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Hexagonal boron nitride is rapidly gaining interest as a platform for photonic quantum technologies, due to its two-dimensional nature and its ability to host defects deep within its large band gap that may act as room-temperature single-photon emitters. In this review paper we provide an overview of (1) the structure, properties, growth and transfer of hexagonal boron nitride; (2) the creationof colour centres in hexagonal boron nitride and assignment of defects by comparison with ab initio calculations for applications in photonic quantum technologies; and (3) heterostructure devices for the electrical tuning and charge control of colour centres that form the basis for photonic quantum technology devices. The aim of this review is to provide readers a summary of progress in both defect engineering and device fabrication in hexagonal boron nitride based photonic quantum technologies.

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Semiconductor spin qubits combine excellent quantum performance with the prospect of manufacturing quantum devices using industry-standard metal-oxide-semiconductor (MOS) processes. This applies also to ion-implanted donor spins, which further afford exceptional coherence times and large Hilbert space dimension in their nuclear spin. Here multiple strategies are demonstrated and integrated to manufacture scale-up donor-based quantum computers. 31PF2 molecule implants are used to triple the placement certainty compared to 31P ions, while attaining 99.99% confidence in detecting the implant. Similar confidence is retained by implanting heavier atoms such as 123Sb and 209Bi, which represent high-dimensional qudits for quantum information processing, while Sb2 molecules enable deterministic formation of closely-spaced qudits. The deterministic formation of regular arrays of donor atoms with 300 nm spacing is demonstrated, using step-and-repeat implantation through a nano aperture. These methods cover the full gamut of technological requirements for the construction of donor-based quantum computers in silicon.

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Controlled interaction between localized and delocalized solid-state spin systems offers a compelling platform for on-chip quantum information processing with quantum spintronics. Hybrid quantum systems (HQSs) of localized nitrogen-vacancy (NV) centers in diamond and delocalized magnon modes in ferrimagnets-systems with naturally commensurate energies-have recently attracted significant attention, especially for interconnecting isolated spin qubits at length-scales far beyond those set by the dipolar coupling. However, despite extensive theoretical efforts, there is a lack of experimental characterization of the magnon-mediated interaction between NV centers, which is necessary to develop such hybrid quantum architectures. Here, we experimentally determine the magnon-mediated NV-NV coupling from the magnon-induced self-energy of NV centers. Our results are quantitatively consistent with a model in which the NV center is coupled to magnons by dipolar interactions. This work provides a versatile tool to characterize HQSs in the absence of strong coupling, informing future efforts to engineer entangled solid-state systems.

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With the aim of creating Cu(II) spin qubits in a rigid metal-organic framework (MOF), this work demonstrates a doping of 5 %, 2 %, 1 %, and 0.1 % mol of Cu(II) ions into a perovskite-type MOF [CH6 N3 ][ZnII (HCOO)3 ]. The presence of dopant Cu(II) sites are confirmed with anisotropic g-factors (gx =2.07, gy =2.12, and gz =2.44) in the S=1/2 system by experimentally and theoretically. Magnetic dynamics indicate the occurrence of a slow magnetic relaxation via the direct and Raman processes under an applied field, with a relaxation time (τ) of 3.5 ms (5 % Cu), 9.2 ms (2 % Cu), and 15 ms (1 % Cu) at 1.8 K. Furthermore, pulse-ESR spectroscopy reveals spin qubit properties with a spin-spin relaxation (phase memory) time (T2 ) of 0.21 µs (2 %Cu), 0.39 µs (1 %Cu), and 3.0 µs (0.1 %Cu) at 10 K as well as Rabi oscillation between MS =±1/2 spin sublevels. T2 above microsecond is achieved for the first time in the Cu(II)-doped MOFs. It can be observed at submicrosecond around 50 K. These spin relaxations are very sensitive to the magnetic dipole interactions relating with cross-relaxation between the Cu(II) sites and can be tuned by adjusting the dopant concentration.

