| 1. |
- Yao, Nannan, et al.
(författare)
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Efficient Charge Transport Enables High Efficiency in Dilute Donor Organic Solar Cells
- 2021
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Ingår i: The Journal of Physical Chemistry Letters. - : American Chemical Society. - 1948-7185. ; 12:20, s. 5039-5044
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Tidskriftsartikel (refereegranskat)abstract
- The donor/acceptor weight ratio is crucial for photovoltaic performance of organic solar cells (OSCs). Here, we systematically investigate the photovoltaic behaviors of PM6:Y6 solar cells with different stoichiometries. It is found that the photovoltaic performance is tolerant to PM6 contents ranging from 10 to 60 wt %. Especially an impressive efficiency over 10% has been achieved in dilute donor solar cells with 10 wt % PM6 enabled by efficient charge generation, electron/ hole transport, slow charge recombination, and field-insensitive extraction. This raises the question about the origin of efficient hole transport in such dilute donor structure. By investigating hole mobilities of PM6 diluted in Y6 and insulators, we find that effective hole transport pathway is mainly through PM6 phase in PM6:Y6 blends despite with low PM6 content. The results indicate that a low fraction of polymer donors combines with near-infrared nonfullerene acceptors could achieve high photovoltaic performance, which might be a candidate for semitransparent windows.
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| 2. |
- You, Xiaohu, et al.
(författare)
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Towards 6G wireless communication networks: vision, enabling technologies, and new paradigm shifts
- 2021
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Ingår i: Science China Information Sciences. - : Science Press. - 1674-733X .- 1869-1919. ; 64:1
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Forskningsöversikt (refereegranskat)abstract
- The fifth generation (5G) wireless communication networks are being deployed worldwide from 2020 and more capabilities are in the process of being standardized, such as mass connectivity, ultra-reliability, and guaranteed low latency. However, 5G will not meet all requirements of the future in 2030 and beyond, and sixth generation (6G) wireless communication networks are expected to provide global coverage, enhanced spectral/energy/cost efficiency, better intelligence level and security, etc. To meet these requirements, 6G networks will rely on new enabling technologies, i.e., air interface and transmission technologies and novel network architecture, such as waveform design, multiple access, channel coding schemes, multi-antenna technologies, network slicing, cell-free architecture, and cloud/fog/edge computing. Our vision on 6G is that it will have four new paradigm shifts. First, to satisfy the requirement of global coverage, 6G will not be limited to terrestrial communication networks, which will need to be complemented with non-terrestrial networks such as satellite and unmanned aerial vehicle (UAV) communication networks, thus achieving a space-air-ground-sea integrated communication network. Second, all spectra will be fully explored to further increase data rates and connection density, including the sub-6 GHz, millimeter wave (mmWave), terahertz (THz), and optical frequency bands. Third, facing the big datasets generated by the use of extremely heterogeneous networks, diverse communication scenarios, large numbers of antennas, wide bandwidths, and new service requirements, 6G networks will enable a new range of smart applications with the aid of artificial intelligence (AI) and big data technologies. Fourth, network security will have to be strengthened when developing 6G networks. This article provides a comprehensive survey of recent advances and future trends in these four aspects. Clearly, 6G with additional technical requirements beyond those of 5G will enable faster and further communications to the extent that the boundary between physical and cyber worlds disappears.
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| 3. |
- Zhang, Jianyun, et al.
(författare)
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Revealing the Critical Role of the HOMO Alignment on Maximizing Current Extraction and Suppressing Energy Loss in Organic Solar Cells
- 2019
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Ingår i: iScience. - : Cell Press. - 2589-0042. ; 19, s. 883-893
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Tidskriftsartikel (refereegranskat)abstract
- For state-of-the-art organic solar cells (OSCs) consisting of a large-bandgap polymer donor and a near-infrared (NIR) molecular acceptor, the control of the HOMO offset is the key to simultaneously achieve small energy loss (Eloss) and high photocurrent. However, the relationship between HOMO offsets and the efficiency for hole separation is quite elusive so far, which requires a comprehensive understanding on how small the driving force can effectively perform the charge separation while obtaining a high photovoltage to ensure high OSC performance. By designing a new family of ZITI-X NIR acceptors (X = S, C, N) with a high structural similarity and matching them with polymer donor J71 forming reduced HOMO offsets, we systematically investigated and established the relationship among the photovoltaic performance, energy loss, and hole-transfer kinetics. We achieved the highest PCEavgs of 14.05 ± 0.21% in a ternary system (J71:ZITI-C:ZITI-N) that best optimize the balance between driving force and energy loss.
