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Journal of Luminescence

Review of condensed matter laser cooling using electric-dipole-allowed transitions

Markus P. Hehlen

Published Sep 6, 2022• 7 citations
Publisher

Abstract

The cooling of solids via laser-excited anti-Stokes luminescence has reached the cryogenic regime and is now being considered for several applications that benefit from vibration-free cryogenic refrigeration. 4f-4f transitions in rare-earth-doped crystals with low phonon energies currently offer the best laser-cooling performance. These transitions, however, are electric-dipole (ED) forbidden and thus have low cross sections, limiting the minimum achievable temperatures in practical materials to the 50–100 K regime. In contrast, ED-allowed transitions may offer greater cross sections and potentially enable lower minimum temperatures or more compact devices. The search for laser cooling with ED-allowed transitions has been an active field of research over the past decades with a wide variety of materials having been studied. This paper reviews the fundamentals of solid-state laser cooling, provides a preliminary theoretical assessment showing that laser-cooling with ED-allowed transitions is in principle possible, and reviews the experimental results reported to date. While cooling with ED-allowed transitions has not yet been realized in the solid state, the existing experimental body of work along with the theoretical considerations presented here suggest that further research on this topic may be fruitful.

DOI
10.1016/j.jlumin.2022.119270

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The cooling of solids via laser-excited anti-Stokes luminescence has reached the cryogenic regime and is now being considered for several applications that benefit from vibration-free cryogenic refrigeration. 4f-4f transitions in rare-earth-doped crystals with low phonon energies currently offer the best laser-cooling performance. These transitions, however, are electric-dipole (ED) forbidden and thus have low cross sections, limiting the minimum achievable temperatures in practical materials to the 50–100 K regime. In contrast, ED-allowed transitions may offer greater cross sections and potentially enable lower minimum temperatures or more compact devices. The search for laser cooling with ED-allowed transitions has been an active field of research over the past decades with a wide variety of materials having been studied. This paper reviews the fundamentals of solid-state laser cooling, provides a preliminary theoretical assessment showing that laser-cooling with ED-allowed transitions is in principle possible, and reviews the experimental results reported to date. While cooling with ED-allowed transitions has not yet been realized in the solid state, the existing experimental body of work along with the theoretical considerations presented here suggest that further research on this topic may be fruitful.
This review discusses the progress and ongoing efforts in optical refrigeration. Optical refrigeration is a process in which phonons are removed from a solid by anti-Stokes fluorescence. The review first summarizes the history of optical refrigeration, noting the success in cooling rare-earth-doped solids to cryogenic temperatures. It then examines in detail a four-level model of rare-earth-based optical refrigeration. This model elucidates the essential roles that the various material parameters, such as the spacing of the energy levels and the radiative quantum efficiency, play in the process of optical refrigeration. The review then describes the experimental techniques for cryogenic optical refrigeration of rare-earth-doped solids employing non-resonant and resonant optical cavities. It then examines the work on laser cooling of semiconductors, emphasizing the differences between optical refrigeration of semiconductors and rare-earth-doped solids and the new challenges and advantages of semiconductors. It then describes the significant experimental results including the observed optical refrigeration of CdS nanostructures. The review concludes by discussing the engineering challenges to the development of practical optical refrigerators, and the potential advantages and uses of these refrigerators.
Laser cooling of solids, also known as optical refrigeration, is an area of optical science investigating the interaction of light with condensed matter to remove thermal energy of a solid through the interaction of the pump photons and phonons in a solid. Apart from being of fundamental scientific interest, this topic addresses a number of important practical issues such as the development of all solid state optical cryo-coolers, and biological applications. A short history of laser cooling as well as latest achievement of optical refrigeration in rare-earth (RE) doped macro-samples are presented and discussed in the paper. The main technique of laser cooling of RE doped solids based on anti-Stokes fluorescence is presented in this paper. The new approach to optical refrigeration based on the Raman cooling is also considered. It is shown that the future prospects of the research are connected with laser cooling of μm- and nm-sized samples, are in their applications in biophysics in the fundamental studies of low-temperature physics.
In recent decades, laser cooling of solids based on anti-Stokes fluorescence, also known as Pringsheim ‘s optical cooling, has garnered a great deal of scientific interest due to its applications, including optical solid-state coolers, radiation-balanced lasers and rare-earth-doped particles for biological applications. This Reprint compiles cutting-edge research on the subject carried out by various scientific teams all over the world. It will be useful to anyone involved in solid-state physics, low-temperature physics or cryogenics.
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.
Optical refrigeration of solids with anti-Stokes fluorescence has been widely explored as a vibration-free cryogenic cooling technology. A minimum temperature of 87 K has been demonstrated with rare-earth-ion-doped crystals using optical refrigeration. However, the depletion of the upper-lying energy levels in the ground-state manifold hinders further cooling to below the liquid nitrogen ( LN 2 ) temperatures, restricting its applications. In this work, we introduce a Purcell-enhanced optical refrigeration method to circumvent this limitation. This approach enhances the emission of high-energy photons by coupling the emitters to an optical cavity, blueshifting the mean emission wavelength. Such Purcell-enhanced emission facilitates cooling starting from a lower-energy level in the ground-state manifold, which exhibits a higher occupation below the LN 2 temperatures. Using experimentally measured optical coefficients, our theoretical analysis predicts a minimum achievable internal temperature of about 38 K for a Yb 3 + : YLiF 4 nanocrystal near a cavity under realistic conditions. The proposed method is applicable to other rare-earth-ion-doped materials and semiconductors and will have applications in creating superconducting and other quantum devices through solid-state cooling.