Microwave Fluorescence Detection of Spin Echoes.

Counting the microwave photons emitted by an ensemble of electron spins when they relax radiatively has recently been proposed as a sensitive method for electron paramagnetic resonance spectroscopy, enabled by the development of operational single microwave photon detectors at millikelvin temperature. Here, we report the detection of spin echoes in the spin fluorescence signal. The echo manifests itself as a coherent modulation of the number of photons spontaneously emitted after a π/2_{X}-τ-π_{Y}-τ-π/2_{Φ} sequence, dependent on the relative phase Φ. We demonstrate experimentally this detection method using an ensemble of Er^{3+} ion spins in a scheelite crystal of CaWO_{4}. We use fluorescence-detected echoes to measure the erbium spin coherence time, as well as the echo envelope modulation due to the coupling to the ^{183}W nuclear spins surrounding each ion. We finally compare the signal-to-noise ratio of inductively detected and fluorescence-detected echoes, and show that it is larger with the fluorescence method.

Single-electron spin resonance detection by microwave photon counting.

Electron spin resonance spectroscopy is the method of choice for characterizing paramagnetic impurities, with applications ranging from chemistry to quantum computing1,2, but it gives access only to ensemble-averaged quantities owing to its limited signal-to-noise ratio. Single-electron spin sensitivity has, however, been reached using spin-dependent photoluminescence3-5, transport measurements6-9 and scanning-probe techniques10-12. These methods are system-specific or sensitive only in a small detection volume13,14, so that practical single-spin detection remains an open challenge. Here, we demonstrate single-electron magnetic resonance by spin fluorescence detection15, using a microwave photon counter at millikelvin temperatures16. We detect individual paramagnetic erbium ions in a scheelite crystal coupled to a high-quality-factor planar superconducting resonator to enhance their radiative decay rate17, with a signal-to-noise ratio of 1.9 in one second integration time. The fluorescence signal shows anti-bunching, proving that it comes from individual emitters. Coherence times up to 3 ms are measured, limited by the spin radiative lifetime. The method has the potential to be applied to arbitrary paramagnetic species with long enough non-radiative relaxation times, and allows single-spin detection in a volume as large as the resonator magnetic mode volume (approximately 10 µm3 in the present experiment), orders of magnitude larger than other single-spin detection techniques. As such, it may find applications in magnetic resonance and quantum computing.

Zeeman spectroscopy and crystal-field analysis of low symmetry centres in Nd3+doped Y2SiO5.

We report on infrared to visible Zeeman absorption spectroscopy and parameterised crystal-field modelling of Nd3+centres in Y2SiO5through the use of experimentally inferred crystal-field energy levels and Zeeman directional electronicgvalues. We demonstrate that good agreement between the calculated and experimental crystal-field energy levels as well as directional Zeemangvalues along all three crystallographic axes can be obtained. Further, we demonstrate that the addition of correlation crystal field effects successfully account for discrepancies that arise between the calculated and experimental values relevant to the2H11/2(2) multiplet in a one-electron crystal field model.

Non-classical correlations over 1250 modes between telecom photons and 979-nm photons stored in 171Yb3+:Y2SiO5.

Quantum repeaters based on heralded entanglement require quantum nodes that are able to generate multimode quantum correlations between memories and telecommunication photons. The communication rate scales linearly with the number of modes, yet highly multimode quantum storage remains challenging. In this work, we demonstrate an atomic frequency comb quantum memory with a time-domain mode capacity of 1250 modes and a bandwidth of 100 MHz. The memory is based on a Y2SiO5 crystal doped with 171Yb3+ ions, with a memory wavelength of 979 nm. The memory is interfaced with a source of non-degenerate photon pairs at 979 and 1550 nm, bandwidth-matched to the quantum memory. We obtain strong non-classical second-order cross correlations over all modes, for storage times of up to 25 µs. The telecommunication photons propagated through 5 km of fiber before the release of the memory photons, a key capability for quantum repeaters based on heralded entanglement and feed-forward operations. Building on this experiment should allow distribution of entanglement between remote quantum nodes, with enhanced rates owing to the high multimode capacity.

Double-heterodyne probing for an ultra-stable laser based on spectral hole burning in a rare-earth-doped crystal.

We present an experimental technique for realizing a specific absorption spectral pattern in a rare-earth-doped crystal at cryogenic temperatures. This pattern is subsequently probed on two spectral channels simultaneously, thereby producing an error signal allowing frequency locking of a laser on the said spectral pattern. Appropriate combination of the two channels leads to a substantial reduction in detection noise, paving the way to realizing an ultra-stable laser for which the detection noise can be made arbitrarily low when using multiple channels. We use this technique to realize a laser with a frequency instability of $ 1.7 \times 1{0^{{\bf - }15}} $1.7×10-15 at 1 s, not limited by the detection noise but by environmental perturbation of the crystal. This is comparable with the lowest instability demonstrated at 1 s to date for rare-earth-doped crystal stabilized lasers.

Optical Spin-Wave Storage in a Solid-State Hybridized Electron-Nuclear Spin Ensemble.

Solid-state impurity spins with optical control are currently investigated for quantum networks and repeaters. Among these, rare-earth-ion doped crystals are promising as quantum memories for light, with potentially long storage time, high multimode capacity, and high bandwidth. However, with spins there is often a tradeoff between bandwidth, which favors electronic spin, and memory time, which favors nuclear spins. Here, we present optical storage experiments using highly hybridized electron-nuclear hyperfine states in ^{171}Yb^{3+}:Y_{2}SiO_{5}, where the hybridization can potentially offer both long storage time and high bandwidth. We reach a storage time of 1.2 ms and an optical storage bandwidth of 10 MHz that is currently only limited by the Rabi frequency of the optical control pulses. The memory efficiency in this proof-of-principle demonstration was about 3%. The experiment constitutes the first optical storage using spin states in any rare-earth ion with electronic spin. These results pave the way for rare-earth based quantum memories with high bandwidth, long storage time, and high multimode capacity, a key resource for quantum repeaters.

