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1.
  • Adamczak, Desiree, et al. (författare)
  • Influence of synthetic pathway, molecular weight and side chains on properties of indacenodithiophene-benzothiadiazole copolymers made by direct arylation polycondensation
  • 2021
  • Ingår i: Journal of Materials Chemistry C. - : Royal Society of Chemistry (RSC). - 2050-7534 .- 2050-7526. ; 9:13, s. 4597-4606
  • Tidskriftsartikel (refereegranskat)abstract
    • Atom-economic protocols for the synthesis of poly(indacenodithiophene-alt-benzothiadiazole) (PIDTBT) are presented in which all C-C coupling steps are achieved by direct arylation. Using two different synthetic pathways, PIDTBT copolymers with different side chains (hexylphenyl, octylphenyl, dodecyl, methyl/2-octyldodecylphenyl, 2-octyldodecylphenyl/2-octyldodecylphenyl) and molecular weight (MW) are prepared. Route A makes use of direct arylation polycondensation (DAP) of indacenodithiophene (IDT) and 4,7-dibromo-2,1,3-benzothiadiazole (BTBr2) leading to PIDTBT in high yields, with adjustable MW and without indications for structural defects. Route B starts from a polyketone precursor also prepared by DAP following cyclization. While route B allows introduction of asymmetric side chains at the IDT unit, polymer analogous cyclization gives rise to defect formation. The absorption coefficient of PIDTBT with alkylphenyl side chains made by route A increases with MW. Field-effect hole mobilities around similar to 10(-2) cm(2) V-1 s(-1) are molecular weight-independent, which is ascribed to a largely amorphous thin film morphology. PIDTBT with linear dodecyl side (C12) chains exhibits a bathochromic shift (20 nm), in agreement with theory, and more pronounced vibronic contributions to absorption spectra. In comparison to alkylphenyl side chains, C12 side chains allow for increased order in thin films, a weak melting endotherm and lower energetic disorder, which altogether explain substantially higher field-effect hole mobilities of similar to 10(-1) cm(2) V-1 s(-1).
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2.
  • Ali Ahmad, Syed Ossama, et al. (författare)
  • Application of two-dimensional materials in perovskite solar cells: recent progress, challenges, and prospective solutions
  • 2021
  • Ingår i: Journal of Materials Chemistry C. - : ROYAL SOC CHEMISTRY. - 2050-7526 .- 2050-7534. ; 9:40, s. 14065-14092
  • Forskningsöversikt (refereegranskat)abstract
    • Perovskite solar cells (per-SCs) with high performance and cost-effective solution processing have been the center of interest for researchers in the past decade. Power conversion efficiencies (PCEs) have been gradually improved up to 25.2% with relatively improved stability, which is an unparalleled progress in all generations of solar cell (SC) technology. However, there are still some prevailing challenges regarding the stability and upscaling of these promising devices. Recently, 2D layered materials (LMs) have been extensively explored to overcome the prevailing challenges of poor stability (under moisture, light soaking and high temperature), halide segregation, hysteresis, involvement of toxic materials (i.e., lead), and upscaling of devices. A critical review addressing the recent developments in the use of 2D materials, especially transition metal dichalcogenides (TMDCs), is hence necessary. The development of novel synthesis and deposition techniques including liquid-metal synthesis and ultrasonic assisted spray pyrolysis has offered more efficient fabrication of 2D-LMs with controlled thickness and morphology. Effective functionalization approaches to increase the dispersability of 2D-LMs in non-polar solvents has boosted their potential application in solar cell technology as well. Moreover, compositing 2D TMDCs with suitable organic/inorganic compounds has enabled superior charge kinetics in all functional parts of per-SCs. In addition, newly developed materials such as graphyne and graphdyine along with 2D metal organic frameworks (MOFs) and covalent organic frameworks (COFs) have been employed in per-SCs to achieve PCEs up to 20%. This review summarizes the recent progress and challenges in the application of 2D-LMs in per-SCs and outlines the future pathways to further extend the PCE of per-SCs beyond 25%. This review particularly focuses on 2D-LMs as electrode materials and additives, the underlying charge (electron-hole) transport phenomenon in the functional layers, and their chemical and structural stability.
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3.
  • Alsufyani, Maryam, et al. (författare)
  • The effect of aromatic ring size in electron deficient semiconducting polymers for n-type organic thermoelectrics
  • 2020
  • Ingår i: Journal of Materials Chemistry C. - : ROYAL SOC CHEMISTRY. - 2050-7526 .- 2050-7534. ; 8:43, s. 15150-15157
  • Tidskriftsartikel (refereegranskat)abstract
    • N-type semiconducting polymers have been recently utilized in thermoelectric devices, however they have typically exhibited low electrical conductivities and poor device stability, in contrast to p-type semiconductors, which have been much higher performing. This is due in particular to the n-type semiconductors low doping efficiency, and poor charge carrier mobility. Strategies to enhance the thermoelectric performance of n-type materials include optimizing the electron affinity (EA) with respect to the dopant to improve the doping process and increasing the charge carrier mobility through enhanced molecular packing. Here, we report the design, synthesis and characterization of fused electron-deficient n-type copolymers incorporating the electron withdrawing lactone unit along the backbone. The polymers were synthesized using metal-free aldol condensation conditions to explore the effect of enlarging the central phenyl ring to a naphthalene ring, on the electrical conductivity. When n-doped with N-DMBI, electrical conductivities of up to 0.28 S cm(-1), Seebeck coefficients of -75 mu V K-1 and maximum Power factors of 0.16 mu W m(-1) K-2 were observed from the polymer with the largest electron affinity of -4.68 eV. Extending the aromatic ring reduced the electron affinity, due to reducing the density of electron withdrawing groups and subsequently the electrical conductivity reduced by almost two orders of magnitude.
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4.
  • Bai, Sai, et al. (författare)
  • Colloidal metal halide perovskite nanocrystals: synthesis, characterization, and applications
  • 2016
  • Ingår i: Journal of Materials Chemistry C. - : ROYAL SOC CHEMISTRY. - 2050-7526 .- 2050-7534. ; 4:18, s. 3898-3904
  • Tidskriftsartikel (refereegranskat)abstract
    • Colloidal metal halide perovskite nanocrystals (NCs) have emerged as promising materials for optoelectronic devices and received considerable attention recently. Their superior photoluminescence (PL) properties provide significant advantages for lighting and display applications. In this Highlight, we discuss recent developments in the design and chemical synthesis of colloidal perovskite NCs, including both organic-inorganic hybrid and all inorganic perovskite NCs. We review the excellent PL properties and current optoelectronic applications of these perovskite NCs. In addition, critical challenges that currently limit the applicability of perovskite NCs are discussed, and prospects for future directions are proposed.
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5.
  • Barghi, Hamidreza, 1970, et al. (författare)
  • Synthesis of an electroconductive membrane using poly(hydroxymethyl-3,4-ethylenedioxythiophene-co-tetramethylene-N-hydrox yethyl adipamide)
  • 2013
  • Ingår i: Journal of Materials Chemistry C. - : Royal Society of Chemistry (RSC). - 2050-7534 .- 2050-7526. ; 1:39, s. 6347-6354
  • Tidskriftsartikel (refereegranskat)abstract
    • Synthesis of a novel electroconductive membrane (ECM) was studied with the aim of producing an electroconductive membrane (ECM) with low electrical resistance and appropriate mechanical properties. The method was based on copolymerization of a highly electroconductive monomer (hydroxymethyl-3,4-ethylenedioxythiophene) with highly mechanical resistant hydrophilized polyamide 46 (polytetramethylene-N-hydroxyethyl adipamide). Due to the lack of hydroxyl groups, polyamide 46 does not have the tendency to take part in any chemical reactions, therefore prior to copolymerization, PA 46 was hydrophilized with acetaldehyde to create reactive sites, which allowed copolymerization to occur. At the final stage, a very thin layer, 566 nm conductive poly(hydroxymethyl-3,4-ethylenedioxythiophene) homopolymer was localised using in situ plasma polymerization in order to improve the electrical conductivity of the obtained copolymer. The result was an adherent, highly conductive, semi-hydrophilic and flexible ECM. The presence of hydroxyl groups in the final product led to improved hydrophilicity of the conductive membrane with a surface tension of 41 mJ m(-2). The electrical resistance of PA 46 was dramatically reduced after copolymerization, to 202 in dry and 54 k Omega cm(-2) in wet conditions; furthermore, after plasma treatment, this reduction continued to 105 in dry and 2 k Omega cm(-2) in wet conditions. Other parameters such as flux flow, roughness, pore size, pore distribution, contact angle, surface energy and thermal stability of the ECM were also investigated.
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6.
