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exciton diffusion and dissociation in organic and quantum-dot solar cells

SmartMat 2023年第6期4卷 11-30页

作者： Dan He Miao Zeng Zhenzhen Zhang Yang Bai Guichuan Xing Hui-Ming Cheng Yuze Lin Department of Metallurgy and Applied Physical Chemistry College of Chemistry and Chemical EngineeringCentral South UniversityChangshaChina Beijing National Laboratory for Molecular Sciences CAS Key Laboratory of Organic SolidsInstitute of ChemistryChinese Academy of SciencesBeijingChina Faculty of Materials Science and Energy Engineering/Institute of Technology for Carbon Neutrality Shenzhen Institute of Advanced TechnologyChinese Academy of SciencesShenzhenChina Joint Key Laboratory of the Ministry of Education Institute of Applied Physics and Materials EngineeringUniversity of MacaoMacaoChina University of Chinese Academy of Sciences BeijingChina Australian Institute for Bioengineering and Nanotechnology The University of Queensland BrisbaneSt LuciaQueenslandAustralia

For the process of photovoltaic conversion in organic solar cells(OSCs)and quantum-dot solar cells(QDSCs),three of four steps are determined by exciton behavior,namely,exciton generation,exciton diffusion,and exciton dissociation.Therefore,it is of great importance to regulate exciton behavior in OSCs and QDSCs for achieving high power conversion efficiency.Due to the rapid development in materials and device fabrication,great progress has been made to manage the exciton behavior to achieve prolonged exciton diffusion length and improved exciton dissociation in recent years.In this review,we first introduce the parameters that affect exciton behavior,followed by the methods to measure exciton diffusion length.Then,we provide an overview of the recent advances with regard to exciton behavior investigation in OSCs and QDSCs,including exciton lifetime,exciton diffusion coefficient,and exciton dissociation.Finally,we propose future directions in deepening the understanding of exciton behavior and boosting the performance of OSCs and QDSCs.

关键词： exciton behavior exciton diffusion exciton dissociation organic solar cells quantum-dot solar cells

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exciton dissociation dynamics and light-driven H2 generation in colloidal 2D cadmium chalcogenide nanoplatelet heterostructures

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Nano Research 2018年第6期11卷 3031-3049页

作者： Qiuyang Li Tianquan Lian Department of Chemistry Emory University 1515 Dickey Drive NE Atlanta GA 30322 USA

Solar-to-H2 conversion is attracting much research attention as a potential approach to meet global renewable energy demands. Although significant advances have been made using metal-tipped colloidal cadmium chalcogenide zero-dimensional （0D） quantum dots and one-dimensional （1D） nanorod heterostructures in solar-to-H2 conversion, their efficiency may be further enhanced using an emerging class of colloidal cadmium chalcogenide nanocrystals, namely two-dimensional （2D） nanoplatelets （NPLs）, because of their unique properties. In this review, we summarize the recent advances on exciton dissociation dynamics and light-driven H2 generation performance of colloidal nanoplatelet heterostructures. Following an introduction on the electronic structure of 2D NPLs, we discuss the dynamics of exciton dissociation by electron transfer to molecular acceptors. The exciton quenching dynamics of CdS NPL-Pt and CdSe NPL-Pt heterostructures are compared to highlight the effect of material properties on the relative contributions of the energy-transfer and electron- transfer pathways. Representative solar-to-H2 conversion performances of 2D NPL-metal heterostructures are discussed and compared with those of 1D nanorod-metal heterostructures. Finally, we discuss the challenges in further improving the solar-to-fuel conversion efficiencies of these systems.

