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EPJ Web of Conferences

Local-Field Effects in the Zero-Phonon Spectral Lines of Single Impurity Molecules in Solid Matrices at Low Temperatures

T. A. Anikushina, M. G. Gladush, А. А. Горшелев, А. В. Наумов

Published Jan 1, 2015• 1 citation
Publisher

Abstract

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.

DOI
10.1051/epjconf/201510305001

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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.
The low temperature spectra of absorption and luminescence of a wide variety of impurity doped organic and inorganic solids comprise very narrow (io 1O cm1) and intense zero-phonon lines (zPL). They arise from the purely electronic transistions in the impurities i.e. from the changes of the electronic state not accompanied by creation or annihilation of the phonons of the host solid. (ZPL may be called the optical analog of the M5sbauer line), Because of their narrowness ZPL's are very sensitive to even very slight differences in the crystal fields at the 1oca tions of impurities and the ZPL spectruim of a body of impu.rities displays a large inhomogeneous broadening (formula available on paper).
The photon echo (PE) spectroscopy and single-molecule spectroscopy (SMS) may be combined to give a very powerful tool for comprehensive study of low-temperature dynamics in dye-doped disordered solids (polymers, glasses). At the same time, this type of studies are likely to reveal discrepancies when comparing characteristic times of optical dephasing T2 and single-molecule zero-phonon spectral lines (ZPL) broadening obtained from PE and SMS, correspondingly, for tetra-tert-butylterrylene in polyisobutylene in the temperature range of a few–dozen of Kelvins [see Phys. Status Solidi B 241, 3480 and 3487 (2004)]. Inexplicably, PE-experiments demonstrated T2-times to be much shorter than it is sufficient to cause the corresponding ZPL broadening. Here we experimentally solve this problem and show that at T = 4.5–15 K the incoherent PE gives T2-times which correspond to the narrowest SM ZPL. On the SM-level there is a pronounced additional ZPL-broadening due to spectral diffusion processes which are strongly dependent on the characteristics time of the measurement (tens of nanoseconds for PE and seconds for SMS). There is also a broad distribution of ZPL spectral widths for different SMs due to different local environments, that contribute differently to both the optical dephasing and the spectral diffusion processes, but always in addition to the value of inverse optical dephasing times measured using a PE technique.
Abstract Optical spectroscopy of a single impurity molecule provides the first truly local probe of host–guest interactions in doped solids. In conventional optical high‐resolution experiments with many molecules only ensemble averages of the microscopic parameters can be obtained. In the single‐molecule regime, the exquisite sensitivity of an individual dopant molecule to both the local environment and to external perturbations has been exploited in recent experiments to reveal a wealth of fascinating novel phenomena such as spectral diffusion in crystals and polymers, optical modification of a single impurity molecule (spectral hole‐burning), local field measurements at the site of a single impurity molecule, and quantum optics in a solid.
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.).