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Reduced exciton binding energy and diverse molecular stacking enable high-performance organic solar cells with V_(OC)over 1.1 V

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Science China Chemistry 2024年第9期67卷 3140-3152页

作者： Tingting Dai Jiahao Lu Ailing Tang Yuhan Meng Peiqing Cong Zongtao Wang Erjun Zhou National Center for Nanoscience and Technology Beijing 100190China Center of Materials Science and Optoelectronics Engineering University of Chinese Academy of SciencesBeijing 100049China College of Chemistry and Chemical Engineering Guangxi Minzu UniversityNanning 530006China Henan Institute of Advanced Technology Zhengzhou UniversityZhengzhou 450003China

High-voltage organic solar cells(OSCs)have received increasing attention because of their promising applications in tandem devices and indoor photovoltaics,but the trade-off between energy loss and charge generation induced by exciton binding energy(E_(b))has become one of the biggest bottlenecks limiting the development of this ***,a wide bandgap(WBG)nonfullerene acceptor BTA503 with reduced E_(b) is designed by changing the phenyl side chain on the central core of Cl-BTA5 to an alkyl *** diverseπ-πinteractions and enhanced molecular stacking of BTA503 are responsible for its reduced E_(b).Furthermore,both the diminished charge recombination and the fast exciton dissociation caused by the small E_(b) favor the generation of more charge carriers for the PTQ10:BTA503 *** efficient Forster resonance energy transfer(FRET)and multiple π-π stacking patterns provide additional charge transfer and transport ***,the PTQ10:BTA503-based OSC device achieves a V_(OC)of 1.112 V and a PCE of 12.70%,which is higher than that of PTQ10:Cl-BTA5(PCE=10.92%).Simultaneously,the thick film(~300 nm)binary device of PTQ10:BTA503 achieves a PCE of 10.13% with a V_(OC)of 1.102 V,which is the best result for thick film high-voltage *** importantly,the ternary device of PTQ10:BTA503:Cl-BTA5(1:0.9:0.1)realizes a champion PCE of 13.12% with a V_(OC)of 1.126 *** study demonstrates that it is an effective strategy to reduce E_(b) of A_(2)-A_(1)-D-A_(1)-A_(2) type WBG acceptors by modulating the side chains on D unit,which further favors the corresponding devices to obtain world-record PCE and improves their potential for commercial applications.

关键词： exciton binding energy intermolecular interaction wide-bandgap acceptor high V_(OC) organic solar cells

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Thermally-enhanced photo-electric response of an organic semiconductor with low exciton binding energy for simultaneous and distinguishable detection of light and temperature

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Science China Chemistry 2022年第1期65卷 145-152页

作者： Yongxu Hu Li Yu Yinan Huang Zhongwu Wang Shuguang Wang Xiaosong Chen Deyang Ji Huanli Dong Jie Li Yajing Sun Liqiang Li Wenping Hu Tianjin Key Laboratory of Molecular Optoelectronic Sciences Department of ChemistryInstitute of Molecular Aggregation ScienceTianjin UniversityTianjin 300072China Joint School of National University of Singapore and Tianjin University International Campus of Tianjin UniversityFuzhou 350207China Beijing National Laboratory for Molecular Sciences Key Laboratory of Organic SolidsInstitute of ChemistryChinese Academy of SciencesBeijing 100190China

Simultaneous and distinguishable detection of external stimuli such as light and temperature is of great interest for a variety of scientific and industrial ***,an organic semiconductor with low exciton binding energy,low thermal activation energy and good charge transporting property produces thermally enhanced photo-electric response in organic phototransistors(OPTs),which thus provides an ideal and effective way to realize the simultaneous and distinguishable detection of temperature and ***,there is no report on such a kind of organic semiconductor until ***,we designed and synthesized a narrow band gap organic small molecule semiconductor 2,5-bis(2-butyloctyl)-3,6-bis(5-(4-(diphenylamino)phenyl)thiophen-2-yl)-2,5-dihydropyrrolo[3,4-c]pyrrole-1,4-dione(DPP-T-TPA)with low exciton binding energy(about 37 meV)and small activation energy(about 61 meV)for distinct thermal-dependence of charge carrier and *** low exciton binding energy enables the semiconductor to exhibit strong thermal dependence of exciton dissociation,which contributes to the thermally-enhanced photo-electric ***,the low thermal activation energy produces the weak thermal dependence of charge transport,which avoids the disturbance of thermally-modulated charge transport on photo-electric *** from these two features,phototransistors based on DPP-T-TPA show great potential in simultaneous and distinguishable detection of light and temperature,which represents a novel and efficient way for bifunctional detection.

