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arXiv:2504.21422 · Physical Review Applied

From heat capacity to coherence in ultranarrow-linewidth solid-state optical emitters at subkelvin temperatures

Diana Serrano, T. Klein, C. Marcenat, Philippe Goldner, M. T. Hartman, Bess Fang, Yann Le Coq, Signe Louise Seidelin

Published Mar 16, 2026• 0 citations
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Abstract

The coherence properties of optical emitters in crystals are crucial for quantum technologies and optical frequency metrology. Cooling to sub-kelvin temperatures can markedly enhance coherence, making it important to identify the parameters governing emitter and host crystal behavior in this regime. We investigate a Czochralski-grown europium-doped yttrium orthosilicate crystal, reporting measurements of its heat capacity and optical coherence. Heat capacity not only informs thermal noise limits in metrology schemes but can also reveal two-level systems (TLS) arising from crystal imperfections via a linear-in-temperature term. Below 1 K, where phonon contributions are suppressed, TLS can drive decoherence, leading to a linear broadening of the homogeneous linewidth. From our data, we place an upper bound on the TLS contribution. This, together with constant optical linewidths between 300 mK and 2 K measured via photon-echo lifetimes, is consistent with a minimal TLS effects in our sample. A low level of TLS is particularly important for the performance of optical quantum devices based on doped crystals, since their presence could otherwise limit further improvements in coherence at sub-kelvin temperatures.

DOI
10.1103/vj7j-jp9y

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The coherence properties of optical emitters in crystals are crucial for quantum technologies and optical frequency metrology. Cooling to sub-kelvin temperatures can markedly enhance coherence, making it important to identify the parameters governing emitter and host crystal behavior in this regime. We investigate a Czochralski-grown europium-doped yttrium orthosilicate crystal, reporting measurements of its heat capacity and optical coherence. Heat capacity not only informs thermal noise limits in metrology schemes but can also reveal two-level systems (TLS) arising from crystal imperfections via a linear-in-temperature term. Below 1 K, where phonon contributions are suppressed, TLS can drive decoherence, leading to a linear broadening of the homogeneous linewidth. From our data, we place an upper bound on the TLS contribution. This, together with constant optical linewidths between 300 mK and 2 K measured via photon-echo lifetimes, is consistent with a minimal TLS effects in our sample. A low level of TLS is particularly important for the performance of optical quantum devices based on doped crystals, since their presence could otherwise limit further improvements in coherence at sub-kelvin temperatures.
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We explore the properties of ultra-narrow spectral holes in ensembles of solid-state emitters in crystals over a range of sub-kelvin temperatures, with a focus on their potential application in frequency stabilization schemes as an alternative to ultrastable cavities. We investigate how the parameters used to burn the spectral hole impact its shape, and how these factors determine the minimum achievable linewidth. In addition to the stability of the hole's center frequency, the linewidth and contrast play a crucial role in frequency locking. At sub-kelvin temperatures, the temperaturedependent T^7 broadening from two-phonon Raman scattering is expected to be negligible, and the spectral hole's linewidth should therefore remain constant in this interval. We observe however a linear broadening with increasing temperature, highlighting the need for further investigation into the mechanisms governing the linewidth at ultra-low temperatures.
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The transportable quantum memory is a feasible solution for realizing the long-distance quantum communication, which requires a storage lifetime of the order of hours. The isotope-enriched 151Eu3+:Y2SiO5 crystal is a promising candidate for this application. However, its optical storage efficiency and spin storage lifetime are limited by the wide inhomogeneous linewidth. In this work, we successfully grow isotope-enriched 151Eu3+:Y2SiO5 crystals with varying doping concentrations by utilizing the Czochralski method. The optical inhomogeneous broadening and spin inhomogeneous broadening are measured by the optical absorption spectroscopy and optically detected magnetic resonance tests, respectively. Notably, in the undoped samples, we identify a baseline level of inhomogeneous linewidths, happening at (390 ± 15) MHz for optical inhomogeneous broadening and (4.6 ± 0.2) kHz for spin inhomogeneous broadening. Our findings reveal that the point defects, induced by the doping ions, significantly contribute to the inhomogeneous broadening. For every increase of 10–6 in doping concentration, the optical inhomogeneous broadening increases by 0.97 MHz, and the spin inhomogeneous broadening increases by 0.014 kHz. Furthermore, we discuss the influence of dislocations on inhomogeneous broadening and propose potential strategies to further mitigate these effects. These advancements are expected to promote the development of ultra-long-lifetime transportable quantum memory applications.
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