Observing changes in molecular structure requires atomic-scale Ångstrom and femtosecond spatio-temporal resolution. We use the Fourier transform (FT) variant of laser-induced electron diffraction (LIED), FT-LIED, to directly retrieve the molecular structure of H2O+ with picometer and femtosecond resolution without a priori knowledge of the molecular structure nor the use of retrieval algorithms or ab initio calculations. We identify a symmetrically stretched H2O+ field-dressed structure that is most likely in the ground electronic state. We subsequently study the nuclear response of an isolated water molecule to an external laser field at four different field strengths. We show that upon increasing the laser field strength from 2.5 to 3.8 V/Å, the O-H bond is further stretched and the molecule slightly bends. The observed ultrafast structural changes lead to an increase in the dipole moment of water and, in turn, a stronger dipole interaction between the nuclear framework of the molecule and the intense laser field. Our results provide important insights into the coupling of the nuclear framework to a laser field as the molecular geometry of H2O+ is altered in the presence of an external field.



Keywords and Phrases

Calculations; Molecular structure, Ab initio calculations; External laser fields; Femto-second resolution; Ground electronic state; Intense laser field; Molecular geometries; Retrieval algorithms; Spatio-temporal resolution, Molecules

International Standard Serial Number (ISSN)

0021-9606; 1089-7690

Document Type

Article - Journal

Document Version

Final Version

File Type





© 2019 The Authors, All rights reserved.

Publication Date

01 Jul 2019

Included in

Physics Commons