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.

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.

Spin Fine Structure Reveals Biexciton Geometry in an Organic Semiconductor.

In organic semiconductors, biexcitons are key intermediates in carrier multiplication and exciton annihilation. Their local geometry governs their electronic properties and yet has been challenging to determine. Here, we access the structure of the recently discovered S=2 quintet biexciton state in an organic semiconductor using broadband optically detected magnetic resonance. We correlate the experimentally extracted spin structure with the molecular crystal geometry to identify the specific molecular pairings on which biexciton states reside.

Multimode Storage of Quantum Microwave Fields in Electron Spins over 100 ms.

We report long coherence times (up to 300 ms) for near-surface bismuth donor electron spins in silicon coupled to a superconducting microresonator, biased at a clock transition. This enables us to demonstrate the partial absorption of a train of weak microwave fields in the spin ensemble, their storage for 100 ms, and their retrieval, using a Hahn-echo-like protocol. Phase coherence and quantum statistics are preserved in the storage.

Two-pulse photon echo area theorem in an optically dense medium.

We perform a theoretical and experimental study of the two-pulse photon echo area conservation law in an optically dense medium. The experimental properties of the echo signal are studied at 4K on the optical transition  3H 6(1)→3H 4(1) (793 nm) of Tm 3+ in a YAG crystal for a wide range of pulse areas of the two incoming light pulses, up to θ 1 r o x4π and θ 2≈7π respectively, with optical depth 1.5. We analyze the experimental data by using the analytic solution of the photon echo area theorem for plane waves. We find that the transverse Gaussian spatial profile of the beam leads to an attenuation of the echo area nutation as function of θ1 and θ2. Additional spatial filtering of the photon echo beam allows to recover this nutation. The experimental data are in good agreement with the solution of photon echo pulse area theorem for weak incoming pulse areas θ 1,2≲π. However at higher pulse areas, the observations diverge from the analytic solution requiring further theoretical and experimental studies.

Selective Optical Addressing of Nuclear Spins through Superhyperfine Interaction in Rare-Earth Doped Solids.

In Er^{3+}:Y_{2}SiO_{5}, we demonstrate the selective optical addressing of the ^{89}Y^{3+} nuclear spins through their superhyperfine coupling with the Er^{3+} electronic spins possessing large Landé g factors. We experimentally probe the electron-nuclear spin mixing with photon echo techniques and validate our model. The site-selective optical addressing of the Y^{3+} nuclear spins is designed by adjusting the magnetic field strength and orientation. This constitutes an important step towards the realization of long-lived solid-state qubits optically addressed by telecom photons.

Strain-mediated ion-ion interaction in rare-earth-doped solids.

It was recently shown that the optical excitation of rare-earth ions produces a local change of the host matrix shape, attributed to a change of the rare-earth ion's electronic orbital geometry. In this work we investigate the consequences of this piezo-orbital backaction and show from a macroscopic model how it yields a disregarded ion-ion interaction mediated by mechanical strain. This interaction scales as1/r3, similarly to the other archetypal ion-ion interactions, namely electric and magnetic dipole-dipole interactions. We quantitatively assess and compare the magnitude of these three interactions from the angle of the instantaneous spectral diffusion mechanism, and re-examine the scientific literature in a range of rare-earth doped systems in the light of this generally underestimated contribution.

Emission of photon echoes in a strongly scattering medium.

We observe the two- and three-pulse photon echo emission from a scattering powder, obtained by grinding a Pr3+:Y2SiO5 rare earth doped single crystal. We show that the collective emission is coherently constructed over several grains. A well defined atomic coherence can therefore be created between randomly placed particles. Observation of photon echo on powders as opposed to bulk materials opens the way to faster material development. More generally, time-domain resonant four-wave mixing offers an attractive approach to investigate coherent propagation in scattering media.

Storage and retrieval of single photons transmitted between remote quantum memories.

