arXiv subjects

Alastair Stacey

Publications and source records attributed to Alastair Stacey.

35 records · Page 2Linked to original sources

arXiv2021

Electrical Control of Quantum Emitters in a Van der Waals Heterostructure

Controlling and manipulating individual quantum systems in solids underpins the growing interest in development of scalable quantum technologies. Recently, hexagonal boron nitride has garnered significant attention in quantum photonic applications due to its ability to host optically stable quantum emitters. However, the large band gap of hBN and the lack of efficient doping inhibits electrical triggering and limits opportunities to study electrical control of emitters. Here, we show an approach to electrically modulate quantum emitters in n hBN graphene van der Waals heterostructure. We show that quantum emitters in hBN can be reversibly activated and modulated by applying a bias across the device. Notably, a significant number of quantum emitters are intrinsically dark, and become optically active at non-zero voltages. To explain the results, we provide a heuristic electrostatic model of this unique behaviour. Finally, employing these devices we demonstrate a nearly coherent source with linewidths of 160 MHz. Our results enhance the potential of hBN for tuneable solid state quantum emitters for the growing field of quantum information science.

physics.optics↗

arXiv2021

Telecommunication-wavelength two-dimensional photonic crystal cavities in a thin single-crystal diamond membrane

We demonstrate two-dimensional photonic crystal cavities operating at telecommunication wavelengths in a single-crystal diamond membrane. We use a high-optical-quality and thin (~ 300 nm) diamond membrane, supported by a polycrystalline diamond frame, to realize fully suspended two-dimensional photonic crystal cavities with a high theoretical quality factor of ~ $8\times10^6$ and a relatively small mode volume of ~2$(λ/n)^3$. The cavities are fabricated in the membrane using electron-beam lithography and vertical dry etching. We observe cavity resonances over a wide wavelength range spanning the telecommunication O- and S-bands (1360 nm-1470 nm) with Q factors of up to ~1800. Our method offers a new direction for on-chip diamond nanophotonic applications in the telecommunication-wavelength range.

physics.optics↗

arXiv2020

Nitrogen overgrowth as a catalytic mechanism during diamond chemical vapour deposition

Nitrogen is frequently included in chemical vapour deposition feed gases to accelerate diamond growth. While there is no consensus for an atomistic mechanism of this effect, existing studies have largely focused on the role of sub-surface nitrogen and nitrogen-based adsorbates. In this work, we demonstrate the catalytic effect of surface-embedded nitrogen in nucleating new layers of (100) diamond. To do so we develop a model of nitrogen overgrowth using density functional theory. Nucleation of new layers occurs through C insertion into a C--C surface dimer. However, we find that C insertion into a C--N dimer has substantially reduced energy requirements. In particular, the rate of the key dimer ring-opening and closing mechanism is increased 400-fold in the presence of nitrogen. Full incorporation of the substitutional nitrogen defect is then facilitated through charge transfer of an electron from the nitrogen lone pair to charge acceptors on the surface. This work provides a compelling mechanism for the role of surface-embedded nitrogen in enhancing (100) diamond growth through the nucleation of new layers. Furthermore, it demonstrates a pathway for substitutional nitrogen formation during chemical vapour deposition which can be extended to study the creation of technologically relevant nitrogen-based defects.

cond-mat.mtrl-sci↗

arXiv2018

Origins of diamond surface noise probed by correlating single spin measurements with surface spectroscopy

The nitrogen vacancy (NV) center in diamond exhibits spin-dependent fluorescence and long spin coherence times under ambient conditions, enabling applications in quantum information processing and sensing. NV centers near the surface can have strong interactions with external materials and spins, enabling new forms of nanoscale spectroscopy. However, NV spin coherence degrades within 100 nanometers of the surface, suggesting that diamond surfaces are plagued with ubiquitous defects. Prior work on characterizing near-surface noise has primarily relied on using NV centers themselves as probes; while this has the advantage of exquisite sensitivity, it provides only indirect information about the origin of the noise. Here we demonstrate that surface spectroscopy methods and single spin measurements can be used as complementary diagnostics to understand sources of noise. We find that surface morphology is crucial for realizing reproducible chemical termination, and use these insights to achieve a highly ordered, oxygen-terminated surface with suppressed noise. We observe NV centers within 10 nm of the surface with coherence times extended by an order of magnitude.

cond-mat.mtrl-sci↗

arXiv2018

Irradiation induced modification of the superconducting properties of heavily boron doped diamond

