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Physical Review Letters

Infrared-Optical Double Resonance in Rare-Earth Crystals

F. Varsanyi

Published May 10, 1965• 23 citations
Publisher
DOI
10.1103/physrevlett.14.786

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We report a double-resonance technique that can substantially increase our knowledge of the many complex and competitive processes operative in materials such as the trivalent rare-earth-doped single crystals. This technique, which modulates the ground-state population, is similar in many respects to the Bloembergen quantum counter and the Varsanyi infrared-optical double-resonance experiment. The similarity and differences of the three techniques are analyzed and discussed. Ground-state modulation has been observed in single crystals of CaW${\mathrm{O}}_{4}$: 2% ${\mathrm{Tm}}^{3+}$ and Cd${\mathrm{F}}_{2}$: 5% ${\mathrm{Ho}}^{3+}$. The applications of this technique to determine the dominant process of competing mechanisms are discussed. This technique may also be used to resolve ambiguities present in optical spectra of the trivalent rare-earth-doped single crystals and as a possible negative \ensuremath{\leftrightarrow} positive image converter.

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Absorption and Emission in Rare Earths

WORLD SCIENTIFIC eBooks•Nov 17, 2014•0 citations
We report a double-resonance technique that can substantially increase our knowledge of the many complex and competitive processes operative in materials such as the trivalent rare-earth-doped single crystals. This technique, which modulates the ground-state population, is similar in many respects to the Bloembergen quantum counter and the Varsanyi infrared-optical double-resonance experiment. The similarity and differences of the three techniques are analyzed and discussed. Ground-state modulation has been observed in single crystals of CaWO4{\mathrm{O}}_{4}O4​: 2% Tm3+{\mathrm{Tm}}^{3+}Tm3+ and CdF2{\mathrm{F}}_{2}F2​: 5% Ho3+{\mathrm{Ho}}^{3+}Ho3+. The applications of this technique to determine the dominant process of competing mechanisms are discussed. This technique may also be used to resolve ambiguities present in optical spectra of the trivalent rare-earth-doped single crystals and as a possible negative \ensuremath{\leftrightarrow} positive image converter.
In this paper, we report the first laser-excited optical double-resonance experiments in rare-earth-doped crystals. Infrared upconversion in LaCl3 : Pr3+ and LaF3 : Pr3+ has been achieved by means of a tunable cw dye laser pump. The quantum efficiency of the upconversion process at 2.03 μ in LaCl3 : Pr3+ is 1.2×10−3, which is an improvement of 4×105 over the highest efficiency found previously with incoherent sources. It is shown that an efficiency of 1 can be easily obtained with higher fluxes and improved crystal quality. Direct excitation of the output fluorescence from the 3P0 level is observed in both LaCl3 : Pr3+ and LaF3 : Pr3+ when the dye laser frequency is resonant with the states of the lower-lying 1D2 manifold in the absence of the infrared input. Detailed assignments of the observed double-resonance transitions have been made from wavelength and polarization measurements.
Numerous bulk crystalline materials exhibit attractive nonlinear and luminescent properties for classical and quantum optical applications. A chip-scale platform for high quality factor optical nanocavities in these materials will enable new optoelectronic devices and quantum light-matter interfaces. In this article, photonic crystal nanobeam resonators fabricated using focused ion beam milling in bulk insulators, such as rare-earth doped yttrium orthosilicate and yttrium vanadate, are demonstrated. Operation in the visible, near infrared, and telecom wavelengths with quality factors up to 27,000 and optical mode volumes close to one cubic wavelength is measured. These devices enable new nanolasers, on-chip quantum optical memories, single photon sources, and non-linear devices at low photon numbers based on rare-earth ions. The techniques are also applicable to other luminescent centers and crystal.