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arXiv:2209.14693 · Physical Review Letters

Overcoming Temperature Limits in the Optical Cooling of Solids Using Light-Dressed States

Luísa Toledo Tude, Conor N. Murphy, P. R. Eastham

Published Jun 27, 2024• 2 citations
arXivHTMLPDF

Abstract

Laser cooling of solids currently has a temperature floor of 50-100 K. We propose a method that could overcome this using defects, such as diamond color centers, with narrow electronic manifolds and bright optical transitions. It exploits the dressed states formed in strong fields which extend the set of phonon transitions and have tunable energies. This allows an enhancement of the cooling power and diminishes the effect of inhomogeneous broadening. We demonstrate these effects theoretically for the silicon vacancy and the germanium vacancy, and discuss the role of background absorption, phonon-assisted emission, and nonradiative decay.

DOI
10.1103/physrevlett.132.266901

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Laser cooling of solids currently has a temperature floor of 50-100 K. We propose a method that could overcome this using defects, such as diamond color centers, with narrow electronic manifolds and bright optical transitions. It exploits the dressed states formed in strong fields which extend the set of phonon transitions and have tunable energies. This allows an enhancement of the cooling power and diminishes the effect of inhomogeneous broadening. We demonstrate these effects theoretically for the silicon vacancy and the germanium vacancy, and discuss the role of background absorption, phonon-assisted emission, and nonradiative decay.
The established approach to laser cooling of solids relies on anti-Stokes fluorescence, for example from rare earth impurities in glass. Although successful, there is a minimum temperature to which such a process can cool set by the electronic level spacing in the impurity. We propose an alternative method which does not suffer from this limitation. Our approach relies on the formation of dressed states under strong laser driving, which generates a spectrum in which the gaps can be tuned to optimize the heat absorption. This allows for a cooling cycle which operates at any temperature with a power comparable to the maximum dictated by thermodynamic principles. While this cooling cycle will compete with heating due to non-radiative decay and other mechanisms, it could in principle allow laser cooling to temperatures which are unachievable with anti-Stokes fluorescence.
Phonon-assisted anti-Stokes photoluminescence (ASPL) up-conversion lies at the heart of optical refrigeration in solids. The thermal energy contained in the lattice vibrations is taken away by the emitted anti-Stokes photons' ASPL process, resulting in laser cooling of solids. To date, net laser cooling of solids is limited in rare-earth (RE)-doped crystals, glasses, and direct band gap semiconductors. Searching more solid materials with efficient phonon-assisted photoluminescence up-conversion is important to enrich optical refrigeration research. Here, we demonstrate the phonon-assisted PL up-conversion process from the silicon vacancy (SiV) center in diamond for the first time by studying ASPL spectra for the dependence of temperature, laser power, and excitation energy. Although net cooling has not been observed, our results show that net laser cooling might be eventually achieved in diamond by improving the external quantum efficiency to higher than 95%. Our work provides a promising route to investigate the laser cooling effect in diamond.
The cooling of solids by optical means only using anti-Stokes emission has a long history of research and achievements. Such cooling methods have many advantages ranging from no moving parts or fluids through to operation in vacuum and may have applications to cryosurgery. However, achieving large optical cryocooling powers has been difficult to manage except in certain rare-earth crystals but these are mostly toxic and not biocompatible. Through study of the emission and absorption cross sections we find that diamond, containing either nitrogen vacancy (NV) or silicon vacancy defects, shows potential for optical cryocooling and, in particular, NV doping shows promise for optical refrigeration. We study the optical cooling of doped diamond microcrystals ranging 10--250 $\ensuremath{\mu}\mathrm{m}$ in diameter trapped either in vacuum or in water. For the vacuum case we find NV-doped microdiamond optical cooling below room temperature could exceed $|\mathrm{\ensuremath{\Delta}}T|>10$ K for irradiation powers of Pin<100{P}_{\text{in}}<100Pin​<100 mW. We predict that such temperature changes should be easily observed via large alterations in the diffusion constant for optically cryocooled microdiamonds trapped in water in an optical tweezer or via spectroscopic signatures such as the zero-phonon line width or Raman line.
Under appropriate conditions, absorption of light by a solid can initiate a process by which it is cooled. In particular, energy is extracted from a material when its absorption of a photon is followed by emission of a photon of higher energy. This up-conversion requires some of the solid's electrons to garner energy from atomic vibrations. Here, two schemes for laser cooling via localized electronic states are addressed. The first scheme utilizes the ground state and an excited state of a localized center. In this two-level scheme, the cooling process is initiated with photon absorption in the extreme low-energy tail of a localized state's vibrationally broadened absorption spectrum. The subsequent atomic relaxation transfers energy of especially large vibratory atomic strains into electrical energy that is then extracted via photon emission. The second scheme involves the ground state and two excited states of a localized center. Cooling is facilitated when (i) the photoexcitation of an electron from its ground state to the lower excited level is followed by (ii) electron-phonon-induced promotion to the uppermost level and the subsequent (iii) return of the electron to its ground state with emission of a photon of higher energy than that of the absorbed photon. However, competing relaxation processes contribute to heating. The net cooling power per unit volume is maximized for both schemes, thereby determining characteristics of localized electronic systems that foster optical cooling. The cooling power per unit volume is greatest at high temperatures and falls rapidly as the thermal energy is reduced below each system's luminescence Stokes shift. Moreover, cooling via the three-level scheme is most effective when (i) the energy separation between excited states is smaller than the thermal energy and (ii) the degeneracy of the highest-lying excited state is much larger than that of the center's middle level. These restrictive conditions appear to be satisfied for the three-level systems that to date exhibit laser cooling at or somewhat below room temperature: severely localized crystal-field-split fff-electron states of rare-earth ions.
Quantum emitters are an integral component for a broad range of quantum technologies, including quantum communication, quantum repeaters, and linear optical quantum computation. Solid-state color centers are promising candidates for scalable quantum optics due to their long coherence time and small inhomogeneous broadening. However, once excited, color centers often decay through phonon-assisted processes, limiting the efficiency of single-photon generation and photon-mediated entanglement generation. Herein, we demonstrate strong enhancement of spontaneous emission rate of a single silicon-vacancy center in diamond embedded within a monolithic optical cavity, reaching a regime in which the excited-state lifetime is dominated by spontaneous emission into the cavity mode. We observe 10-fold lifetime reduction and 42-fold enhancement in emission intensity when the cavity is tuned into resonance with the optical transition of a single silicon-vacancy center, corresponding to 90% of the excited-state energy decay occurring through spontaneous emission into the cavity mode. We also demonstrate the largest coupling strength (g/2π = 4.9 ± 0.3 GHz) and cooperativity (C = 1.4) to date for color-center-based cavity quantum electrodynamics systems, bringing the system closer to the strong coupling regime.