关键词： phototransistor thermally activated photo-electric response exciton binding energy thermal activation energy

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Tuning the exciton binding energy of covalent organic frameworks for efficient photocatalysis

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Chinese Chemical Letters 2024年第2期35卷 577-583页

作者： Zhangjie Gu Zhen Shan Yulan Wang Jinjian Wang Tongtong Liu Xiaoming Li Zhiyang Yu Jian Su Gen Zhang Key Laboratory for Soft Chemistry and Functional Materials of Ministry of Education School of Chemistry and Chemical EngineeringNanjing University of Science and TechnologyNanjing 210094China State Key Laboratory of Photocatalysis on energy and Environment College of ChemistryFuzhou UniversityFuzhou 350002China MIIT Key Laboratory of Advanced Display Material and Devices School of Materials Science and EngineeringNanjing University of Science and TechnologyNanjing 210094China Key Laboratory of Preclinical Study for New Drugs of Gansu Province School of Basic Medical SciencesLanzhou UniversityLanzhou 730000China

Owing to the large exciton binding energy(>100 meV)of most organic materials,the process of exciton dissociation into free electrons and holes is seriously hindered,which plays a key role in the photocatalytic *** this study,a series of chalcogen(S,Se)-substituted mesoporous covalent organic frameworks(COFs)have been synthesized for enhanced photocatalytic organic *** measurements indicate that the introduction of semi-metallic Se atom and the enlargement of conjugation degree can not only reduce the exciton binding energy accelerating the charge separation,but also reduce the band gap of *** a result,the COF-NUST-36 with the lowest exciton binding energy(39.5 meV)shows the highest photocatalytic performance for selective oxidation of amines(up to 98%*** 97.5%Sel.).This work provides a feasible method for designing COFs with high photocatalytic activity by adjusting exciton binding energy.

关键词： Covalent organic frameworks exciton binding energy Atom substitution Extended conjugation Photocatalysis

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Dielectric confinement on exciton binding energy and nonlinear optical properties in a strained Zn_(1-x_(in))Mg_(x(in))Se/Zn_(1-x(out))Mg_(x(out))Se quantum well

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Journal of Semiconductors 2012年第9期33卷 1-7页

作者： J.Abraham Hudson Mark A.John Peter Department of Physics NPR Arts&Science CollegeNathamDindigul-624401India Department of Physics Government Arts CollegeMelur-625106MaduraiIndia

The band offsets for a Zn1-xin Mgxin Se/Zn1-xout Mgxout Se quantum well heterostructure are determined using the model solid theory. The heavy hole exciton binding energies are investigated with various Mg alloy contents. The effect of mismatch between the dielectric constants between the well and the barrier is taken into account. The dependence of the excitonic transition energies on the geometrical confinement and the Mg alloy is discussed. Non-linear optical properties are determined using the compact density matrix approach. The linear, third order non-linear optical absorption coefficient values and the refractive index changes of the exciton are calculated for different concentrations of magnesium. The results show that the occurred blue shifts of the resonant peak due to the Mg incorporation give the information about the variation of two energy levels in the quantum well width.

关键词： interband emission energy exciton binding energy quantum well

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Steric hindrance induced low exciton binding energy enables low-driving-force organic solar cells

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Aggregate 2024年第5期5卷 501-511页

作者： Tianyu Hu Xufan Zheng Ting Wang Aziz Saparbaev Bowen Gao Jingnan Wu Jingyi Xiong Ming Wan Tingting Cong Yuda Li Ergang Wang Xunchang Wang Renqiang Yang Key Laboratory of Optoelectronic Chemical Materials and Devices(Ministry of Education) School of Optoelectronic Materials & TechnologyJianghan UniversityWuhanChina Institute of Ion-Plasma and Laser Technologies National University of UzbekistanTashkentUzbekistan Key Laboratory of Novel Biomass-Based Environmental and energy Materials in Petroleum and Chemical Industry Key Laboratory for Green Process of Ministry of EducationSchool of Chemical Engineering and PharmacyWuhan Institute of TechnologyWuhanChina Department of Chemistry and Chemical Engineering Chalmers University of TechnologyGöteborgSweden

