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Physical Review Letters

Solid State Coherent Transient Measurements Using Hard Optical Pulses

Geoff J. Pryde, Matthew J. Sellars, N. B. Manson

Published Feb 7, 2000• 62 citations
Publisher

Abstract

An isolated and spectrally narrow absorptive feature is prepared via a novel spectral hole burning process in an inhomogeneously broadened optical transition in Eu(3+):Y(2)SiO5. With the narrow feature it is shown that it is feasible to apply complex optical pulse sequences analogous to rf pulse sequences used extensively in NMR.
DOI
10.1103/physrevlett.84.1152

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Optical hole burning is used to study optical dephasing of the 7F0 ⇒ 5D0 transition in samples of Y2O3:Eu3+ grown by both flame fusion and laser-heated pedestal growth. The samples exhibited a wide variation in their low-temperature hole widths, and the measured hole linewidths were in reasonable agreement with homogeneous linewidths obtained from values of T2 that were determined with two-pulse photon echoes. The sample that had the longest value of T2 (510 μs) from the echo measurements gave a hole width of 3.5 kHz. This is believed to be the narrowest spectral feature observed directly in the frequency domain for a solid. Other samples produced wider holes that were not correlated with the Eu3+ impurity concentrations. Time-resolved hole burning in one of the samples showed a slow and continuous broadening of the spectral hole from 130 kHz at 3 ms to 900 kHz at 10 s after hole burning. It is suggested that the additional broadening is associated with some form of disorder modes in this ordered crystalline solid.
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Optical spectroscopy provides a useful tool for probing the structure and dynamics of solids. Over the years, optical methods have evolved from absorption spectroscopy to more complex methods such as spectral hole burning, photon echoes, and luminescence line narrowing. The absorption spectrum provides information about inhomogeneous broadening, while the latter approaches provide information about the systematics of the homogeneous line shape information that is often obscured by inhomogeneous broadening. When external perturbations such as strain or electric fields are applied, details of the local site can be obtained. Recently, the ultimate limit of optical spectroscopy has been attained, in which the spectral properties of individual single impurity molecules in a solid can be measured, with all ensemble averaging removed. This novel regime has provided additional, previously unobtainable, information on a highly local scale, such as the direct observation of the spectral shifting of a single molecule produced by configurational transitions of the host. It is to be expected that further surprises await us in this new frontier of single-molecule spectroscopy in solids.
Laser frequency stabilization giving a 500-Hz Allan deviation for a 2-ms integration time with drift reduced to 7 kHz/min over several minutes was achieved at 1536 nm in the optical communication band. A continuously regenerated spectral hole in the inhomogeneously broadened 4I15/2(1)4I13/2(1){}^{4}{I}_{15/2}{(1)}^{4}{I}_{13/2}(1)4I15/2​(1)4I13/2​(1) optical absorption of an Er3+:Y2SiO5{\mathrm{Er}}^{3+}:{\mathrm{Y}}_{2}{\mathrm{SiO}}_{5}Er3+:Y2​SiO5​ crystal was used as the short-term frequency reference, while a variation on the locking technique allowed simultaneous use of the inhomogeneously broadened absorption line as a long-term reference. The reported frequency stability was achieved without vibration isolation. Spectral hole burning frequency stabilization provides ideal laser sources for high-resolution spectroscopy, real-time optical signal processing, and a range of applications requiring ultra-narrow-band light sources or coherent detection; the time scale for stability and the compatibility with spectral hole burning devices make this technique complementary to other frequency references for laser stabilization.