  • Barghi, H., et al. (författare)
  • Synthesis of an electroconductive membrane using poly(hydroxymethyl-3,4-ethylenedioxythiophene-co-tetramethylene-N-hydroxyethyl adipamide)
  • 2013
  • Ingår i: Journal of Materials Chemistry C. - : R S C Publications. - 2050-7526 .- 2050-7534. ; 1:39, s. 6347-6354
  • Tidskriftsartikel (refereegranskat)abstract
    • Synthesis of a novel electroconductive membrane (ECM) was studied with the aim of producing an electroconductive membrane (ECM) with low electrical resistance and appropriate mechanical properties. The method was based on copolymerization of a highly electroconductive monomer (hydroxymethyl-3,4-ethylenedioxythiophene) with highly mechanical resistant hydrophilized polyamide 46 (polytetramethylene-N-hydroxyethyl adipamide). Due to the lack of hydroxyl groups, polyamide 46 does not have the tendency to take part in any chemical reactions, therefore prior to copolymerization, PA 46 was hydrophilized with acetaldehyde to create reactive sites, which allowed copolymerization to occur. At the final stage, a very thin layer, 566 nm conductive poly(hydroxymethyl-3,4-ethylenedioxythiophene) homopolymer was localised using in situ plasma polymerization in order to improve the electrical conductivity of the obtained copolymer. The result was an adherent, highly conductive, semi-hydrophilic and flexible ECM. The presence of hydroxyl groups in the final product led to improved hydrophilicity of the conductive membrane with a surface tension of 41 mJ m−2. The electrical resistance of PA 46 was dramatically reduced after copolymerization, to 202 in dry and 54 kΩ cm−2 in wet conditions; furthermore, after plasma treatment, this reduction continued to 105 in dry and 2 kΩ cm−2 in wet conditions. Other parameters such as flux flow, roughness, pore size, pore distribution, contact angle, surface energy and thermal stability of the ECM were also investigated.
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7.
  • Baryshnikov, Gleb V., et al. (författare)
  • Nine-ring angular fused biscarbazoloanthracene displaying a solid state based excimer emission suitable for OLED application
  • 2016
  • Ingår i: Journal of Materials Chemistry C. - : Royal Society of Chemistry (RSC). - 2050-7526 .- 2050-7534. ; 4:24, s. 5795-5805
  • Tidskriftsartikel (refereegranskat)abstract
    • A new biscarbazoloanthracene consisting of nine fused aromatic rings, including two pyrrole units, has been obtained in a straightforward and convergent synthesis. Computational chemistry and conformational analysis revealed that the semiconductor's molecule is not planar, the two carbazole moieties being helical twisted from the plane of the anthracene unit. Photophysical and electrochemical measurements showed that this angular fused heteroacene has a low lying HOMO energy level with a wide band gap despite its extended pi-conjugated molecular framework. Based on its relatively low-lying HOMO level, the semiconductor promises a high environmental stability in comparison to other related linear fused acenes and heteroacenes. The biscarbazoloanthracene has been applied as the light emitting layer in a white light emitting diode (WOLED). It is proposed that the white OLED feature is due to dual light emission properties from the active semiconductor layer being based on both the molecular luminescence of the small molecule and a discrete excimer emission made possible by suitable aggregates in the solid state. Noteworthy, this is the first reported example of such a behavior observed in a small molecule heteroacene rather than an oligomer or a polymer.
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8.
  • Bazuev, Gennady V., et al. (författare)
  • The effect of manganese oxidation state on antiferromagnetic order in SrMn1-xSbxO3 (0 < x < 0.5) perovskite solid solutions
  • 2019
  • Ingår i: Journal of Materials Chemistry C. - : Royal Society of Chemistry (RSC). - 2050-7526 .- 2050-7534. ; 7:7, s. 2085-2095
  • Tidskriftsartikel (refereegranskat)abstract
    • The mixed-valence manganese (Mn3+/Mn4+) solid solution, SrMn1-xSbxO3, was prepared for the first time. Two ranges of solid solutions were found: (1) SrMn1-xSbxO3 (0.025 x 0.09) with monoclinically distorted 6H-SrMnO3 polytype (sp. gr. C/2c) and (2) SrMn1-xSbxO3 (0.17 x 0.50) with a tetragonal unit cell (sp. gr. I4/mcm). Crystal structure refinement using X-ray and neutron powder diffraction data showed that the structure of the monoclinic solid solution consists of corner-sharing octahedra around sites occupied by manganese and antimony ions and face-sharing octahedra around sites occupied by manganese ions only, while the tetragonal solid solution has a random distribution of B-site cations. The presence of long-range antiferromagnetic order with a Neel temperature of about 148 K for SrMn0.80Sb0.20O3 and about 280 K for SrMn0.925Sb0.075O3 was found from the results of DC and AC susceptibility and neutron diffraction experiments at 5 K and 80 K.
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9.
  • Benatto, Leandro, et al. (författare)
  • Molecular origin of efficient hole transfer from non-fullerene acceptors : insights from first-principles calculations
  • 2019
  • Ingår i: Journal of Materials Chemistry C. - : Royal Society of Chemistry. - 2050-7526 .- 2050-7534. ; 7:39, s. 12180-12193
  • Tidskriftsartikel (refereegranskat)abstract
    • Due to the strong exciton binding energy (E-b) of organic materials, the energy offset between donor (D) and acceptor (A) materials is essential to promote charge generation in organic solar cells (OSCs). Yet an efficient exciton dissociation from non-fullerene acceptors (NFAs) began to be observed in D/A blends even at very low driving force for hole transfer (Delta H-h). The mechanism behind this efficient photoinduced hole transfer (PHT) remains unclear since current estimates from calculations of isolated molecules indicate that E-b > Delta H-h. Here we rationalize these discrepancies using density functional theory (DFT), the total Gibbs free energy method and the extended Huckel theory (EHT). First, we employed DFT to calculate E-b for NFAs of three representative groups (perylene diimide derivatives, indacenodithiophene and subphthalocyanines) as well as for fullerene acceptors (FAs). Considering isolated molecules in the calculations, we verified that E-b for NFAs is lower than for FAs but still higher than the experimental Delta H-h in which efficient PHT has been observed. Finding the molecular geometry of the excited state, we also obtain that the structural relaxation after photoexcitation tends to further decrease (increase) E-b for NFAs (FAs). This effect helps explain the delayed charge generation measured in some NFA systems. However, this effect is still not large enough for a significant decrease in E-b. We then applied EHT to quantify the decrease of E-b induced by energy levels coupling between stacked molecules in a model aggregate. We then estimated the number of stacked molecules so that E-b approaches Delta H-h's. We found that small NFA aggregates, involving around 5 molecules, are already large enough to explain the experiments. Our results are justified by the low energy barrier to the generation of delocalized states in these systems (especially for the hole delocalization). Therefore, they indicate that molecular systems with certain characteristics can achieve efficient molecular orbital delocalization, which is a key factor to allow an efficient exciton dissociation in low-driving-force systems. These theoretical findings provide a sound explanation to very recent observations in OSCs.
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10.
  • Benesperi, Iacopo, et al. (författare)
  • The researcher's guide to solid-state dye-sensitized solar cells
  • 2018
  • Ingår i: Journal of Materials Chemistry C. - : Royal Society of Chemistry. - 2050-7526 .- 2050-7534. ; 6:44, s. 11903-11942
  • Forskningsöversikt (refereegranskat)abstract
    • In order to sustainably support its ever-increasing energy demand, the human society will have to harvest renewable energy wherever and whenever possible. When converting light to electricity, silicon solar cells are the technology of choice to harvest direct sunlight due to their high performance and continuously dropping price. For diffused light and indoor applications, however, silicon is not the material of choice. To power the next gizmo in your smart home, dye-sensitized solar cells (DSCs) are a viable alternative. Made from inexpensive, earth-abundant, and non-toxic materials, DSCs perform best at low light intensity. So far, issues such as leakage of the liquid electrolyte and its corrosive nature have limited the commercialization of this technology. To overcome these limitations, solid-state DSCs (ssDSCs) - in which the liquid electrolyte is replaced by a solid material - have been developed. For many years their efficiencies have been poor, preventing them from being widely employed. In the past six years, however, research efforts have led them to rival with their liquid counterparts. Here, we will review recent advancements in the field of ssDSCs. Every device component will be acknowledged, from metal oxides and new dyes to novel hole transporters, dopants, counter-electrodes and device architectures. After reviewing materials, long-term stability of devices will be addressed, finally giving an insight into the future that awaits this exciting technology.
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11.
  • Benetti, Daniele, et al. (författare)
  • Functionalized multi-wall carbon nanotubes/TiO2 composites as efficient photoanodes for dye sensitized solar cells
  • 2016
  • Ingår i: Journal of Materials Chemistry C. - 2050-7526 .- 2050-7534. ; 4:16, s. 3555-3562
  • Tidskriftsartikel (refereegranskat)abstract
    • We report on the effects of incorporation of different concentrations of carboxyl group (COOH)-functionalized multi-wall carbon nanotubes (F-MWCNTs) into TiO2 active layers for dye-sensitized solar cells (DSSCs). Standard DSSCs with bare TiO2 exhibit a photo-conversion efficiency (PCE) of 6.05% and a short circuit current density (Jsc) of 13.3 mA cm−2. The presence of 2 wt% F-MWCNTs in the photoanodes increases the PCE up to 7.95% and Jsc up to 17.5 mA cm−2. The photoanodes were characterized using scanning electron microscopy (SEM), Fourier transform infrared (FTIR) spectroscopy and Raman spectroscopy. The electrochemical behaviour of the solar cells was investigated by electrochemical impedance spectroscopy (EIS). We attribute the improved performances to the combined effect of increased dye loading and reduced charge recombination (as clarified by dye loading and EIS measurements), due to the conformal coverage of F-MWCNTs, which allows fast and efficient charge collection in operating solar cells. These results can help in improving the PCE in DSSCs in an elegant and straightforward way, minimizing the need of additional steps (e.g. pre- and post-treatment with TiCl4) for photoanode preparation.
