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Physical review. B, Condensed matter

High-resolution spectroscopy of the zero-phonon line of the deep donor EL2 in GaAs

Christoph Hecht, R. Kummer, M. Thoms, Albrecht Winnacker

Published May 15, 1997• 4 citations
Publisher

Abstract

We investigated the zero-phonon line (ZPL) of the deep donor EL2 in GaAs by means of high-resolution absorption spectroscopy with a narrow-band laser. Frequency-selective bleaching (``spectral-hole burning'') experiments and the measurement of the temperature broadening of the ZPL prove an essentially homogeneous broadening of the transition. The observed asymmetry of the line shape is interpreted to be caused by a Fano resonance of the $^{1}\mathrm{T}_{2}$ excited state with the conduction band. A splitting of the $^{1}\mathrm{T}_{2}$ state as the reason for the asymmetry seems unrealistic. The homogeneous broadening of the ZPL prevents the use of spectral-hole burning spectroscopy to study the effect of external perturbations on the ZPL of the EL2.

DOI
10.1103/physrevb.55.13625

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We investigated the zero-phonon line (ZPL) of the deep donor EL2 in GaAs by means of high-resolution absorption spectroscopy with a narrow-band laser. Frequency-selective bleaching (``spectral-hole burning'') experiments and the measurement of the temperature broadening of the ZPL prove an essentially homogeneous broadening of the transition. The observed asymmetry of the line shape is interpreted to be caused by a Fano resonance of the 1T2^{1}\mathrm{T}_{2}1T2​ excited state with the conduction band. A splitting of the 1T2^{1}\mathrm{T}_{2}1T2​ state as the reason for the asymmetry seems unrealistic. The homogeneous broadening of the ZPL prevents the use of spectral-hole burning spectroscopy to study the effect of external perturbations on the ZPL of the EL2.
Fluorescence—line—narrowing, spectral hole—burning and single molecule spectroscopy are methods of selective spectroscopy using zero-phonon lines (ZPL) to make selection in molecular ensemble. However if electron-phonon coupling is strong or sample temperature is near to room temperature, ZPL are absent and the optical band consists of electron-phonon transitions which are called phonon-side-band (PSB). In these cases the above mentioned methods of selective spectroscopy do not work. Can we get an information concerning a homogeneous optical band from inhomogeneously broadened bands in these cases? The answer is yes if we use femtosecond photon echo.
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:
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.
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.
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.