Theoretical aspects of femtosecond double-pump single-molecule spectroscopy. I. Weak-field regime

Literature Information

Publication Date 2017-11-20
DOI 10.1039/C7CP04809B
Impact Factor 3.676
Authors

Elisa Palacino-González, Maxim F. Gelin, Wolfgang Domcke


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Abstract

We present a theoretical description of double-pump femtosecond single-molecule signals with fluorescence detection. We simulate these signals in the weak-field regime for a model mimicking a chromophore with a Franck–Condon-active vibrational mode. We establish several signatures of these signals which are characteristic for the weak-field regime. The signatures include the quenching of vibrational beatings by electronic dephasing and a pronounced tilt of the phase-time profiles in the two-dimensional (2D) maps. We study how environment-induced slow modulations of the electronic dephasing and relevant chromophore parameters (electronic energy, orientation, vibrational frequency and relative shift of the potential energy surfaces) affect the signals.

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Source Journal

Physical Chemistry Chemical Physics

Physical Chemistry Chemical Physics
CiteScore: 5.5
Self-citation Rate: 10.3%
Articles per Year: 3036

Physical Chemistry Chemical Physics (PCCP) is an international journal co-owned by 19 physical chemistry and physics societies from around the world. This journal publishes original, cutting-edge research in physical chemistry, chemical physics and biophysical chemistry. To be suitable for publication in PCCP, articles must include significant innovation and/or insight into physical chemistry; this is the most important criterion that reviewers and Editors will judge against when evaluating submissions. The journal has a broad scope and welcomes contributions spanning experiment, theory, computation and data science. Topical coverage includes spectroscopy, dynamics, kinetics, statistical mechanics, thermodynamics, electrochemistry, catalysis, surface science, quantum mechanics, quantum computing and machine learning. Interdisciplinary research areas such as polymers and soft matter, materials, nanoscience, energy, surfaces/interfaces, and biophysical chemistry are welcomed if they demonstrate significant innovation and/or insight into physical chemistry. Joined experimental/theoretical studies are particularly appreciated when complementary and based on up-to-date approaches.

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