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12.
  • Beyer, Paul, et al. (författare)
  • Fermi level pinned molecular donor/acceptor junctions : Reduction of induced carrier density by interfacial charge transfer complexes
  • 2020
  • Ingår i: Journal of Materials Chemistry C. - : Royal Society of Chemistry (RSC). - 2050-7534 .- 2050-7526. ; 8:43, s. 15199-15207
  • Tidskriftsartikel (refereegranskat)abstract
    • Increased hole density in an electron donor-type organic semiconductor can be achieved by deposition of a strong acceptor-type molecular layer on top, and has been shown to enable adjusting the carrier density in organic field effect transistors (OFETs). This interfacial charge transfer is due to simultaneous Fermi level (EF) pinning of the donor's highest occupied level and the acceptor's lowest unoccupied level. Here, we investigate the electrical properties of such an EF-pinned junction formed by diindenoperylene (DIP, as donor) and hexafluoro-tetracyano-naphthoquinodimethane (F6, as acceptor) in OFETs, as well as its electronic properties by photoelectron spectroscopy and electrostatic modelling. We find that, in addition to the EF-pinning induced integer charge transfer across the interface, DIP and F6 form charge transfer complexes (CPXs) at their junction. The molecularly thin CPX interlayer acts as insulator and significantly reduces the density of carriers induced on either side of the junction, compared to a scenario without such an interlayer. CPX formation is thus unfavourable for the effectiveness of controlling carrier density at molecular donor/acceptor junctions by EF-pinning. This journal is
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13.
  • Bharmoria, Pankaj, 1985, et al. (författare)
  • Photon upconverting bioplastics with high efficiency and in-air durability
  • 2021
  • Ingår i: Journal of Materials Chemistry C. - : Royal Society of Chemistry (RSC). - 2050-7534 .- 2050-7526. ; 9:35, s. 11655-11661
  • Tidskriftsartikel (refereegranskat)abstract
    • There is an urgent demand for substituting synthetic plastics to bioplastics for sustainable renewable energy production. Here, we report a simple one-step approach to create bioplastics with efficient and durable photon upconversion (UC) by encapsulating non-volatile chromophore solutions into collagen-based protein films. By just drying an aqueous solution of gelatin, surfactant, and UC chromophores (sensitizer and annihilator), liquid surfactant microdroplets containing the UC chromophores are spontaneously confined within the gelatin films. Thanks to the high fluidity of microdroplets and the good oxygen barrier ability of the collagen-based fiber matrices, a high absolute TTA-UC efficiency of 15.6% and low threshold excitation intensity of 14.0 mW cm−2are obtained even in air. The TTA-UC efficiency was retained up to 8.2% after 2 years of storage under ambient conditions, hence displaying the significant durability desired for practical applications.
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14.
  • Boström, Hanna, et al. (författare)
  • Octahedral tilting in Prussian blue analogues
  • 2022
  • Ingår i: Journal of Materials Chemistry C. - : Royal Society of Chemistry (RSC). - 2050-7526 .- 2050-7534. ; 10:37, s. 13690-13699
  • Tidskriftsartikel (refereegranskat)abstract
    • Octahedral tilting is key to the structure and functionality of perovskites. We present a metastudy of published literature showing how these distortions manifest in the related Prussian blue analogues (PBAs): cyanide versions of double perovskites with formula AM[M '(CN)(6)](1-y)(y)center dot nH(2)O (A = alkali metal, M and M ' = transition metals, = vacancy/defect). Tilts are favoured by high values of x if A = Na or K, whereas the transition metals play a less important role. External hydrostatic pressure induces tilt transitions nearly irrespective of the stoichiometry, whereas thermal transitions are only reported for x > 1. Interstitial water can alter the transitions induced by a different stimulus, but (de)hydration per se does not lead to tilts. Finally, the implications for rational design of critical functionality-including improper ferroelectricity and electrochemical performance-are discussed. The results are integral for a fundamental understanding of phase transitions and for the development of functional materials based on PBAs.
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15.
  • Brooke, Robert, et al. (författare)
  • Controlling the electrochromic properties of conductive polymers using UV-light
  • 2018
  • Ingår i: Journal of Materials Chemistry C. - : ROYAL SOC CHEMISTRY. - 2050-7526 .- 2050-7534. ; 6:17, s. 4663-4670
  • Tidskriftsartikel (refereegranskat)abstract
    • The phenomenon of electrochromism in conductive polymers is well known and has been exploited in many scientific reports. Using a newly developed patterning technique for conductive polymers, we manufactured high-resolution electrochromic devices from the complementary polymers PEDOT and polypyrrole. The technique, which combines UV-light exposure with vapor phase polymerization, has previously only been demonstrated with the conductive polymer PEDOT. We further demonstrated how the same technique can be used to control the optical properties and the electrochromic contrast in these polymers. Oxidant exposure to UV-light prior to vapor phase polymerization showed a reduction in polymer electrochromic contrast allowing high-resolution (100 mu m) patterns to completely disappear while applying a voltage bias due to their optical similarity in one redox state and dissimilarity in the other. This unique electrochromic property enabled us to construct devices displaying images that appear and disappear with the change in applied voltage. Finally, a modification of the electrochromic device architecture permitted a dual image electrochromic device incorporating patterned PEDOT and patterned polypyrrole on the same electrode, allowing the switching between two different images.
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16.
  • Brooke, Robert, et al. (författare)
  • Infrared electrochromic conducting polymer devices
  • 2017
  • Ingår i: Journal of Materials Chemistry C. - : The Royal Society of Chemistry. - 2050-7526 .- 2050-7534. ; 5:23, s. 5824-5830
  • Tidskriftsartikel (refereegranskat)abstract
    • The conducting polymer poly(3,4-ethylenedioxythiophene) (PEDOT) is well known for its electrochromic properties in the visible region. Less focus has been devoted to the infrared (IR) wavelength range, although tunable IR properties could enable a wide range of novel applications. As an example, modern day vehicles have thermal cameras to identify pedestrians and animals in total darkness, but road and speed signs cannot be easily visualized by these imaging systems. IR electrochromism could enable a new generation of dynamic road signs that are compatible with thermal imaging, while simultaneously providing contrast also in the visible region. Here, we present the first metal-free flexible IR electrochromic devices, based on PEDOT:Tosylate as both the electrochromic material and electrodes. Lateral electrochromic devices enabled a detailed investigation of the IR electrochromism of thin PEDOT:Tosylate films, revealing large changes in their thermal signature, with effective temperature changes up to 10 [degree]C between the oxidized (1.5 V) and reduced (-1.5 V) states of the polymer. Larger scale (7 [times] 7 cm) vertical electrochromic devices demonstrate practical suitability and showed effective temperature changes of approximately 7 [degree]C, with good optical memory and fast switching (1.9 s from the oxidized state to the reduced state and 3.3 s for the reversed switching). The results are highly encouraging for using PEDOT:Tosylate for IR electrochromic applications.
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17.
  • Brooke, Robert, 1989-, et al. (författare)
  • Infrared electrochromic conducting polymer devices
  • 2017
  • Ingår i: Journal of Materials Chemistry C. - : Royal Society of Chemistry (RSC). - 2050-7526 .- 2050-7534. ; 5:23, s. 5824-5830
  • Tidskriftsartikel (refereegranskat)abstract
    • The conducting polymer poly(3,4-ethylenedioxythiophene) (PEDOT) is well known for its electrochromic properties in the visible region. Less focus has been devoted to the infrared (IR) wavelength range, although tunable IR properties could enable a wide range of novel applications. As an example, modern day vehicles have thermal cameras to identify pedestrians and animals in total darkness, but road and speed signs cannot be easily visualized by these imaging systems. IR electrochromism could enable a new generation of dynamic road signs that are compatible with thermal imaging, while simultaneously providing contrast also in the visible region. Here, we present the first metal-free flexible IR electrochromic devices, based on PEDOT:Tosylate as both the electrochromic material and electrodes. Lateral electrochromic devices enabled a detailed investigation of the IR electrochromism of thin PEDOT:Tosylate films, revealing large changes in their thermal signature, with effective temperature changes up to 10 °C between the oxidized (1.5 V) and reduced (-1.5 V) states of the polymer. Larger scale (7 × 7 cm) vertical electrochromic devices demonstrate practical suitability and showed effective temperature changes of approximately 7 °C, with good optical memory and fast switching (1.9 s from the oxidized state to the reduced state and 3.3 s for the reversed switching). The results are highly encouraging for using PEDOT:Tosylate for IR electrochromic applications.
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18.
  • Brooke, Robert, et al. (författare)
  • Organic energy devices from ionic liquids and conducting polymers
  • 2016
  • Ingår i: Journal of Materials Chemistry C. - : Royal Society of Chemistry. - 2050-7526 .- 2050-7534. ; 4:7, s. 1550-1556
  • Tidskriftsartikel (refereegranskat)abstract
    • The use of smart technologies in our daily lives, from smartphones to auto-dimming windows to touch sensors, has become pervasive. With growing desire for these devices to be conformable and flexible, traditional materials are being replaced to create a class of products known as active organic electronic devices (OEDs). These new devices owe their ability to switch electrical and/or optical function to the intimate interaction between an inherently conducting polymer and electrolyte, typically an ionic liquid. Herein, we provide the first observations that specific ionic liquids can reduce or oxidise conducting polymers upon intimate contact in the absence of any electrical stimuli. The ability to reduce or oxidise the inherently conducting polymer depends on the cation and anion pair within the ionic liquid. Extending the utility of this phenomenon is made by fabricating OEDs such as prototype fuel cells, supercapacitors and smart windows.
