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arXiv:2312.05199 · Applied Physics Letters

Precision multi-mode microwave spectroscopy of paramagnetic and rare-earth ion spin defects in single crystal calcium tungstate

E. Hartman, Michael Edmund Tobar, Ben T. McAllister, Jeremy Bourhill, Maxim Goryachev

Published Oct 14, 2024• 7 citations
arXivHTMLPDF

Abstract

We present experimental observations of dilute ion spin ensemble defects in a low-loss single crystal cylindrical sample of CaWO4 cooled to 30 mK in temperature. Crystal field perturbations were elucidated by constructing a dielectrically loaded microwave cavity resonator from the crystal. The resonator exhibited numerous whispering gallery modes with high Q-factors of up to 3×107, equivalent to a loss tangent of ∼3×10−8. The low loss allowed precision multi-mode spectroscopy of numerous high Q-factor photon–spin interactions. Measurements between 7 and 22 GHz revealed the presence of Gd3+, Fe3+, and another trace species, inferred to be rare-earth, at concentrations on the order of parts per billion. These findings motivate further exploration of prospective uses of this low-loss dielectric material for applications regarding precision and quantum metrology, as well as tests for beyond standard model physics.

DOI
10.1063/5.0224102

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We present experimental observations of dilute ion spin ensemble defects in a low-loss single crystal cylindrical sample of CaWO4 cooled to 30 mK in temperature. Crystal field perturbations were elucidated by constructing a dielectrically loaded microwave cavity resonator from the crystal. The resonator exhibited numerous whispering gallery modes with high Q-factors of up to 3×107, equivalent to a loss tangent of ∼3×10−8. The low loss allowed precision multi-mode spectroscopy of numerous high Q-factor photon–spin interactions. Measurements between 7 and 22 GHz revealed the presence of Gd3+, Fe3+, and another trace species, inferred to be rare-earth, at concentrations on the order of parts per billion. These findings motivate further exploration of prospective uses of this low-loss dielectric material for applications regarding precision and quantum metrology, as well as tests for beyond standard model physics.
Progress in the emerging field of engineered quantum systems requires the development of devices that can act as quantum memories. The realisation of such devices by doping solid state cavities with paramagnetic ions imposes a trade-off between ion concentration and cavity coherence time. Here, we investigate an alternative approach involving interactions between photons and naturally occurring impurity ions in ultra-pure crystalline microwave cavities exhibiting exceptionally high quality factors. We implement a hybrid Whispering Gallery/Electron Spin Resonance method to perform rigorous spectroscopy of an undoped single-crystal sapphire resonator over the frequency range 8{19 GHz, and at external applied DC magnetic fields up to 0.9 T. Measurements of a high purity sapphire cooled close to 100 mK reveal the presence of Fe3+, Cr3+, and V2+ impurities. A host of electron transitions are measured and identified, including the two-photon classically forbidden quadrupole transition (Δms = 2) for Fe3+, as well as hyperfine transitions of V2+.
Progress in the emerging field of engineered quantum systems requires the development of devices that can act as quantum memories. In this thesis, a novel spectroscopic technique using electron spin resonance (ESR) is presented. Microwave whispering gallery modes (WGM) in cylindrical dielectric resonators are used to probe paramagnetic impurities at millikelvin temperatures under the influence of an applied dc magnetic field. This technique couples the naturally high quality factor and the relatively high magnetic filling factor of WGMs in crystalline hosts. Precision spectroscopy has been performed on a number of dielectric samples including, sapphire, ruby, quartz, yttrium orthosilicate (YSO) and yttrium aluminium garnet (YAG). Spectroscopic characterisation of sapphire reveals trace ion impurities at parts per billion, which have been used to control strong coupling between the WGM doublets. Moreover, time-reversal symmetry breaking has been observed when a WGM interacts with an ESR, a result of selection rules being created as a consequence of conservation of angular momentum. Following this, interactions between WGM microwave photons and spin resonances are shown in a range of systems. Results achieved include coupling between WGM photons and Cr3+ ions in ruby with normal mode splitting on the order of 600 MHz at 13.9 GHz, the coupling of iron group ion impurities to WGM photons in YSO, which also revealed a