Diamond, a wide band-gap semiconductor, can be engineered to exhibit superconductivity when doped heavily with boron. The phenomena has been demonstrated in samples grown by chemical vapour deposition where the boron concentration exceeds the critical concentration for the metal-to-insulator transition of $n_{MIT} \gtrsim 4\times10^{20}/\text{cm}^3$. While the threshold carrier concentration for superconductivity is generally well established in the literature, it is unclear how well correlated higher critical temperatures are with increased boron concentration. Previous studies have generally compared several samples grown under different plasma conditions, or on substrates having different crystallographic orientations, in order to vary the incorporation of boron into the lattice. Here, we present a study of a single sample with unchanging boron concentration, and instead modify the charge carrier concentration by introducing compensating defects via high energy ion irradiation. Superconductivity is completely suppressed when the number of defects is sufficient to compensate the hole concentration to below threshold. Furthermore, we show it is possible to recover the superconductivity by annealing the sample in vacuum to remove the compensating defects.

cond-mat.supr-con↗

arXiv2018

Controllable Non-Markovianity for a Spin Qubit in Diamond

We present a flexible scheme to realize non-artificial non-Markovian dynamics of an electronic spin qubit, using a nitrogen-vacancy center in diamond where the inherent nitrogen spin serves as a regulator of the dynamics. By changing the population of the nitrogen spin, we show that we can smoothly tune the non-Markovianity of the electron spin's dynamic. Furthermore, we examine the decoherence dynamics induced by the spin bath to exclude other sources of non-Markovianity. The amount of collected measurement data is kept at a minimum by employing Bayesian data analysis. This allows for a precise quantification of the parameters involved in the description of the dynamics and a prediction of so far unobserved data points.

quant-ph↗

arXiv2018

Evidence for Primal sp2 Defects at the Diamond Surface: Candidates for Electron Trapping and Noise Sources

Diamond materials are central to an increasing range of advanced technological demonstrations, from high power electronics, to nano-scale quantum bio-imaging with unprecedented sensitivity. However, the full exploitation of diamond for these applications is often limited by the uncontrolled nature of the diamond material surface, which suffers from Fermi-level pinning and hosts a significant density of electro-magnetic noise sources. These issues occur despite the oxide-free and air-stable nature of the diamond crystal surface, which should be an ideal candidate for functionalization and chemical-engineering. In this work we reveal a family of previously unidentified and near-ubiquitous primal surface defects which we assign to differently reconstructed surface vacancies. The density of these defects is quantified with X-ray absorption spectroscopy, their energy structures are elucidated by ab initio calculations, and their effect on near-surface quantum probes is measured directly. Subsequent ab-initio calculation of band-bending from these defects suggest they are the source of Fermi-level pinning at most diamond surfaces. Finally, an investigation is conducted on a broad range of post-growth surface treatments and concludes that none of them can reproducibly reduce this defect density below the Fermi-pinning threshold, making this defect a prime candidate as the source for decoherence-limiting noise in near-surface quantum probes.

cond-mat.mes-hall↗

arXiv2017

High precision single qubit tuning via thermo-magnetic field control

Precise control of the resonant frequency of a spin qubit is of fundamental importance to quantum sensing protocols. We demonstrate a control technique on a single nitrogen-vacancy (NV) centre in diamond where the applied magnetic field is modified by fine-tuning a permanent magnet's magnetisation via temperature control. Through this control mechanism, nanoscale cross-relaxation spectroscopy of both electron and nuclear spins in the vicinity of the NV centre are performed. We then show that through maintaining the magnet at a constant temperature an order of magnitude improvement in the stability of the NV qubit frequency can be achieved. This improved stability is tested in the polarisation of a small ensemble of nearby $^{13}$C spins via resonant cross-relaxation and the lifetime of this polarisation explored. The effectiveness and relative simplicity of this technique may find use in the realisation of portable spectroscopy and/or hyperpolarisation systems.

quant-ph↗

arXiv2017

Quantum probe hyperpolarisation of molecular nuclear spins

The hyperpolarisation of nuclear spins within target molecules is a critical and complex challenge in magnetic resonance imaging (MRI) and nuclear magnetic resonance (NMR) spectroscopy. Hyperpolarisation offers enormous gains in signal and spatial resolution which may ultimately lead to the development of molecular MRI and NMR. At present, techniques used to polarise nuclear spins generally require low temperatures and/or high magnetic fields, radio-frequency control fields, or the introduction of catalysts or free-radical mediators. The emergence of room temperature solid-state spin qubits has opened exciting new pathways to circumvent these requirements to achieve direct nuclear spin hyperpolarisation using quantum control. Employing a novel cross-relaxation induced polarisation (CRIP) protocol using a single nitrogen-vacancy (NV) centre in diamond, we demonstrate the first external nuclear spin hyperpolarisation achieved by a quantum probe, in this case of $^1$H molecular spins in poly(methyl methacrylate). In doing so, we show that a single qubit is capable of increasing the thermal polarisation of $\sim 10^6$ nuclear spins by six orders of magnitude, equivalent to an applied magnetic field of $10^5$\,T. The technique can also be tuned to multiple spin species, which we demonstrate using both \C{13} and $^1$H nuclear spin ensembles. Our results are analysed and interpreted via a detailed theoretical treatment, which is also used to describe how the system can be scaled up to a universal quantum hyperpolarisation platform for the production of macroscopic quantities of contrast agents at high polarisation levels for clinical applications. These results represent a new paradigm for nuclear spin hyperpolarisation for molecular imaging and spectroscopy, and beyond into areas such as materials science and quantum information processing.