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19.
  • Bäcklund, Fredrik, et al. (författare)
  • Amyloid fibrils as dispersing agents for oligothiophenes: control of photophysical properties through nanoscale templating and flow induced fibril alignment
  • 2014
  • Ingår i: Journal of Materials Chemistry. - : Royal Society of Chemistry (RSC). - 1364-5501 .- 0959-9428 .- 2050-7526 .- 2050-7534. ; 2:37, s. 7811-7822
  • Tidskriftsartikel (refereegranskat)abstract
    • Herein we report that protein fibrils formed from aggregated proteins, so called amyloid fibrils, serve as an excellent dispersing agent for hydrophobic oligothiophenes such as alpha-sexithiophene (6T). Furthermore, the protein fibrils are capable of orienting 6T along the fibril long axis, as demonstrated by flow-aligned linear dichroism spectroscopy and polarized fluorescence microscopy. The materials are prepared by solid state mixing of 6T with a protein capable of self-assembly. This results in a water soluble composite material that upon heating in aqueous acid undergoes self-assembly into protein fibrils non-covalently functionalized with 6T, with a typical diameter of 5-10 nm and lengths in the micrometre range. The resulting aqueous fibril dispersions are a readily available source of oligothiophenes that can be processed from aqueous solvent, and we demonstrate the fabrication of macroscopic structures consisting of aligned 6T functionalized protein fibrils. Due to the fibril induced ordering of 6T these structures exhibit polarized light emission.
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20.
  • Börjesson, Karl, 1982, et al. (författare)
  • Optically switchable transistors comprising a hybrid photochromic molecule/n-type organic active layer
  • 2015
  • Ingår i: Journal of Materials Chemistry C. - : Royal Society of Chemistry (RSC). - 2050-7534 .- 2050-7526. ; 3:16, s. 4156-4161
  • Tidskriftsartikel (refereegranskat)abstract
    • Organic semiconductors can be easily combined with other molecular building blocks in order to fabricate multifunctional devices, in which each component conveys a specific (opto)electronic function. We have fabricated photoswitchable hybrid thin-film transistors based on an active bi-component material, consisting of an n-type fullerene derivative and a photochromic diarylethene that possesses light-tunable energy levels. The devices can be gated in two independent ways by either using an electrical stimulus via the application of a voltage to the gate electrode or an optical stimulus causing interconversion of the diarylethene molecules between their two isomers. Fine control over the device output current is achieved by engineering the diarylethenes' LUMO that can act as an intra-gap state controlled by a distinct wavelength in the UV or in the visible range. Importantly, the devices based on a mixed diarylethene/fullerene active layer preserve the high mobility of the pristine semiconductor. This journal is
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21.
  • Can, Ayse, et al. (författare)
  • Indenofluorenes for organic optoelectronics: the dance of fused five- and six-membered rings enabling structural versatility
  • 2022
  • Ingår i: Journal of Materials Chemistry C. - : ROYAL SOC CHEMISTRY. - 2050-7526 .- 2050-7534. ; 10:22, s. 8496-8535
  • Forskningsöversikt (refereegranskat)abstract
    • Polycyclic pi-conjugated hydrocarbons (PCHs), either unfunctionalized or structurally modified derivatives, have attracted tremendous interest in the past few decades as high-performance semiconductors for use in new generations of organic (opto)electronic devices. Among several PCHs realized to date, the 6-5-6-5-6 pi-fused-ring backbone of indenofluorene (IF) stands out as a unique semiconducting architecture with great structural and property versatility affording six different regioisomers, diverse functionalization/substitution positions, pi-conjugation/delocalization patterns, aromatic behaviors, and electronic structures. In this review, we summarize and analyze the historical and recent advances in the design and implementation of IF-based semiconductors in organic transistor and solar cell devices, as well as in understanding the chemical structure-molecular property-semiconductivity relationships. Following an introduction to the fascinating properties of an IF pi-framework that distinguishes this core among PCHs, we present IF-based semiconductors and discuss their properties by classifying them into four main families (IF-diones, IF-DCVs/IF-TTFs, pi-IFs, and (un)substituted DH-IFs) considering whether methylene or methine C-bridges are present and how these positions are functionalized or substituted. For each family, design and synthetic approaches, molecular properties, and transistor/solar cell device applicability and/or performance are reviewed and discussed. At the end, we conclude with a section discussing the challenges and opportunities for future progress of IF-based semiconductor materials and related (opto)electronic technologies.
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22.
  • Carrod, Andrew J., 1994, et al. (författare)
  • Modulating TTA efficiency through control of high energy triplet states
  • 2022
  • Ingår i: Journal of Materials Chemistry C. - : Royal Society of Chemistry (RSC). - 2050-7526 .- 2050-7534. ; 10:12, s. 4923-4928
  • Tidskriftsartikel (refereegranskat)abstract
    • An ideal annihilator in triplet-triplet annihilation photon upconversion (TTA-UC) can achieve a maximum of 50% quantum efficiency. This spin statistical limit depends on the energies of the triplet states of the annihilator molecule, with only 20% quantum efficiencies possible in less-optimal energy configurations (ET2 <= 2ET1). Our work utilises three perylene analogues substituted with phenyl in sequential positions. When substituted in the bay position the isomer displays drastically lowered upconversion yields, which can be explained by the system going from an ideal to less-ideal energy configuration. We further concluded position 2 is the best site when functionalising perylene without a wish to affect its photophysics, thus demonstrating how molecular design can influence upconversion quantum efficiencies by controlling the energetics of triplet states through substitution. This will in turn help in the design of molecules that maximise upconversion efficiencies for materials applications.
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23.
  • Chen, Bin, et al. (författare)
  • Full-colour luminescent compounds based on anthracene and 2,2 '-dipyridylamine
  • 2013
  • Ingår i: Journal of Materials Chemistry C. - : Royal Society of Chemistry (RSC). - 2050-7526 .- 2050-7534. ; 1:44, s. 7409-7417
  • Tidskriftsartikel (refereegranskat)abstract
    • Starting from two simple units of anthracene and 2,2'-dipyridylamine, a series of new luminescent compounds 1-8 were designed and synthesized by a combined strategy of changing the connection mode between the two units, extending the conjugation size, and introducing an additional electron donor. Photophysical properties of 1-8 were investigated and discussed on the basis of solvatochromic behaviour, theoretical calculations, crystal structure, and optimized structures. Interestingly, the emission wavelengths of these compounds could be successfully tuned from violet to red both in solutions and the solid-state, and prominent positive solvatochromism was observed for the compounds with a D-p-A framework. Consider compound 7 as an example, it shows peaks at 526 nm and 627 nm in cyclohexane and DMSO, respectively. Meanwhile, the quantum yield was decreased from 0.80 in cyclohexane to 0.12 in DMSO. The introduction of bulky groups was demonstrated to be effective for suppressing the aggregation effect and thus improving the solid state emission quantum yield. These results indicate that the combined structure modulation strategy offers a powerful tool for tuning the emission behaviour. To demonstrate the possibility of practical applications, 2 was employed as the emitting material for the fabrication of deep-blue organic light-emitting diodes (OLEDs), which showed a maximum external quantum efficiency of 2.2%. The CIE coordinates of (0.15, 0.08) are indicative of excellent blue color purity.
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24.
  • Chen, S., et al. (författare)
  • Aggregation-controlled photochromism based on a dithienylethene derivative with aggregation-induced emission
  • 2017
  • Ingår i: Journal of Materials Chemistry C. - : Royal Society of Chemistry. - 2050-7526 .- 2050-7534. ; 5:10, s. 2717-2722
  • Tidskriftsartikel (refereegranskat)abstract
    • We report novel aggregation-induced emission (AIE) characteristics involving aggregation-controlled photochromism properties of a dithienylethene derivative, BTE-EQ, where two quinolinemalononitrile (EQ) units are covalently attached to a dithienylethene core. The typical AIE effect of BTE-EQ has been found to originate from the AIE character of the EQ units with respect to the reference compound BTE, which does not contain an EQ unit. The photochromism study, together with density functional theory calculations, reveals that the photochromic activity of BTE-EQ can be reversibly switched off and on by controlling the aggregation state during the AIE process, which provides a novel route to controlling the photochromism of diarylethenes.
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25.
