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分子聚集体中激子-激子湮灭过程
引用本文:茅江奇,范旭阳,路彦珍,王鹿霞. 分子聚集体中激子-激子湮灭过程[J]. 物理学报, 2021, 0(4): 320-326
作者姓名:茅江奇  范旭阳  路彦珍  王鹿霞
作者单位:北京科技大学数理学院物理系;中国人民大学物理学系
基金项目:国家自然科学基金(批准号:21961132023,11774026)资助的课题.
摘    要:分子的激发能量转移和电荷转移是提高光伏电池和发光二极管效率的关键问题,其中分子聚集体中的激子-激子湮灭过程是影响分子激发能量转移的重要方面,细致研究激子-激子湮灭的动力学过程并与相关的瞬间吸收谱信号对比对相关的理论和实验都有重要意义.本文在分子间弱耦合近似下,用经典的率方程,应用方酸分子的基本参数对激子-激子湮灭过程做...

关 键 词:激子-激子湮灭  率方程  自旋单态湮灭  飞秒激光激发

Exciton-exciton annihilation in molecular aggregations
Mao Jiang-Qi,Fan Xu-Yang,Lu Yan-Zhen,Wang Lu-Xia. Exciton-exciton annihilation in molecular aggregations[J]. Acta Physica Sinica, 2021, 0(4): 320-326
Authors:Mao Jiang-Qi  Fan Xu-Yang  Lu Yan-Zhen  Wang Lu-Xia
Affiliation:(Schoolof Mathematics and Physics,University of Science and Technology Beijing,Beijing 100083,China;Department of Physics,Renmin University of China,Beijing 100876,China)
Abstract:It is of ongoing interest to uncover energy and charge transfer processes in molecular systems,which are essentially important for photovoltaic cells or light emitting diodes.The exciton-exciton annihilation is one of the important aspects in excitation energy transfer in molecular aggregations,so it is important to study its dynamics of exciton-exciton annihilation,and to compare the theoretical parameters with the related transient absorption signal.Upon the excitation of laser pulses,multiple excitons can be produced in molecular aggregations,and its annihilation process is composed of two steps.The first step is that two excitations existing in the first excited state of the molecules move together so that their excitation energy can be used to create a high excited state in one molecule,called exciton fussion.The second step is that an ultrafast internal conversion process brings the molecule which is in the higher excited state back to the first excited state.This paper uses the scheme of classical rate equation in the approximation of weak coupling among molecules to describe the dynamics of exciton-exciton annihilation.With the parameters of squaraine,the effects of external or internal parameters such as the intensity of external field,the dipole configuration in aggregations,the decay rate of molecules on the annihilation process are studied.The relationship between the relaxation time of exciton in the first excited state and the high excited state,between their times of coherent charge transfer,and between their times of exciton and annihilation are studied.These conclusions are suitable to the aggregations with their single molecule having an energy level of Efm≈2Eem.It is found that the J-aggregate has a higher rate of annihilation than the H-aggregate because its coherent energy transfer time is shorter than H-aggregate’s.The high-intensity external field makes high exciton-exciton annihilation rate.The dipole configuration and the decay rate of higher excited state of molecules have strong effects on the annihilation,so one can adjust these factors to control the exciton-exciton annihilation in molecular aggregations.
Keywords:exciton-exciton annihilation  rate equation  singlet state annihilation  excitation of femtosecond laser pulse
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