Unraveling ultrafast dynamics in photoexcited aniline

Gareth M Roberts; Craig A Williams; Jamie D Young; Susanne Ullrich; Martin J Paterson; Vasilios G Stavros

doi:10.1021/ja3029729

Unraveling ultrafast dynamics in photoexcited aniline

Gareth M Roberts, Craig A Williams, Jamie D Young, Susanne Ullrich, Martin J Paterson, Vasilios G Stavros

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74 Citations (Scopus)

Abstract

A combination of ultrafast time-resolved velocity map imaging (TR-VMI) methods and complete active space self-consistent field (CASSCF) ab initio calculations are implemented to investigate the electronic excited-state dynamics in aniline (aminobenzene), with a perspective for modeling (1)ps* mediated dynamics along the amino moiety in the purine derived DNA bases. This synergy between experiment and theory has enabled a comprehensive picture of the photochemical pathways/conical intersections (CIs), which govern the dynamics in aniline, to be established over a wide range of excitation wavelengths. TR-VMI studies following excitation to the lowest-lying (1)pp* state (1(1)pp*) with a broadband femtosecond laser pulse, centered at wavelengths longer than 250 nm (4.97 eV), do not generate any measurable signature for (1)ps* driven N-H bond fission on the amino group. Between wavelengths of 250 and >240 nm (

Original language	English
Pages (from-to)	12578-89
Number of pages	12
Journal	Journal of the American Chemical Society
Volume	134
Issue number	30
DOIs	https://doi.org/10.1021/ja3029729
Publication status	Published - 2012

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10.1021/ja3029729

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title = "Unraveling ultrafast dynamics in photoexcited aniline",

abstract = "A combination of ultrafast time-resolved velocity map imaging (TR-VMI) methods and complete active space self-consistent field (CASSCF) ab initio calculations are implemented to investigate the electronic excited-state dynamics in aniline (aminobenzene), with a perspective for modeling (1)ps* mediated dynamics along the amino moiety in the purine derived DNA bases. This synergy between experiment and theory has enabled a comprehensive picture of the photochemical pathways/conical intersections (CIs), which govern the dynamics in aniline, to be established over a wide range of excitation wavelengths. TR-VMI studies following excitation to the lowest-lying (1)pp* state (1(1)pp*) with a broadband femtosecond laser pulse, centered at wavelengths longer than 250 nm (4.97 eV), do not generate any measurable signature for (1)ps* driven N-H bond fission on the amino group. Between wavelengths of 250 and >240 nm (",

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doi = "10.1021/ja3029729",

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T1 - Unraveling ultrafast dynamics in photoexcited aniline

AU - Roberts, Gareth M

AU - Williams, Craig A

AU - Young, Jamie D

AU - Ullrich, Susanne

AU - Paterson, Martin J

AU - Stavros, Vasilios G

PY - 2012

Y1 - 2012

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Unraveling ultrafast dynamics in photoexcited aniline

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