关键词： colloidal nanoplatelets semiconductor-metal heterostructures exciton dissociation electron transfer hydrogen generation

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Analytical Study on Piezoelectric Effects on exciton dissociation

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Communications in Computational Physics 2016年第6期20卷 179-187页

作者： SeongMin Kim Jaewook Ha Hyeok Kim Jin-Baek Kim The Office of the Theory&Modeling Based Design of Energy Harvesting(private lab) Maetan 3-dongYeongtong-guSuwon-siGyeonggi-do 443-373Korea Department of Chemistry Korea Advanced Institute of Science and TechnologyDaejeon 305-701Korea Photo-Electronic Hybrids Research Center Korea Institute of Science and TechnologySeoul 136-791Korea CAE Platform Technology LabSamsung Advanced Institute of Technology

We analytically and numerically compute the Onsager dissociation rate(exciton dissociation)on an interface induced by a piezoelectric potential in an inorganicorganic hybrid p-n junction system(ZnO+(poly(p-phenylene vinylene));PPV).When a positive piezoelectric potential is created at the interface region owing to the deformation of the system,free electrons accumulate at the interface.Hence,screening effects are observed.It is assumed that the electron layer formed at the interface then attracts free holes from the p-type PPV region,which leads to exciton formation,possibly via the Langevin recombination process.The increased exciton density can then contribute to the Onsager dissociation rate,which is maximum around the interface.This paper focuses on the role of piezoelectric effects in promoting exciton formation at the interface and its relation with the exciton dissociation rate.

关键词： exciton dissociation Onsager rate piezoelectric p-n junction recombination

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配体密度控制促进CsPbBr_(3)量子点激子解离与能量转移实现高效CO_(2)光催化还原

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Science Bulletin 2024年第7期69卷 901-912页

作者：钟丰忆盛剑平杜晨宇何烨孙艳娟董帆 School of Resources and Environment University of Electronic Science and Technology of ChinaChengdu 611731China Research Center for Carbon-Neutral Environmental&Energy Technology Institute of Fundamental and Frontier SciencesUniversity of Electronic Science and Technology of ChinaChengdu 611731China

Perovskite quantum dots(PQDs) hold immense potential as photocatalysts for CO_(2) reduction due to their remarkable quantum properties,which facilitates the generation of multiple excitons,providing the necessary high-energy electrons for CO_(2) photoreduction.However,harnessing multi-excitons in PQDs for superior photocatalysis remains challenging,as achieving the concurrent dissociation of excitons and interparticle energy transfer proves elusive.This study introduces a ligand density-controlled strategy to enhance both exciton dissociation and interparticle energy transfer in CsPbBr_(3) PQDs.Optimized CsPbBr_(3) PQDs with the regulated ligand density exhibit efficient photocatalytic conversion of CO_(2) to CO,achieving a 2.26-fold improvement over unoptimized counterparts while maintaining chemical integrity.Multiple analytical techniques,including Kelvin probe force microscopy,temperaturedependent photoluminescence,femtosecond transient absorption spectroscopy,and density functional theory calculations,collectively affirm that the proper ligand termination promotes the charge separation and the interparticle transfer through ligand-mediated interfacial electron coupling and electronic interactions.This work reveals ligand density-dependent variations in the gas-solid photocatalytic CO_(2) reduction performance of CsPbBr_(3) PQDs,underscoring the importance of ligand engineering for enhancing quantum dot photocatalysis.

关键词： Perovskite quantum dots Ligands Photocatalytic CO_(2)reduction exciton dissociation Electronic coupling

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A simulation study on exciton dissociation in organic photovoltaic cells

A simulation study on exciton dissociation in organic photov...