  • Chen, Shangzhi, et al. (författare)
  • On the anomalous optical conductivity dispersion of electrically conducting polymers : Ultra-wide spectral range ellipsometry combined with a Drude-Lorentz model
  • 2019
  • Ingår i: Journal of Materials Chemistry C. - : Royal Society of Chemistry. - 2050-7526 .- 2050-7534. ; 7:15, s. 4350-4362
  • Tidskriftsartikel (refereegranskat)abstract
    • Electrically conducting polymers (ECPs) are becoming increasingly important in areas such as optoelectronics, biomedical devices, and energy systems. Still, their detailed charge transport properties produce an anomalous optical conductivity dispersion that is not yet fully understood in terms of physical model equations for the broad range optical response. Several modifications to the classical Drude model have been proposed to account for a strong non-Drude behavior from terahertz (THz) to infrared (IR) ranges, typically by implementing negative amplitude oscillator functions to the model dielectric function that effectively reduce the conductivity in those ranges. Here we present an alternative description that modifies the Drude model via addition of positive-amplitude Lorentz oscillator functions. We evaluate this so-called Drude-Lorentz (DL) model based on the first ultra-wide spectral range ellipsometry study of ECPs, spanning over four orders of magnitude: from 0.41 meV in the THz range to 5.90 eV in the ultraviolet range, using thin films of poly(3,4-ethylenedioxythiophene):tosylate (PEDOT:Tos) as a model system. The model could accurately fit the experimental data in the whole ultrawide spectral range and provide the complex anisotropic optical conductivity of the material. Examining the resonance frequencies and widths of the Lorentz oscillators reveals that both spectrally narrow vibrational resonances and broader resonances due to localization processes contribute significantly to the deviation from the Drude optical conductivity dispersion. As verified by independent electrical measurements, the DL model accurately determines the electrical properties of the thin film, including DC conductivity, charge density, and (anisotropic) mobility. The ellipsometric method combined with the DL model may thereby become an effective and reliable tool in determining both optical and electrical properties of ECPs, indicating its future potential as a contact-free alternative to traditional electrical characterization.
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26.
  • Chen, Yongzhen, 1990-, et al. (författare)
  • Image-force effects on energy level alignment at electron transport material/cathode interfaces
  • 2020
  • Ingår i: Journal of Materials Chemistry C. - : ROYAL SOC CHEMISTRY. - 2050-7526 .- 2050-7534. ; 8:1, s. 173-179
  • Tidskriftsartikel (refereegranskat)abstract
    • Electron transport materials (ETMs) are widely used as interlayers to lower the cathode electrode work function in organic solar cells and organic light-emitting diodes, for example. The usual interpretation for their operating principle is a chemical interaction between the ETM and the electrode, inducing partial or integer charge transfer or collectively an intrinsic dipole moment caused by preferential molecular orientation. Herein, we systematically explore the commonly used ETM bathophenanthroline (BPhen) deposited on a series of conducting substrates. The energetics at the BPhen interface follows the typical integer charge transfer (ICT) model with an extra displacement of the vacuum level by up to -1.4 eV. The extra displacement is ascribed to the "double dipole step" formed by the positive and negative charged species and their induced image charges when they are close to the surface of substrates. After n-type doping the displacement is further increased to -1.8 eV, yielding a larger work function modification than obtained using typical electrolytes and zwitterions as cathode interlayer.
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27.
  • Cheng, Qiaoyun, et al. (författare)
  • The conversion of nanocellulose into solvent-free nanoscale liquid crystals by attaching long side-arms for multi-responsive optical materials
  • 2020
  • Ingår i: Journal of Materials Chemistry C. - : ROYAL SOC CHEMISTRY. - 2050-7526 .- 2050-7534. ; 8:32, s. 11022-11031
  • Tidskriftsartikel (refereegranskat)abstract
    • Nanocellulose, with its unique optical and chemical properties, has received increasing attention as feedstock to fabricate sustainable materials. However, achieving a nanocellulose-based solvent-free liquid crystal with good responsiveness still remains a challenge. Herein, for the first time, solvent-free supramolecular liquid crystals were fabricated by attaching long side-arms on the fiber-like nanocellulose derived from tunicate (TCNC) with an average width of 20 nm and 400-3000 nm in length. The side-arms were grafted via surface condensation with a charged organosilane, followed by further functionalization with a counter-ion polyoxyethylene ether. The nanoscale liquid crystals consisted of the stiff TCNC as the core and flexible side-arms as the soft shells, forming the core-shell structure with an average width of 34-36 nm. The resulting solvent-free liquid crystal exhibited transparent and viscous liquid-like fluidity, as well as a bright birefringence between the crossed polarizers at room temperature. In our findings, the stiff core provided crystal-like ordering, whereas the soft shells induced the high mobility of the TCNCs as a result of the increased fractional free volume, as shown by positron annihilation lifetime spectra. The unique flowability enables the possibility of multi-responsiveness to temperature, deformation, and alternating electric fields. In addition, the thermo-responsiveness can be regulated by tailoring the canopy. This work provides a novel strategy for the conversion of solid nanocellulose into a solvent-free nanoscale liquid crystal, which is promising for use as a responsive optical material.
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28.
  • Chesnokov, A., et al. (författare)
  • The local atomic structure and thermoelectric properties of Ir-doped ZnO : hybrid DFT calculations and XAS experiments
  • 2021
  • Ingår i: Journal of Materials Chemistry C. - : Royal Society of Chemistry. - 2050-7526 .- 2050-7534. ; 9:14, s. 4948-4960
  • Tidskriftsartikel (refereegranskat)abstract
    • We combined the hybrid density functional theory (DFT) calculations and X-ray absorption spectroscopy (XAS) experiments in the study of the local atomic structure around Ir ions in ZnO thin films with different iridium content. This was then used in the first principles analysis of the thermoelectric properties of material. The emphasis has been put on the conditions for a positive Seebeck coefficient and p-type electrical conductivity as the functions of the Fermi level. We studied both computationally and experimentally several possible IrOxpolyhedra (complexes) with a different number of surrounding oxygens and Ir oxidation states, including those with the formation of peroxide ions (O22−). In particular, octahedral coordination of iridium ions was identified by reverse Monte Carlo (RMC) simulations of the Ir L3-edge EXAFS spectra of ZnO:Ir thin films as the predominant complex, which is supported by the calculated lowest interstitial oxygen incorporation energies. All the calculated IrOx(x= 4, 5, 6) complexes, regardless of Ir the oxidation state, demonstrate potential for p-type conduction if the Fermi level (μF) falls in the range of 0-0.8 eV from the valence band maximum (VBM) and the Ir concentration is high enough (12.5% in the present DFT calculations). Even though the corresponding calculated Seebeck coefficient (S) around 80-89 μV K−1slightly exceeds the experimental values, we emphasise the presence of an important plateau in the dependence ofSonμFin this range for two complexes with the formation of peroxide ions (O22−). We predicted also that peroxide ions O22−are characterized by the calculated phonon frequencies of 810-942 cm−1in agreement with our previous Raman experimental results. In this light, we discuss the high sensitivity of calculatedS(μF) dependences to the atomic and electronic structure. 
  •  
29.
  • Christensen, M. A., et al. (författare)
  • Mixed valence radical cations and intermolecular complexes derived from indenofluorene-extended tetrathiafulvalenes
  • 2014
  • Ingår i: Journal of Materials Chemistry C. - : Royal Society of Chemistry (RSC). - 2050-7526 .- 2050-7534. ; 2:48, s. 10428-10438
  • Tidskriftsartikel (refereegranskat)abstract
    • Engineering of mixed-valence (MV) radical cations and intermolecular complexes based on pi-extended tetrathiafulvalenes (TTFs) is central for the development of organic conductors. On another front, redox-controlled dimerization of radical cations has recently been recognized as an important tool in supramolecular chemistry. Here we show that pi-extended TTFs based on the indenofluorene core, prepared by Horner-Wadsworth-Emmons reactions, undergo reversible and stepwise one-electron oxidations and that the detectable, intermediate radical cation forms remarkably strong intermolecular MV ([neutral.cation]) and pi-dimer ([cation.cation]) complexes with near-infrared radical cation absorptions. The radical cation itself seems to be a so-called Class III MV species in the Robin-Day classification. The formation of MV dimers was corroborated by ESR spectroelectrochemical studies, revealing two slightly different ESR signals upon oxidation, one assigned to the MV dimer and the other to the cation monomer. Crystals of the radical cation with different anions (PF6- , BF4-, and TaF6-) were grown by electrocrystallization. Conductance studies revealed that the salts behave as semiconductors with the hexafluorotantalate salt exhibiting the highest conductance. Using a custom-built ESR spectrometer with sub-femtomole sensitivity, the magnetic properties of one crystal were investigated. While the spin-to-spin interaction between radical cations was negligible, a high cooperativity coupling to the microwave field was observed - as a result of an exceptionally narrow spin line width and high spin density. This could have great potential for applications in quantum computation where crystalline spin ensembles are exploited for their long coherence times.
  •  
30.
  •  
31.
  • Danielsson, Örjan, et al. (författare)
  • A model for carbon incorporation from trimethyl gallium in chemical vapor deposition of gallium nitride
  • 2016
  • Ingår i: Journal of Materials Chemistry C. - : Royal Society of Chemistry. - 2050-7526 .- 2050-7534. ; 4:4, s. 863-871
  • Tidskriftsartikel (refereegranskat)abstract
    • Gallium nitride (GaN) semiconductor material can become semi-insulating when doping with carbon. Semi-insulating buffer layers are utilized to prevent leakage currents in GaN high power devices. Carbon is inherently present during chemical vapor deposition (CVD) of GaN from the use of trimethyl gallium (TMGa) as precursor. TMGa decomposes in the gas phase, releasing its methyl groups, which could act as carbon source for doping. It is previously known that the carbon doping levels can be controlled by tuning the CVD process parameters, such as temperature, pressure and precursor flow rates. However, the mechanism for carbon incorporation from TMGa is not yet understood. In this paper, a model for predicting carbon incorporation from TMGa in GaN layers grown by CVD is proposed. The model is based on ab initio quantum chemical calculations of molecular adsorption and reaction energies. Using Computational Fluid Dynamics, with a chemical kinetic model for decomposition of the precursors and reactions in the gas phase, to calculate gas phase compositions at realistic process conditions, together with the proposed model, we obtain good correlations with measurements, for both carbon doping concentrations and growth rates, when varying the inlet NH3/TMGa ratio. When varying temperature (800 – 1050°C), the model overpredicts carbon doping concentrations at the lower temperatures, but predicts growth rates well, and the agreement with measured carbon doping concentrations is good above 1000°C.