An elementary quantum network operation involves storing a qubit state in an atomic quantum memory node, and then retrieving and transporting the information through a single photon excitation to a remote quantum memory node for further storage or analysis. Implementations of quantum network operations are thus conditioned on the ability to realize matter-to-light and/or light-to-matter quantum state mappings. Here we report the generation, transmission, storage and retrieval of single quanta using two remote atomic ensembles. A single photon is generated from a cold atomic ensemble at one site , and is directed to another site through 100 metres of optical fibre. The photon is then converted into a single collective atomic excitation using a dark-state polariton approach. After a programmable storage time, the atomic excitation is converted back into a single photon. This is demonstrated experimentally, for a storage time of 0.5 microseconds, by measurement of an anti-correlation parameter. Storage times exceeding ten microseconds are observed by intensity cross-correlation measurements. This storage period is two orders of magnitude longer than the time required to achieve conversion between photonic and atomic quanta. The controlled transfer of single quanta between remote quantum memories constitutes an important step towards distributed quantum networks.

Saturation-induced coherence loss in coherent backscattering of light.

We use coherent backscattering of light by cold strontium atoms to study phase-breaking mechanisms in the multiple-scattering regime. As the probe light intensity is increased, the atomic optical transition starts to be saturated. Nonlinearities and inelastic scattering then occur. The latter induces a characteristic phase-breaking time that reduces the wave coherence. In our experiment, this leads to a strong reduction of the enhancement factor of the coherent backscattering cone. The results at different probe detuning are also presented.

Quantum interference of electromagnetic fields from remote quantum memories.

We observe quantum, Hong-Ou-Mandel, interference of fields produced by two remote atomic memories. High-visibility interference is obtained by utilizing the finite atomic memory time in four-photon delayed coincidence measurements. Interference of fields from remote atomic memories is a crucial element in protocols for scalable entanglement distribution.

Dual-species matter qubit entangled with light.

We propose and demonstrate an atomic qubit based on a cold 85Rb-87Rb isotopic mixture, entangled with a frequency-encoded optical qubit. The interface of an atomic qubit with a single spatial light mode, and the ability to independently address the two atomic qubit states, should provide the basic interferometrically robust element of a quantum network.

Quantum telecommunication based on atomic cascade transitions.

A quantum repeater at telecommunications wavelengths with long-lived atomic memory is proposed, and its critical elements are experimentally demonstrated using a cold atomic ensemble. Via atomic cascade emission, an entangled pair of 1.53 microm and 780 nm photons is generated. The former is ideal for long-distance quantum communication, and the latter is naturally suited for mapping to a long-lived atomic memory. Together with our previous demonstration of photonic-to-atomic qubit conversion, both of the essential elements for the proposed telecommunications quantum repeater have now been realized.

Entanglement of remote atomic qubits.

We report observations of entanglement of two remote atomic qubits, achieved by generating an entangled state of an atomic qubit and a single photon at site , transmitting the photon to site in an adjacent laboratory through an optical fiber, and converting the photon into an atomic qubit. Entanglement of the two remote atomic qubits is inferred by performing, locally, quantum state transfer of each of the atomic qubits onto a photonic qubit and subsequent measurement of polarization correlations in violation of the Bell inequality [EQUATION: SEE TEXT]. We experimentally determine [EQUATION: SEE TEXT]. Entanglement of two remote atomic qubits, each qubit consisting of two independent spin wave excitations, and reversible, coherent transfer of entanglement between matter and light represent important advances in quantum information science.

Observation of dark state polariton collapses and revivals.

By time-dependent variation of a control field, both coherent and single-photon states of light are stored in, and retrieved from, a cold atomic gas. The efficiency of retrieval is studied as a function of the storage time in an applied magnetic field. A series of collapses and revivals is observed, in very good agreement with theoretical predictions. The observations are interpreted in terms of the time evolution of the collective excitation of atomic spin wave and light wave, known as the dark-state polariton.

Deterministic single photons via conditional quantum evolution.

A source of deterministic single photons is proposed and demonstrated by the application of a measurement-based feedback protocol to a heralded single-photon source consisting of an ensemble of cold rubidium atoms. Our source is stationary and produces a photoelectric detection record with sub-Poissonian statistics.

Entanglement of a photon and a collective atomic excitation.

We describe a new experimental approach to probabilistic atom-photon (signal) entanglement. Two qubit states are encoded as orthogonal collective spin excitations of an unpolarized atomic ensemble. After a programmable delay, the atomic excitation is converted into a photon (idler). Polarization states of both the signal and the idler are recorded and are found to be in violation of the Bell inequality. Atomic coherence times exceeding several microseconds are achieved by switching off all the trapping fields--including the quadrupole magnetic field of the magneto-optical trap--and zeroing out the residual ambient magnetic field.