quant-ph↗

arXiv2017

Environmentally mediated coherent control of a spin qubit in diamond

The coherent control of spin qubits forms the basis of many applications in quantum information processing and nanoscale sensing, imaging and spectroscopy. Such control is conventionally achieved by direct driving of the qubit transition with a resonant global field, typically at microwave frequencies. Here we introduce an approach that relies on the resonant driving of nearby environment spins, whose localised magnetic field in turn drives the qubit when the environmental spin Rabi frequency matches the qubit resonance. This concept of environmentally mediated resonance (EMR) is explored experimentally using a qubit based on a single nitrogen-vacancy (NV) centre in diamond, with nearby electronic spins serving as the environmental mediators. We demonstrate EMR driven coherent control of the NV spin-state, including the observation of Rabi oscillations, free induction decay, and spin-echo. This technique also provides a way to probe the nanoscale environment of spin qubits, which we illustrate by acquisition of electron spin resonance spectra of single NV centres in various settings.

cond-mat.mes-hall↗

arXiv2016

Microwave-Free Nuclear Magnetic Resonance at Molecular Scales

The implementation of nuclear magnetic resonance (NMR) at the nanoscale is a major challenge, as conventional systems require relatively large ensembles of spins and limit resolution to mesoscopic scales. New approaches based on quantum spin probes, such as the nitrogen-vacancy (NV) centre in diamond, have recently achieved nano-NMR under ambient conditions. However, the measurement protocols require application of complex microwave pulse sequences of high precision and relatively high power, placing limitations on the design and scalability of these techniques. Here we demonstrate a microwave-free method for nanoscale NMR using the NV centre, which is a far less invasive, and vastly simpler measurement protocol. By utilising a carefully tuned magnetic cross-relaxation interaction between a subsurface NV spin and an external, organic environment of proton spins, we demonstrate NMR spectroscopy of $^1$H within a $\approx(10~{\rm nm})^3$ sensing volume. We also theoretically and experimentally show that the sensitivity of our approach matches that of existing microwave control-based techniques using the NV centre. Removing the requirement for coherent manipulation of either the NV or the environmental spin quantum states represents a significant step towards the development of robust, non-invasive nanoscale NMR probes.

cond-mat.mes-hall↗

arXiv2016

Quantum imaging of current flow in graphene

Since its first isolation in 2004, graphene has been found to host a plethora of unusual electronic transport phenomena, making it a fascinating system for fundamental studies in condensed-matter physics as well as offering tremendous opportunities for future electronic and sensing devices. However, to fully realise these goals a major challenge is the ability to non-invasively image charge currents in monolayer graphene structures and devices. Typically, electronic transport in graphene has been investigated via resistivity measurements, however, such measurements are generally blind to spatial information critical to observing and studying landmark transport phenomena such as electron guiding and focusing, topological currents and viscous electron backflow in real space, and in realistic imperfect devices. Here we bring quantum imaging to bear on the problem and demonstrate high-resolution imaging of current flow in graphene structures. Our method utilises an engineered array of near-surface, atomic-sized quantum sensors in diamond, to map the vector magnetic field and reconstruct the vector current density over graphene geometries of varying complexity, from mono-ribbons to junctions, with spatial resolution at the diffraction limit and a projected sensitivity to currents as small as 1 μA. The measured current maps reveal strong spatial variations corresponding to physical defects at the sub-μm scale. The demonstrated method opens up an important new avenue to investigate fundamental electronic and spin transport in graphene structures and devices, and more generally in emerging two-dimensional materials and thin film systems.

cond-mat.mes-hall↗

arXiv2016

Spin dynamics of diamond nitrogen-vacancy centres at the ground state level anti-crossing and all-optical low frequency magnetic field sensing