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| 4. |
- Chen, Desui, et al.
(författare)
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Shelf-Stable Quantum-Dot Light-Emitting Diodes with High Operational Performance
- 2020
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Ingår i: Advanced Materials. - : Wiley-VCH Verlagsgesellschaft. - 0935-9648 .- 1521-4095. ; 32
-
Tidskriftsartikel (refereegranskat)abstract
- Quantum-dot light-emitting diodes (QLEDs) promise a new generation of high-performance, large-area, and cost-effective electroluminescent devices for both display and solid-state lighting technologies. However, a positive ageing process is generally required to improve device performance for state-of-the-art QLEDs. Here, it is revealed that the in situ reactions induced by organic acids in the commonly used encapsulation acrylic resin lead to positive ageing and, most importantly, the progression of in situ reactions inevitably results in negative ageing, i.e., deterioration of device performance after long-term shelf storage. In-depth mechanism studies focusing on the correlations between the in situ chemical reactions and the shelf-ageing behaviors of QLEDs inspire the design of an electron-transporting bilayer, which delivers both improved electrical conductivity and suppressed interfacial exciton quenching. This material innovation enables red QLEDs exhibiting neglectable changes of external quantum efficiency (>20.0%) and ultralong operational lifetime (T-95: 5500 h at 1000 nits) after storage for 180 days. This work provides design principles for oxide electron-transporting layers to realize shelf-stable and high-operational-performance QLEDs, representing a new starting point for both fundamental studies and practical applications.
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| 5. |
- Hao, Zhengming, et al.
(författare)
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Converting n-Alkanol to Conjugated Polyenal on Cu(110) Surface at Mild Temperature
- 2022
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Ingår i: The Journal of Physical Chemistry Letters. - : AMER CHEMICAL SOC. - 1948-7185. ; 13:14, s. 3276-3282
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Tidskriftsartikel (refereegranskat)abstract
- Achieving C(sp(3))-H activation at a mild temperature is of great importance from both scientific and technologic points of view. Herein, on the basis of the on-surface synthesis strategy, we report the significant reduction of the C(sp(3))-H activation barrier, which results in the full C(sp(3))-H to C(sp(2))-H transformation of n-alkanol (octacosan-1-ol) at a mild temperature as low as 350 K on the Cu(110) surface, yielding the conjugated polyenal (octacosa-tridecaenal) as the final product. The reaction mechanism is revealed by the combined scanning tunneling microscope, density functional theory, and synchrotron radiation photoemission spectroscopy.
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| 6. |
- Hao, Zhengming, et al.
(författare)
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From n-alkane to polyacetylene on Cu (110): Linkage modulation in chain growth
- 2022
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Ingår i: Science in China Series B. - : SCIENCE PRESS. - 1674-7291 .- 1869-1870. ; 65:4, s. 733-739
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Tidskriftsartikel (refereegranskat)abstract
- Direct coupling or transformation of inert alkanes based on the selective C-H activation is of great importance for both chemistry and chemical engineering. Here, we report the coupling of polyenes that are transformed from n-dotriacontane (n-C32H66) through on-surface cascade dehydrogenation on Cu (110) surface, leading to the formation of polyacetylene (PA). Three distinct linkages have been resolved by scanning tunneling microscope (STM) and noncontact atomic force microscope (nc-AFM). Apart from the alpha-type linkage which is the stemless coupling of the terminal C-C double bond in trans-configuration, beta- and gamma-type linkages appear as knots or defects which are, in fact, the C-C couplings in cis-configurations. Interestingly, the "defects" can be effectively suppressed by adjusting the surface coverage, thus making it of general interest for uniform structure modulation.
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| 7. |
- Li, Qing, et al.
(författare)
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Hierarchical Dehydrogenation Reactions on a Copper Surface
- 2018
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Ingår i: Journal of the American Chemical Society. - : AMER CHEMICAL SOC. - 0002-7863 .- 1520-5126. ; 140:19, s. 6076-6082
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Tidskriftsartikel (refereegranskat)abstract
- Hierarchical control of chemical reactions is being considered as one of the most ambitious and challenging topics in modern organic chemistry. In this study, we have realized the one-by-one scission of the X-H bonds (X = N and C) of aromatic amines in a controlled fashion on the Cu(lll) surface. Each dehydrogenation reaction leads to certain metal-organic supramolecular structures, which were monitored in single-bond resolution via scanning tunneling microscopy and noncontact atomic force microscopy. Moreover, the reaction pathways were elucidated from X-ray photoelectron spectroscopy measurements and density functional theory calculations. Our insights pave the way for connecting molecules into complex structures in a more reliable and predictable manner, utilizing carefully tuned stepwise on-surface synthesis protocols.
