TY - JOUR
T1 - Scaling relations of exciton diffusion in linear aggregates with static and dynamic disorder
AU - Kunsel, T.
AU - Jansen, T. L.C.
AU - Knoester, J.
N1 - Publisher Copyright:
© 2021 Author(s).
PY - 2021/10/7
Y1 - 2021/10/7
N2 - Exciton diffusion plays an important role in many opto-electronic processes and phenomena. Understanding the interplay of intermolecular coupling, static energetic disorder, and dephasing caused by environmental fluctuations (dynamic disorder) is crucial to optimize exciton diffusion under various physical conditions. We report on a systematic analysis of the exciton diffusion constant in linear aggregates using the Haken-Strobl-Reineker model to describe this interplay. We numerically investigate the static-disorder scaling of (i) the diffusion constant in the limit of small dephasing rate, (ii) the dephasing rate at which the diffusion is optimized, and (iii) the value of the diffusion constant at the optimal dephasing rate. Three scaling regimes are found, associated with, respectively, fully delocalized exciton states (finite-size effects), weakly localized states, and strongly localized states. The scaling powers agree well with analytically estimated ones. In particular, in the weakly localized regime, the numerical results corroborate the so-called quantum Goldilocks principle to find the optimal dephasing rate and maximum diffusion constant as a function of static disorder, while in the strong-localization regime, these quantities can be derived fully analytically.
AB - Exciton diffusion plays an important role in many opto-electronic processes and phenomena. Understanding the interplay of intermolecular coupling, static energetic disorder, and dephasing caused by environmental fluctuations (dynamic disorder) is crucial to optimize exciton diffusion under various physical conditions. We report on a systematic analysis of the exciton diffusion constant in linear aggregates using the Haken-Strobl-Reineker model to describe this interplay. We numerically investigate the static-disorder scaling of (i) the diffusion constant in the limit of small dephasing rate, (ii) the dephasing rate at which the diffusion is optimized, and (iii) the value of the diffusion constant at the optimal dephasing rate. Three scaling regimes are found, associated with, respectively, fully delocalized exciton states (finite-size effects), weakly localized states, and strongly localized states. The scaling powers agree well with analytically estimated ones. In particular, in the weakly localized regime, the numerical results corroborate the so-called quantum Goldilocks principle to find the optimal dephasing rate and maximum diffusion constant as a function of static disorder, while in the strong-localization regime, these quantities can be derived fully analytically.
UR - http://www.scopus.com/inward/record.url?scp=85116870501&partnerID=8YFLogxK
U2 - 10.1063/5.0065206
DO - 10.1063/5.0065206
M3 - Article
C2 - 34624980
AN - SCOPUS:85116870501
SN - 0021-9606
VL - 155
JO - Journal of Chemical Physics
JF - Journal of Chemical Physics
IS - 13
M1 - 134305
ER -