Monte Carlo fluorescence ray tracing simulation for laser cooling of solids.

We propose an approach to evaluate solid-state media for laser cooling by anti-Stokes fluorescence employing a Monte Carlo-based simulation of fluorescence ray tracing. This approach prompted a revisit of the experimental method, laser-induced thermal modulation spectroscopy (LITMoS), showing that the external quantum efficiency and the background absorption coefficient can be retrieved solely from the two wavelengths where neither cooling nor heating is observed. Our simulation can accurately compute two experimentally inaccessible quantities essential to evaluate laser-cooling media: the mean fluorescence wavelength and the fluorescence escape efficiency. These computed quantities in combination with LITMoS results allow us to retrieve the internal quantum efficiency which is a performance indicator independent of various factors such as the sample size and doping level. Using the proposed approach, we thoroughly investigate the impact of doping level, sample geometry, and refractive index on the fluorescence escape efficiency and reveal its temperature dependency for the example of Yb:YLF. Through comprehensive numerical analysis, we demonstrate that the reduction of sample symmetry is crucial in achieving lower cooling temperatures.

Laser cooling in Yb:KY3F10: a comparison with Yb:YLF.

Laser cooling by anti-Stokes fluorescence is a technology to realize all-solid-state optical cryocoolers. We grew Yb3+-doped KY3F10 (Yb:KYF) crystals as novel laser cooling media and compare their cooling performance to Yb3+-doped LiYF4 (Yb:YLF) crystals also grown in our institute. We present temperature-dependent absorption and emission cross sections as well as the fluorescence lifetime of Yb:KYF, and calculate its material figure-of-merit for laser cooling. Yb:KYF exhibits a higher figure-of-merit than Yb:YLF at temperatures below 200 K. This is because, in contrast to Yb:YLF, the excitation transition from the second-highest Stark level of the ground state is best-suited for cryogenic cooling in Yb:KYF. Thus, it has the potential to achieve unprecedentedly low temperatures below the boiling point of liquid nitrogen. In this work, we observe the first laser cooling of Yb:KYF, and obtain a background absorption coefficient of ∼10-4 cm-1, which is among the lowest ever reported for Yb3+-doped fluoride crystals. A simple model calculation predicts that our Yb:KYF and Yb:YLF crystals can potentially be cooled down to ≈100 K in a high-power cooling setup. Our Yb:KYF crystals still leave room for further improvement through the optimization of the growth process and the use of purer raw materials.

Solid-state laser cooling in Yb:CaF2 and Yb:SrF2 by anti-Stokes fluorescence.

We report on the first example, to the best of our knowledge, of solid-state laser cooling in ytterbium-doped CaF2 and SrF2 crystals by anti-Stokes fluorescence. The crystals were grown by the Czochralski method in a fluorine-rich atmosphere to prevent the formation of divalent ytterbium ions. Using laser-induced thermal modulation spectroscopy (LITMoS), we find the cooling efficiencies for both crystals to be higher than 3% at room temperature. According to model calculations performed using temperature-dependent spectroscopic data, these crystals can be cooled to temperatures as low as 150 K when excited at around 1030 nm.

Temperature-dependent radiative lifetime of Yb:YLF: refined cross sections and potential for laser cooling.

We revisit the spectroscopic characterization of ytterbium-doped LiYF4 (Yb:YLF) for the application of laser cooling. Time-dependent fluorescence spectroscopy reveals a temperature dependence of the radiative lifetime which we explain by the Boltzmann distribution of excited ions in the upper Stark levels. The emission cross sections of Yb:YLF from 17 K to 440 K are revised using the temperature-dependent radiative lifetimes from fluorescence spectra. We provide fit equations for the peak values of important transitions as a function of temperature, which is also useful for the design of Yb:YLF laser oscillators and amplifiers operated at cryogenic temperatures. Based on our spectroscopic data, we show the prerequisite crystal purity to achieve laser cooling below liquid nitrogen temperatures.