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Journal of the Optical Society of America B

Frequency-modulation polarization-spectroscopy detection of persistent spectral holes

M. Romagnoli, M. D. Levenson, Gary C. Bjorklund

Published Aug 1, 1984• 16 citations

Abstract

Frequency-modulation polarization spectroscopy was used to detect persistent and anisotropic spectral holes written in the 607-nm color center in irradiated NaF and in the 683-nm absorption in phthalocyanine free-base-doped polyethylene. The high sensitivity of the technique permitted holes to be detected that had been written with exposure times down to 100 μsec. A general theory of frequency-modulation polarization spectroscopy is developed and specialized to the case of linear pump polarizations. Rate-equation models are presented to describe the anisotropic hole-burning process in a material, such as NaF, for which the absorbing centers have a finite distribution of possible orientations and in amorphous materials for which the distribution is uniform. The erasure of anisotropic holes because of excitation by the probe beam is investigated both theoretically and experimentally. A particular geometry was found to minimize this erasure effect in NaF.

DOI: 10.1364/josab.1.000571

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Frequency-modulation polarization spectroscopy was used to detect persistent and anisotropic spectral holes written in the 607-nm color center in irradiated NaF and in the 683-nm absorption in phthalocyanine free-base-doped polyethylene. The high sensitivity of the technique permitted holes to be detected that had been written with exposure times down to 100 μsec. A general theory of frequency-modulation polarization spectroscopy is developed and specialized to the case of linear pump polarizations. Rate-equation models are presented to describe the anisotropic hole-burning process in a material, such as NaF, for which the absorbing centers have a finite distribution of possible orientations and in amorphous materials for which the distribution is uniform. The erasure of anisotropic holes because of excitation by the probe beam is investigated both theoretically and experimentally. A particular geometry was found to minimize this erasure effect in NaF.

A polarized laser beam can bleach narrow, long-lived, anisotropic holes in the 607-nm zero-phonon line of the NaF

{N}_{1}

center. The width of these holes is twice the homogeneous linewidth, and three orders of magnitude less than the inhomogeneous width of the line. We report a polarization-spectroscopy technique which detects the dichroism and birefringence of the hole with better sensitivity than absorption spectroscopy. A simple rateequation model is developed to account for hole burning, but the recovery of the initial isotropic absorption profile appears to be a complex, slow, and intractable process.

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.

With a ring dye laser persistent spectral hole-burning was measured by fluorescence excitation spectroscopy in the zero-phonon lines of the 2llg ↔ 2llu transition in KI:S2 − and of the 3H4 → 3P0 transition of a defect center with three D− ions in SrF2:Pr3+:D−and also in the zero-phonon line at 462.5 nm of a color center in neutron-irradiated and annealed α-Al2O3. In all three lines holes with a width in the order of 1 GHz could be obtained at 1.5 K with single frequency laser. With broad-band laser in KI:S2 − and SrF2:Pr3+:D− spectral redistribution within the full range of inhomogeneous broadening could be observed which are explained by a photophysical model based on barrier crossing in asymmetric double-well-potentials. In the case of sapphire a photobleaching process is dominant which is effective also for nonselective excitation, and the holes are thermoresistant up to 300 K.

With high-efficiency fluorescence excitation techniques optical spectra of single impurity molecules of perylene in a polyethylene matrix can be obtained at 1.5 K. Analysis of such spectra shows a variety of spectral diffusion effects, including fast (<2 s) resonance frequency changes on the 1–100-MHz scale, which lead to a range of apparent linewidths, as well as discontinuous jumps in the resonance frequency of 10–1000 MHz on a longer time scale. In addition, light-induced changes in the resonance frequency of a single molecule (persistent spectral hole burning) have been conclusively observed by showing that the burning time decreases with increased laser power. Surprisingly, hole-burned single molecules often spontaneously return to the original frequency in 1–100 s. Measurements of the burning time for a large number of hole-burning events for the same single molecule yield an exponential burn-time distribution, which is the first direct measurement to our knowledge of the stochastic kinetics of a single molecule. Analysis of the signal-to-noise function appropriate to these experiments gives the conditions under which other systems may permit single-molecule detection: strong absorption, high fluorescence yield, weak bottlenecks in the optical pumping process, and low hole-burning quantum efficiency.