exciton binding energy(E_(b))has been regarded as a critical parameter in charge separation during photovoltaic *** the E_(b) of the photovoltaic materials can facilitate the exciton dissociation in low-driving force organic solar cells(OSCs)and thus improve the power conversion efﬁciency(PCE);nevertheless,diminishing the E_(b) with deliberate design principles remains a signiﬁcant ***,bulky side chain as steric hindrance structure was inserted into Y-series acceptors to minimize the E_(b) by modulating the intra-and intermolecular *** and experimental results indicate that steric hindrance-induced optimal intra-and intermolecular interaction can enhance molecular polarizability,promote electronic orbital overlap between molecules,and facilitate delocalized charge trans-fer pathways,thereby resulting in a low E_(b).The conspicuously reduced E_(b) obtained in Y-ChC5 with pinpoint steric hindrance modulation can minimize the detrimental effects on exciton dissociation in low-driving-force OSCs,achieving a remarkable PCE of 19.1%with over 95%internal quantum efﬁ*** study provides a new molecular design rationale to reduce the E_(b).

关键词： exciton binding energy exciton dissociation organic solar cells steric hindrance

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Polarization engineering in porous organic polymers for charge separation efficiency and its applications in photocatalytic aerobic oxidations

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Science China Chemistry 2024年第3期67卷 1000-1007页

作者： Kun Wu Pei-Wen Cheng Xin-Yi Liu Ji Zheng Xiao-Wei Zhu Mo Xie Puxin Weng Weigang Lu Dan Li College of Chemistry and Materials Science Guangdong Provincial Key Laboratory of Functional Supramolecular Coordination Materials and ApplicationsJinan UniversityGuangzhou 510632China Guangdong Rare Earth Photofunctional Materials Engineering Technology Research Center School of Chemistry and EnvironmentJiaying UniversityMeizhou 514015China

Photocatalytic aerobic oxidation reactions are largely governed by the efficiency of charge separation and subsequent reactive oxygen species(ROS) generation. Herein, we report a polarization engineering strategy to promote the charge separation and ROS generation efficiency by substituting the benzene unit with furan/thiophene in porous organic polymers(POPs). Benefiting from the extent of local polarization, the thiophene-containing POP(JNU-218) exhibits the best photocatalytic performance in aerobic oxidation reactions, with a yield much higher than those for the furan-containing POP(JNU-217) and the benzenecontaining POP(JNU-216). Experimental studies and theoretical calculations reveal that the increase of local polarization can indeed reduce the exciton binding energy, and therefore facilitate the separation of electron-hole pairs. This work demonstrates a viable strategy to tune charge separation and ROS generation efficiency by modulating the dipole moments of the building blocks in porous polymeric organic semiconductors.

关键词： porous organic polymer local polarization photocatalytic aerobic oxidation charge separation reactive oxygen species exciton binding energy

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Temperature-dependent photoluminescent behavior of millimeter-scale Cs_(4)PbBr_(6)/CsPbBr_(3) bulk crystals and their application to white light-emitting diodes

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Journal of Materials Science & Technology 2024年第12期179卷 57-65页

作者： Qi Wang Sirous Khabbaz Abkenar Matilde Cirignano Hailong Yu Wenzhi Wu Giorgio Divitini School of Electronic Engineering Heilongjiang UniversityHarbin 150030China Electron Spectroscopy and Nanoscopy Istituto Italiano di TecnologiaGenova 16163Italy Dipartimento di Chimica e Chimica Industriale Universitàdegli Studi di GenovaGenova 16146Italy Photonic Nanomaterials Istituto Italiano di TecnologiaGenova 16163Italy

The zero-dimensional perovskite composite Cs_(4)PbBr_(6)/CsPbBr_(3) has attracted significant attention for its remarkable photoluminescence(PL),which remains highly effective even in solid *** work presents a detailed analysis of the steady-state and time-resolved PL(TRPL)behavior of millimeter-scale Cs_(4)PbBr_(6)/CsPbBr_(3) crystals over a temperature range of 80 to 360 K,which covers exciton binding en-ergy,phonon energy,and PL peak energy shifting with increasing *** to the results,Cs_(4)PbBr_(6)/CsPbBr_(3) exhibits high exciton binding energy and phonon energy,with calculated values of 358.7 and 94.8 meV,***,when the temperature is below~235 K,thermal expan-sion dominates to influence the TRPL and peak energy,whereas electron-phonon interaction becomes the dominant factor as temperature rises from 235 to 325 *** is found that Cs_(4)PbBr_(6)/CsPbBr_(3) has a PL behavior similar to CsPbBr_(3),and characterization and TRPL results demonstrate that nanometer-scale CsPbBr_(3) crystals embed in the Cs_(4)PbBr_(6) bulk ***,a white light-emitting diode(WLED)device based on Cs_(4)PbBr_(6)/CsPbBr_(3) with luminous efficiency of 64.56 Im/W is fabricated,and its color coordinate is measured as(0.34,0.31)under 20 mA,which is in close proximity to the standard white color ***,the color gamut of the device is measured as 128.66%of the National Televi-sion Systems Committee(NTSC).The WLED electroluminescence(EL)spectra show high Correlated Color Temperature(CCT)stability for the working current varying from 5 to 100 mA,and after continuous oper-ation for 12 h,the EL intensity decreases and stabilizes at~70%of the initial EL *** findings suggest that Cs_(4)PbBr_(6)/CsPbBr_(3) crystals are a promising candidate for WLEDs.