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| 8. |
- Li, Xuechao, et al.
(författare)
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Direct transformation of n-alkane into all-trans conjugated polyene via cascade dehydrogenation
- 2021
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Ingår i: National Science Review. - : Oxford University Press. - 2095-5138 .- 2053-714X. ; 8:10
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Tidskriftsartikel (refereegranskat)abstract
- Selective C(sp(3))-H activation is of fundamental importance in processing alkane feedstocks to produce high-value-added chemical products. By virtue of an on-surface synthesis strategy, we report selective cascade dehydrogenation of n-alkane molecules under surface constraints, which yields monodispersed all-trans conjugated polyenes with unprecedented length controllability. We are also able to demonstrate the generality of this concept for alkyl-substituted molecules with programmable lengths and diverse functionalities, and more importantly its promising potential in molecular wiring.
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| 9. |
- Wang, Lina, et al.
(författare)
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Tailoring Alkane Uniaxial Self-Assembly via Polymer Modified Step Edges
- 2019
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Ingår i: The Journal of Physical Chemistry C. - : AMER CHEMICAL SOC. - 1932-7447 .- 1932-7455. ; 123:47, s. 28811-28815
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Tidskriftsartikel (refereegranskat)abstract
- Controlling the orientations of molecules in self-assembled monolayers on surfaces is an effective means to construct high quality organic devices. Herein, we utilize linear polymer-modified step edges as a simple and peculiar template for regulating the subsequent self-assembly of alkane molecules (n-C32H66). With this strategy, all the alkane molecules orientate along the step edge ([011] directions). Combining with systematical DFT calculations, we demonstrated that it is the van der Waals interactions between the molecules that leads to (1) the initially adsorbed alkane monomers lie parallel to the polymers; (2) the adjacent alkane molecules show a parallel configuration. Since the polymers anchor on the surface along an exclusive [011] direction, all the adsorbed molecules in the self-assembly islands are regulated along the [011] directions as well.
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| 10. |
- Xia, Xinxin, et al.
(författare)
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Revealing the crystalline packing structure of Y6 in the active layer of organic solar cells: the critical role of solvent additives
- 2023
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Ingår i: Journal of Materials Chemistry A. - : ROYAL SOC CHEMISTRY. - 2050-7488 .- 2050-7496. ; 11:40, s. 21895-21907
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Tidskriftsartikel (refereegranskat)abstract
- The bulk heterojunction (BHJ) morphology of photovoltaic materials is crucial to the fundamental optoelectronic properties of organic solar cells (OSCs). However, in the photoactive layer, the intrinsic crystalline packing structure of Y6, currently the hallmark molecule among Y-series non-fullerene acceptors (NFAs), has not been unambiguously determined. Here, employing grazing-incidence wide-angle X-ray scattering (GIWAXS), we managed to uncover the intrinsic crystalline packing structure of Y6 in the BHJ active layer of OSCs, which is found to be different from its single-crystal structure reported previously. Moreover, we find that solvent additive 1-chloronaphthalene (CN) can induce highly ordered packing of Y6 in BHJ thin films. With the help of atomistic molecular dynamics simulations, it is revealed that pi-pi interactions generally exist between naphthalene derivatives and IC terminals of Y6 analogues, which would essentially improve their long-range ordering. Our work reveals the intrinsic crystalline packing structure of Y6 in the BHJ active layer as well as its crystallization mechanism in thin films, thus providing direct correlations between this crystalline packing and the device characteristics and photophysical properties.
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| 11. |
- Xiong, Shaobing, et al.
