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Updated: Jul 10, 2025

Direct Imaging of Laser-driven Ultrafast Molecular Rotation

Direct Imaging of Laser-driven Ultrafast Molecular Rotation

Published on: February 4, 2017

Ultrafast Molecular Frame Quantum Tomography.

Luna Morrigan¹, Simon P Neville², Margaret Gregory¹

¹Department of Chemistry and Physics, University of Mary Washington, Fredericksburg, Virginia 22401, USA.

Physical Review Letters

|November 24, 2023

Summary

This summary is machine-generated.

We developed a new method for molecular frame quantum tomography (MFQT) to fully characterize molecular dynamics. This technique revealed nuclear motion-induced electronic coherences in ammonia (NH_{3}), offering insights into ultrafast charge migration.

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Area of Science:

Quantum Chemistry
Molecular Dynamics
Spectroscopy

Background:

Understanding ultrafast molecular dynamics is crucial for controlling chemical reactions.
Characterizing electronic and nuclear motion simultaneously in polyatomic molecules remains a challenge.

Purpose of the Study:

To develop and demonstrate a methodology for full molecular frame quantum tomography (MFQT).
To completely characterize an electronically nonadiabatic wave packet in ammonia (NH_{3}).

Main Methods:

Utilized a combination of energy- and time-domain spectroscopic data.
Developed a technique to yield the lab frame density matrix (LFDM) for dynamical polyatomic systems.
Applied MFQT to ammonia (NH_{3}) to analyze electronic and nuclear dynamics.

Main Results:

Successfully characterized an electronically nonadiabatic wave packet in ammonia (NH_{3}).
Observed nuclear dynamics, specifically rotational motion and Coriolis coupling, inducing electronic coherences.
Demonstrated that these nuclear-driven electronic coherences are preserved over extended timescales.
Showcased the ability to construct time-dependent molecular frame electronic probability densities.

Conclusions:

MFQT provides a comprehensive method for characterizing molecular dynamics in the molecular frame.
Nuclear dynamics can nonadiabatically drive electronic motions, leading to charge migration.
This approach can quantify electronic-nuclear entanglement and open new avenues for ultrafast molecular dynamics studies.