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

Takuya Horio, Roman Spesyvtsev, Kazuki Nagashima, Rebecca A. Ingle, Yoshi Ichi Suzuki, Toshinori Suzuki

Research output: Contribution to journalArticle

17 Citations (Scopus)

Abstract

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 S2(ππ) 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 S2(ππ) → S1(nπ) internal conversion in pyrazine using TRPEI with UV pulses, this study presents a complete observation of the dynamics including radiationless transitions from S1 to S0 (internal conversion) and T1(nπ) (intersystem crossing). Also discussed are the role of 1Au(nπ) in the internal conversion and the configuration interaction of the S2(ππ) electronic wave function.

Original languageEnglish
Article number044306
JournalJournal of Chemical Physics
Volume145
Issue number4
DOIs
Publication statusPublished - Jul 28 2016

Fingerprint

Pyrazines
pyrazines
Photoelectrons
photoelectrons
Vacuum
Imaging techniques
internal conversion
vacuum
Wave functions
Molecules
pulses
electronics
deactivation
configuration interaction
wave functions
molecules

All Science Journal Classification (ASJC) codes

  • Physics and Astronomy(all)
  • Physical and Theoretical Chemistry

Cite this

Full observation of ultrafast cascaded radiationless transitions from S2(ππ-) state of pyrazine using vacuum ultraviolet photoelectron imaging. / Horio, Takuya; Spesyvtsev, Roman; Nagashima, Kazuki; Ingle, Rebecca A.; Suzuki, Yoshi Ichi; Suzuki, Toshinori.

In: Journal of Chemical Physics, Vol. 145, No. 4, 044306, 28.07.2016.

Research output: Contribution to journalArticle

Horio, Takuya ; Spesyvtsev, Roman ; Nagashima, Kazuki ; Ingle, Rebecca A. ; Suzuki, Yoshi Ichi ; Suzuki, Toshinori. / Full observation of ultrafast cascaded radiationless transitions from S2(ππ-) state of pyrazine using vacuum ultraviolet photoelectron imaging. In: Journal of Chemical Physics. 2016 ; Vol. 145, No. 4.
@article{d2b811f757544b829ee95cdde6f2bcd1,
title = "Full observation of ultrafast cascaded radiationless transitions from S2(ππ-) state of pyrazine using vacuum ultraviolet photoelectron imaging",
abstract = "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 S2(ππ∗) 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 S2(ππ∗) → S1(nπ∗) internal conversion in pyrazine using TRPEI with UV pulses, this study presents a complete observation of the dynamics including radiationless transitions from S1 to S0 (internal conversion) and T1(nπ∗) (intersystem crossing). Also discussed are the role of 1Au(nπ∗) in the internal conversion and the configuration interaction of the S2(ππ∗) electronic wave function.",
author = "Takuya Horio and Roman Spesyvtsev and Kazuki Nagashima and Ingle, {Rebecca A.} and Suzuki, {Yoshi Ichi} and Toshinori Suzuki",
year = "2016",
month = "7",
day = "28",
doi = "10.1063/1.4955296",
language = "English",
volume = "145",
journal = "Journal of Chemical Physics",
issn = "0021-9606",
publisher = "American Institute of Physics Publising LLC",
number = "4",

}

TY - JOUR

T1 - Full observation of ultrafast cascaded radiationless transitions from S2(ππ-) state of pyrazine using vacuum ultraviolet photoelectron imaging

AU - Horio, Takuya

AU - Spesyvtsev, Roman

AU - Nagashima, Kazuki

AU - Ingle, Rebecca A.

AU - Suzuki, Yoshi Ichi

AU - Suzuki, Toshinori

PY - 2016/7/28

Y1 - 2016/7/28

N2 - 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 S2(ππ∗) 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 S2(ππ∗) → S1(nπ∗) internal conversion in pyrazine using TRPEI with UV pulses, this study presents a complete observation of the dynamics including radiationless transitions from S1 to S0 (internal conversion) and T1(nπ∗) (intersystem crossing). Also discussed are the role of 1Au(nπ∗) in the internal conversion and the configuration interaction of the S2(ππ∗) electronic wave function.

AB - 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 S2(ππ∗) 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 S2(ππ∗) → S1(nπ∗) internal conversion in pyrazine using TRPEI with UV pulses, this study presents a complete observation of the dynamics including radiationless transitions from S1 to S0 (internal conversion) and T1(nπ∗) (intersystem crossing). Also discussed are the role of 1Au(nπ∗) in the internal conversion and the configuration interaction of the S2(ππ∗) electronic wave function.

UR - http://www.scopus.com/inward/record.url?scp=84980348150&partnerID=8YFLogxK

UR - http://www.scopus.com/inward/citedby.url?scp=84980348150&partnerID=8YFLogxK

U2 - 10.1063/1.4955296

DO - 10.1063/1.4955296

M3 - Article

AN - SCOPUS:84980348150

VL - 145

JO - Journal of Chemical Physics

JF - Journal of Chemical Physics

SN - 0021-9606

IS - 4

M1 - 044306

ER -