关键词： Zero-dimensional perovskites Photoluminescence exciton binding energy White light-emitting diode

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Strain- and twist-engineered optical absorption of few-layer black phosphorus

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Science China(Physics,Mechanics & Astronomy) 2016年第9期59卷 86-92页

作者： Qian Jia XiangHua Kong JingSi Qiao Wei Ji Department of Physics and Beijing Key Laboratory of Optoelectronic Functional Materials & Micro-Nano Devices Renmin University of China Beijing 100872 China

Density functional and many-body perturbation theories calculations were carried out to investigate fundamental and optical bandgap, exciton binding energy and optical absorption property of normal and strain- and twist-engineered few-layer black phosphorus （BP）. We found that the fundamental bandgaps of few layer BP can be engineered by layer stacking and in-plane strain, with linear relationships to their associated exciton binding energies. The strain-dependent optical absorption behaviors are also anisotropic that the position of the first absorption peak monotonically blue-shifts as the strain applies to either direction for incident light polarized along the armchair direction, but this is not the case for that along the zigzag direction. Given those striking properties, we proposed two prototype devices for building potentially more balanced light absorbers and light filter passes, which promotes further applications and investigations of BP in nanoelectronics and optoelectronics.

关键词： black phosphorus light absorption strain-engineering exciton binding energy

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Fractional-dimensional approach for excitons in Ga As films on AlxGa(1-x)As substrates

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Chinese Physics B 2016年第3期25卷 375-379页

作者：武振华陈蕾田强 School of Physics and Optoelectronic Engineering Xidian University Xi'an 710071 China School of Science Beijing University of Civil Engineering and Architecture Beijing 100044 China Department of Physics Beijing Normal University Beijing 100875 China

binding energies of excitons in GaAs films on AlxGal-xAs substrates are studied theoretically with the fractional- dimensional approach. In this approach, the real anisotropic ＂exciton ＋ film＂ semiconductor system is mapped into an effective fractional-dimensional isotropic space. For different aluminum concentrations and substrate thicknesses, the exci- ton binding energies are obtained as a function of the film thickness. The numerical results show that, for different aluminum concentrations and substrate thicknesses, the exciton binding energies in GaAs films on AlxGal_xAs substrates all exhibit their maxima with increasing film thickness. It is also shown that the binding energies of heavy-hole and light-hole excitons both have their maxima with increasing film thickness.

关键词： exciton binding energy GaAs film fractional-dimensional approach

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Polaronic Effects of an exciton in a Cylindrical Quantum Wire

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Communications in Theoretical Physics 2005年第1期43卷 169-174页

作者： WANGRui-Qiang XIEHong-Jing GUOKang-Xian YUYou-Bin DENGYong-Qing DepartmentofPhysics GuihuagangCampusGuangzhouUniversityGuangzhou510405China

The effects of exciton-optical phonon interaction on the binding energy and the total and reduced effective masses of an exciton in a cylindrical quantum wire have been investigated. We adopt a perturbative-PLL [T.D. Lee,F. Low, and D. Pines, Phys. Rev. B90 (1953) 297] technique to construct an effective Hamiltonian and then use a variational solution to deal with the exciton-phonon system. The interactions of exciton with the longitudinal-optical phonon and the surface-optical phonon have been taken into consideration. The numerical calculations for GaAs show that the influences of phonon modes on the exciton in a quasi-one-dimensional quantum wire are considerable and should not be neglected. Moreover the numerical results for heavy- and light-hole exciton are obtained, which show that the polaronic effects on two types of excitons are very different but both depend heavily on the sizes of the wire.

关键词： exciton binding energy polaronic effect cylindrical quantum wire

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