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Spectral Hole-Burning and Related Spectroscopies: Science and Applications

Microwave-Induced Hole Burning of the 638 Nm Zero-Phonon Transition and Frequency-Dependent Dephasing of the N-V Center in Diamond

Max Glasbeek, Eric van Oort

Published Jan 1, 1991• 0 citations
Publisher

Abstract

In recent years the microscopic description of inhomogeneous broadening of electronic transitions of chromophores in crystals and glasses has attracted much interest [1–3]. In the phenomenological model proposed by Selzer [1], it is assumed that the energies of the initial and final states involved in the optical transition exhibit a one-to-one correlation. In an alternative approach by Lee et al [2], the two states are considered as completely uncorrelated. Very recently, a more general microscopic theory has been presented by Laird and Skinner [3]. In the latter theory the aforementioned models are obtained as limiting cases. So far relatively few experiments have been reported which focus on the origin of inhomogeneous broadening.

DOI
10.1364/pshb.1991.sb2

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We have applied the results of the nonperturbative theory of zero-phonon linewidths of impurities in crystals discussed by Osad’ko and us, and further developed by us in papers I and II of this series, to the analysis of several absorption, photon echo, and hole burning experiments. Two (relatively) high temperature absorption experiments on 1,3-diazaazulene in naphthalene and dilute ruby were analyzed with a model of Debye acoustic phonons. In both cases the Debye temperature was obtained from independent experiment or theory, and a one-parameter fit was performed on the temperature-dependent linewidth. It was found that (especially for diazaazulene) the systems are not in the weak coupling limit. For several low temperature experiments, where the dephasing is presumably due to pseudolocal phonons, the nonperturbative theory, coupled with the results of deBree and Wiersma, provides a reasonably complete understanding of the observed dephasing rates.
We present a theory of frequency-dependent optical dephasing as measured by narrow-band photon-echo experiments. We consider a substitutionally disordered crystal with inhomogeneous broadening (diagonal disorder) and electronic interactions between occupied sites. We include the possibility of site-energy correlations. We find that the frequency dependence of the dephasing rate 1/T2{T}_{2}T2​ is very sensitive to the ratio \ensuremath{\xi}/a, where \ensuremath{\xi} is the correlation length and a is the lattice spacing. When \ensuremath{\xi}/a\ensuremath{\rightarrow}\ensuremath{\infty}, and there are macroscopic domains of resonant ions, 1/T2{T}_{2}T2​ becomes frequency independent. In the other limit when \ensuremath{\xi}/a\ensuremath{\rightarrow}0, and the site energies are uncorrelated (microscopic broadening), 1/T2{T}_{2}T2​ is proportional to the inhomogeneous line shape. We have compared our results to experiments by Macfarlane and Shelby on Y2{\mathrm{Y}}_{2}Y2​O3{\mathrm{O}}_{3}O3​:Eu3+{\mathrm{Eu}}^{3+}Eu3+ (2 at. %) and EuP5{\mathrm{EuP}}_{5}EuP5​O14{\mathrm{O}}_{14}O14​. We find reasonable agreement with experiment when \ensuremath{\xi} is less than a few lattice sites. Thus, for these systems the model of microscopic broadening is more appropriate than that of macroscopic broadening.
New satellite features and antiholes in the persistent hole-burning spectrum of N–V centers in diamond, as well as their dependences on applied electric fields and frequency within the inhomogeneous absorption line, are reported. These results, together with reassignments of spin states of this center, permit an understanding of the origin of the satellite holes as well as of possible mechanisms for the persistent hole-burning phenomenon itself. In addition we report narrow optical interference fringes in heterodyne-detected spectra of persistent spectral holes in the N–V defect center in diamond and discuss a recent suggestion for high-resolution Ramsey-fringe hole-burning spectroscopy of solids based on phase-separated fields.
Abstract Inhomogeneous broadening is often considered a nuisance in solid state spectroscopy, and the usual treatment of it is phenomenological. In fact, the inhomogeneous broadening of absorption spectra, coupled with a microscopic theory, can provide one with interesting information about the nature of disorder in different systems. More sophisticated experiments can provide more detailed information about disorder by probing certain correlations between energy levels. For example, flourescence line narrowing spectra of isolated impurities involve correlations among three different vibronic levels. Pressure effects on hole burning spectra probe correlations of impurity transition energies before and after the pressure change. For interacting impurity systems, photon echo experiments involve transition energy correlations between different impurities. Efforts to understand these effects within a microscopic framework are discussed.