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International Conference on Luminescence - 1984

Laser Study of No-phonon Lines in the Inhomogeneously Broadened Spectra via Photochemical Hole Burning.

Karl K. Rebane

Published Jan 1, 1984• 0 citations
Publisher

Abstract

When the inhomogeneous broadening (IHB) is eliminated, the no-phonon lines (NPL) in optical spectra (absorption, luminescence, hot luminescence, light-scattering, excitation of luminescence) actually become the optical analogues of the Mössbauer γ-resonance lines. The basic reason of this analogue lies in the symmetry of the Hamiltonian of the harmonic oscillator in coordinates and momenta[1,2]

DOI
10.1364/icol.1984.tha2

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When the inhomogeneous broadening (IHB) is eliminated, the no-phonon lines (NPL) in optical spectra (absorption, luminescence, hot luminescence, light-scattering, excitation of luminescence) actually become the optical analogues of the Mössbauer γ-resonance lines. The basic reason of this analogue lies in the symmetry of the Hamiltonian of the harmonic oscillator in coordinates and momenta[1,2]
Many investigations have been done on the field of frequency domain optical memories based on photochemical hole burning (PHB). This effect offers an extra dimension for the organization of an optical memory. At cryogenic temperatures several solid state materials such as aggregate color centers in alkali halide crystals exhibit inhomogeneously broadened absorption lines. In such an absorption line permanent narrow holes can be burnt by photochemical processes induced by exposure to intense laser radiation with a wavelength within the inhomogeneously broadened line.
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.
In inhomogeneously broadened lines, selective photochemistry with narrow band lasers leads to photochemical hole burning. We describe this phenomenon with particular reference to free-base porphyrin (H2P) and chlorin molecules in n-alkane matrices at low temperatures. It is shown that hole burning, which is permanent at low temperatures, can be used to study homogeneous optical dephasing processes as a function of temperature, to measure fast vibronic relaxation, and to assign complex vibronic spectra. Some of the parameters that are important to the potential use of photochemical hole burning for information storage in inhomogeneously broadened lines are measured and discussed.
High inhomogeneous broadening of impurity spectra in amorphous media reflects one type of dispersion, characteristic for disordered systems: dispersion of electronic transition frequency. In principle, there can exist a pronounced dispersion of other parameters: homogeneous line width (Γ), Debay-Waller factor (α), hole burning efficiency (ϕ), etc. The problem of the burning efficiency dispersion (BED) was extensively discussed in the recent years ([1-6] and references therein). The nonexponentiality of the burning kinetics was treated in some publications [1-3,6] as an evidence of such dispersion. But burning kinetics is always nonexponential in strongly inhomogeneously broadened systems, if a burning laser line width Δνl is much less then Γ. That was found experimentally and treated theoretically in one of the first publications on a hole burning [7] (see, also [8]). All other sources of the nonexponentiality are, in fact, additional to this one. So, it’s not easy to attain experimentally the BED parameters on such background. The procedure of a numerical fit ting of the burning kinetic with BED, developed in [4,5], is correct, but it looks unreliable due to many fitting parameters.
Persistent spectral hole-burning (PHB) of inhomogeneously broadened absorption lines in solids occurs when a homogeneous class of absorbing centers in resonance with a narrowband laser beam undergoes a photolnduced change in optical absorption that persists for times longer than any excited state lifetime. Persistent spectral holes for impurity centers in solids can provide important information about guest–light and guest–host interactions, such as dephasing, Zeeman and Stark splittings, and photochemical reaction mechanisms.