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第十五届全国化学动力学会议

作者：闫亚明 Linze Song Qiang Shi Beijing National Laboratory for Molecular Sciences State Key Laboratory for Structural Chemistry of Unstable and Stable SpeciesInstitute of ChemistryChinese Academy of Sciences University of Chinese Academy of Sciences

The quite high efficiency of exciton dissociation observed in organic photovoltaic solar cells is a confusing problem because of the high coulomb exciton binding energy in those materials [1-4]. By employing several lattice model systems, we investigate how several important factors affect the charge separation barrier in organic photovoltaic（OPV） cells. The combined effects of external electric field, dimensionality, and charge delocalization are found to reduce the free energy barrier for charge separation significantly. The dynamic disorder reduces charge carrier delocalization and results in increased charge separation barrier, while the effect of static disorder is more complex. It is found that, under a reasonable set of parameters, the charge separation barrier can be reduced to several kBT. The current results also indicate that only a small energy offset between the band gap and the lowest energy charge transfer state is needed to achieve efficient free charge generation in OPV devices. Besides, we also performed quantum dynamic study, which reveal that hot vibronic exciton can fascinate the dissociation process.

关键词： Organic photovoltaic exciton dissociation HEOM IT-PIMC

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Design of ultranarrow-bandgap acceptors for efficient organic photovoltaic cells and highly sensitive organic photodetectors

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Journal of Energy Chemistry 2022年第9期31卷 388-394,I0011页

作者： Ye Xu Tao Zhang Huifeng Yao Jingwen Wang Pengqing Bi Jianhui Hou Beijing National Laboratory for Molecular Sciences State Key Laboratory of Polymer Physics and ChemistryCAS Research/Education Center for Excellence in Molecular SciencesInstitute of ChemistryChinese Academy of SciencesBeijing 100190China School of Chemical Sciences University of Chinese Academy of SciencesBeijing 100049China

The fabrication of multifunctional electronic devices based on the intriguing natures of organic semiconductors is crucial for organic electronics.Ultranarrow-bandgap materials are in urgent demand for fabricating high-performance organic photovoltaic(OPV)cells and highly sensitive near-infrared organic photodetectors(OPDs).By combining alkoxy modification and an asymmetric strategy,three narrowbandgap electronic acceptors(BTP-4F,DO-4F,and QO-4F)were synthesized with finely tuned molecular electrostatic potential(ESP)distributions.Through the careful modulation of electronic configurations,the optical absorption onsets of DO-4F and QO-4F exceeded 1μm.The experimental and theoretical results suggest that the small ESP of QO-4F is beneficial for achieving a low nonradiative voltage loss,while the large ESP of BTP-4F can help obtain high exciton dissociation efficiency.By contrast,the asymmetric acceptor DO-4F with a moderate ESP possesses balanced voltage loss and exciton dissociation,yielding the best power conversion efficiency of 13.6%in the OPV cells.OPDs were also fabricated based on the combination of PBDB-T:DO-4F,and the as-fabricated device outputs a high shot-noise-limited specific detectivity of 3.05×10^(13) Jones at 850 nm,which is a very good result for near-infrared OPDs.This work is anticipated to provide a rational way of designing high-performance ultranarrow-bandgap organic semiconductors by modulating the molecular ESP.

关键词： Ultranarrow-bandgap acceptors Asymmetric design strategies Molecular electrostatic potentials exciton dissociation Non-radiative energy loss

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Understanding the roles of carbon in carbon/g-C_(3)N_(4)based photocatalysts for H2 evolution

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Nano Research 2023年第4期16卷 4539-4545页

作者： Mu Xiao Yalong Jiao Bin Luo Songcan Wang Peng Chen Miaoqiang Lyu Aijun Du Lianzhou Wang Nanomaterials Centre School of Chemical Engineering and Australian Institute for Bioengineering and NanotechnologyThe University of QueenslandSt LuciaQLD 4072Australia School of Chemistry Physics and Mechanical EngineeringScience and Engineering Faculty Queensland University of TechnologyBrisbane CityQLD 4000Australia Faculty for Chemistry and Food Chemistry TU Dresden01069 DresdenGermany Frontiers Science Center for Flexible Electronics Shaanxi Institute of Flexible Electronics&Shaanxi Institute of Biomedical

