Theoretical aspects of femtosecond double-pump single-molecule spectroscopy. II. Strong-field regime

Literature Information

Publication Date 2017-11-20
DOI 10.1039/C7CP04810F
Impact Factor 3.676
Authors

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


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Abstract

We investigate femtosecond double-pump single-molecule signals in the strong-field regime, which is characterized by nonlinear scaling of the signal with the intensity of the pump pulses. The signals can be decomposed into population and coherence contributions. In contrast to the weak-field regime (in which only the coherence contribution is important) both contributions are relevant in the strong-field regime and reveal the vibrational dynamics of the chromophore. Other than in the weak-field regime, the detection of vibrational beatings is not limited by the electronic dephasing time of the chromophore. Moreover, the signals in the strong-field regime are more robust with respect to the environment-induced modulation of the chromophore parameters. It is shown that excited-state absorption in chromophores with three electronic states is reflected in the phase dependence of single-molecule signals. The simulations reveal that the information content of femtosecond double-pump single-molecule signals is enhanced in the strong-coupling regime.

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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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