(författare)
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Reducing nonradiative recombination for highly efficient inverted perovskite solar cells via a synergistic bimolecular interface
- 2024
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Ingår i: Nature Communications. - : NATURE PORTFOLIO. - 2041-1723. ; 15:1
-
Tidskriftsartikel (refereegranskat)abstract
- Reducing interface nonradiative recombination is important for realizing highly efficient perovskite solar cells. In this work, we develop a synergistic bimolecular interlayer (SBI) strategy via 4-methoxyphenylphosphonic acid (MPA) and 2-phenylethylammonium iodide (PEAI) to functionalize the perovskite interface. MPA induces an in-situ chemical reaction at the perovskite surface via forming strong P-O-Pb covalent bonds that diminish the surface defect density and upshift the surface Fermi level. PEAI further creates an additional negative surface dipole so that a more n-type perovskite surface is constructed, which enhances electron extraction at the top interface. With this cooperative surface treatment, we greatly minimize interface nonradiative recombination through both enhanced defect passivation and improved energetics. The resulting p-i-n device achieves a stabilized power conversion efficiency of 25.53% and one of the smallest nonradiative recombination induced Voc loss of only 59 mV reported to date. We also obtain a certified efficiency of 25.05%. This work sheds light on the synergistic interface engineering for further improvement of perovskite solar cells. Reducing interface nonradiative recombination is important for realizing highly efficient perovskite solar cells. Here, the authors employ a bimolecular interlayer to functionalize the perovskite interface, achieving cooperative surface treatment and certified power conversion efficiency of 25.05%.
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| 12. |
- Yang, Biao, et al.
(författare)
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Abiotic Formation of an Amide Bond via Surface-Supported Direct Carboxyl-Amine Coupling
- 2022
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Ingår i: Angewandte Chemie International Edition. - : WILEY-V C H VERLAG GMBH. - 1433-7851 .- 1521-3773. ; 61:5
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Tidskriftsartikel (refereegranskat)abstract
- Amide bond formation is one of the most important reactions in biochemistry, notably being of crucial importance for the origin of life. Herein, we combine scanning tunneling microscopy and X-ray photoelectron spectroscopy studies to provide evidence for thermally activated abiotic formation of amide bonds between adsorbed precursors through direct carboxyl-amine coupling under ultrahigh-vacuum conditions by means of on-surface synthesis. Complementary insights from temperature-programmed desorption measurements and density functional theory calculations reveal the competition between cross-coupling amide formation and decarboxylation reactions on the Au(111) surface. Furthermore, we demonstrate the critical influence of the employed metal support: whereas on Au(111) the coupling readily occurs, different reaction scenarios prevail on Ag(111) and Cu(111). The systematic experiments signal that archetypical bio-related molecules can be abiotically synthesized in clean environments without water or oxygen.
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| 13. |
- Yang, Biao, et al.
(författare)
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Synthesis of Surface Covalent Organic Frameworks via Dimerization and Cyclotrimerization of Acetyls
- 2015
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Ingår i: Journal of the American Chemical Society. - : American Chemical Society. - 0002-7863 .- 1520-5126. ; 137:15, s. 4904-4907
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Tidskriftsartikel (refereegranskat)abstract
- The formation of additional phenyl rings on surfaces is of particular interest because it allows for the building-up of surface covalent organic frameworks. In this work, we show for the first time that the cyclotrimerization of acetyls to aromatics provides a promising approach to 2D conjugated covalent networks on surfaces under ultrahigh vacuum. With the aid of scanning tunneling microscopy, we have systematically studied the reaction pathways and the products. With the combination of density functional theory calculations and X-ray photoemission spectroscopy, the surface-assisted reaction mechanism, which is different from that in solution, was explored.
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| 14. |
- Zhou, Zichun, et al.
(författare)
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Subtle Molecular Tailoring Induces Significant Morphology Optimization Enabling over 16% Efficiency Organic Solar Cells with Efficient Charge Generation
- 2020
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Ingår i: Advanced Materials. - : WILEY-V C H VERLAG GMBH. - 0935-9648 .- 1521-4095. ; 32:4
-
Tidskriftsartikel (refereegranskat)abstract
- Manipulating charge generation in a broad spectral region has proved to be crucial for nonfullerene-electron-acceptor-based organic solar cells (OSCs). 16.64% high efficiency binary OSCs are achieved through the use of a novel electron acceptor AQx-2 with quinoxaline-containing fused core and PBDB-TF as donor. The significant increase in photovoltaic performance of AQx-2 based devices is obtained merely by a subtle tailoring in molecular structure of its analogue AQx-1. Combining the detailed morphology and transient absorption spectroscopy analyses, a good structure-morphology-property relationship is established. The stronger pi-pi interaction results in efficient electron hopping and balanced electron and hole mobilities attributed to good charge transport. Moreover, the reduced phase separation morphology of AQx-2-based bulk heterojunction blend boosts hole transfer and suppresses geminate recombination. Such success in molecule design and precise morphology optimization may lead to next-generation high-performance OSCs.
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| 15. |
- Chen, Hao, et al.
