| 1. |
- Alcer, David, et al.
(författare)
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Comparison of Triethylgallium and Trimethylgallium Precursors for GaInP Nanowire Growth
- 2021
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Ingår i: Physica Status Solidi (B) Basic Research. - : Wiley. - 0370-1972. ; 258:2
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Tidskriftsartikel (refereegranskat)abstract
- Nanowire (NW) arrays containing a top segment of GaxIn1–xP are investigated, comparing NWs grown using two different Ga precursors, trimethylgallium (TMGa) and triethylgallium (TEGa). TMGa is the precursor commonly used for the particle-assisted vapor–liquid–solid (VLS) growth of GaxIn1–xP NWs. However, it shows inefficient pyrolysis at typical NW growth conditions. The use of the alternative precursor TEGa is investigated by making a direct comparison between NWs grown using TEGa and TMGa at otherwise identical growth conditions. Growth rates, resulting NW materials composition, and time-resolved photoluminescence (TRPL) lifetimes are investigated. With increasing Ga content of the NWs, the TRPL lifetimes decrease, indicating trap states that are associated with GaP. Somewhat longer TRPL lifetimes for the samples grown using TEGa indicate a lower concentration of deep trap states. For doped NWs, it is found that the strong effect of the p-type dopant diethylzinc (DEZn) on the NW composition, observed for GaxIn1–xP NWs grown using TMGa, is absent when using TEGa.
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| 2. |
- Alvarez, Sol Laura Gutierrez, et al.
(författare)
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Morphology-Dependent One- and Two-Photon Absorption Properties in Blue Emitting CsPbBr3Nanocrystals
- 2022
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Ingår i: Journal of Physical Chemistry Letters. - : American Chemical Society (ACS). - 1948-7185. ; 13:22, s. 4897-4904
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Tidskriftsartikel (refereegranskat)abstract
- The linear and nonlinear optical parameters and morphologic dependence of CsPbBr3 nanocrystals (NCs) are crucial for device engineering. In particular, such information in asymmetric nanocrystals is still insufficient. We characterized the OPLA (σ1) and TPA cross sections (σ2) of a series CsPbBr3 nanocrystals with various aspect ratios (AR) using femtosecond transient absorption spectroscopy (TAS). The σ1 presents a linear volume dependence of all the samples, which agrees with the previous behavior in CsPbBr3 QDs. However, the σ2 values do not exhibit conventional power dependency of the crystal volume but are also modulated by the shape-dependent local field factors. In addition, the local field effect in CsPbBr3 NCs is contributed by their asymmetric morphologies and polar ionic lattices, which is more pronounced than in conventional semiconductor NCs. Finally, we revealed that the lifetimes of photogenerated multiexcitonic species of those nanocrystals feature identical morphology independence in both OPLA and TPA.
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| 3. |
- An, Rui, et al.
(författare)
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Photostability and Photodegradation Processes in Colloidal CsPbI3 Perovskite Quantum Dots
- 2018
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Ingår i: ACS Applied Materials and Interfaces. - : American Chemical Society (ACS). - 1944-8244 .- 1944-8252. ; 10:45, s. 39222-39227
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Tidskriftsartikel (refereegranskat)abstract
- All-inorganic CsPbI3 perovskite quantum dots (QDs) have attracted intense attention for their successful application in photovoltaics (PVs) and optoelectronics that are enabled by their superior absorption capability and great photoluminescence (PL) properties. However, their photostability remains a practical bottleneck and further optimization is highly desirable. Here, we studied the photostability of as-obtained colloidal CsPbI3 QDs suspended in hexane. We found that light illumination does induce photodegradation of CsPbI3 QDs. Steady-state spectroscopy, X-ray diffraction, Fourier transform infrared spectroscopy, transmission electron microscopy, and transient absorption spectroscopy verified that light illumination leads to detachment of the capping agent, collapse of the CsPbI3 QD surface, and finally aggregation of surface Pb0. Both dangling bonds containing surface and Pb0 serve as trap states causing PL quenching with a dramatic decrease of PL quantum yield. Our work provides a detailed insight about the correlation between the structural and photophysical consequences of the photodegradation process in CsPbI3 QDs and may lead to the optimization of such QDs toward device applications.
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| 4. |
- Bericat Vadell, Robert, et al.
(författare)
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Single-electron transfer reactions on surface-modified gold plasmons
- 2023
-
Ingår i: Materials Today Chemistry. - : Elsevier. - 2468-5194. ; 34
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Tidskriftsartikel (refereegranskat)abstract
- Photoredox catalysis's relevance in organic synthesis research and innovation will increase in the coming decades. However, the processes rely almost exclusively on expensive noble metal complexes, most notably iridium complexes, to absorb light and transfer a single charge to a substrate or a catalyst to initiate cascade transformations. Light-triggered plasmon resonances generate a non-Fermi-Dirac energy distribution with many hot carriers that decay in similar to 1 ps. Their ultrafast relaxation makes performing single electron transfer (SET) transformations challenging. Herein, a novel photosystem is proposed based on surface-modified gold nanoparticles (aka plasmon "molecularization"), which improved charge separation and, more importantly, enabled SET reactions, expanding the portfolio of photocatalysts available for photoredox catalysis. The photosystem was made into an electrode, permitting its use in photoelectrochemical arrangements that leverage electro- and photo-chemical approaches' benefits and chemical engineering solutions, helping the synthetic chemistry efforts towards greener synthesis and synthesis of more complex structures on a scale.