  •  
32.
  • Di Marcantonio, M., et al. (författare)
  • Green-yellow emitting hybrid light emitting electrochemical cell
  • 2017
  • Ingår i: Journal of Materials Chemistry C. - : Royal Society of Chemistry (RSC). - 2050-7526 .- 2050-7534. ; 5:46, s. 12062-12068
  • Tidskriftsartikel (refereegranskat)abstract
    • Light-emitting electrochemical cells (LECs) are attractive candidates for future low-cost lighting applications such as light-emitting smart tags, thanks to their simplicity, fully solution-based fabrication and flexibility. However, high brightness and efficiency in combination with satisfactory operation lifetimes need to be achieved for different emission colours bearing future device commercialization in mind. LECs emitting in the yellow-green spectral range, where the human eye is most sensitive are thereby particularly attractive. Here we present an improved hybrid LEC based on an Ir-iTMC, [Ir(4-Fppy)(2)(pbpy)][PF6] (4-Fppy = 2-(4-fluorophenyl) pyridinato, pbpy = 6-phenyl-2,2'-bipyridine) emitting at 557 nm. It features a luminance of 2400 cd m(-2) when driven at a constant voltage of 4 V, and a lifetime of 271 h at a luminance of 1500 cd m(-2) under pulsed current operation. The hybrid LEC shows an enhanced performance compared to a LEC solely based on the Ir-ITMC where operation lifetimes of 165 h at a luminance above 1200 cd m(-2) under pulsed current operation conditions were observed. The performance improvement was achieved by addition of a solution-processed ZnO nanoparticle film on top.
  •  
33.
  • DInnocenzo, V., et al. (författare)
  • Two-dimensional charge transport in molecularly ordered polymer field-effect transistors
  • 2016
  • Ingår i: JOURNAL OF MATERIALS CHEMISTRY C. - : ROYAL SOC CHEMISTRY. - 2050-7526 .- 2050-7534. ; 4:47, s. 11135-11142
  • Tidskriftsartikel (refereegranskat)abstract
    • Nanometer-thick Langmuir-Schafer monolayers of an electron transporting polymer display charge transport, optical and electro-optical properties that do not depend on the number of layers deposited one above the other. This phenomenon can be rationalized with the micro-structure of the specific multi-layers, which introduces an interlayer hopping penalty confining transport to a neat 2D regime, with a channel not extending beyond a single similar to 3 nm thick polymer strand, as confirmed by kinetic Monte Carlo simulations. Such findings are critical to establish a quantitative structure-property nexus in high mobility polymer semiconductors and in the control of charge transport at a molecular scale.
  •  
34.
  • dos Santos, John Marques, et al. (författare)
  • Color tuning of multi-resonant thermally activated delayed fluorescence emitters based on fully fused polycyclic amine/carbonyl frameworks
  • 2023
  • Ingår i: Journal of Materials Chemistry C. - : Royal Society of Chemistry. - 2050-7526 .- 2050-7534. ; 11:24, s. 8263-8273
  • Tidskriftsartikel (refereegranskat)abstract
    • Two novel π-extended amine/carbonyl-based multi-resonance thermally activated delayed fluorescence (MR-TADF) emitters have been designed and synthesized. The two emitters are isomeric, composed of nine fused rings and show green-yellow emission. Sym-DiDiKTa and Asym-DiDiKTa possess tert-butyl groups distributed in a symmetrical and asymmetrical fashion, respectively, which significantly impact the single-crystal packing structure. The two compounds possess similar singlet-triplet energy gaps, ΔEST, of around 0.23 eV, narrowband emission characterized by a full-width at half-maximum, FWHM, of 29 nm and a photoluminescence quantum yield, ΦPL, of 70% and 53% for the symmetric and asymmetric counterparts, respectively, in toluene. Investigation in OLEDs demonstrated that the devices with Sym-DiDiKTa and Asym-DiDiKTa displayed electroluminescence maxima of 543 and 544 nm, and maximum external quantum efficiencies (EQEmax) of 9.8% and 10.5%, respectively. The maximum EQE was further improved to 19.9% by employing a hyperfluorescence strategy. We further present the first example of a neutral MR-TADF emitter incorporated in a LEC device where Sym-DiDiKTa acts as the emitter. The LEC shows a λEL at 551 nm and FWHM of 60 nm with luminance of 300 cd m−2 and a fast turn-on time of less than 2 s to 100 cd m−2
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35.
  • Eklund, Per, et al. (författare)
  • Transition-metal-nitride-based thin films as novel energy harvesting materials
  • 2016
  • Ingår i: Journal of Materials Chemistry C. - : ROYAL SOC CHEMISTRY. - 2050-7526 .- 2050-7534. ; 4:18, s. 3905-3914
  • Tidskriftsartikel (refereegranskat)abstract
    • The last few years have seen a rise in the interest in early transition-metal and rare-earth nitrides, primarily based on ScN and CrN, for energy harvesting by thermoelectricity and piezoelectricity. This is because of a number of important advances, among those the discoveries of exceptionally high piezoelectric coupling coefficient in (Sc,Al)N alloys and of high thermoelectric power factors of ScN-based and CrN-based thin films. These materials also constitute well-defined model systems for investigating thermodynamics of mixing for alloying and nanostructural design for optimization of phase stability and band structure. These features have implications for and can be used for tailoring of thermoelectric and piezoelectric properties. In this highlight article, we review the ScN-and CrN-based transition-metal nitrides for thermoelectrics, and drawing parallels with piezoelectricity. We further discuss these materials as a models systems for general strategies for tailoring of thermoelectric properties by integrated theoretical-experimental approaches.
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36.
  • Elfwing, Anders, et al. (författare)
  • Protein nanowires with conductive properties
  • 2015
  • Ingår i: Journal of Materials Chemistry C. - : Royal Society of Chemistry. - 2050-7526 .- 2050-7534. ; 3:25, s. 6499-6504
  • Tidskriftsartikel (refereegranskat)abstract
    • Herein we report on the investigation of self-assembled protein nanofibrils functionalized with metallic organic compounds. We have characterized the electronic behaviour of individual nanowires using conductive atomic force microscopy. In order to follow the self assembly process we have incorporated fluorescent molecules into the protein and used the energy transfer between the internalized dye and the metallic coating to probe the binding of the polyelectrolyte to the fibril.
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37.
  • Fabiano, Simone, et al. (författare)
  • On the fundamentals of organic mixed ionic/electronic conductors
  • 2023
  • Ingår i: Journal of Materials Chemistry C. - : ROYAL SOC CHEMISTRY. - 2050-7526 .- 2050-7534. ; 11:42, s. 14527-14539
  • Tidskriftsartikel (refereegranskat)abstract
    • The first Telluride Science meeting (formerly TSRC) on organic mixed ionic and electronic conductors (OMIECs), Oct 3-7, 2022, brought together researchers across the field to understand the fundamental processes and identify out-standing questions related to this exciting class of materials. OMIECs are organic materials that promote the transport of mobile electronic charge carriers while simultaneously supporting ionic transport and ionic-electronic coupling. These properties open up broad areas of applications from energy to bioelectronics. Devices include batteries, supercapacitors, actuators, electrochromic displays, and organic electrochemical transistors (OECTs). They possess the key strengths of traditional organic electronic materials, such as synthetic tunability and low-temperature processing. Despite the recent advances in devices and applications achieved with such materials, many challenges and gaps in understanding remain. These topics hold the key to designing next-generation materials and devices that continue to push the limits of performance and stability and facilitate novel functionality. This perspective aims to summarize the current understanding, conversations, and debates that made this TSRC particularly engaging, enabling new directions and searching for missing pieces of the OMIEC puzzle. This perspective offers insights from discussions conducted during the Telluride Science meeting on organic mixed ionic and electronic conductors, outlining the challenges associated with understanding the behavior of this intriguing materials class.
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38.
  • Fazzi, Daniele, et al. (författare)
  • Polarons in pi-conjugated ladder-type polymers: a broken symmetry density functional description
  • 2019
  • Ingår i: Journal of Materials Chemistry C. - : ROYAL SOC CHEMISTRY. - 2050-7526 .- 2050-7534. ; 7:41, s. 12876-12885
  • Tidskriftsartikel (refereegranskat)abstract
    • Electronic charged states (i.e., polarons) play a crucial role in governing charge transfer, spin, thermo-electric and redox mechanisms in organic functional materials. An accurate description at the quantum-chemical level is mandatory to understand their response and transport properties. We report a comprehensive computational investigation concerning the polaron properties of a high electron conductivity (n-type) pi-conjugated ladder-type polymer, namely polybenzimidazobenzophenanthroline (BBL). We show how spin polarized unrestricted Density Functional Theory (UDFT) and restricted (RDFT) methods can lead to solutions of the polaron and bipolaron electronic wavefunctions which are not the most stable ones. This aspect can be traced back to the multiconfigurational character of the electronic charged states wavefunction. We demonstrate how broken symmetry DFT (BS-UDFT) can circumvent this issue, well describing the polaron/bipolaron localization in terms of spin densities and structural deformations, thus providing a correct assessment of the electron transport parameters (e.g., reorganization energy), otherwise incorrectly computed at the UDFT/RDFT levels. Our calculations are further validated by comparing the IR spectra of polaronic species with the experimental one, as measured on doped BBL films. Our study calls for an urgent and careful computational assessment of the electronic charged states (e.g., polaron, bipolaron, etc.), in high performance pi-conjugated materials, such as ladder-type polymers and other donor-acceptor derivatives, for a correct understanding of their charge, heat, and spin transport mechanisms.