(författare)
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Surface-Directed Structural Transition of Amyloidogenic Aggregates and the Resulting Neurotoxicity
- 2020
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Ingår i: ACS Omega. - : American Chemical Society (ACS). - 2470-1343. ; 5:6, s. 2856-2864
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Tidskriftsartikel (refereegranskat)abstract
- The transition of amyloidogenic species into ordered structures (i.e., prefibrillar oligomers, protofibrils, mature fibrils, and amyloidogenic aggregates) is closely associated with many neurodegenerative disease pathologies. It is increasingly appreciated that the liquid-solid interface contributes to peptide aggregation under physiological conditions. However, much remains to be explored on the molecular mechanism of surface-directed amyloid formation. We herein demonstrate that physical environmental conditions (i.e., negatively charged surface) affect amyloid formation. Nontoxic amyloid aggregates quickly develop into intertwisting fibrils on a negatively charged mica surface. These fibrillar structures show significant cytotoxicity on both neuroblastoma cell-lines (SH-SY5Y) and primary neural stem cells. Our results suggest an alternative amyloid development pathway, following which A beta peptides form large amyloidogenic aggregates upon stimulation, and later transit into neurotoxic fibrillar structures while being trapped and aligned by a negatively charged surface. Conceivably, the interplay between chemical and physical environmental conditions plays important roles in the development of neurodegenerative diseases.
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| 16. |
- He, Chengliang, et al.
(författare)
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Near infrared electron acceptors with a photoresponse beyond 1000 nm for highly efficient organic solar cells
- 2020
-
Ingår i: Journal of Materials Chemistry A. - : ROYAL SOC CHEMISTRY. - 2050-7488 .- 2050-7496. ; 8:35, s. 18154-18161
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Tidskriftsartikel (refereegranskat)abstract
- Developing near infrared (NIR) organic semiconductors is indispensable for promoting the performance of organic solar cells (OSCs), but addressing the trade-off between voltage and current density thus achieving high efficiency with low energy loss is still an urgent challenge. Herein, NIR acceptors (H1, H2 and H3) with a photoresponse beyond 1000 nm were developed by conjugating dithienopyrrolobenzothiadiazole to 2-(5,6-difluoro-3-oxo-2,3-dihydro-1H-inden-1-ylidene)malononitrileviavaried alkyl thiophene bridges. It was found that the linear outward chains in thiophene bridges could mitigate both the conformation disorder of H3 and the electronic disorder of the PBDB-T:H3 blends, which could help to form a favorable blend morphology, facilitating highly efficient photoelectric conversion in the resultant OSCs. As a result, devices based on PBDB-T:H3 achieve a high efficiency of 13.75% with a low energy loss of 0.55 eV, which is one of the highest efficiencies and the lowest energy loss among OSCs with an optoelectronic response near 1000 nm. This work provides a new design strategy towards NIR acceptors for efficient OSCs and future exploration of functional optoelectronics.
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| 17. |
- Li, Shuixing, et al.
(författare)
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Asymmetric Electron Acceptors for High-Efficiency and Low-Energy-Loss Organic Photovoltaics
- 2020
-
Ingår i: Advanced Materials. - : WILEY-V C H VERLAG GMBH. - 0935-9648 .- 1521-4095. ; 32
-
Tidskriftsartikel (refereegranskat)abstract
- Low energy loss and efficient charge separation under small driving forces are the prerequisites for realizing high power conversion efficiency (PCE) in organic photovoltaics (OPVs). Here, a new molecular design of nonfullerene acceptors (NFAs) is proposed to address above two issues simultaneously by introducing asymmetric terminals. Two NFAs, BTP-S1 and BTP-S2, are constructed by introducing halogenated indandione (A(1)) and 3-dicyanomethylene-1-indanone (A(2)) as two different conjugated terminals on the central fused core (D), wherein they share the same backbone as well-known NFA Y6, but at different terminals. Such asymmetric NFAs with A(1)-D-A(2) structure exhibit superior photovoltaic properties when blended with polymer donor PM6. Energy loss analysis reveals that asymmetric molecule BTP-S2 with six chlorine atoms attached at the terminals enables the corresponding devices to give an outstanding electroluminescence quantum efficiency of 2.3 x 10(-2)%, one order of magnitude higher than devices based on symmetric Y6 (4.4 x 10(-3)%), thus significantly lowering the nonradiative loss and energy loss of the corresponding devices. Besides, asymmetric BTP-S1 and BTP-S2 with multiple halogen atoms at the terminals exhibit fast hole transfer to the donor PM6. As a result, OPVs based on the PM6:BTP-S2 blend realize a PCE of 16.37%, higher than that (15.79%) of PM6:Y6-based OPVs. A further optimization of the ternary blend (PM6:Y6:BTP-S2) results in a best PCE of 17.43%, which is among the highest efficiencies for single-junction OPVs. This work provides an effective approach to simultaneously lower the energy loss and promote the charge separation of OPVs by molecular design strategy.
