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.

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.

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.

We investigated the influence of Yb2+ on the spectroscopic properties of Yb:CaF2. A strong nonradiative decay of Yb3+ was observed in an Yb2+-rich crystal, so Yb2+ is highly detrimental for lasing and optical refrigeration.

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