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Optics and Spectroscopy

Hole burning spectroscopy with preliminary photoselection of impurity molecules

G. M. Svishchev

Published Jan 1, 2001• 0 citations
Publisher

Abstract

The photoselection of impurity molecules caused by spectral hole burning produces a specific spectral angular distribution of the molecules in low-temperature amorphous matrices: All the molecules, whose zero-phonon absorption lines lie within a selected narrow spectral interval, have a specified distribution of their orientations relative to the laboratory coordinate system. In this paper, the possibility of application of known methods of hole burning in this spectral interval is studied and the outlook for combination of these methods with preliminary photoselection is demonstrated by the example of the Stark effect.

DOI
10.1134/1.1343545

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The photoselection of impurity molecules caused by spectral hole burning produces a specific spectral angular distribution of the molecules in low-temperature amorphous matrices: All the molecules, whose zero-phonon absorption lines lie within a selected narrow spectral interval, have a specified distribution of their orientations relative to the laboratory coordinate system. In this paper, the possibility of application of known methods of hole burning in this spectral interval is studied and the outlook for combination of these methods with preliminary photoselection is demonstrated by the example of the Stark effect.
A method of selective (relative to the magnitude of the linear Stark effect in zero-dipole impurity molecules) burning of holes in the spectra of amorphous matrices is studied. It is shown that this method makes it possible not only to select a subensemble of impurity molecules having both preset energy of the 0-0 transition and magnitude of the matrix-induced Stark moment, but also to divide this subensemble into two fractions whose Stark moments are predominantly oriented either along the transition moment or perpendicular to it. The possibility of experimental verification of the most popular hypothesis about the origin of induced Stark moments, which neglects a possible correlation between the direction of the Stark moment and that of the transition dipole moment, is considered. The method described also allows one to study experimentally the correlation of some other photophysical parameters of impurity molecules with the direction of local internal fields relative to the vector of the transition dipole moment.
The shape of a multiwell hole, which is produced upon burning a number of closely spaced equidistant spectral holes in the low-temperature absorption spectrum of an impurity amorphous solid, is studied. When the bottom of such a hole is probed by the wavelength-modulated light, the transmission and luminescence of the sample become modulated. This modulation is caused by a subsystem of impurity molecules, which differs from a total ensemble by a smaller scatter in the zero-phonon linewidth and a smaller (by a factor of 2–3) mean value of this width. The study of the photophysical parameters of this subsystem can yield useful information for simulating the nanostructure of an amorphous body.
A method of selective (with respect to the Stark effect) burning of a spectral hole in the 0-0 absorption band of zero-dipole impurity molecules is suggested. It is shown that in combination with the Stark modulation of the optical density of a sample, this method makes it possible to determine that contribution to the total absorption and luminescence of the sample that the impurity molecules with a preset magnitude of the matrix-induced Stark moment (provided this magnitude exceeds the mean value for the entire ensemble) make. This allows one to experimentally study both the distribution of impurity molecules over the magnitude of the Stark moment and the correlation of the Stark moment with other parameters of impurity molecules.
Persistent spectral hole-burning (PSHB) is a versatile tool to study Stark effect in solids where impurity spectra is strongly inhomogeneously broadened. At liquid helium temperatures impurity homogeneous zero-phonon line widths are small (γhom~10–2-10–4cm–1) and narrow holes can be burnt in the inhomogeneous distribution by illumination with narrow band laser(Δνlaser < γhom) U1- Stark effect alters the shape of narrow spectral holes depending on the Stark shift (splitting) of impurity energy levels, orientation of the impurities, strength and orientation of the electric field, as well as on the properties of the matrix [2].
Zero-phonon lines in impurity optical spectra and their inhomogeneous broadening are discussed. Photoburning of persistent spectral holes is not only an effective method to eliminate the inhomogeneous broadening and perform high resolution spectroscopy, but it serves also as a powerful tool to control by means of illumination the absorption coefficient and refractive index of the matter. It opens new horizons for frequency-selective optical memories, data storage and data processing. Hole burning by picosecond pulses and the time-and space-domain holography based on it are discussed and the results of the experiments described.