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| 18. |
- Li, Shuixing, et al.
(författare)
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Unveiling structure-performance relationships from multi-scales in non-fullerene organic photovoltaics
- 2021
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Ingår i: Nature Communications. - : Nature Publishing Group. - 2041-1723. ; 12:1
-
Tidskriftsartikel (refereegranskat)abstract
- Unveiling the correlations among molecular structures, morphological characteristics, macroscopic properties and device performances is crucial for developing better photovoltaic materials and achieving higher efficiencies. To achieve this goal, a comprehensive study is performed based on four state-of-the-art non-fullerene acceptors (NFAs), which allows to systematically examine the above-mentioned correlations from different scales. Its found that extending conjugation of NFA shows positive effects on charge separation promotion and non-radiative loss reduction, while asymmetric terminals can maximize benefits from both terminals. Another molecular optimization is from alkyl chain tuning. The shortened alkyl side chain results in strengthened terminal packing and decreased pi-pi distance, which contribute high carrier mobility and finally the high charge collection efficiency. With the most-acquired benefits from molecular structure and macroscopic factors, PM6:BTP-S9-based organic photovoltaics (OPVs) exhibit the optimal efficiency of 17.56% (certified: 17.4%) with a high fill factor of 78.44%, representing the best among asymmetric acceptor based OPVs. This work provides insight into the structure-performance relationships, and paves the way toward high-performance OPVs via molecular design. Understanding correlations between molecular structures and macroscopic properties is critical in realising highly efficient organic photovoltaics. Here, the authors conduct a comprehensive study based on four non-fullerene acceptors revealing how the extended conjugation, asymmetric terminals and alkyl chain length can affect device performance.
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| 19. |
- Li, Xuechao, et al.
(författare)
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Pyridinic Nitrogen Modification for Selective Acetylenic Homocoupling on Au(111)
- 2023
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Ingår i: Journal of the American Chemical Society. - : AMER CHEMICAL SOC. - 0002-7863 .- 1520-5126. ; 145:8, s. 4545-4552
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Tidskriftsartikel (refereegranskat)abstract
- On-surface acetylenic homocoupling has been proposed to construct carbon nanostructures featuring sp hybrid-ization. However, the efficiency of linear acetylenic coupling is far from satisfactory, often resulting in undesired enyne products or cyclotrimerization products due to the lack of strategies to enhance chemical selectivity. Herein, we inspect the acetylenic homocou-pling reaction of polarized terminal alkynes (TAs) on Au(111) with bond-resolved scanning probe microscopy. The replacement of benzene with pyridine moieties significantly prohibits the cyclotrimerization pathway and facilitates the linear coupling to produce well-aligned N-doped graphdiyne nanowires. Combined with density functional theory calculations, we reveal that the pyridinic nitrogen modification substantially differentiates the coupling motifs at the initial C-C coupling stage (head-to-head vs head-to-tail), which is decisive for the preference of linear coupling over cyclotrimerization.
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| 20. |
- Li, Yaokai, et al.
(författare)
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Mechanism study on organic ternary photovoltaics with 18.3% certified efficiency: from molecule to device
- 2022
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Ingår i: Energy & Environmental Science. - : ROYAL SOC CHEMISTRY. - 1754-5692 .- 1754-5706. ; 15:2, s. 855-865
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Tidskriftsartikel (refereegranskat)abstract
- Multi-component organic photovoltaics (OPVs), e.g., ternary blends, are effective for high performance, while the fundamental understanding from the molecular to device level is lacking. To address this issue, we here systematically study the working mechanism of ternary OPVs based on non-fullerene acceptors (NFAs). With both molecular dynamics simulations and morphology characterization, we identify that when adding another larger band gap and highly miscible NFA, namely IT-4F or BTP-S2, into the PBDB-TF:BTP-eC9 blend, the NFAs undergo molecular intermixing selectively with BTP-eC9. This causes the composition-dependent band gap and charge recombination, and hence the composition-dependent V-OC. While the charge recombination still dominantly occurs at the PBDB-TF:BTP-eC9 interface, BTP-S2 or IT-4F plays an auxiliary role in facilitating charge transfer and suppressing non-radiative decay. Interestingly, intermolecular end-group packing in the intermixed blend is improved compared to that in pristine films, leading to higher carrier mobility. These synergistic effects significantly improve the power conversion efficiency of the device to an outstanding value of 18.7% (certified value of 18.3%).
