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Spectral Hole-Burning and Related Spectroscopies: Science and Applications

High-resolution nonlinear laser spectroscopy and its applications using rare-earth-doped crystals

Masaharu Mitsunaga, Urs P. Wild, Stefan B. Altner, Hiroko Sasaki, Koichi Karaki

Published Jan 1, 1994• 0 citations
Publisher

Abstract

Due to their ultralong dephasing times, rare-earth-ion-doped crystals can be a powerful tool for investigating small interactions undergoing in the crystal. Furthermore, narrow spectral holes along with persistent lifetimes make them an ideal candidate of high-density optical data storage. We present some recent topics in this area.
DOI
10.1364/shbs.1994.wc2

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Recently, we showed the first high-resolution spectroscopy and manipulation of single Pr3+ ions in the solid state using rare-earth doped crystals. The special feature of these systems is access to the hyperfine splitting caused by the interaction of the 4f electrons and the nucleus, leading to sets of sublevels with exceptionally long coherence times at cryogenic temperatures, on the order of minutes and hours. This ground state splitting can serve as a lambda level scheme, a key ingredient for many prospective applications in quantum optics, in particular for qubit storage and manipulation. In this presentation, we discuss our latest results and future challenges in reducing spectral diffusion and line broadening down to the expected natural linewidth, prospects for the use of microcavities or plasmonic nano-antennas to enhance the photon yield, and schemes for on-chip integration.
Unique spectroscopic properties of isolated rare earth ions in solids offer optical linewidths rivaling those of trapped single atoms and enable a variety of recent applications. We design rare-earth-doped crystals, ceramics, and fibers with persistent or transient "spectral hole" recording properties for applications including high-bandwidth optical signal processing where light and our solids replace the high-bandwidth portion of the electronics; quantum cryptography and information science including the goal of storage and recall of single photons; and medical imaging technology for the 700-900 nm therapeutic window. Ease of optically manipulating rare-earth ions in solids enables capturing complex spectral information in 105 to 108 frequency bins. Combining spatial holography and spectral hole burning provides a capability for processing high-bandwidth RF and optical signals with sub-MHz spectral resolution and bandwidths of tens to hundreds of GHz for applications including range-Doppler radar and high bandwidth RF spectral analysis. Simply stated, one can think of these crystals as holographic recording media capable of distinguishing up to 108 different colors. Ultra-narrow spectral holes also serve as a vibration-insensitive sub-kHz frequency reference for laser frequency stabilization to a part in 1013 over tens of milliseconds. The unusual properties and applications of spectral hole burning of rare earth ions in optical materials are reviewed. Experimental results on the promising Tm3+:LiNbO3 material system are presented and discussed for medical imaging applications. Finally, a new application of these materials as dynamic optical filters for laser noise suppression is discussed along with experimental demonstrations and theoretical modeling of the process.
Rare-earth doped insulators have been widely recognized as excellent candidate materials for optical quantum computing and information processing. This is principally due to a combination of optical coherence times of up to milliseconds and ground-state hyperfine coherence times of seconds exhibited by rare-earth 4𝑓 𝑁 states. A key contender among rare-earth doped materials is Er3+:Y2SiO5, for which homogeneous linewidths as narrow as 50 Hz have been reported, and for which transitions between the ground and first excited states fall within the 1.5 𝜇m telecommunications wavelength band. However, attempts to utilize this material for spin-wave storage have been hampered by the complexity of the excited-state hyperfine structure, which inhibits the necessary theoretical work required to predict the location of zero first-order zeeman transitions. To address this, a novel crystal-field fitting method was developed to allow an accurate analysis of the 𝐶1 point-group symmetry sites of Y2SiO5. This work was complemented with spectral hole-burning spectroscopy, which revealed ground-state hyperfine level storage with a lifetime of 1.6 ± 0.4 seconds for the 4I15/2𝑍1 → 4F9/2𝐷1 transition. This type of storage time is uncharacteristic for erbium without an external magnetic field, since spin-flips of the unpaired electron in nearby Er3+ ions are typically understood to lead to fast hole filling. The development process of the theoretical and experimental tools required to perform the above work enabled several additional investigations. In particular, the novel crystal-field fitting methods were applied to the 𝑆4 site of Ce3+:LiYF4 and to the 𝐶2𝑣 site of Sm3+:Na+/Li+:CaF2/SrF2. These studies consisted of excellent tests for the developed methods yet also amounted to interesting investigations in their own respect. Similarly, the experimental work afforded an opportunity to directly determine the hyperfine splittings of the 5I8𝑍1 → 5F5𝐷1 transition in Ho3+:KY3F10. This was achieved using high-resolution excitation spectroscopy. Furthermore, the experimentally determined hyperfine structure could be accurately reproduced using a crystal field model. Finally, a lifetime measurement of the 6H7/2 state of Sm3+:LiYF4 was conducted. By utilizing an infrared free-electron laser, pico-second pump-probe spectroscopy allowed for a direct measurements of one of the shortest lifetimes of an RE3+ doped insulator reported in the literature to date. This confirmed the previously suggested two-gradient modification required for the energy-gap law at very short time scales.