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Updated: Jul 1, 2025

$Measurements of Long-range Electronic Correlations During Femtosecond Diffraction Experiments Performed on Nanocrystals of Buckminsterfullerene$

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Published on: August 22, 2017

Quantum tomography of molecules using ultrafast electron diffraction.

Jiayang Jiang¹, Ming Zhang², Aosheng Gu¹

¹Departments of Chemistry and Physics, University of Toronto, Toronto, Ontario M5S 3H6, Canada.

The Journal of Chemical Physics

|March 8, 2024

Summary

We developed a quantum tomography method to reconstruct molecular electronic states from ultrafast electron diffraction. This technique allows visualizing electronic dynamics, like a "molecular movie," capturing coherence and population transfer.

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Published on: June 9, 2018

Area of Science:

Quantum Chemistry
Spectroscopy
Chemical Physics

Background:

Ultrafast electron diffraction (UED) probes molecular dynamics.
Reconstructing electronic state evolution from UED is challenging.

Purpose of the Study:

To develop a quantum tomography (QT) approach for retrieving time-evolving reduced density matrices.
To visualize electronic degrees of freedom in molecular dynamics using UED.

Main Methods:

Simulated nuclear wavepacket dynamics and UED of photoexcited pyrrole using ab initio CASSCF.
Applied QT to reconstruct the density matrix from simulated time-resolved diffraction data.

Main Results:

Successfully retrieved the evolving density matrix in a diabatic basis.
Revealed the symmetry of the excited pyrrole wavepacket.
Demonstrated QT's capability to capture electronic state coherence and population transfer.

Conclusions:

The proposed QT approach enables quantum-level "molecular movies" of electronic dynamics.
UED can now reveal electronic state coherence, relaxation, and population transfer dynamics.