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Physical review. B, Condensed matter

Polarization-spectroscopy measurement of the homogeneous linewidth of an inhomogeneously broadened color-center band

M. D. Levenson, R. M. Macfarlane, Robert M. Shelby

Published Nov 15, 1980• 36 citations
Publisher

Abstract

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.

DOI
10.1103/physrevb.22.4915

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Applied Physics Letters•Oct 8, 2001•8 citations
A polarized laser beam can bleach narrow, long-lived, anisotropic holes in the 607-nm zero-phonon line of the NaF N1{N}_{1}N1​ 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.
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.
We report reversible hole burning in the inhomogeneously broadened zero-phonon line of F3+{{F}_{3}}^{+}F3​+ in NaF at 5456 \AA{}. The hole recovery time shows two components: 2.5 sec assigned to triplet-state relaxation and 70 min assigned to electron tunneling from an adjacent center. These holes were used to measure the homogeneous linewidth (17 MHz) and the linear Stark effect. We find the excited 1E^{1}E1E level has a distribution of zero-field splittings inside the inhomogeneous lines, which quenches the first-order Zeeman effect.
At very low temperatures, the spread in the different environments of matrix embedded dye molecules results in an inhomogeneously broadened S1 ← S0 band. Spectroscopic techniques based on the appearence of optical zero phonon lines, such as fluorescence line narrowing, spectral hole-burning, and single molecule spectroscopy provide an experimental resolution limited by the homogeneous linewidth. From the investigation of the homogeneous line width as a function of different parameters (time, temperature) information on the guest host interactions responsible for the observed linewidth is obtained. Spectrally narrow features are extremely sensitive probes for external perturbations, such as electric fields, magnetic fields, or hydrostatic pressure.
The study of optical relaxation processes in solids at low temperature has progressed tremendously in the last 20 years due to the development of coherent optical techniques. The latter would not have been possible without the advent of narrow-band tunable lasers, on the one hand, and lasers with very short pulses (picoseconds, femtosecoods) on the other hand. Such coherent techniques are necessary because spectral line shapes of solids doped with guest molecules are seldom determined by dynamical interactions but principally by strain or structural disorder. This gives rise to inhomogeneous broadening, rlOh, which in crystalline hosts at low temperature varies between ' 0.1 and 10 cm -I, whereas in glasses it may amount to � 100-500 em-I. One of the techniques to achieve narrowing of spectral lines is site­ selection spectroscopy (1-3). A sub-ensemble of molecules within thc inhomogeneously broadened absorption band is selectively excited by mcans of a narrow-band laser, and the fluorescence or phosphoresccnce signal is detected with a high-resolution monochromator and/or a Fabry­ Perot interferometer. Fluorescence line-narrowing ( I) is a special case of this technique (for a review see 3). The intrinsic or homogeneous spectral linewidth, r hom, which yields information on the relaxation processes of the excited state, is given by the effective optical dephasing time, T2:
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.
Luminescence and absorption spectra of LiF crystals with F2− color centers (CCs) were studied in the 14–300 K temperature range. The Huang–Rhys factors measured from absorption and emission spectra were equal in magnitude and calculated to be 3.2 and 2.72 at 77 and 300 K, respectively. It was shown that below 40 K inhomogeneous broadening of the zero phonon line of the F2− CC prevails over homogeneous broadening. Inhomogeneous broadening of the zero phonon line was observed to vary from 5 to 15 cm−1 for different crystal preparations. Persistent spectral hole burning stable at room temperature was realized in LiF:F2− crystals.