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In the development of two-qubit quantum gates, precise control over the intramolecular spin-spin interaction between molecular spin units plays a pivotal role. A weak but measurable exchange coupling is especially important for achieving selective spin addressability that allows controlled manipulation of the computational basis states |00⟩ |01⟩ |10⟩ |11⟩ by microwave pulses. Here, we report the synthesis and Electron Paramagnetic Resonance (EPR) study of a heterometallic meso-meso (m-m) singly-linked VIV O-CuII porphyrin dimer. X-band continuous wave EPR measurements in frozen solutions suggest a ferromagnetic exchange coupling of ca. 8 ⋅ 10-3  cm-1 . This estimation is supported by Density Functional Theory calculations, which also allow disentangling the ferro- and antiferromagnetic contributions to the exchange. Pulsed EPR experiments show that the dimer maintains relaxation times similar to the monometallic CuII porphyrins. The addressability of the two individual spins is made possible by the different g-tensors of VIV and CuII -ions, in contrast to homometallic dimers where tilting of the porphyrin planes plays a key role. Therefore, single-spin addressability in the heterometallic dimer can be maintained even with small tilting angles, as expected when deposited on surface, unlocking the full potential of molecular quantum gates for practical applications.

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Noise spectroscopy elucidates the fundamental noise sources in spin systems, thereby serving as an essential tool toward developing spin qubits with long coherence times for quantum information processing, communication, and sensing. But existing techniques for noise spectroscopy that rely on microwave fields become infeasible when the microwave power is too weak to generate Rabi rotations of the spin. Here, we demonstrate an alternative all-optical approach to performing noise spectroscopy. Our approach utilizes coherent Raman rotations of the spin state with controlled timing and phase to implement Carr-Purcell-Meiboom-Gill pulse sequences. Analyzing the spin dynamics under these sequences enables us to extract the noise spectrum of a dense ensemble of nuclear spins interacting with a single spin in a quantum dot, which has thus far been modeled only theoretically. By providing spectral bandwidths of over 100 MHz, our approach enables studies of spin dynamics and decoherence for a broad range of solid-state spin qubits.

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The small size and excellent integrability of silicon metal-oxide-semiconductor (SiMOS) quantum dot spin qubits make them an attractive system for mass-manufacturable, scaled-up quantum processors. Furthermore, classical control electronics can be integrated on-chip, in-between the qubits, if an architecture with sparse arrays of qubits is chosen. In such an architecture qubits are either transported across the chip via shuttling or coupled via mediating quantum systems over short-to-intermediate distances. This paper investigates the charge and spin characteristics of an elongated quantum dot-a so-called jellybean quantum dot-for the prospects of acting as a qubit-qubit coupler. Charge transport, charge sensing, and magneto-spectroscopy measurements are performed on a SiMOS quantum dot device at mK temperature and compared to Hartree-Fock multi-electron simulations. At low electron occupancies where disorder effects and strong electron-electron interaction dominate over the electrostatic confinement potential, the data reveals the formation of three coupled dots, akin to a tunable, artificial molecule. One dot is formed centrally under the gate and two are formed at the edges. At high electron occupancies, these dots merge into one large dot with well-defined spin states, verifying that jellybean dots have the potential to be used as qubit couplers in future quantum computing architectures.

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Molecular platforms are regarded as promising candidates in the generation of units of information for quantum computing. Herein, a strategy combining spin-crossover metal ions and radical ligands is proposed from a model Hamiltonian first restricted to exchange interactions. Unusual spin states structures emerge from the linkage of a singlet/triplet commutable metal centre with two doublet-radical ligands. The ground state nature is modulated by charge transfers and can exhibit a mixture of triplet and singlet local metal spin states. Besides, the superposition reaches a maximum for 2 K M = K 1 + K 2 ${2{K}_{M}={K}_{1}+{K}_{2}}$ , suggesting a necessary competition between the intramolecular K M ${{K}_{M}}$ and inter-metal-ligand K 1 ${{K}_{1}}$ and K 2 ${{K}_{2}}$ direct exchange interactions. The results promote spinmerism, an original manifestation of quantum entanglement between the spin states of a metal centre and radical ligands. The study provides insights into spin-coupled compounds and inspiration for the development of molecular spin-qubits.

Asunto(s)

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SignificanceAtomic defects in solid-state materials are promising candidates as quantum bits, or qubits. New materials are actively being investigated as hosts for new defect qubits; however, there are no unifying guidelines that can quantitatively predict qubit performance in a new material. One of the most critical property of qubits is their quantum coherence. While cluster correlation expansion (CCE) techniques are useful to simulate the coherence of electron spins in defects, they are computationally expensive to investigate broad classes of stable materials. Using CCE simulations, we reveal a general scaling relation between the electron spin coherence time and the properties of qubit host materials that enables rapid and quantitative exploration of new materials hosting spin defects.

