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Picosecond polarized fluorescence studies of anisotropic fluid media. I. Theory

Bain, AJ; Chandna, P; Bryant, J; (2000) Picosecond polarized fluorescence studies of anisotropic fluid media. I. Theory. The Journal of Chemical Physics , 112 (23) 10418 - 10434. 10.1063/1.481678. Green open access

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Abstract

Recent work has demonstrated the production of substantial molecular alignment in a free ethylene glycol jet. Using variably polarized photoselection, a range of initial nonequilibrium orientational distributions can be prepared and their subsequent relaxation monitored via polarization resolved time correlated single photon counting. The imposition of order in a fluid is seen to have a profound effect on molecular motion and a strong anisotropy in theta and phi diffusion is indicated. In this work (Papers I and II) we describe a detailed investigation of this phenomenon. Here (Paper I) we develop the formalism necessary to describe the interaction of polarized laser pulses with an anisotropic medium, allowing a full description of the initially photoselected distribution. The relaxation of the nonequilibrium distributions is considered via a perturbation treatment of the anisotropic rotational diffusion equation. New "selection rules" for orientational relaxation can be deduced from symmetry arguments and the form of the cylindrically symmetric (theta diffusion) and asymmetric alignment decays (phi diffusion) are predicted. (C) 2000 American Institute of Physics. [S0021-9606(00)00117-3].

Type: Article
Title: Picosecond polarized fluorescence studies of anisotropic fluid media. I. Theory
Open access status: An open access version is available from UCL Discovery
DOI: 10.1063/1.481678
Publisher version: https://doi.org/10.1063/1.481678
Language: English
Additional information: This version is the version of record. For information on re-use, please refer to the publisher’s terms and conditions.
Keywords: LASER TECHNIQUES, LIQUID-CRYSTALS, ROTATIONAL DIFFUSION, DEPOLARIZATION, ORDER, COLLISIONS, MEMBRANES, EMISSION, DECAY
UCL classification: UCL > Provost and Vice Provost Offices
UCL > Provost and Vice Provost Offices > UCL BEAMS
UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Maths and Physical Sciences
UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Maths and Physical Sciences > Dept of Physics and Astronomy
URI: https://discovery.ucl.ac.uk/id/eprint/113001
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