Much of a Muchness: On the Origins of Two- and Three-Photon Absorption Activity of Dipolar Y-Shaped Chromophores

Autor:	Marta Chołuj, Rojalini Behera, Elizaveta F. Petrusevich, Wojciech Bartkowiak, Md. Mehboob Alam, Robert Zaleśny
Rok vydání:	2022
Předmět:	Photons Physical and Theoretical Chemistry
Zdroj:	The Journal of Physical Chemistry A. 126:752-759
ISSN:	1520-5215 1089-5639
DOI:	10.1021/acs.jpca.1c10098
Popis:	The molecular origin of two- (2PA) and three-photon absorption (3PA) activity in three experimentally studied chromophores, prototypical dipolar systems, is investigated. To that end, a generalized few-state model (GFSM) formula is derived for the 3PA transition strength for nonhermitian theories and employed at the coupled-cluster level of theory. Using various computational techniques such as molecular dynamics, linear and quadratic response theories, and GFSM, an in-depth analysis of various optical channels involved in 2PA and 3PA processes is presented. It is found that the four-state model involving the second and third excited singlet states as intermediates is the smallest model among all considered few-state approximations that produces 2PA and 3PA transition strengths (for S
Databáze:	OpenAIRE
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