strong coupling regime with very low magnetic field, and coupling of Er3+ to WGMs in YAG with evidence of dilute ferromagnetism - the first observation of such an effect outside of iron group doped semiconductors. In addition a novel double-post re-entrant cavity is presented, which is able to focus the rf magnetic field into a small sample, in this case a sub-millimetre sized Yttrium Iron Garnet (YIG) ferrite microsphere that supports magnon resonances. Ultra-high cooperatively of 105 between photon and magnon modes is demonstrated at millikelvin temperatures and microwave frequencies. A coupling strength (normal mode splitting) of 2 GHz at 20 GHz, equivalent to 76 cavity linewidths, is achieved for the bright cavity mode. This constitutes about 10% of the photon energy and shows that ultra-strong coupling is possible in spin systems at microwave frequencies.
Progress in the emerging field of engineered quantum systems requires the development of devices that can act as quantum memories. The realisation of such devices by doping solid state cavities with paramagnetic ions imposes a trade-off between ion concentration and cavity coherence time. Here, we investigate an alternative approach involving interactions between photons and naturally occurring impurity ions in ultra-pure crystalline microwave cavities exhibiting exceptionally high quality factors. We implement a hybrid Whispering Gallery/Electron Spin Resonance method to perform rigorous spectroscopy of an undoped single-crystal sapphire resonator over the frequency range 8--19 GHz, and at external applied DC magnetic fields up to 0.9 T. Measurements of a high purity sapphire cooled close to 100 mK reveal the presence of Fe3+^{3+}3+, Cr3+^{3+}3+, and V2+^{2+}2+ impurities. A host of electron transitions are measured and identified, including the two-photon classically forbidden quadrupole transition (Δms=2Δm_s =2Δms​=2) for Fe3+^{3+}3+, as well as hyperfine transitions of V2+^{2+}2+.
Progress in the emerging field of engineered quantum systems requires the development of devices that can act as quantum memories. The realization of such devices by doping solid-state cavities with paramagnetic ions imposes a tradeoff between ion concentration and cavity coherence time. Here, we investigate an alternative approach involving interactions between photons and naturally occurring impurity ions in ultrapure crystalline microwave cavities exhibiting exceptionally high quality factors. We implement a hybrid whispering gallery/electron spin resonance method to perform rigorous spectroscopy of an undoped single-crystal sapphire resonator over the frequency range 8--19 GHz, and at external applied DC magnetic fields up to 0.9 T. Measurements of high-purity sapphire cooled close to 100 mK reveal the presence of Fe3+{}^{3+}3+, Cr3+{}^{3+}3+, and V2+{}^{2+}2+ impurities. A host of electron transitions are measured and identified, including the two-photon classically forbidden quadrupole transition ($\ensuremath{\Delta}{m}_{s}=2$) for Fe3+{}^{3+}3+, as well as hyperfine transitions of V2+{}^{2+}2+.
The microwave properties of a crystalline sapphire dielectric whispering gallery mode resonator have been measured at very low excitation strength (E/ℏω≈1) and low temperatures (T≈30 mK). The measurements were sensitive enough to observe saturation due to a highly detuned electron spin resonance, which limited the loss tangent of the material to about 2×10−8 measured at 13.868 and 13.259 GHz. Small power dependent frequency shifts were also measured which correspond to an added magnetic susceptibility of order 10−9. This work shows that quantum limited microwave resonators with Q-factors >108 are possible with the implementation of a sapphire whispering gallery mode system.
Abstract The low dielectric losses of an isotopically pure single crystal 28Si sample were determined at a temperature of 20 mK and at powers equivalent to that of a single photon. Whispering Gallery Mode (WGM) analysis revealed large Quality Factors of order 2 × 106 (dielectric loss ~5 × 10−7) at high powers, degrading to 7 × 105 (dielectric loss ~1.4 × 10−6) at single photon energy. A very low-loss narrow line width paramagnetic spin flip transition was detected with extreme sensitivity in 28Si, with very small concentration below 1011 cm−3 (less than 10 parts per trillion) and g-factor of 1.995 ± 0.008. Such determination was only possible due to the low dielectric photonic losses combined with the long lifetime of the spin transition (low magnetic loss), which enhances the magnetic AC susceptibility. Such low photonic loss at single photon energy combined with the narrow line width of the spin ensemble, indicate that single crystal 28Si could be an important crystal for future cavity QED experiments.