Time-resolved high-harmonic spectroscopy of nonadiabatic dynamics in NO2

被引：40

作者：

Kraus, P. M. ^{[1
]}

Arasaki, Y. ^{[2
]}

Bertrand, J. B. ^{[3
,4
]}

Patchkovskii, S. ^{[3
,4
]}

Corkum, P. B. ^{[3
,4
]}

Villeneuve, D. M. ^{[3
,4
]}

Takatsuka, K. ^{[2
]}

Woerner, H. J. ^{[1
]}

机构：

[1] ETH, Lab Phys Chem, CH-8093 Zurich, Switzerland

[2] Univ Tokyo, Grad Sch Arts & Sci, Dept Basic Sci, Tokyo 1538902, Japan

[3] Natl Res Council Canada, Joint Attosecond Sci Lab, Ottawa, ON K1A 0R6, Canada

[4] Univ Ottawa, Ottawa, ON K1A 0R6, Canada

来源：

PHYSICAL REVIEW A | 2012年 / 85卷 / 04期

基金：

瑞士国家科学基金会;

关键词：

Harmonic analysis;

D O I：

10.1103/PhysRevA.85.043409

中图分类号：

O43 [光学];

学科分类号：

070207 ; 0803 ;

摘要：

Time-resolved high-harmonic spectroscopy is an emerging approach to measuring coupled electronic and nuclear dynamics in photochemical reactions. A general conceptual and theoretical model for the technique is derived from first principles and applied to study the sensitivity of the technique to nonadiabatic dynamics. By comparing the model with detailed experimental data on photoexcited NO2 molecules, we find that time-resolved high-harmonic spectroscopy is primarily sensitive to electronic population dynamics. The coordinate dependence of the vertical ionization potential and photorecombination matrix elements contribute also, but much less significantly, to the observed dynamics because of the rapid spreading of the wave packet in the excited state. We discuss the extension of the method to larger polyatomic molecules in light of this insight.

引用

页数：5