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| 5. |
- Cai, Zekai, et al.
(författare)
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Charge photogeneration dynamics in non-fullerene polymer solar cells with fluorinated and non-fluorinated acceptors
- 2024
-
Ingår i: Journal of Chemical Physics. - 0021-9606. ; 160:7
-
Tidskriftsartikel (refereegranskat)abstract
- In this work, charge photogeneration and recombination processes of PM6:IDIC-4F and PM6:IDIC blend films were investigated by the steady-state and time-resolved spectroscopies, as well as the time-dependent density functional theory calculations. The peaks in absorption and photoluminescence (PL) spectra of IDIC and IDIC-4F solutions were assigned by combining the experiment and the simulation of UV-vis absorption and PL spectra. For neat acceptor films, the exciton diffusion length of neat IDIC and IDIC-4F films was estimated as ∼28.9 and ∼19.9 nm, respectively. For PM6-based blend films, we find that the fluorine substitution engineering on the IDIC acceptor material can increase the phase separate size of acceptor material in blend films, resulting in the reduction of dissociation efficiencies of acceptor excitons. In addition, we find that the charge recombination in PM6:IDIC-4F is dominated by bimolecular recombination, in comparison to geminate type carrier recombination in PM6:IDIC blend films. In addition, we find that thermal annealing treatment has a weak influence on carrier recombination but slightly reduces the exciton dissociation efficiency of acceptor in PM6:IDIC blend films, leading to a slightly reduced power conversion efficiency of PM6:IDIC solar cells. These results may shed light on the design of high-performance semiconductor molecules for application in solar cells.
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| 6. |
- Dong, Jianqi, et al.
(författare)
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Centimeter-long III-Nitride nanowires and continuous-wave pumped lasing enabled by graphically epitaxial lift-off
- 2020
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Ingår i: Nano Energy. - : Elsevier BV. - 2211-2855. ; 78
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Tidskriftsartikel (refereegranskat)abstract
- It remains a big challenge to elongate one-dimensional (1D) semiconductor nanowires (NWs), which can be attractive platforms for miniaturizing and/or integrating macroscopic devices, into centimeter-scale length. Herein, we report the innovative preparation of single-crystalline III-nitride NWs, with unprecedented length above 2 cm and the aspect ratio above 6000, by graphically epitaxial lifting-off (GELO) the epitaxial films on sapphire. The proposed GELO technology involves isotropic dry etching and selectively electrochemical (EC) etching. Reaction kinetics study of the EC etching indicate that two-steps processes are included, which is, to our best knowledge, firstly revealed and experimentally confirmed. Centimeter-long freestanding NWs, with predesigned structure of homogeneous GaN, p-GaN/(InGaN/GaN)6 quantum-wells/n-GaN (simply InGaN/GaN QWs) and AlGaN/AlN/GaN heterostructure, are successfully obtained and exhibit superior morphological uniformity and robust flexibility. Optical properties of the released InGaN/GaN QW-NWs were well optimized owing to the relieved intrinsic strain. Random lasing behavior was unexpectedly observed by continuous-wave excitation of the individual InGaN/GaN QW-NW, with a low threshold of 232 kW•cm-2. This work represents a low-cost and economic approach to yield structure-engineerable super-long III-nitride NWs, which would promote the development and integration of optoelectronic nanodevices.
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| 7. |
- Feng, Junyi, et al.
(författare)
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Aggregation-Induced Emission in a Polymeric Photovoltaic Donor Material
- 2022
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Ingår i: Journal of Physical Chemistry C. - : American Chemical Society (ACS). - 1932-7447 .- 1932-7455. ; 126:48, s. 20275-20283
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Tidskriftsartikel (refereegranskat)abstract
- In this work, we report the aggregation-induced emission in a polymeric donor material poly(bis(2-butyloctyl)[2,2′:5′,2″-terthiophene]-4,4″-dicarboxylate-5,5′-diyl-vinylene) (PTVT-T), which exhibits a high device performance for the application of photovoltaics. Time-dependent density functional theory calculations and steady-state and time-resolved spectroscopy have been employed to reveal the underlying emission mechanism. We find that the aggregation of the PTVT-T polymer chain in solution increases the exciton luminescence lifetime and exciton emission quantum yield, which is related to the effective torsional inhibition of carbon-carbon single bonds. Compared with the aggregates in solution, the exciton emission quantum yield of the aggregates in PTVT-T film is reduced. It is attributable to exciton delocalization caused by the improvement of molecular planarity in film. We also observe that the as-cast film and thermally annealed film show distinctly different emission behaviors. This work can shed light on designing optoelectronic polymer materials with the integration of photovoltaic and light-emitting functions.
