Imaging an isolated water molecule using a single electron wave packet

TL;DR

This paper demonstrates a novel laser-induced electron diffraction technique to directly image and observe ultrafast structural changes in an isolated water molecule with atomic and femtosecond resolution, revealing how external laser fields alter molecular geometry.

Contribution

The study introduces FT-LIED for direct, real-time imaging of molecular structure without prior knowledge or complex algorithms, applied to water molecules under laser fields.

Findings

Water molecule structure can be directly imaged with femtosecond resolution.

Increasing laser field strength causes water to stretch and bend.

Molecular dipole moment increases as structure changes under laser influence.

Abstract

Observing changes in molecular structure requires atomic-scale {\AA}ngstrom 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 ${\rm H_2O^+}$ with picometre 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 ${\rm H_2O^+}$ 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/{\AA}, 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 ${\rm H_2O^+}$ is altered in the presence of an external field.