Assignment of caroteneS* state features to the vibrationally hot ground electronic state

Literature Information

Publication Date 2010-06-07
DOI 10.1039/B925071A
Impact Factor 3.676
Authors

Thomas Lenzer, Florian Ehlers, Mirko Scholz, Rainer Oswald, Kawon Oum


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Abstract

The so-called S* state has been suggested to play an important role in the photophysics of β-carotene and other carotenoids in solution and photosynthetic light-harvesting complexes, yet its origin has remained elusive. The present experiments employing temperature-dependent steady-state absorption spectroscopy and ultrafast pump-supercontinuum probe (PSCP) transient absorption measurements of β-carotene in solution demonstrate that the spectral features of S* are due to vibrationally excited molecules in the ground electronic state S0. Characteristic spectral signatures, such as a highly structured bleach below 500 nm and absorption in the range 500–660 nm result from the superposition of hot S0 absorption (“S0*”) on top of the ground-state bleach of room-temperature molecules. Appearance and disappearance of the S0* molecules can be completely described by a global kinetic analysis employing time-dependent species-associated spectra without the need to invoke the population of an intermediate electronically excited state.

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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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