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arXiv:2411.16687 · Physical Review Letters

Anomalous Subkelvin Thermal Frequency Shifts of Ultranarrow Linewidth Solid State Emitters

Xiuji Lin, M. T. Hartman, Benjamin Pointard, Rodolphe Le Targat, Philippe Goldner, Signe Louise Seidelin, Bess Fang, Yann Le Coq

Published Oct 29, 2024• 6 citations
arXivHTMLPDF

Abstract

We investigate the frequency response of narrow spectral holes in a doped crystal structure as a function of temperature below 1 K. We identify a particular regime in which this response significantly deviates from the expected two-phonon Raman scattering theory. Namely, near 290 mK, we observed a behavior exhibiting a temperature-dependent frequency shift of zero to first order. This is of particular interest for applications that require high frequency stability, such as laser frequency stabilization, as by operating the scheme at this specific point would result in the spectral hole frequency being highly immune to temperature fluctuations, providing the potential for a laser fractional frequency instability as low as ∼2×10^{-22} at 1 s.

DOI
10.1103/physrevlett.133.183803

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Conference on Lasers and Electro-Optics Europe & European Quantum Electronics Conference (CLEO/Europe-EQEC)•Jun 21, 2021•1 citation
We investigate the frequency response of narrow spectral holes in a doped crystal structure as a function of temperature below 1 K. We identify a particular regime in which this response significantly deviates from the expected two-phonon Raman scattering theory. Namely, near 290 mK, we observed a behavior exhibiting a temperature-dependent frequency shift of zero to first order. This is of particular interest for applications that require high frequency stability, such as laser frequency stabilization, as by operating the scheme at this specific point would result in the spectral hole frequency being highly immune to temperature fluctuations, providing the potential for a laser fractional frequency instability as low as ∼2×10^{-22} at 1 s.
We explore the properties of ultranarrow spectral holes in ensembles of solid-state emitters in crystals over a range of sub-kelvin temperatures, as a new step toward leveraging their exceptional coherence properties more effectively. As an example, we consider the potential gain observed in their application in frequency stabilization schemes. 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 temperature-dependent T7 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.
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.
The possibility of generating a narrow spectral hole in a rare-earth doped crystal opens the gateway to a variety of applications, one of which is the realization of an ultrastable laser. As this is achieved by locking in a prestabilized laser to the narrow hole, a prerequisite is the elimination of frequency fluctuations of the spectral hole. One potential source of such fluctuations can arise from temperature instabilities. However, when the crystal is surrounded by a buffer gas subject to the same temperature as the crystal, the effect of temperature-induced pressure changes may be used to counterbalance the direct effect of temperature fluctuations. For a particular pressure, it is indeed possible to identify a temperature for which the spectral hole resonant frequency is independent of the first-order thermal fluctuations. Here, we measure frequency shifts as a function of temperature for different values of the pressure of the surrounding buffer gas, and identify the ``magic'' environment within which the spectral hole is largely insensitive to temperature.
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.
The coherence properties of optical emitters in crystals are critical for quantum technologies and optical frequency metrology. Cooling to sub-kelvin temperatures can significantly enhance their coherence, making it essential to identify the key parameters governing emitter and host crystal behavior in this ultra cold regime. We investigate a Czochralski-grown europium doped yttrium orthosilicate crystal, and we report measurements of the heat capacity, a parameter fundamental to evaluating thermal noise limits in metrology schemes based on spectral hole stabilization in such samples. In parallel, we characterize optical coherence via photon echo measurements as a function of temperature. Below 1 K, where phonon contributions diminish, two-level systems (TLS) associated with crystal imperfections may emerge as a limiting factor. A linear-in-temperature term in the heat capacity serves as a signature of TLS, and from our data, we establish an upper bound on this contribution. This, combined with the optical homogeneous linewidth from photon-echo measurements being constant in the interval from 300 mK to 2 K demonstrates a minimal TLSrelated effects in our sample. These findings highlight the promise of ultralow-temperature operation for enhancing the performance of optical quantum devices based on doped crystals.
Spectral hole burning in rare earth doped crystal can provide frequency references based on the optical transition of the dopant ions [1] . The narrow spectral patterns can be used to improve laser frequency stabilization [2] , [3] and provide a new generation of ultra-stable lasers with lower thermal noise benefiting from the cryogenic environment and better quality factor of the crystal than the amorphous glass typically used in the Fabry-Perot cavity. We utilize Europium doped yttrium silicon oxide (Eu:YSO) in our experiments, which allow realization of long lived (hours or more depending on temperature) narrow spectral holes ( kHz or less) well suited for high precision experiment applications. We will describe our novel double-heterodyne detection method [4] , used to decrease the detection noise, as well as experiments assessing quantitatively the sensitivity of the spectral pattern to crystal deformation [5] , [6] , application of electric field [7] and temperature fluctuations. We currently demonstrate a state-of-the-art laser frequency stability at 1.7 × 10 − 15 at 1s [4] , limited by the latter effect, for which improvement strategies have been demonstrated elsewhere [2] and which we are currently implementing. The other effects which we have quantitatively studied are compatible with a few 10 − 18 frequency stability at 1s time scale. This work is particularly promising in the context of optical frequency lattice clocks, for which the ultra-stable laser used for probing the clock transition is a strong limiting factor of the frequency stability.