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Journal of the Optical Society of America B

Coherent pumping for fast laser cooling of doped crystals

Andrei V. Ivanov, Yu. Rozhdestvensky, E. Yu. Perlin

Published Apr 14, 2015• 11 citations
Publisher

Abstract

A mechanism for laser cooling of crystals doped with rare-earth ions is proposed. The mechanism involves two-photon Raman scattering through the dipole-allowed 5d ion level, electron–phonon transitions between the Stark-split sublevels, and fluorescence from the excited ion level. It is shown that, under the conditions of coherent pumping, the total population of the ground level is transferred to the excited level of the rare-earth ion, thus increasing the cooling power and accelerating the cooling process. The involvement of dipole-allowed transitions yields an increase in the cooling efficiency by 14% compared to the efficiency of direct pumping at transitions between the 4f levels. Estimations show that the temperature of the sample cooled by the proposed mechanism can reach 82.9 K for current materials with a background absorption coefficient of 4.0×10−4 cm−1.

DOI
10.1364/josab.32.000b47

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A mechanism for laser cooling of crystals doped with rare-earth ions is proposed. The mechanism involves two-photon Raman scattering through the dipole-allowed 5d ion level, electron–phonon transitions between the Stark-split sublevels, and fluorescence from the excited ion level. It is shown that, under the conditions of coherent pumping, the total population of the ground level is transferred to the excited level of the rare-earth ion, thus increasing the cooling power and accelerating the cooling process. The involvement of dipole-allowed transitions yields an increase in the cooling efficiency by 14% compared to the efficiency of direct pumping at transitions between the 4f levels. Estimations show that the temperature of the sample cooled by the proposed mechanism can reach 82.9 K for current materials with a background absorption coefficient of 4.0×10−4 cm−1.
Methods of coherent pumping through dipole-allowed 5d levels of RE ion are proposed for laser cooling. The coherent and complete population transfer between the ground and the first excited levels of 4f multiplet is achieved by using the different Raman techniques, namely two-photon scattering, adiabatic passage method, and π-pulse pumping. It is shown that the multiplication of the number of electrons that participate in cooling cycle leads to increasing of the cooling power and to acceleration of the cooling process. The increasing of cooling efficiency of 0.5% compared to the direct pumping between 4f levels is attained through the use of dipole-allowed optical transitions. Performed estimates show that the sample temperature can achieve 94 K for current purity materials. The calculations are obtained for Yb3+:CaF2 system.
A vibronic model of laser cooling for crystals doped with Yb3+ ions is proposed. The model involves the stimulated Raman adiabatic passage pumping through dipole-allowed 4f–5d transitions, electron transitions between Stark-split sublevels due to vibronic interaction, and anti-Stokes fluorescence from the excited ion state. Dynamics of the cooling process are described by the density matrix formalism. It is shown that the cooling power in the case of vibronic interaction is higher at least by a factor of 3.4 compared to the case of electron–phonon interaction. In the proposed model, an increase in the cooling power yields deeper and faster refrigeration of a crystal doped with Yb3+ ions. Estimations show that, on cooling by the stimulated Raman adiabatic passage pumping, the temperature of a crystal with an irradiated volume of 2.12×10−4 cm3 can reach 64 K in a time of 2 s. In the proposed model, the cooling temperature is 30 K lower and the cooling process is 100 times faster compared to the traditional model of direct pumping. The estimates are applicable to present-day materials of technologically attainable purity.