We investigate the photo-induced spin dynamics of single nitrogen-vacancy (NV) centres in diamond near the electronic ground state level anti-crossing (GSLAC), which occurs at an axial magnetic field around 1024 G. Using optically detected magnetic resonance spectroscopy, we first find that the electron spin transition frequency can be tuned down to 100 kHz for the \NV{14} centre, while for the \NV{15} centre the transition strength vanishes for frequencies below about 2 MHz owing to the GSLAC level structure. Using optical pulses to prepare and readout the spin state, we observe coherent spin oscillations at 1024 G for the \NV{14}, which originate from spin mixing induced by residual transverse magnetic fields. This effect is responsible for limiting the smallest observable transition frequency, which can span two orders of magnitude from 100 kHz to tens of MHz depending on the local magnetic noise. A similar feature is observed for the \NV{15} centre at 1024 G. As an application of these findings, we demonstrate all-optical detection and spectroscopy of externally-generated fluctuating magnetic fields at frequencies from 8 MHz down to 500 kHz, using a \NV{14} centre. Since the Larmor frequency of most nuclear spin species lies within this frequency range near the GSLAC, these results pave the way towards all-optical, nanoscale nuclear magnetic resonance spectroscopy, using longitudinal spin cross-relaxation.

cond-mat.mes-hall↗

arXiv2016

Wide-band, nanoscale magnetic resonance spectroscopy using quantum relaxation of a single spin in diamond

We demonstrate a wide-band all-optical method of nanoscale magnetic resonance (MR) spectroscopy under ambient conditions. Our method relies on cross-relaxation between a probe spin, the electronic spin of a nitrogen-vacancy centre in diamond, and target spins as the two systems are tuned into resonance. By optically monitoring the spin relaxation time ($T_1$) of the probe spin while varying the amplitude of an applied static magnetic field, a frequency spectrum of the target spin resonances, a $T_1$-MR spectrum, is obtained. As a proof of concept, we measure $T_1$-MR spectra of a small ensemble of $^{14}$N impurities surrounding the probe spin within the diamond, with each impurity comprising an electron spin 1/2 and a nuclear spin 1. The intrinsically large bandwidth of the technique and probe properties allows us to detect both electron spin transitions -- in the GHz range -- and nuclear spin transitions -- in the MHz range -- of the $^{14}$N spin targets. The measured frequencies are found to be in excellent agreement with theoretical expectations, and allow us to infer the hyperfine, quadrupole and gyromagnetic constants of the target spins. Analysis of the strength of the resonances obtained in the $T_1$-MR spectrum reveals that the electron spin transitions are probed via dipole interactions, while the nuclear spin resonances are dramatically enhanced by hyperfine coupling and an electron-mediated process. Finally, we investigate theoretically the possibility of performing $T_1$-MR spectroscopy on nuclear spins without hyperfine interaction and predict single-proton sensitivity using current technology. This work establishes $T_1$-MR as a simple yet powerful technique for nanoscale MR spectroscopy, with broadband capability and a projected sensitivity down to the single nuclear spin level.

quant-ph↗

arXiv2015

Extremely high negative electron affinity of diamond via magnesium adsorption

We report large negative electron affinity (NEA) on diamond (100) using magnesium adsorption on a previously oxygen-terminated surface. The measured NEA is up to $(-2.01\pm0.05)$ eV, the largest reported negative electron affinity to date. Despite the expected close relationship between the surface chemistry of Mg and Li species on oxygen-terminated diamond, we observe differences in the adsorption properties between the two. Most importantly, a high-temperature annealing step is not required to activate the Mg-adsorbed surface to a state of negative electron affinity. Diamond surfaces prepared by this procedure continue to possess negative electron affinity after exposure to high temperatures, air and even immersion in water.

cond-mat.mtrl-sci↗

arXiv2013

Electronic properties and metrology of the diamond NV- center under pressure

The negatively charged nitrogen-vacancy (NV-) center in diamond has realized new frontiers in quantum technology. Here, the center's optical and spin resonances are observed under hydrostatic pressures up to 60 GPa. Our observations motivate powerful new techniques to measure pressure and image high pressure magnetic and electric phenomena. Our observations further reveal a fundamental inadequacy of the current model of the center and provide new insight into its electronic structure.

cond-mat.mtrl-sci↗

arXiv2009

A new, enhanced diamond single photon emitter in the near infra-red

Individual color centers in diamond are promising for near-term quantum technologies including quantum key distribution and metrology. Here we show fabrication of a new color center which has photophysical properties surpassing those of the two main-stay centers, namely the nitrogen vacancy and NE8 centers. The new center is fabricated using focused ion beam implantation of nickel into isolated chemical vapor deposited diamond micro-crystals. Room temperature photoluminescence studies reveal a narrow emission in the near infrared region centered at 768 nm with a lifetime as short as 2 ns. Its focused ion beam compatibility opens the prospect to fabrication with nanometer resolution and realization of integrated quantum photonic devices. Preliminary investigations suggest that this center arises from an as-yet uncharacterized nickel-silicon complex.

cond-mat.mtrl-sci↗