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| 21. |
- Song, Luying, et al.
(författare)
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Synthesis of Two-Dimensional Metal-Organic Frameworks via Dehydrogenation Reactions on a Cu(111) Surface
- 2020
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Ingår i: The Journal of Physical Chemistry C. - : AMER CHEMICAL SOC. - 1932-7447 .- 1932-7455. ; 124:23, s. 12390-12396
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Tidskriftsartikel (refereegranskat)abstract
- Metal-organic frameworks prepared on surfaces (SMOFs) have been considered to have potential applications in various research fields. Traditionally, the SMOFs are prepared by coadsorbing organic ligands and metal atoms on surfaces. In this article, we successfully construct the SMOFs via the dehydrogenation reactions of aromatic amines on the Cu(111) surfaces. The dehydrogenated nitrogen radicals interact with the copper adatoms, forming the N-Cu-N bonds. Combining with the scanning tunneling microscopy and the density functional theory calculations, we obtain the structural models of the SMOFs.
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| 22. |
- Wang, Cheng-Xiang, et al.
(författare)
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On the Road to 6G: Visions, Requirements, Key Technologies, and Testbeds
- 2023
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Ingår i: IEEE Communications Surveys and Tutorials. - : IEEE-INST ELECTRICAL ELECTRONICS ENGINEERS INC. - 1553-877X. ; 25:2, s. 905-974
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Tidskriftsartikel (refereegranskat)abstract
- Fifth generation (5G) mobile communication systems have entered the stage of commercial deployment, providing users with new services, improved user experiences as well as a host of novel opportunities to various industries. However, 5G still faces many challenges. To address these challenges, international industrial, academic, and standards organizations have commenced research on sixth generation (6G) wireless communication systems. A series of white papers and survey papers have been published, which aim to define 6G in terms of requirements, application scenarios, key technologies, etc. Although ITU-R has been working on the 6G vision and it is expected to reach a consensus on what 6G will be by mid-2023, the related global discussions are still wide open and the existing literature has identified numerous open issues. This paper first provides a comprehensive portrayal of the 6G vision, technical requirements, and application scenarios, covering the current common understanding of 6G. Then, a critical appraisal of the 6G network architecture and key technologies is presented. Furthermore, existing testbeds and advanced 6G verification platforms are detailed for the first time. In addition, future research directions and open challenges are identified to stimulate the on-going global debate. Finally, lessons learned to date concerning 6G networks are discussed.
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| 23. |
- Xu, Qiang, et al.
(författare)
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Theoretical prediction, synthesis, and crystal structure determination of new MAX phase compound V2SnC
- 2020
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Ingår i: JOURNAL OF ADVANCED CERAMICS. - : SPRINGER. - 2226-4108 .- 2227-8508. ; 9:4, s. 481-492
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Tidskriftsartikel (refereegranskat)abstract
- Guided by the theoretical prediction, a new MAX phase V2SnC was synthesized experimentally for the first time by reaction of V, Sn, and C mixtures at 1000 degrees C. The chemical composition and crystal structure of this new compound were identified by the cross-check combination of first-principles calculations, X-ray diffraction (XRD), energy dispersive X-ray spectroscopy (EDS), and high resolution scanning transmission electron microscopy (HR-STEM). The stacking sequence of V2C and Sn layers results in a crystal structure of space group P6(3)/mmc. Thea- andc-lattice parameters, which were determined by the Rietveld analysis of powder XRD pattern, are 0.2981(0) nm and 1.3470(6) nm, respectively. The atomic positions are V at 4f (1/3, 2/3, 0.0776(5)), Sn at 2d (2/3, 1/3, 1/4), and C at 2a (0, 0, 0). A new set of XRD data of V2SnC was also obtained. Theoretical calculations suggest that this new compound is stable with negative formation energy and formation enthalpy, satisfied Born-Huang criteria of mechanical stability, and positive phonon branches over the Brillouin zone. It also has low shear deformation resistancec(44)(second-order elastic constant,c(ij)) and shear modulus (G), positive Cauchy pressure, and low Pughs ratio (G/B= 0.500 < 0.571), which is regarded as a quasi-ductile MAX phase. The mechanism underpinning the quasi-ductility is associated with the presence of a metallic bond.
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| 24. |
- Zhong, Qigang, et al.