Coupling graphitic carbon nitride(CN)with carbonaceous materials is an effective strategy to improve photocatalytic performance,but the contributions of carbonaceous materials are not fully understood.Herein,a new type of carbon/CN(CCN)complex photocatalyst is synthesized with a 6-fold enhancement of H2 evolution rate compared to that of pristine CN.The role of carbon in photocatalytic H2 evolution reaction is systemically studied and it is experimentally and theoretically revealed that carbon mainly contributes to the improved capability of exciton dissociation and enhanced electric conductivity for charge transfer,leading to an increased population of photo-carriers for photocatalytic reactions.Interestingly,the enhanced light absorption originated from carbon barely generates charge carriers for H2 evolution activity.These new findings will inspire the rational design of carbon-based photocatalysts for efficient solar fuel production.

关键词： carbon nitride carbon exciton dissociation charge transfer photocatalysis

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Critical Role of Molecular Electrostatic Potential on Charge Generation in Organic Solar Cells

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Chinese Journal of Chemistry 2018年第6期36卷 491-494页

作者： Huifeng Yao Deping Qian Hao Zhang Yunpeng Qin Bowei Xu Yong Cui Runnan Yu Feng Gao Jianhui Hou Beijing National Laboratory for Molecular Sciences State Key Laboratory of Polymer Physics and Chemistry CAS Research/Education Center for Excellence in Molecular Sciences Institute of Chemistry Chinese Academy of Sciences Beijing 100190 China Department of Physics Chemistry and Biology (IFM) Linkoping University Linkoping 58183 Sweden University of Chinese Academy of Sciences Beijing 100049 China

Revealing the charge generation is a crucial step to understand the organic photovoltaics. Recent development in non-fullerene organic solar cells （OSCs） indicates efficient charge separation even with negligible energetic offset between the donor and acceptor materials. These new findings trigger a critical question concerning the charge separation mechanism in OSCs, traditionally believed to result from sufficient energetic offset between the polymer donor and fullerene acceptor. We propose a new mechanism, which involves the molecular electrostatic potential, to explain efficient charge separation in non-fullerene OSCs. Together with the new mechanism, we demonstrate a record efficiency of -12% for systems with negligible energetic offset between donor and acceptor materials. Our analysis also rationalizes different requirement of the energetic offset between fullerene-based and non-fullerene OSCs, and paves the way for further design of OSC materials with both high photocurrent and high photovottage at the same time.

关键词： organic solar cells non-fullerene acceptor molecular electrostatic potential exciton dissociation

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Improved Device Performance of Polymer Solar Cells by Using a SnO2/ZnO Stacked Structure as Cathode Interfacial Layer

Improved Device Performance of Polymer Solar Cells by Using ...

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第四届新型太阳能电池学术研讨会

作者： Shuai Huang Si Shen Xin Chen Bonan Kang State Key Laboratory on Integrated Optoelectronics College of Electronic Science and Engineering Jilin University

In the inverted structure, an interfacial layer plays a significant role in high-efficiency PSCs such as offering favorable ohmic contacts with electrodes, suppressing charge recombination and serving as an optical spacer layer for light manipulation.We prepared a highly efficient inverted polymer photovoltaic cell based on P3HT:PCBM by incorporating a SnO/ZnO stacked structure as a cathode interfacial layer.Compared to the inverted polymer photovoltaic cells with ZnO interfacial layer, the stacked SnO/ZnO not only facilitate electron injection and reduce the energy loss in the process of charge separation due to the optimum band matching, but also inhibit carrier recombination and enhance exciton dissociation at the interface of photoactive layer and cathode, hence all the device parameters of P3HT-based solar cells are simultaneously improved, yielding higher power conversion efficiency(PCE) up to 4.25% compared with the control one(PCE 3.10%).Furthermore, the PCE of device with stacked SnO/ZnO still remained 85% of its initial value during the device storage in a glove box for 23 day.

关键词： polymer solar cells stacked interfacial layer work function electron injection exciton dissociation

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