| 1. |
- Chen, Xian-Kai, et al.
(författare)
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A unified description of non-radiative voltage losses in organic solar cells
- 2021
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Ingår i: Nature Energy. - : Springer Nature. - 2058-7546. ; 6:8, s. 799-806
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Tidskriftsartikel (refereegranskat)abstract
- Organic solar cells based on non-fullerene acceptors have enabled high efficiencies yet their charge dynamics and its impact on the photovoltaic parameters are not fully understood. Now, Chen et al. provide a general description of non-radiative voltage losses in both fullerene and non-fullerene solar cells. Recent advances in organic solar cells based on non-fullerene acceptors (NFAs) come with reduced non-radiative voltage losses (Delta V-nr). Here we show that, in contrast to the energy-gap-law dependence observed in conventional donor:fullerene blends, the Delta V-nr values in state-of-the-art donor:NFA organic solar cells show no correlation with the energies of charge-transfer electronic states at donor:acceptor interfaces. By combining temperature-dependent electroluminescence experiments and dynamic vibronic simulations, we provide a unified description of Delta V-nr for both fullerene- and NFA-based devices. We highlight the critical role that the thermal population of local exciton states plays in low-Delta V-nr systems. An important finding is that the photoluminescence yield of the pristine materials defines the lower limit of Delta V-nr. We also demonstrate that the reduction in Delta V-nr (for example, <0.2 V) can be obtained without sacrificing charge generation efficiency. Our work suggests designing donor and acceptor materials with high luminescence efficiency and complementary optical absorption bands extending into the near-infrared region.
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| 2. |
- Crispin, Xavier, 1968-, et al.
(författare)
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Local density functional study of copper clusters: A comparison between real clusters, model surface clusters, and the actual metal surface
- 1999
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Ingår i: European Journal of Inorganic Chemistry. - : Wiley-VCH Verlag Berlin. - 1434-1948 .- 1099-1948. ; :2, s. 349-360
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Tidskriftsartikel (refereegranskat)abstract
- Density Functional Theory is used to study the influence of the size of copper clusters modeling the Cu(100) surface, on the electronic properties: ionization potential, electron affinity, electronic chemical potential, and chemical hardness. The model clusters are chosen to have a bilayer structure and range in size from 9 to 20 copper atoms. The chemical hardness being identified as the relaxation energy of the frontier levels when an electron is removed or added to the system, a simple expression is proposed to estimate its value from the eigenenergies of the frontier levels in neutral and partially ionized systems. A detailed comparison of the geometric and electronic structures is made between the model surface copper clusters, real copper clusters, and the actual metal surface; it is seen that the model surface clusters provide an easy extrapolation to the properties of the metal surface.
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| 3. |
- He, Chengliang, et al.
(författare)
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Asymmetric electron acceptor enables highly luminescent organic solar cells with certified efficiency over 18%
- 2022
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Ingår i: Nature Communications. - : NATURE PORTFOLIO. - 2041-1723. ; 13:1
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Tidskriftsartikel (refereegranskat)abstract
- Enhancing the luminescence property without sacrificing the charge collection is one key to high-performance organic solar cells (OSCs), while limited by the severe non-radiative charge recombination. Here, we demonstrate efficient OSCs with high luminescence via the design and synthesis of an asymmetric non-fullerene acceptor, BO-5Cl. Blending BO-5Cl with the PM6 donor leads to a record-high electroluminescence external quantum efficiency of 0.1%, which results in a low non-radiative voltage loss of 0.178 eV and a power conversion efficiency (PCE) over 15%. Importantly, incorporating BO-5Cl as the third component into a widely-studied donor:acceptor (D:A) blend, PM6:BO-4Cl, allows device displaying a high certified PCE of 18.2%. Our joint experimental and theoretical studies unveil that more diverse D:A interfacial conformations formed by asymmetric acceptor induce optimized blend interfacial energetics, which contributes to the improved device performance via balancing charge generation and recombination. High-performance organic solar cells call for novel designs of acceptor molecules. Here, He et al. design and synthesize a non-fullerene acceptor with an asymmetric structure for diverse donor:acceptor interfacial conformations and report a certificated power conversion efficiency of 18.2%.
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| 4. |
- Knippenberg, Stefan, et al.
(författare)
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Benchmarking Post-Hartree-Fock Methods To Describe the Nonlinear Optical Properties of Polymethines : An Investigation of the Accuracy of Algebraic Diagrammatic Construction (ADC) Approaches
- 2016
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Ingår i: Journal of Chemical Theory and Computation. - : American Chemical Society. - 1549-9618 .- 1549-9626. ; 12:11, s. 5465-5476
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Tidskriftsartikel (refereegranskat)abstract
- Third-order nonlinear optical (NLO) properties of polymethine dyes have been widely studied for applications such as all-optical switching. However, the limited accuracy of the current computational methodologies has prevented a comprehensive understanding of the nature of the lowest excited states and their influence on the molecular optical and NLO properties. Here, attention is paid to the lowest excited-state energies and their energetic ratio, as these characteristics impact the figure-of-merit for all-optical switching. For a series of model polymethines, we compare several algebraic diagrammatic construction (ADC) schemes for the polarization propagator with approximate second-order coupled cluster (CC2) theory, the widely used INDO/MRDCI approach and the symmetry adapted cluster configuration interaction (SAC-CI) algorithm incorporating singles and doubles linked excitation operators (SAC-CI SD-R). We focus in particular on the ground-to-excited state transition dipole moments and the corresponding state dipole moments, since these quantities are found to be of utmost importance for an effective description of the third-order polarizability gamma and two-photon absorption spectra. A sum-overstates expression has been used, which is, found to quickly converge. While ADC(3/2) has been found to be the most appropriate method to calculate these properties, CC2 performs poorly.
