Collisional decoherence and rotational quasirevivals in asymmetric-top molecules

Ian F. Tenney, Maxim Artamonov, Tamar Seideman, and Philip H. Bucksbaum

Phys. Rev. A 93, 013421 – Published 25 January 2016

Abstract

We demonstrate the observation of quasiperiodic revivals out to 27 ps in an impulsively aligned asymmetric-top molecule, sulfur dioxide $({SO}_{2})$ , at high sample temperature and density (295 K, 0.5 bar). We find that the asymmetric top exhibits a strong correlation between population alignment and population lifetime $(r = 0.97)$ , in accordance with the trend observed in linear molecules. We use a linear birefringence measurement fit to a full quantum simulation of the asymmetric rotor and are able to separately measure both the population $(T_{1})$ and coherence $(T_{2})$ lifetimes of the rotational wave packet. Additionally, we observe a high rate of elastic decoherence $(T_{2}^{*} = 9.6 ps)$ and attribute this to long-range interactions mediated by the permanent dipole of the ${SO}_{2}$ molecule. We propose the use of birefringence measurements to study intermolecular interactions in a coherent ensemble, as a step toward using field-free alignment to investigate reaction dynamics and dissipative processes.

Received 26 November 2015

DOI:https://doi.org/10.1103/PhysRevA.93.013421

Physics Subject Headings (PhySH)

Molecule trapping & guiding

Atomic, Molecular & Optical

Authors & Affiliations

Ian F. Tenney^*

Department of Physics, Stanford University, Stanford, California 94305, USA and Stanford PULSE Institute, SLAC National Accelerator Laboratory, Menlo Park, California 94025, USA

Maxim Artamonov^† and Tamar Seideman^‡

Department of Chemistry, Northwestern University, Evanston, Illinois 60208, USA

Philip H. Bucksbaum^§

Department of Physics and Department of Applied Physics, Stanford University, Stanford, California 94305, USA and Stanford PULSE Institute, SLAC National Accelerator Laboratory, Menlo Park, California 94025, USA

^*Author to whom correspondence should be addressed: iftenney@stanford.edu
^†m-artamonov@northwestern.edu
^‡t-seideman@northwestern.edu
^§phb@slac.stanford.edu

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Vol. 93, Iss. 1 — January 2016

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