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Journal of Optical Technology

Laser cooling of solutions of complex molecules

В. В. Данилов, V. A. Smirnov, В. Б. Шилов

Published Feb 1, 2004• 2 citations
Publisher

Abstract

This paper theoretically discusses possible ways of increasing the efficiency of optical cooling accompanying anti-Stokes excitation of the fluorescence of solutions of complex molecules. It is concluded that it is promising for these purposes to use the "photoinduced" luminescence effect, which makes it possible to speed up the photoluminescence process without causing additional population of the excited states of the molecule. © 2004 Optical Society of America

DOI
10.1364/jot.71.000123

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This paper theoretically discusses possible ways of increasing the efficiency of optical cooling accompanying anti-Stokes excitation of the fluorescence of solutions of complex molecules. It is concluded that it is promising for these purposes to use the "photoinduced" luminescence effect, which makes it possible to speed up the photoluminescence process without causing additional population of the excited states of the molecule. © 2004 Optical Society of America
Publisher Summary This chapter focuses on the concept of laser cooling of a solid, which may occur when the average energy of the photons emitted by the solid is larger than the energy of the ones it absorbs. More formally, the anti-Stokes emission, which occurs at frequencies larger than that of the pump laser, must dominate the Stokes emission that occurs at smaller frequencies. A crucial additional requirement is that the nonradiative decay rates of the laser-pumped states be negligible in comparison to their radiative decay rates. For the sake of specificity, these states will be taken to be those of a set of isolated ions embedded within an insulating host, although in general they could equally well be those of gas-, liquid-, or solid-phase neutral atoms or molecules, or even those of the energy bands of intrinsic semiconductors. Outside the realm of impurity-doped insulators, recent experiments with semiconductors make net anti-Stokes fluorescence cooling of these materials appear achievable. A long-term idea for improving laser cooling of solids takes advantage of photonic band gap materials. The idea is to fabricate a refractive-index structure within the cooling element that would establish a three-dimensional photonic gap immediately below the pump frequency. In this way, emission at Stokes frequencies falling within the gap would be inhibited, thereby enhancing the cooling power derived from the anti-Stokes emission.
Cold and ultracold molecules are highly desirable for a diverse range of applications in physics and chemistry such as precision measurements, tests of fundamental physics, quantum simulation and information processing, quantum chemistry, and the physics of strongly correlated quantum matter. Laser cooling is usually infeasible in molecules because their rotational and vibrational transitions make is difficult to come up with a closed scattering cycle. Recently, a narrow range of diatomic molecules, one of which is CaF, has been shown to possess a convenient electronic structure and a highly-diagonal Franck-Condon matrix and thus be amenable to laser cooling. This thesis describes experiments on laser cooling of CaF radicals produced in a supersonic source. We first investigate the increased fluorescence when multi-frequency resonant light excites the molecules from the four hyperfine levels of the ground X²∑+(N = 1, v = 0) state to the first excited A²π½ (J’ = 1=2; v’ = 0) state. The number of photons scattered per molecule increases significantly from one or two in the single frequency case to more than 50 before the molecules get pumped into the X²∑+(N = 1; v = 1) state. We demonstrate laser cooling and slowing of CaF using counter-propagating laser light which causes the molecules to scatter more than a thousand photons on the X (N = 1, v = 0, 1) <->A (J’ = 1=2; v’ = 0) transition. The effect of the laser cooling is to slow a group of molecules from 600 ms-1 to about 580 ms-1 and to narrow their velocity distribution from an initial temperature of 3 K down to 300 mK. In addition, chirping the frequency of the cooling light to keep it on resonance with the decelerating molecules doubles the deceleration and further compresses the velocity distribution. The effect of the laser cooling is limited by the optical pumping of molecules in the X (N = 1, v = 2) state.
Laser cooling of solids is also called anti-Stokes fluorescent cooling, it is a new optical cooling technology in recent years. We propose a two-level model to analyze the absorption and stimulated-emission processes between the Yb3+2F7/2 ground-state manifold and the 2F5/2 excited-state manifold, and discuss several parameters that influence the cooling power, and find some ways to improve the cooling power. The influences of the doped concentration, pumping power and the effective pump-spot area on cooling are particularly analyzed. At the same time, we make computer simulation about the cooling process and obtain the temperature as a function of the cooling time, which is similar to the experimental results. So this shows that our model is reasonable.
Optical refrigeration using anti-Stokes photoluminescence is now well established, especially for rare-earth-doped solids where cooling to cryogenic temperatures has recently been achieved. The cooling efficiency of optical refrigeration is constrained by the requirement that the increase in entropy of the photon field must be greater than the decrease in entropy of the sample. Laser radiation has been used in all demonstrated cases of optical refrigeration with the intention of minimizing the entropy of the absorbed photons. In this presentation, I will show that as long as the incident radiation is unidirectional, the loss of coherence does not significantly affect the cooling efficiency. Using a general formulation of radiation entropy as the von Neumann entropy of the photon field, I will show how the cooling efficiency depends on the properties of the light source such as wavelength, coherence, and directionality. These results suggest that the laws of thermodynamics permit optical cooling of materials with incoherent sources such as light emitting diodes and filtered sunlight almost as efficiently as with lasers.
Laser cooling of solids with anti-Stokes fluorescence is currently attracting widespread attention because of the wide range of its applications, including all-optical cryocooling for airborne and space-based applications, heat suppression in high-power lasers, and cooling of nanoparticles for biological and mesoscopic physics. This laser cooling process has typically very low (only a few%) efficiency and its enhancement is therefore highly desirable. In this work, we propose to leverage Mie resonance to enhance anti-Stokes fluorescence cooling in RE-doped nanoparticles. As an example, we consider an Yb3+:YAG nanosphere pumped at the long wavelength tail of the Yb3+ absorption spectrum, at 1030 nm. We show that if the radius of the nanosphere is adjusted to the pump wavelength in such a manner that the pump excites some of the Mie resonant modes of the sample, the cooling power density generated in the sample is considerably enhanced and the temperature of the sample is consequently appreciably decreased.