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| 5. |
- Qian, Deping, et al.
(författare)
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Correlating the Hybridization of Local-Exciton and Charge-Transfer States with Charge Generation in Organic Solar Cells
- 2023
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Ingår i: Advanced Energy Materials. - : WILEY-V C H VERLAG GMBH. - 1614-6832 .- 1614-6840. ; 13
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Tidskriftsartikel (refereegranskat)abstract
- In organic solar cells with very small energetic-offset (& UDelta;ELE - CT), the charge-transfer (CT) and local-exciton (LE) states strongly interact via electronic hybridization and thermal population effects, suppressing the non-radiative recombination. Here, we investigated the impact of these effects on charge generation and recombination. In the blends of PTO2:C8IC and PTO2:Y6 with very small, ultra-fast CT state formation was observed, and assigned to direct photoexcitation resulting from strong hybridization of the LE and CT states (i.e., LE-CT intermixed states). These states in turn accelerate the recombination of both CT and charge separated (CS) states. Moreover, they can be significantly weakened by an external-electric field, which enhanced the yield of CT and CS states but attenuated the emission of the device. This study highlights that excessive LE-CT hybridization due to very low , whilst enabling direct and ultrafast charge transfer and increasing the proportion of radiative versus non-radiative recombination rates, comes at the expense of accelerating recombination losses competing with exciton-to-charge conversion process, resulting in a loss of photocurrent generation.
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| 6. |
- Qian, Deping, et al.
(författare)
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Design rules for minimizing voltage losses in high-efficiency organic solar cells
- 2018
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Ingår i: Nature Materials. - : NATURE PUBLISHING GROUP. - 1476-1122 .- 1476-4660. ; 17:8, s. 703-
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Tidskriftsartikel (refereegranskat)abstract
- The open-circuit voltage of organic solar cells is usually lower than the values achieved in inorganic or perovskite photovoltaic devices with comparable bandgaps. Energy losses during charge separation at the donor-acceptor interface and non-radiative recombination are among the main causes of such voltage losses. Here we combine spectroscopic and quantum-chemistry approaches to identify key rules for minimizing voltage losses: (1) a low energy offset between donor and acceptor molecular states and (2) high photoluminescence yield of the low-gap material in the blend. Following these rules, we present a range of existing and new donor-acceptor systems that combine efficient photocurrent generation with electroluminescence yield up to 0.03%, leading to non-radiative voltage losses as small as 0.21 V. This study provides a rationale to explain and further improve the performance of recently demonstrated high-open-circuit-voltage organic solar cells.
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| 7. |
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| 8. |
- Wan, Li, et al.
(författare)
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Sensitive near-infrared circularly polarized light detection via non-fullerene acceptor blends
- 2023
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Ingår i: Nature Photonics. - : NATURE PORTFOLIO. - 1749-4885 .- 1749-4893. ; 17:8, s. 649-655
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Tidskriftsartikel (refereegranskat)abstract
- Circularly polarized light (CPL) is widely used for various applications in sensing and imaging(1-3). An ongoing challenge is to realize high-quality CPL detection using chiral organic semiconductors, especially in the near-infrared (NIR) region(4). Chiral molecules tend to rely on twisted stereogenic moieties; however, conventional approaches to reduce the bandgap of organic semiconductors are based on the use of co-planar backbones that commonly lead to molecular symmetries preventing chirality. Here we report a widely applicable strategy to directly induce chiroptical activity in planar non-fullerene acceptors(5-7), which are widely used for high-performance organic photovoltaics and provide a wealth of opportunities to fill the spectral gap of CPL detection in the NIR regime. We demonstrate proof-of-concept circularly polarized organic photodiodes using chiroptically active non-fullerene acceptor blends, which exhibit strong circular dichroism and hence great sensitivity to CPL in the NIR region. Importantly, this strategy is found to be effective in a wide series of state-of-the-art non-fullerene acceptor families including ITIC5, o-IDTBR6 and Y6 analogues(7), which substantially broadens the range of materials applicable to NIR CPL detection.
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| 9. |
- 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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| 10. |
- Zhang, Tiankai, et al.
(författare)
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Ion-modulated radical doping of spiro-OMeTAD for more efficient and stable perovskite solar cells
- 2022
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Ingår i: Science. - : AMER ASSOC ADVANCEMENT SCIENCE. - 0036-8075 .- 1095-9203. ; 377:6605, s. 495-501
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Tidskriftsartikel (refereegranskat)abstract
- Record power conversion efficiencies (PCEs) of perovskite solar cells (PSCs) have been obtained with the organic hole transporter 2,2,7,7-tetrakis(N,N-di-p-methoxyphenyl-amine)9,9-spirobifluorene (spiro-OMeTAD). Conventional doping of spiro-OMeTAD with hygroscopic lithium salts and volatile 4-tert-butylpyridine is a time-consuming process and also leads to poor device stability. We developed a new doping strategy for spiro-OMeTAD that avoids post-oxidation by using stable organic radicals as the dopant and ionic salts as the doping modulator (referred to as ion-modulated radical doping). We achieved PCEs of >25% and much-improved device stability under harsh conditions. The radicals provide hole polarons that instantly increase the conductivity and work function (WF), and ionic salts further modulate the WF by affecting the energetics of the hole polarons. This organic semiconductor doping strategy, which decouples conductivity and WF tunability, could inspire further optimization in other optoelectronic devices.
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