Report

Tracing orbital images on ultrafast time scales

See allHide authors and affiliations

Science  18 Feb 2021:
eabf3286
DOI: 10.1126/science.abf3286

You are currently viewing the abstract.

View Full Text

Log in to view the full text

Log in through your institution

Log in through your institution

Abstract

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 to observe ultrafast electron motion in time and space.

View Full Text

Stay Connected to Science