Optically addressable molecular spins for quantum information processing.

Spin-bearing molecules are promising building blocks for quantum technologies as they can be chemically tuned, assembled into scalable arrays, and readily incorporated into diverse device architectures. In molecular systems, optically addressing ground-state spins would enable a wide range of applications in quantum information science, as has been demonstrated for solid-state defects. However, this important functionality has remained elusive for molecules. Here, we demonstrate such optical addressability in a series of synthesized organometallic, chromium(IV) molecules. These compounds display a ground-state spin that can be initialized and read out using light and coherently manipulated with microwaves. In addition, through atomistic modification of the molecular structure, we vary the spin and optical properties of these compounds, indicating promise for designer quantum systems synthesized from the bottom-up.

Correlating dynamic strain and photoluminescence of solid-state defects with stroboscopic x-ray diffraction microscopy.

Control of local lattice perturbations near optically-active defects in semiconductors is a key step to harnessing the potential of solid-state qubits for quantum information science and nanoscale sensing. We report the development of a stroboscopic scanning X-ray diffraction microscopy approach for real-space imaging of dynamic strain used in correlation with microscopic photoluminescence measurements. We demonstrate this technique in 4H-SiC, which hosts long-lifetime room temperature vacancy spin defects. Using nano-focused X-ray photon pulses synchronized to a surface acoustic wave launcher, we achieve an effective time resolution of ~100 ps at a 25 nm spatial resolution to map micro-radian dynamic lattice curvatures. The acoustically induced lattice distortions near an engineered scattering structure are correlated with enhanced photoluminescence responses of optically-active SiC quantum defects driven by local piezoelectric effects. These results demonstrate a unique route for directly imaging local strain in nanomechanical structures and quantifying dynamic structure-function relationships in materials under realistic operating conditions.

Quantum control of surface acoustic-wave phonons.

One of the hallmarks of quantum physics is the generation of non-classical quantum states and superpositions, which has been demonstrated in several quantum systems, including ions, solid-state qubits and photons. However, only indirect demonstrations of non-classical states have been achieved in mechanical systems, despite the scientific appeal and technical utility of such a capability1,2, including in quantum sensing, computation and communication applications. This is due in part to the highly linear response of most mechanical systems, which makes quantum operations difficult, as well as their characteristically low frequencies, which hinder access to the quantum ground state3-7. Here we demonstrate full quantum control of the mechanical state of a macroscale mechanical resonator. We strongly couple a surface acoustic-wave8 resonator to a superconducting qubit, using the qubit to control and measure quantum states in the mechanical resonator. We generate a non-classical superposition of the zero- and one-phonon Fock states and map this and other states using Wigner tomography9-14. Such precise, programmable quantum control is essential to a range of applications of surface acoustic waves in the quantum limit, including the coupling of disparate quantum systems15,16.

Electrometry by optical charge conversion of deep defects in 4H-SiC.

Optically active point defects in various host materials, such as diamond and silicon carbide (SiC), have shown significant promise as local sensors of magnetic fields, electric fields, strain, and temperature. Modern sensing techniques take advantage of the relaxation and coherence times of the spin state within these defects. Here we show that the defect charge state can also be used to sense the environment, in particular high-frequency (megahertz to gigahertz) electric fields, complementing established spin-based techniques. This is enabled by optical charge conversion of the defects between their photoluminescent and dark charge states, with conversion rate dependent on the electric field (energy density). The technique provides an all-optical high-frequency electrometer which is tested in 4H-SiC for both ensembles of divacancies and silicon vacancies, from cryogenic to room temperature, and with a measured sensitivity of [Formula: see text] Finally, due to the piezoelectric character of SiC, we obtain spatial 3D maps of surface acoustic wave modes in a mechanical resonator.

Suppressing Spectral Diffusion of Emitted Photons with Optical Pulses.

