Relative detection sensitivity in ultrafast spectroscopy: state lifetime and laser pulse duration effects

Literature Information

Publication Date 2017-10-27
DOI 10.1039/C7CP05426B
Impact Factor 3.676
Authors

Nikoleta Kotsina


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Abstract

We present a numerical modelling study employing a kinetic model based on rate equations to investigate the role of excited state lifetime and laser pulse duration on effective relative detection efficiency in time-resolved pump–probe spectroscopy. The work begins to address the critical outstanding problem of photochemical branching ratio determination when excited state population evolves via competing relaxation pathways in molecular systems. Our findings reveal significant differences in detection sensitivity, which can exceed an order of magnitude under typical experimental conditions for excited state lifetimes ranging between 10 fs and 1 ps. We frame our discussion within the widely used approach of ultrafast photoionization for interrogating excited state populations, but our overall treatment may be readily extended to consider a broader range of experimental methodologies and timescales.

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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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