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Physical Review B

Enhanced laser cooling of rare-earth-ion-doped nanocrystalline powders

Xiulin Ruan, Massoud Kaviany

Published Apr 21, 2006• 72 citations
Publisher

Abstract

The enhanced laser cooling performance of rare-earth-ion-doped nanocrystalline powders is predicted, compared to the bulk material, using ${\mathrm{Yb}}^{3+}:{\mathrm{Y}}_{2}{\mathrm{O}}_{3}$ 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.

DOI
10.1103/physrevb.73.155422

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Proceedings of SPIE, the International Society for Optical Engineering/Proceedings of SPIE•Mar 10, 2015•7 citations
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.
Nonradiative relaxation and photoluminescence quenching in nanocrystalline powders doped with rare-earth elements are of interest in optical bistability, random laser, and other optoelectronic applications. Here, the luminescence quenching of a one-dimensional random medium made of multilayer nanoparticles (Y2O3) doped with rare-earth elements (Yb3+) is analyzed by considering the transport, transition, and interaction of the fundamental energy carriers. The nonradiative decay and luminescence quenching in random media are enhanced compared to single crystals, due to multiple scattering, enhanced absorption, and low thermal conductivity. The coherent wave treatment is used to calculate the photon absorption, allowing for field enhancement and photon localization. The luminescent and thermal emission is considered as incoherent. The size-dependent absorption coefficient and penetration depth are observed. The nonradiative decay is identified as a multiphonon relaxation process, and is found to be enhanced compared to bulk materials. The luminescence quenching and nonlinear thermal emission, occurring with increasing irradiation intensity, are predicted.
The material metrics for optimal laser cooling of ion-doped solids are derived using atomic and molecular dynamics properties of the constituents. The anti-Stokes process is modeled as an optical phonon coupling of the bound electron, followed by a photon absorption. The transition dipole moment is estimated using a simplified charge-displacement model and the Judd--Ofelt theory of rare-earth ions both suggesting that transitions with high-energy gaps and similar angular momentum states should be used. The electron-phonon coupling is interpreted as a derivative of electronic energy with respect to displacement of the nearest neighboring ligands whose stretching mode frequency is approximated using the molecular data. The Debye-Gaussian model is used for the phonon density of states of diatomic crystal. Then, the Fermi golden rule is used for photon-induced, phonon-assisted electronic transition probability and applied to the cooling rate equation by defining a phonon-assisted transition dipole moment. Based on the material metrics, an example blend is investigated for its cooling performance and a general guide is proposed for selection of better performing laser cooling hosts. Furthermore, the cooling rate limits are discussed and three distinct characteristic times are identified with the photon-induced, phonon-assisted transition time controlling the rate. The metrics guide the selection of host materials for optimal cooling, and predict a noticeable increase in the absorption rate when using a blend of cation atoms.
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.
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.
To overcome the ETU-induced heating and realize efficient and enhanced laser cooling in Ho3+-doped solids, in Section 4.3, we will provide a modified excitation scheme based on ground-state absorption (GSA) of 5I8 Æ 5I7 at around 2.07 μm and ESA of 5I5 Æ 5F5 at around 2.28 μm. Compared with the conventional pumping scheme, the co-pumping scheme ameliorates the cooling performance significantly through alleviating the upconversion-quenching-induced heat [12], that is, the heat-producing 5I5 Ho3+ions are pumped to the 5F5 state by the laser at 2.28 μm. Fortunately, the 5F5 Ho3+ ions barely transit to the lower nearby state and tend to decay radiatively. Therefore, major heat produced in the conventional laser cooling of Ho3+-doped solids is avoided, and both cooling efficiency and cooling power density can be improved. In Section 4.4, we broaden the research domain of optical refrigeration to rare earth ion co-doped systems. Specifically, when Ho3+–Tm3+ co-doped YLiF4 crystals are pumped at around 2.07 μm, Ho3+ ions will populate at the 5I7 manifold. Meanwhile, Tm3+ ions will also be sensitized by absorbing energy transferred from 5I7 Ho3+ ions. Since the average energy of fluorescence photons generated by Tm3+3F4 Æ 3H6 radiative transitions is higher than that generated by Ho3+5I7 Æ 5I8 radiative transitions, energy transfer (ET) from Ho3+ to Tm3+ ions will induce annihilation of host phonons, and bring enhancement in both the cooling efficiency and the cooling power. Therefore, this cooling mechanism is referred next as energy transfer-enhanced laser cooling (ETLC) of solids [11]. 4.2 Conventional Laser Cooling of Holmium- The main upconversion process and the anti-Stokes fluorescence cooling (ASFC) processes of Ho3+-doped fluoride crystals are illustrated in Fig. 4.1. The ground-state (5I8) Ho3+ ions are pumped to the first excited state (5I7) with laser excitations of energy hν (solid red arrow on the left) and then relax thermally among the Stark levels in a timescale of picoseconds with host phonon absorption. Part of the Ho3+5I7 ions de-excite by emitting fluorescence photons of mean energy hν10 (solid blue arrow, ν10 > ν), which accounts for the ASFC process. The rest of the 5I7 Ho3+ ions de-excited and transfer their energy to the neighboring 5I7 Ho3+ ions, causing population accumulation at the third excited state (5I5) with host phonon absorption (solid green arrows). Comparison between the energy mismatch and the host phonon energy (for YLiF4 crystal host, ħω ≈ 450 cm-1) indicates that about two host phonons are annihilated for each ETU process (see Table 4.1).
This paper reports on the characterization of nanocrystalline powders of ytterbium doped YLiF4 for applications in optical refrigeration. Here we used powders with nanocrystals of Yb 3+ concentrations of (10, 15, 20) mol % and lengths (70, 66, 96) nm. Our preliminary spectroscopic measurements did not show an enhancement in the absorption at the long-wavelength tail of the spectra of the nanocrystalline powder when compared with bulk Yb:YLiF4, indicating that the increase of the phonon-assisted excitation is not large enough to play a significant role in cooling in the present conditions. One advantage of nanocrystalline powders over bulk crystals is the possibility of enhancing the absorption by the realization of cavity-less pump recycling through photon localization [1]. While photon localization also increases the reabsorption of the fluorescence depending on the quantum efficiency of the material and can mitigate cooling, it allows the use of crystals of low enough concentrations to avoid deleterious effects such as ion-ion energy transfer followed by quenching. The pump intensity enhancement favors upconversion luminescence to visible wavelengths, which can be used for optical refrigeration and extends the scope of the application for the material. We observed both green and blue emission from the samples and investigate the processes which lead to it. We present the experimental investigation of the nanocrystals’ absorption and emission spectra and the first excited state lifetime measurements, which are used to estimate the nanocrystal’s photoluminescence quantum efficiency.