  •  
39.
  • Gamage, Sampath, et al. (författare)
  • Transparent nanocellulose metamaterial enables controlled optical diffusion and radiative cooling
  • 2020
  • Ingår i: Journal of Materials Chemistry C. - : Royal Society of Chemistry. - 2050-7526 .- 2050-7534. ; 8:34, s. 11687-11694
  • Tidskriftsartikel (refereegranskat)abstract
    • Materials that provide independent control of infrared thermal radiation and haze in the visible could benefit many areas and applications, including clothing, packaging and photovoltaics. Here, we study this possibility for a metamaterial composite paper based on cellulose nanofibrils (CNF) and silicon dioxide (SiO2) microparticles with infrared (IR) Fröhlich phonon resonances. This CNF-SiO2composite shows outstanding transparency in the visible wavelength range, with the option of controlling light diffusion and haze from almost zero to 90% by varying the SiO2microparticle concentration. We further show that the transparent metamaterial paper could maintain high thermal emissivity in the atmospheric IR window, as attributed to strong IR absorption of both the nanocellulose and the resonant SiO2microparticles. The high IR emissivity and low visible absorption make the paper suitable for passive radiative cooling and we demonstrate cooling of the paper to around 3 °C below ambient air temperature by exposing it to the sky. 
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40.
  • Geng, Wenping, et al. (författare)
  • Permanent charged domain walls under tip-poling engineering
  • 2021
  • Ingår i: Journal of Materials Chemistry C. - : Royal Society of Chemistry. - 2050-7526 .- 2050-7534. ; 9:44, s. 15797-15803
  • Tidskriftsartikel (refereegranskat)abstract
    • Charged domain walls (CDWs) have attracted considerable attention owing to their tunable properties related to high-density information storage and nanoelectronics devices. The excellent time endurance of conductivity is a pressing need, which is directly related to the domain stability and boundary conditions. In this study, we propose an effective method to promote the permanent formation of charged domain walls aimed with tip-induced electric fields. The permanent domain structures and CDWs are attributed to the robust stimulus with tip dimensions combined with effective screening conditions. This interesting conductivity near the domain walls is three orders of magnitude higher than the domain inner, and exhibits attractive anti-fatigue properties with the value of ∼60 pA for the duration of more than one month. In addition, the tunable mechanism of CDWs in LiNbO3 thin films is related to carrier gathering near the domain walls for the inclined boundary. These inclined head-to-head domain walls exhibit conductive features only along the negative direction, which can be modulated by the application of a sub-coercive voltage. The results demonstrate the stable manipulation of domain reversal and charged domain walls in LiNbO3 thin films, highlighting them as a critical component, especially for multiple-state logic circuits and potential ferroelectric diode applications in non-volatile memories and nanoelectronics devices.
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41.
  • Ghasemi, Shima, 1993, et al. (författare)
  • Exploring the impact of select anchor groups for norbornadiene/quadricyclane single-molecule switches
  • 2023
  • Ingår i: Journal of Materials Chemistry C. - 2050-7534 .- 2050-7526. ; 11:44, s. 15379-15776
  • Tidskriftsartikel (refereegranskat)abstract
    • To achieve the ultimate limit of device miniaturization, it is necessary to have a comprehensive understanding of the structure–property relationship in functional molecular systems used in single-molecule electronics. This study reports the synthesis and characterization of a novel series of norbornadiene derivatives capped with thioether and thioester anchor groups. Utilizing the mechanically controllable break junction technique, the impact of these capping groups on conductance across single-molecule junctions is investigated. Among the selection of anchor groups, norbornadiene capped with thioacetate and tert-butyl groups exhibits higher conductance (G ≈ 4 × 10−4 G0) compared to methyl thioether (G ≈ 2 × 10−4 G0). Electronic transmission through the considered set of single-molecule junctions has been simulated. The computational results for electron transport across these junctions align closely with the experimental findings, with the thioacetate- and tert-butyl-substituted systems outperforming the methyl thioether-capped derivative. In terms of junction stability, the methyl thioether-capped system is the most resilient, maintaining consistent conductance even after approximately 10 000 cycles. Meanwhile, the likelihood of observing molecular plateaus in both the thioacetate- and tert-butyl-substituted systems declines over time. These findings substantially advance both the design and understanding of functional molecular systems in the realm of single-molecule electronics, particularly in the context of molecular photoswitches.
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42.
  • Gilzad Kohan, Mojtaba, et al. (författare)
  • Optical field coupling in ZnO nanorods decorated with silver plasmonic nanoparticles
  • 2021
  • Ingår i: Journal of Materials Chemistry C. - : Royal Society of Chemistry. - 2050-7526 .- 2050-7534. ; 9:43, s. 15452-15462
  • Tidskriftsartikel (refereegranskat)abstract
    • Characterizing carrier redistribution due to optical field modulation in a plasmonic hot-electron/semiconductor junction can be used to raise the framework for harnessing the carrier decay of plasmonic metals in more efficient conversion systems. In this work we comprehensively studied the carrier redistribution mechanisms of a 1-dimensional (1D) metal-semiconductor Schottky architecture, holding the dual feature of a hot-electron plasmonic system and a simple metal/semiconductor junction. We obtained a strongly enhanced external quantum efficiency (EQE) of the plasmonic Ag decorated ZnO semiconductor in both the band-edge region of ZnO and the corresponding plasmonic absorption profile of the Ag NPs (visible region). Simultaneously, the insertion of an insulating Al2O3 intermediate layer between Ag NPs and ZnO resulted in a parallel distinction of the two main non-radiative carrier transfer mechanisms of plasmonic NPs, i.e. direct electron transfer (DET) and plasmonic induced resonance energy transfer (PIRET). The multi-wavelength transient pump-probe spectroscopy indicated the very fast plasmonic radiative transfer dynamics of the system in <500 fs below 389 nm. We demonstrate a 13% increase of photogenerated current in ZnO upon visible irradiation as a result of non-radiative plasmonic hot-electron injection from Ag NPs. Overall, our device encompasses several effective solutions for designing a plasmonic system featuring non-radiative electron-electron plasmonic dephasing and high photoconversion efficiencies.
  •  
43.
  • Giri, Anupam, et al. (författare)
  • Rational surface modification of Mn3O4 nanoparticles to induce multiple photoluminescence and room temperature ferromagnetism
  • 2013
  • Ingår i: Journal of Materials Chemistry C. - : Royal Society of Chemistry. - 2050-7526 .- 2050-7534. ; 1:9, s. 1885-1895
  • Tidskriftsartikel (refereegranskat)abstract
    • Surface modification can have a significant influence on the materials behavior at the nanoscale and can lead to nanostructures with novel properties. Here, we demonstrate the surface modification induced multiple photoluminescence and room temperature ferromagnetic activation of Mn3O4 nanoparticles (NPs). Employing a systematic variation of the ligands, their functional groups and the structural position of the functional groups, we have identified the necessary and sufficient structural requirements of the surface co-ordinating ligands, in order to induce unprecedented optical/magnetic responses from the NPs. Using a multitude of spectroscopic techniques, we have investigated the mechanism behind the emergence of the multiple photoluminescence (PL), and it is revealed that the presence of a α-hydroxy carboxylate moiety in the ligands is necessary to activate the Jahn-Teller (J-T) splitting of Mn3+ ions on the NP surface and the corresponding d-d transitions along with the ligand-to-metal charge transfer transitions (LMCT, associated with Mn2+/3+-ligand interactions) is the key factor. However, the presence of a carboxylate group on the surface coordinating ligands is sufficient to activate the room temperature ferromagnetism of the NPs. Moreover, it has been observed that the ligands that induced the smallest crystal field splitting energy (CFSE) resulted in the strongest ferromagnetic activation of the NPs. Finally, the functionalized material has been identified as an efficient catalyst for the photo-degradation of a model cationic organic dye. Apart from the fundamental scientific interest, these results represent a promising route for the rational design of Mn 3O4 NPs adaptable to diverse applications.
  •  
44.