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| 8. |
- Feng, Junyi, et al.
(författare)
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The Role of Energy Offsets on Charge Photogeneration Dynamics in Y-Series Molecules-Based Polymer Solar Cells
- 2023
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Ingår i: Solar RRL. - 2367-198X. ; 7:16
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Tidskriftsartikel (refereegranskat)abstract
- Recent research has revealed that low-energy offset polymer solar cells (PSCs) are capable of a power conversion efficiency of over 19%. However, it is unclear how energy offsets and the charge photogeneration process are correlated. Herein, the effect of energy offsets on charge photogeneration dynamics for Y-series molecules (Y5, Y6, Y10, and BTP-4F-12)-based PSCs with the variations of the lowest unoccupied molecular orbital energy offsets (ΔELUMO) of 0.11–0.42 eV and the highest occupied molecular orbital energy offsets (ΔEHOMO) of 0.08–0.23 eV utilizing steady-state and time-resolved spectroscopies is studied. The steady-state measurement shows that the probability of photoluminescence quenching via energy transfer for the donor exciton reduces with the increasing ΔELUMO. It is found that even in PM6:Y6 with the highest ΔELUMO, ≈18% of PM6 exciton dissociated via the path of “energy transfer first and then hole transfer,” manifesting the energy transfer also plays a vital role in the process of exciton dissociation. Furthermore, it is found that the PM6 exciton can efficiently dissociate under the ΔELUMO of 0.11 eV. After photoexcitation of the Y-series molecule acceptors, the exciton dissociation efficiency enhances with the increase of ΔEHOMO. Besides, the higher energy offsets, the lower charge recombination rate in the ultrafast timescale has been found from the transient absorption measurement. These findings reveal that energy offsets are important for charge photogeneration and recombination in an ultrafast timescale for Y-series molecule-based PSCs, which may shed light on the design of high-performance PSCs.
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| 9. |
- Geng, Huifang, et al.
(författare)
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Controlled synthesis of highly stable lead-free bismuth halide perovskite nanocrystals : tructures and photophysics
- 2023
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Ingår i: SCIENCE CHINA Materials. - : Springer Science and Business Media LLC. - 2095-8226 .- 2199-4501. ; 66:5, s. 2079-2089
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Tidskriftsartikel (refereegranskat)abstract
- Recently, cesium bismuth halide perovskites have emerged as potential substitutes to their counterparts, cesium lead halide perovskites, owing to their low toxicity. However, the photophysics of cesium-bismuth halides nanocrystals (NCs) have not yet been fully rationalized because their structures remain highly debated. The ultraviolet-visible (UV-vis) absorption along with other photophysical properties such as the nature and lifetime of the excited states vary considerably across the previous reports. Here, we successfully synthesize pure Cs3BiBr6 and Cs3Bi2Br9 NCs via a modified hot-injection method, where the structure can be easily controlled by tuning the reaction temperature. The UV-vis absorption spectrum of the pure Cs3Bi2Br9 NCs features two characteristic peaks originating from the absorption of the first exciton and second exciton, respectively, which ultimately clarifies the debate in the previous reports. Using femtosecond transient absorption spectroscopy, we systematically investigate the excited state dynamics of the Cs3Bi2Br9 NCs and reveal that the photoexcited carriers undergo a self-trapping process within 3 ps after excitation. More intriguingly, the Cs3Bi2Br9 NCs prepared by this method show much better photostability than those prepared by the ligand-assisted reprecipitation process. Photodetectors based on these Cs3Bi2Br9 NCs show a sensitive light response, demonstrating the definite potential for breakthrough optoelectronic applications. [Figure not available: see fulltext.].
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| 10. |
- Geng, Xinjian, et al.
(författare)
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Can photoluminescence quenching be a predictor for perovskite solar cell efficiencies?
- 2023
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Ingår i: Physical Chemistry, Chemical Physics - PCCP. - : Royal Society of Chemistry. - 1463-9076 .- 1463-9084. ; 25:34, s. 22607-22613
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Tidskriftsartikel (refereegranskat)abstract
- Bromide-based perovskites have large bandgaps, making them attractive for tandem solar cells developed to overcome the Shockley–Queisser limit. A perovskite solar cell architecture employs transporting layers to improve charge extraction and transport. Due to the wide variety of materials and preparation methods, it is critical to devise fast screening methods to rank transporting layers. Herein, we evaluate perovskite fluorescence quenching followed by time- and energy-resolved photoluminescence (TER-PL) and analyse the intensity dependence as a potential method to qualify charge-transporting layers rapidly. The capability of the technique was evaluated with TiO2/FAPbBr3 and SnO2/FAPbBr3, the most commonly used electron transporting layers, which were prepared using standard protocols to make best-performing devices. The results revealed that TiO2 is the most effective quencher due to the higher density of states in the conduction band, consistent with Marcus-Gerischer's theory. However, record-performance devices use SnO2 as the electron transport layer. This shows that the relationship between photoluminescence quenching and device performance is not bidirectional. Therefore, additional measurements like conductivity are also needed to provide reliable feedback for device performance.
