Tracing orbital images on ultrafast time scales

被引：55

作者：

Wallauer, R. ^{[1
,2
]}

Raths, M. ^{[3
,4
,5
]}

Stallberg, K. ^{[1
,2
]}

Muenster, L. ^{[1
,2
]}

Brandstetter, D. ^{[6
]}

Yang, X. ^{[3
,4
,5
]}

Guedde, J. ^{[1
,2
]}

Puschnig, P. ^{[6
]}

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

Kumpf, C. ^{[3
,4
,5
]}

Bocquet, F. C. ^{[3
,4
]}

Tautz, F. S. ^{[3
,4
,5
]}

Hoefer, U. ^{[1
,2
]}

机构：

[1] Philipps Univ Marburg, Fachbereich Phys, Renthof 5, D-35032 Marburg, Germany

[2] Philipps Univ Marburg, Zentrum Mat Wissensch, Renthof 5, D-35032 Marburg, Germany

[3] Forschungszentrum Julich, Peter Grunberg Inst PGI 3, D-52425 Julich, Germany

[4] Julich Aachen Res Alliance JARA, Fundamentals Future Informat Technol, D-52425 Julich, Germany

[5] Rhein Westfal TH Aachen, Expt Phys 4, Otto Blumenthal Str, D-52074 Aachen, Germany

[6] Karl Franzens Univ Graz, Inst Phys, NAWI Graz, A-8010 Graz, Austria

来源：

SCIENCE | 2021年 / 371卷 / 6533期

基金：

奥地利科学基金会;

关键词：

D O I：

10.1126/science.abf3286

中图分类号：

O [数理科学和化学]; P [天文学、地球科学]; Q [生物科学]; N [自然科学总论];

学科分类号：

07 ; 0710 ; 09 ;

摘要：

Frontier orbitals determine fundamental molecular properties such as chemical reactivities. Although electron distributions of occupied orbitals can be imaged in momentum space by photoemission tomography, it has so far been impossible to follow the momentum-space dynamics of a molecular orbital in time, for example, through an excitation or a chemical reaction. Here, we combined time-resolved photoemission using high laser harmonics and a momentum microscope to establish a tomographic, femtosecond pump-probe experiment of unoccupied molecular orbitals. We measured the full momentum-space distribution of transiently excited electrons, connecting their excited-state dynamics to real-space excitation pathways. Because in molecules this distribution is closely linked to orbital shapes, our experiment may, in the future, offer the possibility of observing ultrafast electron motion in time and space.

引用

页码：1056 / +

页数：30

共 47 条

[1] Time-Resolved Molecular Frame Dynamics of Fixed-in-Space CS2 Molecules [J].