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 Fe 3+ , Cr 3+ , and V 2+ impurities. A host of electron transitions are measured and identified, including the two-photon classically forbidden quadrupole transition (∆ms = 2) for Fe 3+ , as well as hyperfine transitions of V 2+ .

We present new results on a cryogenic solid-state maser frequency standard, which relies on the excitation of whispering gallery (WG) modes within a doped monocrystalline sapphire resonator (alpha-Al2O3). Included substitutively within the highest purity HEMEX-grade sapphire crystal lattice are Fe2+ impurities at a concentration of parts per million, an unavoidable result of the manufacturing process. Mass conversion of Fe2+ to Fe3+ ions was achieved by thermally annealing the sapphire in air. Above-threshold maser oscillation was then excited in the resonator at zero applied DC magnetic field by pumping high-Q WG modes coincident in frequency with the electron spin resonance (ESR) energy levels of the Fe3+ spin population. A 2 stage annealing process was undertaken for a sapphire resonator with exceptionally low Fe3+ concentration, resulting in an improvement of 6 orders of magnitude in output power for this particular crystal, and exceeding the previous best implementation of our scheme in another crystal by nearly 20 dB. This represents an output signal 7 orders of magnitude more powerful than a typical commercial hydrogen maser. At this power level, we estimate a limit on the frequency stability of order 1 x 10(-17)/square root(tau) due to the Schawlow-Townes fundamental thermal noise limit.

We report observations of the Schawlow-Townes noise limit in a cryogenic sapphire secondary frequency standard. The effect causes a fundamental limit to the frequency stability, and was measured through the novel excitation of a bimodal maser oscillation of a Whispering Gallery doublet at 12.04 GHz. The beat frequency of 10 kHz between the oscillations enabled a sensitive probe for this measurement of fractional frequency instability of 10(-14) tau(-1/2) with only 0.5 pW of output power.