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| 11. |
- Geng, Xinjian, et al.
(författare)
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Transient Energy-Resolved Photoluminescence Study of Excitons and Free Carriers on FAPbBr3 and FAPbBr3/SnO2 Interfaces
- 2023
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Ingår i: The Journal of Physical Chemistry C. - : American Chemical Society (ACS). - 1932-7447 .- 1932-7455. ; 127:6, s. 3085-3092
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Tidskriftsartikel (refereegranskat)abstract
- Lead bromide perovskites have a larger band gap and are significantly more stable than their iodine counterparts, offering the perspective for higher voltage, tandem photovoltaics exceeding the Shockley-Queisser limit, and shorter time to deployment of photovoltaics. However, their efficiencies still need to be rivaling the iodine ones. Herein, the photophysics of FAPbBr(3) and the ones behind electron transfer from FAPbBr(3) to SnO2, one of the most effective electron transporting materials (ETMs), are reported. Time- and energy-resolved photoluminescence studies revealed the existence of two emitting states in the perovskite, which were assigned to bounded excitons and free carriers. SnO2 extracted electrons from excitons and free carriers, with a selectivity related to the SnO2 surface treatment. This new insight helps explain SnO2's unique qualities as an ETM to produce photovoltaics with reduced voltage losses. Furthermore, this study illustrates the importance of performing time- and energy-resolved photoluminescence to capture the intricacies of the photophysical process.
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| 12. |
- Hrachowina, Lukas, et al.
(författare)
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Imaging the influence of oxides on the electrostatic potential of photovoltaic InP nanowires
- 2021
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Ingår i: Nano Research. - : Springer Science and Business Media LLC. - 1998-0124 .- 1998-0000. ; 14:11, s. 4087-4092
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Tidskriftsartikel (refereegranskat)abstract
- Nanowires require surface passivation due to their inherent large surface to volume ratio. We investigate the effect of embedding InP nanowires in different oxides with respect to surface passivation by use of electron beam induced current measurements enabled by a nanoprobe based system inside a scanning electron microscope. The measurements reveal remote doping due to fixed charge carriers in the passivating POx/Al2O3 shell in contrast to results using SiOx. We used time-resolved photoluminescence to characterize the lifetime of charge carriers to evaluate the success of surface passivation. In addition, spatially resolved internal quantum efficiency simulations support and correlate the two applied techniques. We find that atomic-layer deposited POx/Al2O3 has the potential to passivate the surface of InP nanowires, but at the cost of inducing a field-effect on the nanowires, altering their electrostatic potential profile. The results show the importance of using complementary techniques to correctly evaluate and interpret processing related effects for optimization of nanowire-based optoelectronic devices. [Figure not available: see fulltext.].
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| 13. |
- Irish, Austin, et al.
(författare)
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Nitrogen plasma passivation of GaAs nanowires resolved by temperature dependent photoluminescence
- 2022
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Ingår i: NANO EXPRESS. - : Institute of Physics (IOP). - 2632-959X. ; 3:4
-
Tidskriftsartikel (refereegranskat)abstract
- We demonstrate a significant improvement in the optical performance of GaAs nanowires achieved using a mixed nitrogen-hydrogen plasma which passivates surface states and reduces the rate of nonradiative recombination. This has been confirmed by time-resolved photoluminescence measurements. At room temperature, the intensity and lifetime of radiative recombination in the plasma-treated nanowires was several times greater than that of the as-grown GaAs nanowires. Low-temperature measurements corroborated these findings, revealing a dramatic increase in photoluminescence by two orders of magnitude. Photoelectron spectroscopy of plasma passivated nanowires demonstrated a yearlong stability achieved through the replacement of surface oxygen with nitrogen. Furthermore, the process removed the As-0 defects observed on non-passivated nanowires which are known to impair devices. The results validate plasma as a nitridation technique suitable for nanoscale GaAs crystals. As a simple ex situ procedure with modest temperature and vacuum requirements, it represents an easy method for incorporating GaAs nanostructures into optoelectronic devices.
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| 14. |
- Li, Chuanshuai, et al.
