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 tune the spin and optical properties of these compounds, paving the way for designer quantum systems synthesized from the bottom-up.
Optically addressable spins are a promising platform for quantum information science due to their combination of a long-lived qubit with a spin-optical interface for external qubit control and read out. The ability to chemically synthesize such systems - to generate optically addressable molecular spins - offers a modular qubit architecture which can be transported across different environments, and atomistically tailored for targeted applications through bottom-up design and synthesis. Here we demonstrate how the spin coherence in such optically addressable molecular qubits can be controlled …
Optically connecting quantum bits can effectively reduce decoherence and facilitate long-distance communication. Optically addressable spin-bearing molecules have been demonstrated to have a good potential for quantum computing. In this report optically induced exchange interactions and spin dynamics, which are inherently important for spin-based quantum computing, have been calculated for a bi-radical - a potential quantum computing circuit unit. Consistent with the previous experimental observation of spin coherence induced by optical excitation, our work demonstrated an optically driven qua…
Coherent Microwave Control of Optically Addressable Donor Qubits in ZnO
University of Washington（华盛顿大学）；University of Wisconsin-Madison（威斯康星大学麦迪逊分校）；California Institute of Technology（加州理工学院）；Institute for Quantum Information and Matter, California Institute of Technology（加州理工学院量子信息与物质研究所）；University of Tokyo（东京大学）；RIKEN（理化学研究所）
Solid-state defect qubit systems with spin-photon interfaces show great promise for quantum information and metrology applications. Photon collection efficiency, however, presents a major challenge for defect qubits in high refractive index host materials. Inverse-design optimization of photonic devices enables unprecedented flexibility in tailoring critical parameters of a spin-photon interface including spectral response, photon polarization and collection mode. Further, the design process can incorporate additional constraints, such as fabrication tolerance and material processing limitatio…
Optically Addressable Molecular Spins at 2D Surfaces
HUN-REN Wigner Research Centre for Physics（匈牙利科学院维格纳研究物理中心）；ELTE Eötvös Loránd University（罗兰大学）；University of Stuttgart（斯图加特大学）；Max Planck Institute for Solid State Research（马克斯·普朗克固体研究所）
Optically detected and radio wave-controlled spin chemistry in flavoproteins
Technical University of Munich, TUM School of Natural Sciences, Chemistry Department（慕尼黑工业大学）；Munich Center for Quantum Science and Technology (MCQST)（慕尼黑量子科学与技术中心）；Albert Ludwigs-Universität Freiburg, Institute of Physical Chemistry（弗赖堡大学）；Marburg University, Chemistry Department（马尔堡大学）
We show that several qubits can be integrated in a single magnetic ion, using its internal electronic spin states with energies tuned by a suitably chosen molecular environment. This approach is illustrated with a nearly-isotropic Gd(III) ion entrapped in a polyoxometalate molecule. Experiments with microwave technologies, either three dimensional cavities or quantum superconducting circuits, show that this magnetic molecule possesses the number of spin states and the set of coherently addressable transitions connecting these states that are needed to perform a universal three-qubit processor …
Artificial magnetic molecules are suitable hosts to one or several spin qubits, which could then implement small-scale algorithms. In order to become of practical use, such molecular spin processors need to increase the dimension $d$ of the available computational space and fulfill the highly demanding conditions that warrant universal operations. Here, we design, synthesize and fully characterize dissymetric molecular dimers hosting either one or two Gd(III) ions. The strong sensitivity of Gd(III) magnetic anisotropy to the symmetry of its local coordination gives rise to different zero-field…
Silicon carbide has recently been developed as a platform for optically addressable spin defects. In particular, the neutral divacancy in the 4H polytype displays an optically addressable spin-1 ground state and near-infrared optical emission. Here, we present the Purcell enhancement of a single neutral divacancy coupled to a photonic crystal cavity. We utilize a combination of nanolithographic techniques and a dopant-selective photoelectrochemical etch to produce suspended cavities with quality factors exceeding 5,000. Subsequent coupling to a single divacancy leads to a Purcell factor of ~50…
Optically addressable spins in materials are important platforms for quantum technologies, such as repeaters and sensors. Identification of such systems in two-dimensional (2d) layered materials offers advantages over their bulk counterparts, as their reduced dimensionality enables more feasible on-chip integration into devices. Here, we report optically detected magnetic resonance (ODMR) from previously identified carbon-related defects in 2d hexagonal boron nitride (hBN). We show that single-defect ODMR contrast can be as strong as 6% and displays a magnetic-field dependence with both positi…
