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Single Molecules

Influence of the Optical Anisotropy of a Crystalline Host on the Radiative Line Width of a Single Impurity Molecule

Inna Rebane

Published Mar 1, 2001• 4 citations
Publisher

Abstract

We calculate the dependence of the spontaneous emission rate of a single impurity molecule on the orientation of the transition dipole moment vector with respect to the principal axis of a birefringent host crystal. We find that e.g. in naphthalene crystal the orientation-dependent spontaneous emission rate varies between 1.91 γ0 and 8.26 γ0 , where γ0 is the spontaneous emission rate in the vacuum.

DOI
10.1002/1438-5171(200103)2:1<31::aid-simo31>3.0.co;2-8

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We calculate the dependence of the spontaneous emission rate of a single impurity molecule on the orientation of the transition dipole moment vector with respect to the principal axis of a birefringent host crystal. We find that e.g. in naphthalene crystal the orientation-dependent spontaneous emission rate varies between 1.91 γ0 and 8.26 γ0 , where γ0 is the spontaneous emission rate in the vacuum.
Abstract The influence of the anisotropy of the host crystal on the spontaneous emission rate of the single‐impurity molecule and thus also on the radiative line width has taken into account. The anisotropy reveals itself in the dependence of the spontaneous emission rate on the orientation of the radiative transition dipole moment in the crystal. In this paper calculations of the relative spontaneous emission rate (the spontaneous emission rate divided by the spontaneous emission rate in the case when the transition dipole moment is parallel to the optical axis) of the quadrupole transition in a uniaxial host crystal are presented in the form which is convenient for experimenters. (© 2008 WILEY‐VCH Verlag GmbH & Co. KGaA, Weinheim)
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We study theoretically the spontaneous emission rate of a two-level quantum emitter in any nanophotonic system. We derive a general representation of the rate on the orientation of the transition dipole by only invoking symmetry of the Green function. The rate depends quadratically on orientation and is determined by rates along three principal axes, which greatly simplifies visualization: emission rate surfaces provide insight on how preferred orientations for enhancement (or inhibition) depend on emission frequency and location, as shown for a mirror, a plasmonic sphere, and a photonic band-gap crystal. Moreover, insight is provided on means to ``switch'' the emission rates by actively controlling the orientation of the emitters' transition dipole.