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Journal of Applied Physics

Coherent Emission from Rare Earth Ions in Electro-optic Crystals

L. F. Johnson, A. A. Ballman

Published Jan 1, 1969• 259 citations
Publisher

Abstract

We report the observation of coherent emission from three rare-earth ions in electro-optic crystals. Oscillation is observed from Nd3+ ions in Bi4Ge3O12, LiNbO3, and Ba0.75Ca0.25Nb26O at room temperature, and from Tm3+ and Ho3+ ions in LiNbO3 at 77°K. Second-harmonic radiation is obtained from LiNbO3:Tm3+ and electric-field modulation of threshold is observed for certain crystals of LiNbO3:Nd3+. The latter effect is believed to arise from crystal strain. The propagation angle for phase-matched second-harmonic generation is calculated to lie at 43° to the c axis for both LiNbO3:Tm3+ and LiNbO3:Ho3+ at 77°K. Phasematched second-harmonic generation from LiNbO3:Nd3+ is not possible, since the maser line is an extraordinary wave. However, the polarization of the maser line in LiNbO3:Nd3+ is appropriate for phasematched parametric frequency conversion in the near infrared. Attempts to observe such radiation were not successful due to the limited power available in the fundamental.

DOI
10.1063/1.1657047

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•Jan 1, 1998•5 citations
We report the observation of coherent emission from three rare-earth ions in electro-optic crystals. Oscillation is observed from Nd3+ ions in Bi4Ge3O12, LiNbO3, and Ba0.75Ca0.25Nb26O at room temperature, and from Tm3+ and Ho3+ ions in LiNbO3 at 77°K. Second-harmonic radiation is obtained from LiNbO3:Tm3+ and electric-field modulation of threshold is observed for certain crystals of LiNbO3:Nd3+. The latter effect is believed to arise from crystal strain. The propagation angle for phase-matched second-harmonic generation is calculated to lie at 43° to the c axis for both LiNbO3:Tm3+ and LiNbO3:Ho3+ at 77°K. Phasematched second-harmonic generation from LiNbO3:Nd3+ is not possible, since the maser line is an extraordinary wave. However, the polarization of the maser line in LiNbO3:Nd3+ is appropriate for phasematched parametric frequency conversion in the near infrared. Attempts to observe such radiation were not successful due to the limited power available in the fundamental.
Most investigations of rare-earth ions in solids for quantum information have used crystals where the rare-earth ion is a dopant. Here, we analyze the conversion of quantum information from microwave photons to optical frequencies using crystals where the rare-earth ions, rather than being dopants, are part of the host crystal. These concentrated crystals are attractive for frequency conversion because of their large ion densities and small linewidths. We show that conversion with both high efficiency and large bandwidth is possible in these crystals. In fact, the collective coupling between the rare-earth ions and the optical and microwave cavities is large enough that the limitation on the bandwidth of the devices will instead be the spacing between magnon modes in the crystal.
We demonstrate optical probing of spectrally resolved single Nd^{3+} rare-earth ions in yttrium orthovanadate. The ions are coupled to a photonic crystal resonator and show strong enhancement of the optical emission rate via the Purcell effect, resulting in near radiatively limited single photon emission. The measured high coupling cooperativity between a single photon and the ion allows for the observation of coherent optical Rabi oscillations. This could enable optically controlled spin qubits, quantum logic gates, and spin-photon interfaces for future quantum networks.
Rare-earth-ion doped materials are studied for a quantum information protocol, controlled reversible inhomogeneous broadening, for storing single photons. Coherence properties of Er-doped silicate optical fibers and Er-doped LiNbO3 waveguiding structures are investigated. Spectral hole burning spectroscopy is performed in Erbium and Neodymium doped crystals and spectral tailoring is demonstrated in Nd³?:YVO4. The preservation of information encoded into the relative phase and amplitudes of optical pulses during storage and retrieval in an optical memory based on stimulated photon echo is demonstrated. Furthermore photon echoes stored in spatially separated optical memories in several temporal modes, are retrieved and then combined at a beam splitter. They show almost perfect interference demonstrating both phase preserving storage and indistinguishability of photon echoes. Finally, we report an interference experiment of spontaneous emission of light from two distant solid-state ensembles of atoms and the resulting high fringe visibility implies that the observed spontaneous emission is coherent.
Solids containing rare earth (RE) ions have attracted spectroscopists' attention since the beginning of this century.In the last 30 years, their extremely narrow spectral features in combination with the use of non linear spectroscopy have served to sensitively measure ion-solid interactions and to progressively observe narrower homogeneous linewidths.The potential for using RE ion doped crystals as optical storage materials and processors has lately been a driving force in their investigations, Here, the ratio of inhomogeneous to homogeneous linewidth is regarded as an adequate measure of storage density and can become as big as 10 7 at cryogenic temperatures.Therefore, the analysis of line broadening is of fundamental as well as applied interest.This work is concerned with the investigation of interactions of RE ions with their environment.By means of a laser with a kilohertz resolution and non-linear spectroscopy, spectral dynamics as a function of intrinsic, external electric field, or light-pulse induced perturbations are analyzed on different time scales.In the first part, the theoretical background for the spectroscopy of RE ion doped crystals is outlined.The energy levels are presented and it is shown that due to their electronic properties RE ions have spectrally narrow electronic transitions, sometimes in the sub-kHz regime.The investigations of these narrow spectral features on the seconds to minutes time scale require very stable tunable laser sources.At present, such devices are not commercially available.In the second part, the performance of ahorne built laser system is characterized using persistent spectral holes, The results show that frequency selective materials can be used as powerful tools for the high resolution Vlll Abstract spectral analysis of laser sources.Complementary to that, they give a measure for the long term evolution of the spectral holes for the particular hole burning substance.In the third part, the effect of an external electric field on RE ion doped crystals is investigated.It is shown that for these systems the electric field induced frequency shifts are fully reversible.A general theory of Stark splittings of RE doped crystals is introduced and two methods are presented which allow for the determination of the magnitude and orientation of the electric dipole moment differences with sub-degree accuracy.Finally in the last part, spectral line broadening mechanisms of RE ion doped crystals are discussed and investigated by means of two-pulse photon echoes.Through variation of the experimental parameters, a discrimination between the different contributions is partly achieved and characteristic properties for different dephasing mechanisms are presented.In combination with the measurements from the third part, quantitative predictions of the electric dipole-dipole induced broadening are carried out, which are compared to the experimental results,