title: Davydov Ansatz as an efficient tool for the simulation of nonlinear optical response of molecular aggregates.
abstract: We have developed a variational approach to the description of four-wave-mixing signals of molecular aggregates, in which the third-order response functions are evaluated in terms of the Davydov Ansätze. Our theory treats both singly and doubly excited excitonic states, handling the contributions due to stimulated emission, ground state bleach, and excited state absorption. As an illustration, we simulate a series of optical two-dimensional spectra of model J-aggregates. Our approach may become suitable for the computation of femtosecond optical four-wave-mixing signals of molecular aggregates with intermediate-to-strong exciton-phonon and exciton-exciton coupling strengths.
authors.affiliation: School of Science, Hangzhou Dianzi University, Hangzhou 310018, China.
authors.forename: Ke-Wei
authors.initials: KW
authors.lastname: Sun
authors.affiliation: Department of Chemistry, Technische Universität München, Garching D-85747, Germany.
authors.forename: Maxim F
authors.initials: MF
authors.lastname: Gelin
authors.affiliation: Division of Materials Science, Nanyang Technological University, 50 Nanyang Avenue, Singapore 639798, Singapore.
authors.forename: Vladimir Y
authors.initials: VY
authors.lastname: Chernyak
authors.affiliation: Division of Materials Science, Nanyang Technological University, 50 Nanyang Avenue, Singapore 639798, Singapore.
authors.forename: Yang
authors.initials: Y
authors.lastname: Zhao