Optically addressable spins associated with defects in wide-bandgap semiconductors are versatile platforms for quantum information processing and nanoscale sensing, where spin-dependent inter-system crossing (ISC) transitions facilitate optical spin initialization and readout. Recently, the van der Waals material hexagonal boron nitride (h-BN) has emerged as a robust host for quantum emitters (QEs), but spin-related effects have yet to be observed. Here, we report room-temperature observations of strongly anisotropic photoluminescence (PL) patterns as a function of applied magnetic field for s…
Silicon carbide (SiC) has become a key player in realization of scalable quantum technologies due to its ability to host optically addressable spin qubits and wafer-size samples. Here, we have demonstrated optically detected magnetic resonance (ODMR) with resonant excitation, and clearly identified the ground state energy levels of the NV centers in 4H-SiC. Coherent manipulation of NV centers in SiC has been achieved with Rabi and Ramsey oscillations. Finally, we show the successful generation and characterization of single nitrogen vacancy (NV) center in SiC employing ion implantation. Our re…
Optically-addressable solid-state spin defects are promising candidates for storing and manipulating quantum information using their long coherence ground state manifold; individual defects can be entangled using photon-photon interactions, offering a path toward large scale quantum photonic networks. Quantum computing protocols place strict limits on the acceptable photon losses in the system. These low-loss requirements cannot be achieved without photonic engineering, but are attainable if combined with state-of-the-art nanophotonic technologies. However, most materials that host spin defect…
Optically active spin defects in wide-bandgap materials have many potential applications in quantum information and quantum sensing. Spin defects in two-dimensional layered van der Waals materials are just emerging to be investigated. Here we demonstrate that optically-addressable spin ensembles in hexagonal boron nitride (hBN) can be generated by femtosecond laser irradiation. We observe optically detected magnetic resonance (ODMR) of hBN spin defects created by laser irradiation. We show that the creation of spin defects in hBN is strongly affected by the pulse energy of the femtosecond lase…
Hyperfine spectroscopy and fast, all-optical arbitrary state initialization and readout of a single, ten-level ${}^{73}$Ge vacancy nuclear spin qudit in diamond
We demonstrate that the spin of optically addressable point defects can be coherently driven with AC electric fields. Based on magnetic-dipole forbidden spin transitions, this scheme enables spatially confined spin control, the imaging of high-frequency electric fields, and the characterization of defect spin multiplicity. While we control defects in SiC, these methods apply to spin systems in many semiconductors, including the nitrogen-vacancy center in diamond. Electrically driven spin resonance offers a viable route towards scalable quantum control of electron spins in a dense array.
In a radiative Auger process, optical decay is accompanied by simultaneous excitation of other carriers. The radiative Auger process gives rise to weak red-shifted satellite peaks in the optical emission spectrum. These satellite peaks have been observed over a large spectral range: in the X-ray emission of atoms; close to visible frequencies on donors in semiconductors and quantum emitters; and at infrared frequencies as shake-up lines in two-dimensional systems. So far, all the work on the radiative Auger process has focussed on detecting the spontaneous emission. However, the fact that the …
We study the physics of a magnetic molecule described by a "giant" spin with multiple ($d > 2$) spin states interacting with the quantized cavity field produced by a superconducting resonator. By means of the input-output formalism, we derive an expression for the output modes in the dispersive regime of operation. It includes the effect of magnetic anisotropy, which makes different spin transitions addressable. We find that the measurement of the cavity transmission allows to uniquely determine the spin state of the qudits. We discuss, from an effective Hamiltonian perspective, the conditions…
We consider two new quantum gate mechanisms based on nuclear spins in hyperpolarized solid $^{129}Xe$ and HCl mixtures and inorganic semiconductors. We propose two schemes for implementing a controlled NOT (CNOT) gate based on nuclear magnetic resonance (NMR) spectroscopy and magnetic resonance imaging (MRI) from hyperpolarized solid $^{129}Xe$ and HCl mixtures and optically pumped NMR in semiconductors. Such gates might be built up with particular spins addressable based on MRI techniques and optical pumping and optical detection techniques. The schemes could be useful for implementing actual…
Optically-Induced Modulation and Programming of Diamond Photonic Cavities
Institute of Physics, Swiss Federal Institute of Technology Lausanne (EPFL)（洛桑联邦理工学院物理研究所）；Center of Quantum Science and Engineering, Swiss Federal Institute of Technology Lausanne (EPFL)（洛桑联邦理工学院量子科学与工程中心）；Photonics Research Group, Department of Information Technology (INTEC), Ghent University - IMEC（根特大学信息技朮系光子研究组（与IMEC联合））；University of Stuttgart（斯图加特大学）
Engineering and Probing a One-Dimensional Dipolar Spin Ensemble in Diamond
University of California, Santa Barbara（加州大学圣塔芭芭拉分校）；California Institute of Technology（加州理工学院）；Stanford University（斯坦福大学）；Harvard University（哈佛大学）；Boston University（波士顿大学）；Max-Planck-Institut für Physik Komplexer Systeme（马克斯·普朗克复杂系统物理研究所）
