A laboratory frame density matrix for ultrafast quantum molecular dynamics

Author:

Gregory Margaret1,Neville Simon2,Schuurman Michael23ORCID,Makhija Varun1ORCID

Affiliation:

1. Department of Chemistry and Physics, University of Mary Washington, 1301 College Avenue, Fredericksburg, Virginia 22401, USA

2. National Research Council Canada, 100 Sussex Drive, Ottawa, Ontario K1A 0R6, Canada

3. Department of Chemistry and Biomolecular Sciences, University of Ottawa, 150 Louis Pasteur, Ottawa, Ontario K1N 6N5, Canada

Abstract

In most cases, the ultrafast dynamics of resonantly excited molecules are considered and almost always computed in the molecular frame, while experiments are carried out in the laboratory frame. Here, we provide a formalism in terms of a lab frame density matrix, which connects quantum dynamics in the molecular frame to those in the laboratory frame, providing a transparent link between computation and measurement. The formalism reveals that in any such experiment, the molecular frame dynamics vary for molecules in different orientations and that certain coherences, which are potentially experimentally accessible, are rejected by the orientation-averaged reduced vibronic density matrix. Instead, molecular angular distribution moments are introduced as a more accurate representation of experimentally accessible information. Furthermore, the formalism provides a clear definition of a molecular frame quantum tomography and specifies the requirements to perform such a measurement enabling the experimental imaging of molecular frame vibronic dynamics. Successful completion of such a measurement fully characterizes the molecular frame quantum dynamics for a molecule at any orientation in the laboratory frame.

Publisher

AIP Publishing

Subject

Physical and Theoretical Chemistry,General Physics and Astronomy

Cited by 2 articles. 订阅此论文施引文献 订阅此论文施引文献,注册后可以免费订阅5篇论文的施引文献,订阅后可以查看论文全部施引文献

1. Ultrafast Molecular Frame Quantum Tomography;Physical Review Letters;2023-11-07

2. Topical Review: Extracting molecular frame photoionization dynamics from experimental data;Journal of Physics B: Atomic, Molecular and Optical Physics;2023-05-11

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