(författare)
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Graphitic Carbon Nitride/CdSe Quantum Dot/Iron Carbonyl Cluster Composite for Enhanced Photocatalytic Hydrogen Evolution
- 2021
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Ingår i: ACS Applied Nano Materials. - : American Chemical Society (ACS). - 2574-0970. ; 4:6, s. 6280-6289
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Tidskriftsartikel (refereegranskat)abstract
- A g-C3N4/CdSe quantum dot/[Fe2S2(CO)6] composite has been successfully constructed. The structure and chemical composition of the composite were investigated via, inter alia, transmission electron microscopy (TEM), Fourier transform infrared spectroscopy (FTIR), and X-ray photoelectron spectroscopy (XPS). The ability of the assembly to act as a photocatalyst for proton reduction to form hydrogen gas was studied. With visible light irradiation for 4 h, the total H2 production catalyzed by the g-C3N4/CdSe quantum dot/[Fe2S2(CO)6] composite was found to be 9 times as high as a corresponding CdSe/[Fe2S2(CO)6] assembly and significantly higher than either the CdSe quantum dots or g-C3N4 alone. The g-C3N4 support/matrix was found to enhance the stability and efficiency of the CdSe quantum dot/iron carbonyl cluster assembly in the photocatalytic hydrogen evolution process. Results from recycling tests showed that the g-C3N4/CdSe quantum dot/[Fe2S2(CO)6] composite is a sustainable and robust photocatalyst, maintaining the same activity after three cycles. The photoinduced charge carrier transfer dynamics in the g-C3N4/CdSe quantum dot/[Fe2S2(CO)6] composite system has been investigated by transient absorption (TA) and time-resolved photoluminescence (TRPL) spectroscopies. The spectroscopic results indicate efficient hole transfer from the valence band of the excited CdSe quantum dots to the molecular iron carbonyl clusters and from the defect state of the quantum dots to g-C3N4 in the g-C3N4/CdSe quantum dot/[Fe2S2(CO)6] composite, which significantly inhibits the recombination of photogenerated charge carriers in CdSe quantum dots and boosts the photocatalytic activity and stability for hydrogen evolution. Energy transfer from g-C3N4 to the CdSe quantum dot/[Fe2S2(CO)6] assembly with a time constant of 0.7 ns also contributed to the charge transfer process.
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| 15. |
- Liang, Mingli, et al.
(författare)
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Electronic Structure and Trap States of Two-Dimensional Ruddlesden–Popper Perovskites with the Relaxed Goldschmidt Tolerance Factor
- 2020
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Ingår i: ACS Applied Electronic Materials. - : American Chemical Society (ACS). - 2637-6113. ; 2:5, s. 1402-1412
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Tidskriftsartikel (refereegranskat)abstract
- Two-dimensional Ruddlesden–Popper perovskites (2D RPPs) have been considered as promising building blocks for optoelectronic applications owing to optical properties comparable to the ones of 3D perovskites, together with superior stability. In addition, the more flexible structure adopted by such perovskites leads to a relaxation of the Goldschmidt tolerance factor (τ) requirement. Herein, we compare the crystalline and electronic structures, as well as the photophysics of two 2D perovskite single crystals (n-BA)2(MA)2Pb3I10 (BMAPI) and (n-BA)2(EA)2Pb3I10 (BEAPI) (n-BA = n-butylamine) containing small A-cations (MA, methylammonium) and large A-cations (EA, ethylammonium), respectively. The latter presents a relaxed τ (τEA > 1) compared with the requirement of a stable phase in 3D perovskites (τ < 1). Such relaxed τ is beneficial from the structural flexibility of the long organic cation bilayer and the pronounced lattice distortions in the 2D perovskite structures. We further elucidate how the greater lattice distortions concurrently modulate the electronic structure as well as trap densities in these 2D RPPs. The electronic band gap (Eg) of BEAPI (2.08 ± 0.03 eV) is ∼0.17 eV larger than the one of BMAPI (1.91 ± 0.03 eV). This is mainly because of a shift in the valence band maximum associated with the expansion of the Pb–I bond length in BEAPI. In addition, the overall trap state densities for BMAPI and BEAPI are calculated to be ∼2.18 × 1016 and ∼3.76 × 1016 cm–3, respectively, as extracted from the time-resolved photoluminescence studies. The larger trap density in BEAPI can be attributed to the stronger interfacial lattice distortion that sets in when large EA cations are contained into the inorganic crystal lattice.
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| 16. |
- Liang, Mingli, et al.
(författare)
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Free Carriers versus Self-Trapped Excitons at Different Facets of Ruddlesden-Popper Two-Dimensional Lead Halide Perovskite Single Crystals
- 2021
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Ingår i: Journal of Physical Chemistry Letters. - : American Chemical Society (ACS). - 1948-7185. ; 12:20, s. 4965-4971
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Tidskriftsartikel (refereegranskat)abstract
- The physical origin of sub-band gap photoluminescence in Ruddlesden-Poppers two-dimensional (2D) lead halide perovskites (LHPs) is still under debate. In this paper, we studied the photoluminescence features from two different facets of 2D LHP single crystals: the in-plane facet (IF) containing the 2D inorganic layers and the facet perpendicular to the 2D layers (PF). At the IF, the free carriers (FCs) dominate due to the weak electron-phonon coupling in a symmetric lattice. At the PF, the strain accumulation along the 2D layers enhances the electron-phonon coupling and facilitates self-trapped exciton (STE) formation. The time-resolved PL studies indicate that free carriers (FCs) at the IF can move freely and display the trapping by the intrinsic defects. The STEs at the PF are not likely trapped by the defects due to the reduced mobility. However, with increasing STE density, the STE transport is promoted, enabling the trapping of STE by the intrinsic defects.
