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Chinese Physics Letters

Infrared Spectral Hole-Burning and Spectral Diffusion of Vibrational N-D Bands in a Disordered Tutton Salt

Hongwei Song, Herbert L. Strauss

Published Dec 19, 2001• 1 citation
Publisher

Abstract

We have studied infrared spectral hole burning of the N-D stretching bands of NH 3 D + in salt [(NH 4 ) 2 Co 0.25 Ni 0.75 (H 2 O) 6 (SO 4 ) 2 ] at 10 K. We have observed that the spectral line broadening occurred on a logarithmic timescale, which is consistent with the theoretical prediction of a standard two-level system. The temperature of 10 K is also beyond the temperature limit in previous studies on spectral diffusion.

DOI
10.1088/0256-307x/19/1/314

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We have studied infrared spectral hole burning of the N-D stretching bands of NH 3 D + in salt [(NH 4 ) 2 Co 0.25 Ni 0.75 (H 2 O) 6 (SO 4 ) 2 ] at 10 K. We have observed that the spectral line broadening occurred on a logarithmic timescale, which is consistent with the theoretical prediction of a standard two-level system. The temperature of 10 K is also beyond the temperature limit in previous studies on spectral diffusion.
The population hole burned within the inhomogeneously broadened ir fundamental absorption band of 12C^{12}\mathrm{C}12C17O^{17}\mathrm{O}17O in solid N2{\mathrm{N}}_{2}N2​ by a narrow-band pulsed laser is detected as an antihole in the transient absorption of a tunable cw probe beam whose frequency is swept through the $v=1\ensuremath{\rightarrow}v=2$ resonance. The time development of the transient profile demonstrates that spectral diffusion is governed by an energy-dependent process, contrary to what has been observed in many disordered systems.
In the first experimental search for persistent spectral hole burning in an elemental semiconductor, we examined a variety of electronic defects in Si and in a Si:Ge alloy. No persistent spectral changes have been observed for Be-Li, Se0, or thermal donors in Si; however, spectral holes which persist for ~5 ms have been produced in the 1s-2p absorption lines of a sulfur-hydrogen complex in Si. The addition of 0.7% Ge to the Si host ensures that an inhomogeneously broadened system is being studied. Measurements combining a CO2 laser pump with a Fourier transform spectrometer probe reveal that the hole burning is due to migration of electrons from the S-H centers to shallow traps. The large observed hole width (4.6 cm−1) is attributed to spectral diffusion by resonant excitation transfer. The hole burning behavior of the 2p± line is temperature independent below 30 K, whereas the hole burning of the 2p0 line exhibits strong temperature dependence, suggesting that the ionization of the laser-excited centers in the 2p± hole burning process occurs via energy transfer between neighboring excited centers rather than by thermal ionization.
Holes burnt into the absorption spectrum of terrylene in hexadecane have quite unusual features: spectral diffusion behavior under thermal cycles shows a narrowing regime at very low temperatures (2-5 K) followed by a plateau region (up to about 13 K) and a broadening regime (T>13 K). Thermal line broadening (quasihomogeneous linewidth) shows a nonmonotonous behavior as a function of temperature: at around 4 K there is a maximum followed by a flat minimum and the onset of strong broadening at higher temperatures. Finally, the central hole shows one-sided narrowly spaced side features. This behavior is interpreted within the frame of a two-site model. One of the two sites can be well described by a standard two level system; the other, however, shows characteristic features of a multilevel system. The two sites are characterized by strongly different optical linewidths, phototransformation yields, and thermal stabilities.
Spectral holes which persist for \ensuremath{\sim}5 msec have been produced in the spectrum of a sulfur-hydrogen complex in a Si-0.1 at.% Ge alloy crystal maintained at 1.7 K. Measurements which combine an infrared laser pump with a Fourier-transform spectrometer probe show that the hole burning is due to migration of electrons from the S-H centers to shallow traps. The large observed hole width (4.6 ${\mathrm{cm}}^{\ensuremath{-}1}$) is attributed to spectral diffusion by resonant excitation transfer. The lack of temperature dependence of the hole burning of the $2{p}_{\ifmmode\pm\else\textpm\fi{}}$ line below 30 K suggests that excitation transfer is also responsible for the ionization of laser-excited centers in the hole-burning process.
Photon gated spectral hole-burning was first observed in a samarium doped crystal, BaFCl:Sm2+ [1]. This material was of interest to the developement of optical memories as the holes were found to be stable to room temperature thermal cycling. Holes could be burnt at liquid helium temperatures but as the temperature was raised the line quickly became homogeneously broadened. The addition of bromine to the melt succeeded in broadening the inhomogeneous linewidths to about 2 nm through substitutional disorder [2] and persistent holes were observed at 77 K [3]. Subsequently, a study of the parameters for spectral hole-burning in a BaFCl0.5Br0.5:Sm2+ crystalline powder was performed [4] and the highest temperature for which persistent hole-burning had been observed was raised to 133 K. Here we report spectral hole-burning at room temperature (figure 1) in a related compound, Sr0.5Mg0.5FCl0.5Br0.5:Sm2+.