Extending Phenomenological Crystal-Field Methods to C_{1} Point-Group Symmetry: Characterization of the Optically Excited Hyperfine Structure of

We show that crystal-field calculations for C_{1} point-group symmetry are possible, and that such calculations can be performed with sufficient accuracy to have substantial utility for rare-earth based quantum information applications. In particular, we perform crystal-field fitting for a C_{1}-symmetry site in ^{167}Er^{3+}:Y_{2}SiO_{5}. The calculation simultaneously includes site-selective spectroscopic data up to 20 000 cm^{-1}, rotational Zeeman data, and ground- and excited-state hyperfine structure determined from high-resolution Raman-heterodyne spectroscopy on the 1.5 µm telecom transition. We achieve an agreement of better than 50 MHz for assigned hyperfine transitions. The success of this analysis opens the possibility of systematically evaluating the coherence properties, as well as transition energies and intensities, of any rare-earth ion doped into Y_{2}SiO_{5}.

All-optical control of long-lived nuclear spins in rare-earth doped nanoparticles.

Nanoscale systems that coherently couple to light and possess spins offer key capabilities for quantum technologies. However, an outstanding challenge is to preserve properties, and especially optical and spin coherence lifetimes, at the nanoscale. Here, we report optically controlled nuclear spins with long coherence lifetimes (T2) in rare-earth-doped nanoparticles. We detect spins echoes and measure a spin coherence lifetime of 2.9 ± 0.3 ms at 5 K under an external magnetic field of 9 mT, a T2 value comparable to those obtained in bulk rare-earth crystals. Moreover, we achieve spin T2 extension using all-optical spin dynamical decoupling and observe high fidelity between excitation and echo phases. Rare-earth-doped nanoparticles are thus the only nano-material in which optically controlled spins with millisecond coherence lifetimes have been reported. These results open the way to providing quantum light-atom-spin interfaces with long storage time within hybrid architectures.

Dispersive heterodyne probing method for laser frequency stabilization based on spectral hole burning in rare-earth doped crystals.

Frequency-locking a laser to a spectral hole in rare-earth doped crystals at cryogenic temperature has been shown to be a promising alternative to the use of high finesse Fabry-Perot cavities when seeking a very high short term stability laser (M. J. Thorpe et al., Nature Photonics 5, 688 (2011)). We demonstrate here a novel technique for achieving such stabilization, based on generating a heterodyne beat-note between a master laser and a slave laser whose dephasing caused by propagation near a spectral hole generate the error signal of the frequency lock. The master laser is far detuned from the center of the inhomogeneous absorption profile, and therefore exhibits only limited interaction with the crystal despite a potentially high optical power. The demodulation and frequency corrections are generated digitally with a hardware and software implementation based on a field-programmable gate array and a Software Defined Radio platform, making it straightforward to address several frequency channels (spectral holes) in parallel.

Low-repetition-rate femtosecond operation in extended-cavity mode-locked Yb:CALGO laser.

We report on an extended-cavity mode-locked laser based on an Yb:CALGO crystal operating either at 27 MHz and 93 fs pulse duration or at 15 MHz and 170 fs duration single-pulse regime. To the best of our knowledge this is the first demonstration of an extended-cavity oscillator based on Yb-doped crystal producing sub-100 fs pulses. The pulse energy was 24 nJ directly at the output of the oscillator (and 17 nJ after compression). Based on a similar design, we also demonstrate an unprecedented double-pulse dual-wavelength femtosecond regime. An explanation of this atypical regime is proposed.

Continuous-wave and femtosecond laser operation of Yb:CaGdAlO4 under high-power diode pumping.

We demonstrate the generation of 68 fs secant hyperbolic pulses at a 105 MHz repetition rate with an average power of 520 mW from a diode-pumped Yb(3+):CaGdAlO(4) mode-locked laser. A semiconductor saturable absorber allows passive mode locking, and a 15 W diode laser is used to pump directly the crystal. To our knowledge this represents the highest average power ever obtained for a sub-100 fs diode-pumped Yb-bulk laser.

47-fs diode-pumped Yb3+:CaGdAlO4 laser.

The experimental demonstration of a diode-pumped passively mode-locked femtosecond laser based on an Yb3+:CaGdAlO4 single crystal is reported. The oscillator is directly diode pumped by a high-brightness 5 W fiber coupled laser diode, and pulses are produced by use of a semiconductor saturable-absorber mirror. It permits the production of pulses as short as 47 fs at 1050 nm, which are to our knowledge the shortest laser pulses obtained from an oscillator based on Yb3+-doped bulk materials. The average power is 38 mW, and the repetition rate is 109 MHz.

Laser oscillation with low quantum defect in Yb:GdVO4, a crystal with high thermal conductivity.

A Yb:GdVO4 single crystal was grown by the Czochralski process. Its thermal conductivity was measured by photothermal analysis and reached 8.1 and 7.1 W m(-1) K(-1) along and perpendicular to the c axis, respectively. These values are in good agreement with the predicted ones. The optical spectroscopy of the crystal, such as its absorption and emission cross sections under the two polarizations, its fluorescence lifetime, and its laser parameters, is investigated. Cw laser oscillation is obtained for what is to our knowledge the first time in this material under titanium sapphire pumping at 984 nm. We obtain 420 mW of output power for a 2% output coupler at 1029 nm. With a thin sample, the laser wavelength decreases to 1015 nm. In this case the quantum defect is as small as 2.9%. The weak heat release of the material suggests good prospects for its use in high-power applications.