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| 17. |
- Lin, Weihua, et al.
(författare)
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Combining two-photon photoemission and transient absorption spectroscopy to resolve hot carrier cooling in 2D perovskite single crystals : the effect of surface layer
- 2022
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Ingår i: Journal of Materials Chemistry C. - : Royal Society of Chemistry (RSC). - 2050-7526 .- 2050-7534. ; 10:44, s. 16751-16760
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Tidskriftsartikel (refereegranskat)abstract
- We investigate hot carrier (HC) cooling in two-dimensional (2D) perovskite single crystals by applying two complementary ultrafast spectroscopy techniques - transient absorption (TA) and time-resolved two-photon photoemission (TR-2PPE) spectroscopies. TR-2PPE directly maps the hot electron distribution and its dynamics in the conduction band to the detected photoelectron distribution. While TR-2PPE selectively probes the upper layer of the material, TA provides information on the whole bulk. Two cooling regimes are resolved in both techniques. The fast timescale of 100-200 fs is related to the electron scattering by longitudinal optical (LO) phonons and the slow timescale of 3-4 ps corresponds to the LO phonon relaxation. The HC cooling dynamic of TA measurement has faster initial stage and higher starting temperature for the slower stage than in TR-2PPE measurements. Conclusions about spatial sensitivity of the cooling dynamics across the 2D perovskite single crystals constitute valuable information that can guide the future development of HC solar cells and thermoelectric applications based on 2D perovskites.
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| 18. |
- Liu, Shungang, et al.
(författare)
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The role of connectivity in significant bandgap narrowing for fused-pyrene based non-fullerene acceptors toward high-efficiency organic solar cells
- 2020
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Ingår i: Journal of Materials Chemistry A. - : Royal Society of Chemistry (RSC). - 2050-7488 .- 2050-7496. ; 8:12, s. 5995-6003
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Tidskriftsartikel (refereegranskat)abstract
- Great attention has been paid to developing low bandgap non-fullerene acceptors (NFAs) for matching wide bandgap donor polymers to increase the photocurrent and therefore the power conversion efficiencies (PCEs) of NFA organic solar cells, while pyrene-core based acceptor-donor-acceptor (A-D-A) NFAs have been mainly reported via the 2,9-position connection due to their bisthieno[3′,2′-b']thienyl[a,h]pyrene fused via a five-membered ring bridge at the ortho-position of pyrene as the representative one named FPIC5, which has prohibited further narrowing their energy gap. Herein, an acceptor FPIC6 was exploited by creating the 1,8-position connection through fusing as bisthieno[3′,2′-b′]thienyl[f-g,m-n]pyrene linked at the bay-position via a six-membered bridge, with enhanced push-pull characteristics within such A-D-A structure. As a structural isomer of FPIC5, FPIC6 exhibited a much lower bandgap of 1.42 eV (1.63 eV for FPIC5). Therefore, the photocurrent and PCE of PTB7-Th:FPIC6 cells were improved to 21.50 mA cm-2 and 11.55%, respectively, due to the balanced mobilities, better photoluminescence quenching efficiency and optimized morphology, which are both ∼40% better than those of PTB7-Th:FPIC5 cells. Our results clearly proved that a pyrene fused core with 1,8-position connection with electron-withdrawing end groups instead of 2,9-position connection is an efficient molecular design strategy to narrow the optical bandgap and improve the photovoltaic performance of NFA based OSCs.
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| 19. |
- Meng, Jie, et al.
(författare)
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Optimizing the quasi-equilibrium state of hot carriers in all-inorganic lead halide perovskite nanocrystals through Mn doping : fundamental dynamics and device perspectives
- 2022
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Ingår i: Chemical Science. - : Royal Society of Chemistry (RSC). - 2041-6520 .- 2041-6539. ; 13:6, s. 1734-1745
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Tidskriftsartikel (refereegranskat)abstract
- Hot carrier (HC) cooling accounts for the significant energy loss in lead halide perovskite (LHP) solar cells. Here, we study HC relaxation dynamics in Mn-doped LHP CsPbI3 nanocrystals (NCs), combining transient absorption spectroscopy and density functional theory (DFT) calculations. We demonstrate that Mn2+ doping (1) enlarges the longitudinal optical (LO)-acoustic phonon bandgap, (2) enhances the electron-LO phonon coupling strength, and (3) adds HC relaxation pathways via Mn orbitals within the bands. The spectroscopic study shows that the HC cooling process is decelerated after doping under band-edge excitation due to the dominant phonon bandgap enlargement. When the excitation photon energy is larger than the optical bandgap and the Mn2+ transition gap, the doping accelerates the cooling rate owing to the dominant effect of enhanced carrier-phonon coupling and relaxation pathways. We demonstrate that such a phenomenon is optimal for the application of hot carrier solar cells. The enhanced electron-LO phonon coupling and accelerated cooling of high-temperature hot carriers efficiently establish a high-temperature thermal quasi-equilibrium where the excessive energy of the hot carriers is transferred to heat the cold carriers. On the other hand, the enlarged phononic band-gap prevents further cooling of such a quasi-equilibrium, which facilitates the energy conversion process. Our results manifest a straightforward methodology to optimize the HC dynamics for hot carrier solar cells by element doping. This journal is
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| 20. |
- Mone, Mariza, 1992, et al.
