Visualization of Hot Exciton Energy Relaxation from Coherent to Diffusive Regimes in Conjugated Polymers: A Theoretical Analysis.
The unified coherent-to-diffusive energy relaxation of hot exciton in organic aggregates or polymers, which still remains largely unclear and is also a great challenge theoretically, is investigated from a time-dependent wavepacket diffusive approach. The results demonstrate that in the multiple time scale energy relaxation dynamics, the fast relaxation time essentially corresponds to the dephasing time of excitonic coherence motion, whereas the slow time is related to a hopping migration, and a suggested kinetic model successfully connects these two processes. The dependencies of those times on the initial energy and delocalization of exciton wavepacket as well as exciton-phonon interactions are further analyzed. The proposed method together with quantum chemistry calculations has explained an experimental observation of hot exciton energy relaxation in the low-bandgap copolymer PBDTTPD.
State Key Laboratory of Physical Chemistry of Solid Surfaces, Collaborative Innovation Center of Chemistry for Energy Materials, Fujian Provincial Key Lab of Theoretical and Computational Chemistry, and College of Chemistry and Chemical Engineering, Xiamen University, Xiamen 361005, People's Republic of China.
Yaling
Y
Ke
State Key Laboratory of Physical Chemistry of Solid Surfaces, Collaborative Innovation Center of Chemistry for Energy Materials, Fujian Provincial Key Lab of Theoretical and Computational Chemistry, and College of Chemistry and Chemical Engineering, Xiamen University, Xiamen 361005, People's Republic of China.
Yuxiu
Y
Liu
State Key Laboratory of Physical Chemistry of Solid Surfaces, Collaborative Innovation Center of Chemistry for Energy Materials, Fujian Provincial Key Lab of Theoretical and Computational Chemistry, and College of Chemistry and Chemical Engineering, Xiamen University, Xiamen 361005, People's Republic of China.
Yi
Y
Zhao
PBDTTPD; Quantum Coherence; Time-Dependent Wavepacket Diffusion Method; Ultrafast Energy Relaxation