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Journal of Luminescence

Differences of the radiative line width in single-impurity molecule spectroscopy

Inna Rebane

Published Feb 5, 2004• 6 citations
Publisher
DOI
10.1016/j.jlumin.2003.12.019

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A pure-electronic zero-phonon line, which represents an optical analog of the Mössbauer γ-resonance line, is a cornerstone of three remarkable areas of spectroscopy and optics of impurity solids, namely, ultrahigh-resolution spectroscopy, persistent hole-burning spectroscopy, and spectroscopy of single impurity molecules. In recent experiments made by the photon echo technique, a zero-phonon line width as small as 78 Hz was achieved (with the Q -factor, i.e., the ratio of the transition frequency to the line width being 2×10 14 :78≈ 10 12 ), which is several tenfold lower than the frequency shift of the vibronic spectrum caused by the momentum of the absorbed or emitted photon of optical range. We estimate the position, intensity, and width of zero-phonon lines under conditions when these characteristics, as well as properties of the phonon wing, are determined not only by Stokes losses but also by the photon recoil effect. It is shown that the latter effect, within the approximation used, does not lead to strong and easily detectable phenomena. They, however, take place, and their study is becoming more topical with improving accuracy and sophistication of the experimental technique (in the photon echo configurations, etc.).

Optics and Spectroscopy•May 1, 2001•2 citations
In this work, we study the relation between the widths of the zero-phonon lines (ZPL) of single impurity molecules (SM) in solid matrices with local effective values of the refractive index n. Since at ultralow temperatures the width of SM ZPL is determined mainly by the radiative lifetime T1, while the local-field effects produce the function T1(n), SM spectroscopy makes it possible to measure the distribution of n local values in solids. The approach proposed here for studying local fluctuations of n has been tested on the example of doped polymers and molecular crystals.
A pure-electronic zero-phonon line, which represents an optical analog of the Mössbauer γ-resonance line, is a cornerstone of three remarkable areas of spectroscopy and optics of impurity solids, namely, ultrahigh-resolution spectroscopy, persistent hole-burning spectroscopy, and spectroscopy of single impurity molecules. In recent experiments made by the photon echo technique, a zero-phonon line width as small as 78 Hz was achieved (with the Q -factor, i.e., the ratio of the transition frequency to the line width being 2×10 14 :78≈ 10 12 ), which is several tenfold lower than the frequency shift of the vibronic spectrum caused by the momentum of the absorbed or emitted photon of optical range. We estimate the position, intensity, and width of zero-phonon lines under conditions when these characteristics, as well as properties of the phonon wing, are determined not only by Stokes losses but also by the photon recoil effect. It is shown that the latter effect, within the approximation used, does not lead to strong and easily detectable phenomena. They, however, take place, and their study is becoming more topical with improving accuracy and sophistication of the experimental technique (in the photon echo configurations, etc.).