(författare)
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Near-Infrared Emission by Tuned Aggregation of a Porphyrin Compound in a Host–Guest Light-Emitting Electrochemical Cell
- 2021
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Ingår i: Advanced Optical Materials. - : Wiley. - 2195-1071 .- 2162-7568. ; 9:6
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Tidskriftsartikel (refereegranskat)abstract
- The synthesis of 5,10,15,20-tetrakis((5,10-bis((2-hexyldecyl)oxy)dithieno[3,2-c:3′,2′-h][1,5]naphthyridin-2-yl)ethynyl)porphyrin zinc(II) (Por4NT), a near-infrared (NIR) emitting compound, comprising a zinc porphyrin core linked with triple bonds through its meso positions to four 5,10-bis((2-hexyldecyl)oxy)dithieno[3,2-c:3′,2′-h][1,5]naphthyridine (NT) arms is reported. Por4NT featured high solubility in common non-polar solvents, which is ideal for easy processing through solution techniques, and high photoluminescence (PL) efficiency of ≈30% in dilute toluene solution. It also exhibited a strong tendency for aggregation because of its flat conformation, and this aggregation resulted in a strong redshifted emission and a drop in PL efficiency. A well-matched PBDTSi-BDD-Py “host” terpolymer is therefore designed, which is capable of mitigating the aggregation of the Por4NT “guest”. An optimized blend of the host, guest, and an ionic-liquid electrolyte is utilized as the active material in a light-emitting electrochemical cell (LEC), which delivered strong NIR radiance of 134 µW cm-2 with a long wavelength maximum at 810 nm at a low drive voltage of 5.0 V. The attainment of the strong NIR emission from the host–guest LEC is attributed to a tuned aggregation of the Por4NT emitter, which resulted in the desired aggregation-induced redshift of the emission at a reasonably retained efficiency.
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| 21. |
- Su, Xiaojun, et al.
(författare)
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Effect of hydrogen chloride etching on carrier recombination processes of indium phosphide nanowires
- 2019
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Ingår i: Nanoscale. - : Royal Society of Chemistry (RSC). - 2040-3364 .- 2040-3372. ; 11:40, s. 18550-18558
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Tidskriftsartikel (refereegranskat)abstract
- Introduction of in situ HCl etching to an epitaxial growth process has been shown to suppress radial growth and improve the morphology and optical properties of nanowires. In this paper, we investigate the dynamics of photo-generated charge carriers in a series of indium phosphide nanowires grown with varied HCl fluxes. Time resolved photo-induced luminescence, transient absorption and time resolved terahertz spectroscopy were employed to investigate charge trapping and recombination processes in the nanowires. Since the excitation photons generate charges predominantly in less than a half length of the nanowires, we can selectively assess the charge carrier dynamics at their top and bottom. We found that the photoluminescence decay is dominated by the decay of the mobile hole population due to trapping, which is affected by the HCl etching. The hole trapping rate is in general faster at the top of the nanowires than at the bottom. In contrast, electrons remain highly mobile until they recombine non-radiatively with the trapped holes. The slowest hole trapping as well as the least efficient non-radiative recombination was recorded for etching using the HCl molar fraction of χHCl = 5.4 × 10-5
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| 22. |
- Su, Xiaojun, et al.
(författare)
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Understanding of photophysical processes in dio additive-treated ptb7:Pc71 bm solar cells
- 2021
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Ingår i: Crystals. - : MDPI AG. - 2073-4352. ; 11:9
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Tidskriftsartikel (refereegranskat)abstract
- 1,8-diiodooctane (DIO) additive is an important method for optimizing the morphology and device performance of polythieno[3,4-b]-thiophene-co-benzodithiophene (PTB7)-based polymer solar cells. However, the effect of DIO additive on charge photogeneration dynamics of PTB7-based polymer solar cells is still poorly understood. In this work, the effect of DIO additive on the carrier photogeneration dynamics, as well as device performance of PTB7: [6,6]-phenyl-C71-butyric acid methyl ester (PC71 BM) solar cells was studied. Bias-dependent photoluminescence (PL) experiments of a neat PTB7 device show that the exciton cannot be dissociated by the electric field in the device within the operating voltage range, but it can be effectively dissociated by the high electric field. PL and time-resolved PL studies show that DIO additive reduces the phase size of PTB7 in the blend film, resulting in an increased exciton dissociation efficiency. The carrier recombination processes were studied by transient absorption, which shows geminate carrier recombination was suppressed in the DIO-treated PTB7:PC71 BM device in ultrafast time scale. The increased exciton dissociation efficiency and suppressed carrier recombination in ultrafast time scale play an important role for DIO-treated PTB7:PC71 BM solar cells to attain a higher power conversion efficiency.