In many quantum architectures the solid-state qubits, such as quantum dots or color centers, are interfaced via emitted photons. However, the frequency of photons emitted by solid-state systems exhibits slow uncontrollable fluctuations over time (spectral diffusion), creating a serious problem for implementation of the photon-mediated protocols. Here we show that a sequence of optical pulses applied to the solid-state emitter can stabilize the emission line at the desired frequency. We demonstrate efficiency, robustness, and feasibility of the method analytically and numerically. Taking nitrogen-vacancy center in diamond as an example, we show that only several pulses, with the width of 1 ns, separated by few ns (which is not difficult to achieve) can suppress spectral diffusion. Our method provides a simple and robust way to greatly improve the efficiency of photon-mediated entanglement and/or coupling to photonic cavities for solid-state qubits.

Decoherence of Near-Surface Nitrogen-Vacancy Centers Due to Electric Field Noise.

We show that electric field noise from surface charge fluctuations can be a significant source of spin decoherence for near-surface nitrogen-vacancy (NV) centers in diamond. This conclusion is based on the increase in spin coherence observed when the diamond surface is covered with high-dielectric-constant liquids, such as glycerol. Double-resonance experiments show that improved coherence occurs even though the coupling to nearby electron spins is unchanged when the liquid is applied. Multipulse spin-echo experiments reveal the effect of glycerol on the spectrum of NV frequency noise.

Proton magnetic resonance imaging using a nitrogen-vacancy spin sensor.

Magnetic resonance imaging, with its ability to provide three-dimensional, elementally selective imaging without radiation damage, has had a revolutionary impact in many fields, especially medicine and the neurosciences. Although challenging, its extension to the nanometre scale could provide a powerful new tool for the nanosciences, especially if it can provide a means for non-destructively visualizing the full three-dimensional morphology of complex nanostructures, including biomolecules. To achieve this potential, innovative new detection strategies are required to overcome the severe sensitivity limitations of conventional inductive detection techniques. One successful example is magnetic resonance force microscopy, which has demonstrated three-dimensional imaging of proton NMR with resolution on the order of 10 nm, but with the requirement of operating at cryogenic temperatures. Nitrogen-vacancy (NV) centres in diamond offer an alternative detection strategy for nanoscale magnetic resonance imaging that is operable at room temperature. Here, we demonstrate two-dimensional imaging of (1)H NMR from a polymer test sample using a single NV centre in diamond as the sensor. The NV centre detects the oscillating magnetic field from precessing protons as the sample is scanned past the NV centre. A spatial resolution of ∼12 nm is shown, limited primarily by the scan resolution.

Multipulse double-quantum magnetometry with near-surface nitrogen-vacancy centers.

We discuss multipulse magnetometry that exploits all three magnetic sublevels of the S=1 nitrogen-vacancy center in diamond to achieve enhanced magnetic field sensitivity. Based on dual frequency microwave pulsing, the scheme is twice as sensitive to ac magnetic fields as conventional two-level magnetometry. We derive the spin evolution operator for dual frequency microwave excitation and show its effectiveness for double-quantum state swaps. Using multipulse sequences of up to 128 pulses under optimized conditions, we show enhancement of the SNR by up to a factor of 2 in detecting NMR statistical signals, with a 4× enhancement theoretically possible.

Probing surface noise with depth-calibrated spins in diamond.

Sensitive nanoscale magnetic resonance imaging of target spins using nitrogen-vacancy (NV) centers in diamond requires a quantitative understanding of dominant noise at the surface. We probe this noise by applying dynamical decoupling to shallow NVs at calibrated depths. Results support a model of NV dephasing by a surface bath of electronic spins having a correlation rate of 200 kHz, much faster than that of the bulk N spin bath. Our method of combining nitrogen delta-doping growth and nanoscale depth imaging paves a way for studying spin noise present in diverse material surfaces.

Current-induced spin polarization in anisotropic spin-orbit fields.

The magnitude and direction of current-induced spin polarization and spin-orbit splitting are measured in In0.04Ga0.96 As epilayers as a function of in-plane electric and magnetic fields. We show that, contrary to expectation, the magnitude of the current-induced spin polarization is smaller for crystal directions corresponding to larger spin-orbit fields. Furthermore, we find that the steady-state in-plane spin polarization does not align along the spin-orbit field, an effect due to anisotropy in the spin relaxation rate.

