Full observation of ultrafast cascaded radiationless transitions from S2(ππ*) state of pyrazine using vacuum ultraviolet photoelectron imaging

被引：43

作者：

Horio, Takuya ^{[1
]}

Spesyvtsev, Roman ^{[1
,2
]}

Nagashima, Kazuki ^{[1
]}

Ingle, Rebecca A. ^{[1
,3
]}

Suzuki, Yoshi-ichi ^{[1
,4
]}

Suzuki, Toshinori ^{[1
]}

机构：

[1] Kyoto Univ, Grad Sch Sci, Dept Chem, Sakyo Ku, Kitashirakawa Oiwake Cho, Kyoto 6068502, Japan

[2] Univ St Andrews, Sch Phys & Astron, SUPA, St Andrews KY16 9SS, Fife, Scotland

[3] Univ Bristol, Sch Chem, Cantocks Close, Bristol BS8 1TS, Avon, England

[4] Hlth Sci Univ Hokkaido, Fac Pharmaceut Sci, Ishikari, Hokkaido 0610293, Japan

来源：

JOURNAL OF CHEMICAL PHYSICS | 2016年 / 145卷 / 04期

关键词：

CONICAL INTERSECTION DYNAMICS; VIBRONIC LEVEL FLUORESCENCE; AB-INITIO; CONFIGURATION-INTERACTION; ELECTRONIC STATES; QUANTUM DYNAMICS; FS DEEP; TIME; SPECTROSCOPY; MOLECULES;

D O I：

10.1063/1.4955296

中图分类号：

O64 [物理化学（理论化学）、化学物理学];

学科分类号：

070304 ; 081704 ;

摘要：

A photoexcited molecule undergoes multiple deactivation and reaction processes simultaneously or sequentially, which have been observed by combinations of various experimental methods. However, a single experimental method that enables complete observation of the photo-induced dynamics would be of great assistance for such studies. Here we report a full observation of cascaded electronic dephasing from S-2(pi pi*) in pyrazine (C4N2H4) by time-resolved photoelectron imaging (TRPEI) using 9.3-eV vacuum ultraviolet pulses with a sub-20 fs time duration. While we previously demonstrated a real-time observation of the ultrafast S-2(pi pi*) -> S-1(n pi*) internal conversion in pyrazine using TRPEI with UV pulses, this study presents a complete observation of the dynamics including radiationless transitions from S-1 to S-0 (internal conversion) and T-1(n pi*) (intersystem crossing). Also discussed are the role of (1)A(u)(n pi*) in the internal conversion and the configuration interaction of the S-2(pi pi*) electronic wave function. Published by AIP Publishing.

引用

页数：10

共 59 条

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