(författare)
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Substrate-Modulated Synthesis of Metal-Organic Hybrids by Tunable Multiple Aryl-Metal Bonds
- 2022
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Ingår i: Journal of the American Chemical Society. - : AMER CHEMICAL SOC. - 0002-7863 .- 1520-5126. ; 144:18, s. 8214-8222
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Tidskriftsartikel (refereegranskat)abstract
- Assembly of semiconducting organic molecules with multiple aryl-metal covalent bonds into stable one- and two- dimensional (1D and 2D) metal-organic frameworks represents a promising route to the integration of single-molecule electronics in terms of structural robustness and charge transport efficiency. Although various metastable organometallic frameworks have been constructed by the extensive use of single aryl-metal bonds, it remains a great challenge to embed multiple aryl-metal bonds into these structures due to inadequate knowledge of harnessing such complex bonding motifs. Here, we demonstrate the substrate-modulated synthesis of 1D and 2D metal-organic hybrids (MOHs) with the organic building blocks (perylene) interlinked solely with multiple aryl-metal bonds via the stepwise thermal dehalogenation of 3,4,9,10-tetrabromo-1,6,7,12-tetrachloroperylene and subsequent metal-organic connection on metal surfaces. More importantly, the conversion from 1D to 2D MOHs is completely impeded on Au(111) but dominant on Ag(111). We comprehensively study the distinct reaction pathways on the two surfaces by visually tracking the structural evolution of the MOHs with high-resolution scanning tunneling and noncontact atomic force microscopy, supported by first-principles density functional theory calculations. The substrate-dependent structural control of the MOHs is attributed to the variation of the M-X (M = Au, Ag; X = C, Cl) bond strength regulated by the nature of the metal species.
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| 25. |
- Zhou, Jingmin, et al.
(författare)
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Rationale and design of the beta-blocker in heart failure with normal left ventricular ejection fraction (beta-PRESERVE) study.
- 2010
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Ingår i: European journal of heart failure : journal of the Working Group on Heart Failure of the European Society of Cardiology. - : Wiley. - 1879-0844. ; 12:2, s. 181-5
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Tidskriftsartikel (refereegranskat)abstract
- Chronic heart failure with normal left ventricular ejection fraction (HFNEF) is not only common, but also carries a high risk of substantial morbidity and mortality. However, few studies have been conducted in this population and no proven treatment is available. Although beta-blockers are evidence-based first-line therapy in systolic heart failure, they have not been well studied in HFNEF.
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| 26. |
- Zhu, Zhenke, et al.
(författare)
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Microorganisms maintain C:N stoichiometric balance by regulating the priming effect in long-term fertilized soils
- 2021
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Ingår i: Applied Soil Ecology. - : Elsevier BV. - 0929-1393. ; 167
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Tidskriftsartikel (refereegranskat)abstract
- Labile carbon (C) inputs affect the soil carbon:nitrogen (C:N) ratio and microbial stoichiometric homeostasis, which control the intensity and direction of the priming effect (PE). Here, we clarified how soil microorganisms regulate enzyme production and PE to maintain the C:N stoichiometric balance. Specifically, we conducted an incubation experiment by adding 13C-labeled glucose to four long-term fertilized paddy soils: no fertilization; fertilization with mineral nitrogen, phosphorus, and potassium (NPK); NPK combined with straw; and NPK with manure (NPKM). After glucose addition, the dissolved organic carbon-to-ammonium (DOC:NH4+) ratio (24–39) initially increased, but subsequently decreased after day 2 following glucose exhaustion. In parallel, the microbial C:N imbalance [(DOC:NH4+):(microbial biomass C:microbial biomass N)] rapidly decreased from day 2 (4.6–7.2) to day 20 (<0.5). Thus, microorganisms became C limited after 20 days of incubation. Excess C, resulting from glucose addition, increased N-hydrolase (chitinase) production and N mining from soil organic matter (SOM) through positive PEs. However, C hydrolase (β-1,4-glucosidase and β-xylosidase) activity increased, while that of N hydrolase (chitinase) decreased, following glucose exhaustion. Consequently, the C:N microbial biomass ratio increased as the DOC:NH4+ ratio decreased, leading to negative PEs. NPKM-fertilized soil had the largest cumulative PE (2.3% of soil organic carbon) because it had the highest microbial biomass and iron (Fe) reduction rate. Thus, this increased N mining from SOM maintained the microbial C:N stoichiometric balance. We concluded that soil microorganisms regulate C- and N-hydrolase production to control the intensity and direction of PE, maintaining the C:N stoichiometric balance in response to labile C inputs.
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