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In the last 20 years, silicon quantum dots have received considerable attention from academic and industrial communities for research on readout, manipulation, storage, near-neighbor and long-range coupling of spin qubits. In this paper, we introduce how to realize a single spin qubit from Si-MOS quantum dots. First, we introduce the structure of a typical Si-MOS quantum dot and the experimental setup. Then, we show the basic properties of the quantum dot, including charge stability diagram, orbital state, valley state, lever arm, electron temperature, tunneling rate and spin lifetime. After that, we introduce the two most commonly used methods for spin-to-charge conversion, i.e., Elzerman readout and Pauli spin blockade readout. Finally, we discuss the details of how to find the resonance frequency of spin qubits and show the result of coherent manipulation, i.e., Rabi oscillation. The above processes constitute an operation guide for helping the followers enter the field of spin qubits in Si-MOS quantum dots.

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To design molecular spin qubits with enhanced quantum coherence, a control of the coupling between the local vibrations and the spin states is crucial, which could be realized in principle by engineering molecular structures via coordination chemistry. To this end, understanding the underlying structural factors that govern the spin relaxation is a central topic. Here, we report the investigation of the spin dynamics in a series of chemically designed europium(II)-based endohedral metallofullerenes (EMFs). By introducing a unique structural difference, i. e. metal-cage binding site, while keeping other molecular parameters constant between different complexes, these manifest the key role of the three low-energy metal-displacing vibrations in mediating the spin-lattice relaxation times (T1 ). The temperature dependence of T1 can thus be normalized by the frequencies of these low energy vibrations to show an unprecedentedly universal behavior for EMFs in frozen CS2 solution. Our theoretical analysis indicates that this structural difference determines not only the vibrational rigidity but also spin-vibration coupling in these EMF-based qubit candidates.

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We combine top-down and bottom-up nanolithography to optimize the coupling of small molecular spin ensembles to 1.4 GHz on-chip superconducting resonators. Nanoscopic constrictions, fabricated with a focused ion beam at the central transmission line, locally concentrate the microwave magnetic field. Drops of free-radical molecules have been deposited from solution onto the circuits. For the smallest ones, the molecules were delivered at the relevant circuit areas by means of an atomic force microscope. The number of spins Neff effectively coupled to each device was accurately determined combining Scanning Electron and Atomic Force Microscopies. The collective spin-photon coupling constant has been determined for samples with Neff ranging between 2 × 106 and 1012 spins, and for temperatures down to 44 mK. The results show the well-known collective enhancement of the coupling proportional to the square root of Neff. The average coupling of individual spins is enhanced by more than 4 orders of magnitude (from 4 mHz up to above 180 Hz), when the transmission line width is reduced from 400 µm down to 42 nm, and reaches maximum values near 1 kHz for molecules located on the smallest nanoconstrictions.

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Spin qubits in silicon quantum dots offer a promising platform for a quantum computer as they have a long coherence time and scalability. The charge sensing technique plays an essential role in reading out the spin qubit as well as tuning the device parameters, and therefore, its performance in terms of measurement bandwidth and sensitivity is an important factor in spin qubit experiments. Here we demonstrate fast and sensitive charge sensing by radio frequency reflectometry of an undoped, accumulation-mode Si/SiGe double quantum dot. We show that the large parasitic capacitance in typical accumulation-mode gate geometries impedes reflectometry measurements. We present a gate geometry that significantly reduces the parasitic capacitance and enables fast single-shot readout. The technique allows us to distinguish between the singly- and doubly occupied two-electron states under the Pauli spin blockade condition in an integration time of 0.8 µs, the shortest value ever reported in silicon, by the signal-to-noise ratio of 6. These results provide a guideline for designing silicon spin qubit devices suitable for the fast and high-fidelity readout.

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Quantum bits (qubits) constitute the most elementary building-blocks of any quantum technology, where information is stored and processed in the form of quantum superpositions between discrete energy levels. In particular, the fabrication of quantum processors is a key long-term goal that will allow us conducting specific tasks much more efficiently than the most powerful classical computers can do. Motivated by recent experiments in which three addressable spin qubits are defined on a potential single-molecule quantum processor, namely the [Gd(H2O)P5W30O110]12- polyoxometalate, we investigate the decohering effect of magnetic noise on the encoded quantum information. Our state-of-the-art model, which provides more accurate results than previous estimates, show a noticeable contribution of magnetic noise in limiting the survival timescale of the qubits. Yet, our results suggest that it might not be the only dephasing mechanism at play but other mechanisms, such as lattice vibrations and physical movement of magnetic nuclei, must be considered to understand the whole decoherence process.