The enhanced laser cooling performance of rare-earth-ion-doped nanocrystalline powders is predicted, compared to the bulk material, using Yb3+:Y2O3{\mathrm{Yb}}^{3+}:{\mathrm{Y}}_{2}{\mathrm{O}}_{3}Yb3+:Y2​O3​ as the model material. This is achieved by enhancing the off-resonance, phonon-assisted absorption, which is proportional to the three factors considered in this paper: the dopant concentration, the pumping field energy, and the excitation coefficient. Using the energy transfer theory for concentration quenching, the optimum concentration corresponding to the maximum cooling power is found to be considerably larger than the currently used value, suggesting noticeable enhancement effects for laser cooling. The pumping field energy is enhanced in random nanopowders compared with bulk crystals under the same irradiation, due to the multiple scattering of photons. Photons are thus localized in the medium and do not propagate through, increasing the photon absorption of the pumping beam (and it is shown that the reabsorption of the fluorescence is negligible). Using molecular dynamics simulations, the phonon density of states (DOS) of the nanopowder is calculated, and found to have broadened modes, and extended small tails at low and high frequencies. The second-order electronic transition rate for the anti-Stokes luminescence is calculated using the Fermi golden rule, which includes the influence of this phonon DOS, and is shown to have enhancement effects on the laser cooling efficiency using nanopowders. It is finally concluded that these three enhancement mechanisms are essentially to increase the population of the three participating carriers (electron, photon, and phonon) in the interacting volume, and this also points out directions for enhancing laser cooling performance in bulk materials.
The recent achievements devoted to cooling of solids with a laser are presented in this paper. We discuss the latest results of traditional laser cooling of solids based on rare earth ions and new techniques based on colloidal lead-salt quantum dots doped in a glass host, laser cooling in Tm3+-doped oxy-fluoride glass ceramic. Relatively short (microsecond) lifetime of the excited level of the PbSe QDs compared to the millisecond lifetime of the excited level of RE ions allows an acceleration of the cooling process and provides an opportunity to use new materials with higher phonon energy as hosts, which are normally considered unsuitable for cooling with RE ions. Another new approach to the laser cooling problem based on super-radiance has been considered in this paper. The advantages of optical refrigeration with rare earth doped semiconductors, in which not only optically active electrons of the 4f shell but the valence and conduction bands of the host material are involved in cooling cycle is discussed. It is shown that involving the valence and conduction bands of the host in the cooling cycle allows the pump wavelength to be shorter than mean fluorescence wavelength. Raman laser cooling of solids as well as observation of spontaneous Brillouin cooling have been presented.
We present a theoretical scheme for laser cooling of rare-earth-doped solids with optical superradiance (SR), which is the coherent, sharply directed spontaneous emission of photons by a system of laser-excited rare-earth ions in the solid-state host (glass or crystal). We consider an Yb+{}^{+}+-doped ZnF4{}_{4}4​-BaF2{}_{2}2​-LaF3{}_{3}3​-AlF3{}_{3}3​-NaF (ZBLAN) sample pumped at a wavelength 1015 nm, with a rectangular pulsed source with a power of \ensuremath{\sim}433 W and a duration of 10 ns. The intensity of the SR is proportional to the square of the number of excited ions. This unique feature of SR permits an increase in the rate of the cooling process in comparison with the traditional laser cooling of the rare-earth-doped solids with anti-Stokes spontaneous incoherent radiation (fluorescence). This scheme overcomes the limitation of using only low phonon energy glasses for laser cooling.
Laser cooling of rare-earth doped solids has been demonstrated across a wide range of material platforms, inspiring the development of simple phenomenological models such as the four-level model to elucidate the universal properties of laser cooling under various operating conditions. However, these models usually require the input of full absorption spectra that must be provided experimentally or by additional complicated atomic modeling. In this Letter, we propose that a four-level model, when extended to admit effective energy levels adaptive to the pumping photon energy, can accurately predict the cooling efficiency as a function of temperature and pumping frequency using only few inputs such as the absorption coefficient measured at a single frequency and temperature. Our model exploits the quasi-equilibrium properties of the excitation of rare-earth ions for the determination of the effective four energy levels. The model is validated against published experimental results for a span of materials including ytterbium/thulium-doped glass and crystals. With the verified model, we derive explicit expressions for the optimal frequency and the operating bandwidth of pumping lasers. Our model significantly simplifies the modeling process of laser cooling and is expected to stimulate further development of optical refrigeration.