Simulation of ultrafast transient absorption spectra of a perylene-based light harvesting antenna

Perez-Castillo, Royle; Freixas, Victor M.; Martinez-Mesa, Aliezer; Uranga-Piña, Llinersy; Gelin, Maxim F.; Tretiak, Sergei; Fernandez-Alberti, Sebastian

doi:10.1039/D5SC03157E

Simulation of ultrafast transient absorption spectra of a perylene-based light harvesting antenna

Journal Article · Mon Jun 23 00:00:00 EDT 2025 · Chemical Science

DOI:https://doi.org/10.1039/D5SC03157E· OSTI ID:2583264

^[1]; ^[2]; Martinez-Mesa, Aliezer ^[3]; Uranga-Piña, Llinersy ^[4]; Gelin, Maxim F. ^[5]; ^[6]; ^[1]

Universidad Nacional de Quilmes, Bernal (Argentina)
Univ. of California, Irvine, CA (United States)
Univ. of Havana (Cuba)
Univ. of Havana (Cuba); Univ. of Toulouse (France)
Hangzhou Dianzi Univ. (China)
Los Alamos National Laboratory (LANL), Los Alamos, NM (United States)

Atomistic simulations of photo-induced responses in artificial light-harvesting molecular systems help to reveal the mechanisms of ultrafast intramolecular energy transfer between individual chromophores. These light-induced processes mimic the primary events occurring in natural photosynthesis. Modeling studies contribute to the design of more efficient molecular architectures enabling performance optimization for applications in light harvesting, energy conversion, and optoelectronics. Within this context, the direct comparison between simulated and experimental transient absorption pump–probe (TA-PP) spectra are especially valuable for validating theoretical approaches and deepening mechanistic understanding. Herein, we investigate the photoinduced dynamics of an antenna system composed of two naphthalene monoimides donor units covalently linked to a perylene derived acceptor. Following photoexcitation, the exciton rapidly self-traps on one of the donor units. Thereafter, efficient ultrafast energy transfer to the acceptor unit takes place via two possible pathways: either through transient exciton localization on the second donor unit or by direct transfer to the acceptor. The simulated TA-PP spectra clearly capture these distinct energy transfer pathways and enable a detailed comparison of their relative efficiencies. This highlights the system's potential for tunable exciton dynamics towards advancing light-harvesting and optoelectronic molecular materials.

View Accepted Manuscript (DOE)

Research Organization:: Los Alamos National Laboratory (LANL), Los Alamos, NM (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: 89233218CNA000001

OSTI ID:: 2583264

Report Number(s):: LA-UR--25-24053; 2041-6539; 10.1039/D5SC03157E

Journal Information:: Chemical Science, Journal Name: Chemical Science Journal Issue: 29 Vol. 16; ISSN 2041-6539; ISSN 2041-6520

Publisher:: Royal Society of ChemistryCopyright Statement

Country of Publication:: United States

Language:: English

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