Nanoscale nuclear magnetic resonance with a nitrogen-vacancy spin sensor.

Extension of nuclear magnetic resonance (NMR) to nanoscale samples has been a longstanding challenge because of the insensitivity of conventional detection methods. We demonstrated the use of an individual, near-surface nitrogen-vacancy (NV) center in diamond as a sensor to detect proton NMR in an organic sample located external to the diamond. Using a combination of electron spin echoes and proton spin manipulation, we showed that the NV center senses the nanotesla field fluctuations from the protons, enabling both time-domain and spectroscopic NMR measurements on the nanometer scale.

Spin coherence during optical excitation of a single nitrogen-vacancy center in diamond.

We examine the quantum spin state of a single nitrogen-vacancy (NV) center in diamond at room temperature as it makes a transition from the orbital ground state (GS) to the orbital excited state (ES) during nonresonant optical excitation. While the fluorescence readout of NV-center spins relies on conservation of the longitudinal spin projection during optical excitation, the question of quantum phase preservation has not been examined. Using Ramsey measurements and quantum process tomography of the optical excitation process, we measure a trace fidelity of F=0.87±0.03, which includes ES spin dephasing during measurement. Extrapolation to the moment of optical excitation yields F≈0.95. This result provides insight into the interaction between spin coherence and nonresonant optical absorption through a vibronic sideband.

Decoherence-protected quantum gates for a hybrid solid-state spin register.

Protecting the dynamics of coupled quantum systems from decoherence by the environment is a key challenge for solid-state quantum information processing. An idle quantum bit (qubit) can be efficiently insulated from the outside world by dynamical decoupling, as has recently been demonstrated for individual solid-state qubits. However, protecting qubit coherence during a multi-qubit gate is a non-trivial problem: in general, the decoupling disrupts the interqubit dynamics and hence conflicts with gate operation. This problem is particularly salient for hybrid systems, in which different types of qubit evolve and decohere at very different rates. Here we present the integration of dynamical decoupling into quantum gates for a standard hybrid system, the electron-nuclear spin register. Our design harnesses the internal resonance in the coupled-spin system to resolve the conflict between gate operation and decoupling. We experimentally demonstrate these gates using a two-qubit register in diamond operating at room temperature. Quantum tomography reveals that the qubits involved in the gate operation are protected as accurately as idle qubits. We also perform Grover's quantum search algorithm, and achieve fidelities of more than 90% even though the algorithm run-time exceeds the electron spin dephasing time by two orders of magnitude. Our results directly allow decoherence-protected interface gates between different types of solid-state qubit. Ultimately, quantum gates with integrated decoupling may reach the accuracy threshold for fault-tolerant quantum information processing with solid-state devices.

Measurements of nanoscale domain wall flexing in a ferromagnetic thin film.

We use the high spatial sensitivity of the anomalous Hall effect in the ferromagnetic semiconductor Ga(1-x)Mn(x)As, combined with the magneto-optical Kerr effect, to probe the nanoscale elastic flexing behavior of a single magnetic domain wall in a ferromagnetic thin film. Our technique allows position sensitive characterization of the pinning site density, which we estimate to be ∼10(14) cm(-3). Analysis of single site depinning events and their temperature dependence yields estimates of pinning site forces (10 pN range) as well as the thermal deactivation energy. Our data provide evidence for a much higher intrinsic domain wall mobility for flexing than previously observed in optically probed µm scale measurements.

Spin-seebeck effect: a phonon driven spin distribution.

Here we report on measurements of the spin-Seebeck effect in GaMnAs over an extended temperature range alongside the thermal conductivity, specific heat, magnetization, and thermoelectric power. The amplitude of the spin-Seebeck effect in GaMnAs scales with the thermal conductivity of the GaAs substrate and the phonon-drag contribution to the thermoelectric power of the GaMnAs, demonstrating that phonons drive the spin redistribution. A phenomenological model involving phonon-magnon drag explains the spatial and temperature dependence of the measured spin distribution.