  • Goetz, Katelyn P., et al. (författare)
  • Remarkable performance recovery in highly defective perovskite solar cells by photo-oxidation
  • 2023
  • Ingår i: Journal of Materials Chemistry C. - : Royal Society of Chemistry (RSC). - 2050-7526 .- 2050-7534. ; 11:24, s. 8007-8017
  • Tidskriftsartikel (refereegranskat)abstract
    • Exposure to environmental factors is generally expected to cause degradation in perovskite films and solar cells. Herein, we show that films with certain defect profiles can display the opposite effect, healing upon exposure to oxygen under illumination. We tune the iodine content of methylammonium lead triiodide perovskite from understoichiometric to overstoichiometric and expose them to oxygen and light prior to the addition of the top layers of the device, thereby examining the defect dependence of their photooxidative response in the absence of storage-related chemical processes. The contrast between the photovoltaic properties of the cells with different defects is stark. Understoichiometric samples indeed degrade, demonstrating performance at 33% of their untreated counterparts, while stoichiometric samples maintain their performance levels. Surprisingly, overstoichiometric samples, which show low current density and strong reverse hysteresis when untreated, heal to maximum performance levels (the same as untreated, stoichiometric samples) upon the photooxidative treatment. A similar, albeit smaller-scale, effect is observed for triple cation and methylammonium-free compositions, demonstrating the general application of this treatment to state-of-the-art compositions. We examine the reasons behind this response by a suite of characterization techniques, finding that the performance changes coincide with microstructural decay at the crystal surface, reorientation of the bulk crystal structure for the understoichiometric cells, and a decrease in the iodine-to-lead ratio of all films. These results indicate that defect engineering is a powerful tool to manipulate the stability of perovskite solar cells.
  •  
45.
  • Gorski, Krzysztof, et al. (författare)
  • The interplay of intersystem crossing and internal conversion in quadrupolar tetraarylpyrrolo[3,2-b]pyrroles
  • 2024
  • Ingår i: Journal of Materials Chemistry C. - : ROYAL SOC CHEMISTRY. - 2050-7526 .- 2050-7534.
  • Tidskriftsartikel (refereegranskat)abstract
    • Adding nitro groups to aromatic compounds usually quenches their fluorescence via intersystem crossing (ISC) or internal conversion (IC). Herein, we investigated centrosymmetric 1,4-dihydropyrrolo[3,2-b]pyrroles linked to variously substituted nitro-heteroaryls. A 1,4-orientation of the nitro substituent versus the electron rich 1,4-dihydropyrrolo[3,2-b]pyrrole core invokes a strong fluorescence in non-polar solvents and intense two-photon absorption while a 1,3-orientation of push-pull substituents results in a dramatic hypsochromic shift of absorption, weak, bathochromically shifted emission and weak two-photon absorption. The combined experimental and computational study indicates that the primary responsible factors are: (1) the difference in electron density distribution in the LUMO; (2) the difference in mu 10. IC is a dominant mechanism of non-radiative dissipation of energy in all these dyes but as long as the distribution of electron density within the HOMO and LUMO is delocalized on the 1,4-dihydropyrrolo[3,2-b]pyrrole core as well as on the nitroaromatic moieties its rate is slower than the fluorescence rate in non-polar solvents.
  •  
46.
  • Gray, Victor, 1988, et al. (författare)
  • Photophysical characterization of the 9,10-disubstituted anthracene chromophore and its applications in triplet-triplet annihilation photon upconversion
  • 2015
  • Ingår i: Journal of Materials Chemistry C. - : Royal Society of Chemistry (RSC). - 2050-7526 .- 2050-7534. ; 3:42, s. 11111-11121
  • Tidskriftsartikel (refereegranskat)abstract
    • Molecules based on anthracene are commonly used in applications such as OLEDs and triplet-triplet annihilation upconversion. In future design of blue emitting materials it is useful to know which part of the molecule can be altered in order to obtain new physical properties without losing the inherent optical properties. We have studied the effect of substitution of 9,10-substituted anthracenes. Eight anthracenes with aromatic phenyl and thiophene substituents were synthesised, containing both electron donating and accepting groups. The substitutions were found to affect the UV/Vis absorption only to a small extent, however the fluorescence properties were more affected with the thiophene substituents that decreased the fluorescence quantum yield from unity to
  •  
47.
  • Gray, Victor, Dr, 1988-, et al. (författare)
  • Triplet transfer from PbS quantum dots to tetracene ligands : is faster always better?
  • 2022
  • Ingår i: Journal of Materials Chemistry C. - : Royal Society of Chemistry. - 2050-7526 .- 2050-7534. ; 10:43, s. 16321-16329
  • Tidskriftsartikel (refereegranskat)abstract
    • Quantum dot-organic semiconductor hybrid materials are gaining increasing attention as spin mixers for applications ranging from solar harvesting to spin memories. Triplet energy transfer between the inorganic quantum dot (QD) and organic semiconductor is a key step to understand in order to develop these applications. Here we report on the triplet energy transfer from PbS QDs to four energetically and structurally similar tetracene ligands. Even with similar ligands we find that the triplet energy transfer dynamics can vary significantly. For TIPS-tetracene derivatives with carboxylic acid, acetic acid and methanethiol anchoring groups on the short pro-cata side we find that triplet transfer occurs through a stepwise process, mediated via a surface state, whereas for monosubstituted TIPS-tetracene derivative 5-(4-benzoic acid)-12-triisopropylsilylethynyl tetracene (BAT) triplet transfer occurs directly, albeit slower, via a Dexter exchange mechanism. Even though triplet transfer is slower with BAT the overall yield is greater, as determined from upconverted emission using rubrene emitters. This work highlights that the surface-mediated transfer mechanism is plagued with parasitic loss pathways and that materials with direct Dexter-like triplet transfer are preferred for high-efficiency applications.
  •  
48.
  • Grybauskaite-Kaminskiene, Gintare, et al. (författare)
  • Contribution of TADF and exciplex emission for efficient "warm-white" OLEDs
  • 2018
  • Ingår i: Journal of Materials Chemistry C. - : Royal Society of Chemistry. - 2050-7526 .- 2050-7534. ; 6:6, s. 1543-1550
  • Tidskriftsartikel (refereegranskat)abstract
    • The bicarbazole derivative 4,4'-(9H, 9'H-[3,3'-bicarbazole]-9,9'-diyl) bis(3-(trifluoromethyl) benzonitrile), denoted as pCNBCzoCF(3), was synthesized and tested for white OLED applications. pCNBCzoCF3 demonstrated an extremely small value of the singlet-triplet energy gap that caused intensive thermally activated delayed fluorescence (TADF). In addition, this compound is able to form exciplex-type excited states at the interface with star-shaped 4,40,400-tris[phenyl(m-tolyl) amino] triphenylamine (m-MTDATA). Combining the TADF emission of pCNBCzoCF3 with the exciplex emission from the pCNBCzoCF(3) m-MTDATA interface, we fabricated a number of highly efficient "warm-white'' OLEDs, the electroluminescence of which was close to candle emission. The best device demonstrated a very high brightness of 40 900 Cd m(-2) (at 15 V), current efficiency of 53.8 Cd A(-1) and power efficiency of 19.3 lm W-1, while the external quantum efficiency reached 18.8%. The fabricated devices demonstrated high emission characteristics even for the standard test at 1000 Cd m(-2) (current efficiency of 46.2 Cd A(-1), power efficiency of 10.6 lm W-1, EQE of 17.0%).
  •  
49.
  • Gryszel, Maciej, et al. (författare)
  • Vertical Organic Electrochemical Transistor Platforms for Efficient Electropolymerization of Thiophene Based Oligomers
  • 2024
  • Ingår i: Journal of Materials Chemistry C. - : ROYAL SOC CHEMISTRY. - 2050-7526 .- 2050-7534.
  • Tidskriftsartikel (refereegranskat)abstract
    • Organic electrochemical transistors (OECTs) have emerged as promising candidates for various fields, including bioelectronics, neuromorphic computing, biosensors, and wearable electronics. OECTs operate in aqueous solutions, exhibit high amplification properties, and offer ion-to-electron signal transduction. The OECT channel consists of a conducting polymer, with PEDOT:PSS receiving the most attention to date. While PEDOT:PSS is highly conductive, and benefits from optimized protocols using secondary dopants and detergents, new p-type and n-type polymers are emerging with desirable material properties. Among these, low-oxidation potential oligomers are highly enabling for bioelectronics applications, however the polymers resulting from their polymerization lag far behind in conductivity compared with the established PEDOT:PSS. In this work we show that by careful design of the OECT geometrical characteristics, we can overcome this limitation and achieve devices that are on-par with transistors employing PEDOT:PSS. We demonstrate that the vertical architecture allows for facile electropolymerization of a family of trimers that are polymerized in very low oxidation potentials, without the need for harsh chemicals or secondary dopants. Vertical and planar OECTs are compared using various characterization methods. We show that vOECTs are superior platforms in general and propose that the vertical architecture can be expanded for the realization of OECTs for various applications.
  •  
50.
  • Gschneidtner, Tina, 1985, et al. (författare)
  • Progress in self-assembled single-molecule electronic devices
  • 2013
  • Ingår i: Journal of Materials Chemistry C. - : Royal Society of Chemistry (RSC). - 2050-7534 .- 2050-7526. ; 1:43, s. 7127-7133
  • Tidskriftsartikel (refereegranskat)abstract
    • Recent years have seen progress in several areas regarding single molecule electronic devices. A number of interesting structure-property relationships have been observed, including vibronic effects, spin transitions, and molecular electronic interference known as quantum interference. Together, these observations highlight what the rich opportunities in molecular design might bring in terms of advanced device properties. Pertinent challenges are related to development of high yield preparative procedures for fabrication of single molecule devices in a parallel and reproducible way. With this highlight article we review recent progress in the field considering self-assembled formation of metal nanogaps incorporating single molecules for single molecule electronics applications. We discuss methods for the formation of the nanogaps as well as methods attempting to achieve single molecule functionality in each individual device.
  •  
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