Realization of devices based on quantum laws might lead to building processors that outperform their classical analogues and establishing unconditionally secure communication protocols. Solids do usually present a serious challenge to quantum coherence. However, owing to their spin-free lattice and low spin orbit coupling, carbon materials and particularly diamond are suitable for hosting robust solid state quantum registers. We show that scalable quantum logic elements can be realized by exploring long range magnetic dipolar coupling between individually addressable single electron spins asso…
The ability to optically initialize the electronic spin of the nitrogen-vacancy (NV) center in diamond has long been considered a valuable resource to enhance the polarization of neighboring nuclei, but efficient polarization transfer to spin species outside the diamond crystal has proven challenging. Here we demonstrate variable-magnetic-field, microwave-enabled cross-polarization from the NV electronic spin to protons in a model viscous fluid in contact with the diamond surface. Slight changes in the cross-relaxation rate as a function of the wait time between successive repetitions of the t…
Correlating spin and optical properties of quantum emitters in hBN
University of Technology Sydney（悉尼科技大学）；ARC Centre of Excellence for Transformative Meta-Optical Systems（变革性超光学系统卓越研究中心）；National Institute for Materials Science（国立材料研究所）
Cold inelastic collisions between confined cesium (Cs) atoms and Cs$\_2$ molecules are investigated inside a CO$\_2$ laser dipole trap. Inelastic atom-molecule collisions can be observed and measured with a rate coefficient of $\sim 2.5 \times 10^{-11} $cm$^3$ s$^{-1}$, mainly independent of the molecular ro-vibrational state populated. Lifetimes of purely atomic and molecular samples are essentially limited by rest gas collisions. The pure molecular trap lifetime ranges 0,3-1 s, four times smaller than the atomic one, as is also observed in a pure magnetic trap. We give an estimation of the i…
Optically addressable spins in widebandgap semiconductors have become one of the most prominent platforms for exploring fundamental quantum phenomena. While several candidates in 3D crystals including diamond and silicon carbide have been extensively studied, the identification of spindependent processes in atomically thin 2D materials has remained elusive. Although optically accessible spin states in hBN are theoretically predicted, they have not yet been observed experimentally. Here, employing rigorous electron paramagnetic resonance techniques and photoluminescence spectroscopy, we identif…
The silicon-vacancy center in diamond offers attractive opportunities in quantum photonics due to its favorable optical properties and optically addressable electronic spin. Here, we combine both to achieve all-optical coherent control of its spin states. We utilize this method to explore spin dephasing effects in an impurity-rich sample beyond the limit of phonon-induced decoherence: Employing Ramsey and Hahn-echo techniques at 12mK base temperature we identify resonant coupling to a substitutional nitrogen spin bath as the limiting decoherence source for the electron spin.
Molecular imaging refers to a class of noninvasive biomedical imaging techniques with the sensitivity and specificity to image biochemical variations in-vivo. An ideal molecular imaging technique visualizes a biochemical target according to a range of criteria, including high spatial and temporal resolution, high contrast relative to non-targeted tissues, depth-independent penetration into tissue, lack of harm to the organism under study, and low cost. Because no existing molecular imaging modality is ideal for all purposes, new imaging approaches are needed. Here we demonstrate a novel molecu…
Optically addressable spin defects in wide-bandage semiconductors as promising systems for quantum information and sensing applications have attracted more and more attention recently. Spin defects in two-dimensional materials are supposed to have unique superiority in quantum sensing since their atomatic thickness. Here, we demonstrate that the negatively boron charged vacancy (V$ _\text{B}^{-} $) with good spin properties in hexagonal boron nitride can be generated by ion implantation. We carry out optically detected magnetic resonance measurements at room temperature to characterize the spi…
Quantum networks based on optically addressable spin qubits promise to enable secure communication, distributed quantum computing, and tests of fundamental physics. Scaling up quantum networks based on solid-state luminescent centers requires coherent spin and optical transitions coupled to photonic resonators. Here we investigate single $\mathrm{{}^{171}Yb^{3+}}$ ions in yttrium orthovanadate coupled to a nanophotonic cavity. These ions possess optical and spin transitions that are first-order insensitive to magnetic field fluctuations, enabling optical linewidths less than 1 MHz and spin coh…
Solid-state nuclear spins surrounding individual, optically addressable qubits provide a crucial resource for quantum networks, computation and simulation. While hosts with sparse nuclear spin baths are typically chosen to mitigate qubit decoherence, developing coherent quantum systems in nuclear spin-rich hosts enables exploration of a much broader range of materials for quantum information applications. The collective modes of these dense nuclear spin ensembles provide a natural basis for quantum storage, however, utilizing them as a resource for single spin qubits has thus far remained elus…