Electrical tuning of single nitrogen-vacancy center optical transitions enhanced by photoinduced fields.

We demonstrate precise control over the zero-phonon optical transition energies of individual nitrogen-vacancy (NV) centers in diamond by applying multiaxis electric fields, via the dc Stark effect. The Stark shifts display surprising asymmetries that we attribute to an enhancement and rectification of the local electric field by photoionized charge traps in the diamond. Using this effect, we tune the excited-state orbitals of strained NV centers to degeneracy and vary the resulting degenerate optical transition frequency by >10 GHz, a scale comparable to the inhomogeneous frequency distribution. This technique will facilitate the integration of NV-center spins within photonic networks.

Spin-light coherence for single-spin measurement and control in diamond.

The exceptional spin coherence of nitrogen-vacancy centers in diamond motivates their function in emerging quantum technologies. Traditionally, the spin state of individual centers is measured optically and destructively. We demonstrate dispersive, single-spin coupling to light for both nondestructive spin measurement, through the Faraday effect, and coherent spin manipulation, through the optical Stark effect. These interactions can enable the coherent exchange of quantum information between single nitrogen-vacancy spins and light, facilitating coherent measurement, control, and entanglement that is scalable over large distances.

Observation of the spin-Seebeck effect in a ferromagnetic semiconductor.

Reducing the heat generated in traditional electronics is a chief motivation for the development of spin-based electronics, called spintronics. Spin-based transistors that do not strictly rely on the raising or lowering of electrostatic barriers can overcome scaling limits in charge-based transistors. Spin transport in semiconductors might also lead to dissipation-less information transfer with pure spin currents. Despite these thermodynamic advantages, little experimental literature exists on the thermal aspects of spin transport in solids. A recent and surprising exception was the discovery of the spin-Seebeck effect, reported as a measurement of a redistribution of spins along the length of a sample of permalloy (NiFe) induced by a temperature gradient. This macroscopic spatial distribution of spins is, surprisingly, many orders of magnitude larger than the spin diffusion length, which has generated strong interest in the thermal aspects of spin transport. Here, the spin-Seebeck effect is observed in a ferromagnetic semiconductor, GaMnAs, which allows flexible design of the magnetization directions, a larger spin polarization, and measurements across the magnetic phase transition. This effect is observed even in the absence of longitudinal charge transport. The spatial distribution of spin currents is maintained across electrical breaks, highlighting the local nature of this thermally driven effect.

Quantum computing with defects.

Identifying and designing physical systems for use as qubits, the basic units of quantum information, are critical steps in the development of a quantum computer. Among the possibilities in the solid state, a defect in diamond known as the nitrogen-vacancy (NV(-1)) center stands out for its robustness--its quantum state can be initialized, manipulated, and measured with high fidelity at room temperature. Here we describe how to systematically identify other deep center defects with similar quantum-mechanical properties. We present a list of physical criteria that these centers and their hosts should meet and explain how these requirements can be used in conjunction with electronic structure theory to intelligently sort through candidate defect systems. To illustrate these points in detail, we compare electronic structure calculations of the NV(-1) center in diamond with those of several deep centers in 4H silicon carbide (SiC). We then discuss the proposed criteria for similar defects in other tetrahedrally coordinated semiconductors.

Spin control of drifting electrons using local nuclear polarization in ferromagnet-semiconductor heterostructures.

We demonstrate methods to locally control the spin rotation of moving electrons in a GaAs channel. The Larmor frequency of optically injected spins is modulated when the spins are dragged through a region of spin-polarized nuclei created at a MnAs/GaAs interface. The effective field created by the nuclei is controlled either optically or electrically using the ferromagnetic proximity polarization effect. Spin rotation is also tuned by controlling the carrier traverse time through the polarized region. We demonstrate coherent spin rotations of 5π   rad during transport.