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Quantum dot arrays are a versatile platform for the implementation of spin qubits, as high-bandwidth sensor dots can be integrated with single-, double-, and triple-dot qubits yielding fast and high-fidelity qubit readout. However, for undoped silicon devices, reflectometry off sensor ohmics suffers from the finite resistivity of the two-dimensional electron gas (2DEG), and alternative readout methods are limited to measuring qubit capacitance, rather than qubit charge. By coupling a surface-mount resonant circuit to the plunger gate of a high-impedance sensor, we realized a fast charge sensing technique that is compatible with resistive 2DEGs. We demonstrate this by acquiring at high speed charge stability diagrams of double- and triple-dot arrays in Si/SiGe heterostructures as well as pulsed-gate single-shot charge and spin readout with integration times as low as 2.4 µs.

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The strong atomistic spin-orbit coupling of holes makes single-shot spin readout measurements difficult because it reduces the spin lifetimes. By integrating the charge sensor into a high bandwidth radio frequency reflectometry setup, we were able to demonstrate single-shot readout of a germanium quantum dot hole spin and measure the spin lifetime. Hole spin relaxation times of about 90 µs at 500 mT are reported, with a total readout visibility of about 70%. By analyzing separately the spin-to-charge conversion and charge readout fidelities, we have obtained insight into the processes limiting the visibilities of hole spins. The analyses suggest that high hole visibilities are feasible at realistic experimental conditions, underlying the potential of hole spins for the realization of viable qubit devices.

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Silicon carbide is a promising platform for single photon sources, quantum bits (qubits), and nanoscale sensors based on individual color centers. Toward this goal, we develop a scalable array of nanopillars incorporating single silicon vacancy centers in 4H-SiC, readily available for efficient interfacing with free-space objective and lensed-fibers. A commercially obtained substrate is irradiated with 2 MeV electron beams to create vacancies. Subsequent lithographic process forms 800 nm tall nanopillars with 400-1400 nm diameters. We obtain high collection efficiency of up to 22 kcounts/s optical saturation rates from a single silicon vacancy center while preserving the single photon emission and the optically induced electron-spin polarization properties. Our study demonstrates silicon carbide as a readily available platform for scalable quantum photonics architecture relying on single photon sources and qubits.

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We investigate a spin-to-charge conversion mechanism which maps the spin singlet and triplet states to two charge states differing by one electron mediated by an intermediate metastable charge state. This mechanism allows us to observe fringes in the spin-unblocked region beyond the triplet transition line in the measurement of the exchange oscillations between singlet and triplet states in a four-electron double quantum dot. Moreover, these fringes are amplified and π-phase shifted, compared with those in the spin blockade region. Unlike the signal enhancement mechanism reported before which produces similar effects, this mechanism only requires one dot coupling to the lead, which is a commonly encountered case especially in imperfect devices. Besides, the crucial tunnel rate asymmetry is provided by the dependence on spin state, not by the asymmetric couplings to the leads. We also design a scheme to control the amplification process, which enables us to extract the relevant time parameters. This mechanism will have potential applications in future investigations of spin qubits.

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Hole spins in silicon represent a promising yet barely explored direction for solid-state quantum computation, possibly combining long spin coherence, resulting from a reduced hyperfine interaction, and fast electrically driven qubit manipulation. Here we show that a silicon-nanowire field-effect transistor based on state-of-the-art silicon-on-insulator technology can be operated as a few-hole quantum dot. A detailed magnetotransport study of the first accessible hole reveals a g-factor with unexpectedly strong anisotropy and gate dependence. We infer that these two characteristics could enable an electrically driven g-tensor-modulation spin resonance with Rabi frequencies exceeding several hundred mega-Hertz.

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Large-scale quantum computers must be built upon quantum bits that are both highly coherent and locally controllable. We demonstrate the quantum control of the electron and the nuclear spin of a single (31)P atom in silicon, using a continuous microwave magnetic field together with nanoscale electrostatic gates. The qubits are tuned into resonance with the microwave field by a local change in electric field, which induces a Stark shift of the qubit energies. This method, known as A-gate control, preserves the excellent coherence times and gate fidelities of isolated spins, and can be extended to arbitrarily many qubits without requiring multiple microwave sources.