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| 23. |
- Sun, Huiliang, et al.
(författare)
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Reducing energy loss via tuning energy levels of polymer acceptors for efficient all-polymer solar cells
- 2020
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Ingår i: Science China Chemistry. - : Springer Science and Business Media LLC. - 1869-1870 .- 1674-7291. ; 63:12, s. 1785-1792
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Tidskriftsartikel (refereegranskat)abstract
- The open-circuit voltage (Voc) of all-polymer solar cells (all-PSCs) is typically lower than 0.9 V even for the most efficient ones. Large energy loss is the main reason for limiting Voc and efficiency of all-PSCs. Herein, through materials design using electron deficient building blocks based on bithiophene imides, the lowest unoccupied molecular orbital (LUMO) energy levels of polymer acceptors can be effectively tuned, which resulted in a reduced energy loss induced by charge generation and recombination loss due to the suppressed charge-transfer (CT) state absorption. Despite a negligible driving force, all-PSC based on the polymer donor and acceptor combination with well-aligned energy levels exhibited efficient charge transfer and achieved an external quantum efficiency over 10% while maintaining a large Voc of 1.02 V, leading to a 9.21% efficiency. Through various spectroscopy approaches, this work sheds light on the mechanism of energy loss in all-PSCs, which paves an avenue to achieving efficient all-PSCs with large Voc and drives the further development of all-PSCs.
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| 24. |
- Sun, Huiliang, et al.
(författare)
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Reducing energy lossviatuning energy levels of polymer acceptors for efficient all-polymer solar cells
- 2020
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Ingår i: Science China Chemistry. - : Science China Press and Springer-Verlag GmbH Germany. - 1674-7291 .- 1869-1870. ; 63, s. 1785-1792
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Tidskriftsartikel (refereegranskat)abstract
- The open-circuit voltage (V-oc) of all-polymer solar cells (all-PSCs) is typically lower than 0.9 V even for the most efficient ones. Large energy loss is the main reason for limitingV(oc)and efficiency of all-PSCs. Herein, through materials design using electron deficient building blocks based on bithiophene imides, the lowest unoccupied molecular orbital (LUMO) energy levels of polymer acceptors can be effectively tuned, which resulted in a reduced energy loss induced by charge generation and recombination loss due to the suppressed charge-transfer (CT) state absorption. Despite a negligible driving force, all-PSC based on the polymer donor and acceptor combination with well-aligned energy levels exhibited efficient charge transfer and achieved an external quantum efficiency over 10% while maintaining a largeV(oc)of 1.02 V, leading to a 9.21% efficiency. Through various spectroscopy approaches, this work sheds light on the mechanism of energy loss in all-PSCs, which paves an avenue to achieving efficient all-PSCs with largeV(oc)and drives the further development of all-PSCs.
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| 25. |
- Tang, Yingying, et al.
(författare)
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Photodetector Based on Spontaneously Grown Strongly Coupled MAPbBr3/N-rGO Hybrids Showing Enhanced Performance
- 2020
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Ingår i: ACS Applied Materials and Interfaces. - : American Chemical Society (ACS). - 1944-8244 .- 1944-8252. ; 12:1, s. 858-867
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Tidskriftsartikel (refereegranskat)abstract
- Recently, metal-halide perovskites have emerged as a candidate for optoelectronic applications such as photodetectors. However, the poor device performance and instability have limited their future commercialization. Herein, we report the spontaneous growth of perovskite/N-rGO hybrid structures using a facile solution method and their applications for photodetectors. In the hybrid structures, perovskites were homogeneously wrapped by N-rGO sheets through strong hydrogen bonding. The strongly coupled N-rGOs facilitate the charge carrier transportation across the perovskite crystals but also distort the surface lattice of the perovskite creating a potential barrier for charge transfer. We optimize the addition of N-rGO in the hybrid structures to balance interfacial structural distortion and the intercrystal conductivity. High-performance photodetection up to 3 × 104 A/W, external quantum efficiency exceeding 105%, and detectivity up to 1012 Jones were achieved in the optimal device with the weight ratio between perovskites and N-rGO to be 8:1.5. The underlying mechanism behind the optimal N-rGO addition ratio in the hybrids has also been rationalized via time-resolved spectroscopic studies as a reference for future applications.
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