arXiv subjects

Alastair Stacey

Publications and source records attributed to Alastair Stacey.

At least 19 recordsLinked to original sources

arXiv2026

Efficient and Robust p-type Transistor based on Ultra-wide-bandgap Semiconductor

The p-type transistor is an indispensable component of semiconductor technology, enabling complementary operation with n-channel transistors for computation, storage, and communication. Achieving both high robustness and high efficiency is highly desirable but challenging for p-type transistors due to limited semiconductors with reliable hole transport and their high activation energies. Here, we achieved a robust yet efficient p-type transistor by heterogeneously integrating an ultra-wide-bandgap semiconductor and a high-k dielectric layer through van der Waals integration. The p-type transistor employs a two-dimensional hole channel on hydrogenated diamond (bandgap 5.6 eV) combined with a high-k (30.5) SrTiO3 perovskite membrane. At room temperature, the transistor exhibits stable operation with a high on-current (~200 mA/mm), low subthreshold swing (70 mV/dec), high hole mobility (566 cm^2/Vs to 572 cm^2/Vs) and high on-off ratio (~10^9). Furthermore, tuning annealing temperature allows operation in either enhancement or depletion mode. The robust p-type transistor with high efficiency holds great potential for future power electronics, UV optoelectronics, and harsh-environment electronic applications.

cond-mat.mtrl-sci↗

arXiv2025

Control of Neuronal Survival and Development Using Conductive Diamond

This study demonstrates the control of neuronal survival and development using nitrogen-doped ultrananocrystalline diamond (N-UNCD). We highlight the role of N-UNCD in regulating neuronal activity via near-infrared illumination, demonstrating the generation of stable photocurrents that enhance neuronal survival and neurite outgrowth and foster a more active, synchronized neuronal network. Whole transcriptome RNA sequencing reveals that diamond substrates improve cellular-substrate interaction by upregulating extracellular matrix and gap junction-related genes. Our findings underscore the potential of conductive diamond as a robust and biocompatible platform for noninvasive and effective neural tissue engineering.

physics.bio-ph↗

arXiv2025

The properties of the nitrogen-vacancy center in milled chemical vapor deposition nanodiamonds

Fluorescent nanodiamonds (FNDs) containing negatively charged nitrogen-vacancy (NV-) centers are vital for many emerging quantum sensing applications from magnetometry to intracellular sensing in biology. However, developing a scalable fabrication method for FNDs hosting color centers with consistent bulk-like photoluminescence (PL) and spin coherence properties remains a highly desired but unrealized goal. Here, we investigate optimized ball milling of single-crystal diamonds produced via chemical vapor deposition (CVD) and containing 2 ppm of substitutional nitrogen and 0.3 ppm of NV- to achieve this goal. The NV charge state, PL lifetime, and spin properties of bulk CVD diamond samples are directly compared to milled CVD FNDs and commercial high-pressure high-temperature (HPHT) FNDs. We find that on average, the relative contribution of the NV- charge state to the total NV PL is lower and the NV PL lifetime is longer in CVD FNDs compared to HPHT FNDs, both likely due to the lower Ns0 concentration in CVD FNDs. The CVD bulk and CVD FNDs on average show similar average T1 spin relaxation times of 3.2 $\pm$ 0.7 ms and 4.7 $\pm$ 1.6 ms, respectively, compared to 0.17 $\pm$ 0.01 ms for commercial HPHT FNDs. Our results demonstrate that ball milling of CVD diamonds enables the large-scale fabrication of NV ensembles in FNDs with bulk-like T1 spin relaxation properties.

cond-mat.mes-hall↗

arXiv2025

Nitrogen-vacancy centre formation via local femto-second laser annealing of diamond

Emerging quantum technologies based on the nitrogen-vacancy (NV) centre in diamond require carefully engineered material with controlled defect density, optimised NV formation processes, and minimal crystal strain. The choice of NV generation technique plays a crucial role in determining the quality and performance of these centres. In this work, we investigate NV centre formation in nitrogen-doped diamond using femtosecond (fs) laser processing. We systematically examine the effect of laser pulse energy on NV production and quality using photoluminescence and optically detected magnetic resonance measurements. We also probe the role of pre-existing lattice defects formed by electron irradiation and consider defect evolution over extended dwell times. Finally, we are able to identify a regime where the main action of the fs-laser is to diffuse rather than create vacancies. This local annealing capability expands the toolkit for tailored NV production and presents opportunities for fine tuning defect populations.

cond-mat.mtrl-sci↗

arXiv2025

Robust quantification of the diamond nitrogen-vacancy center charge state via photoluminescence spectroscopy

Nitrogen vacancy (NV) centers in diamond are at the heart of many emerging quantum technologies, all of which require control over the NV charge state. Hence, methods for quantification of the relative photoluminescence (PL) intensities of the NV$^0$ and NV$^-$ charge state, i.e., a charge state ratio, are vital. Several approaches to quantify NV charge state ratios have been reported but are either limited to bulk-like NV diamond samples or yield qualitative results. We propose an NV charge state quantification protocol based on the determination of sample- and experimental setup-specific NV$^0$ and NV$^-$ reference spectra. The approach employs blue (400-470 nm) and green (480-570 nm) excitation to infer pure NV$^0$ and NV$^-$ spectra, which are then used to quantify NV charge state ratios in subsequent experiments via least squares fitting. We test our dual excitation protocol (DEP) for a bulk diamond NV sample, 20 and 100 nm nanodiamond particles and compare results with those obtained via other commonly used techniques such as zero-phonon line fitting and non-negative matrix factorization. We find that DEP can be employed across different samples and experimental setups and yields consistent and quantitative results for NV charge state ratios that are in agreement with our understanding of NV photophysics. By providing robust NV charge state quantification across sample types and measurement platforms, DEP will support the development of NV-based quantum technologies.

cond-mat.mes-hall↗

arXiv2024

The $N_2V$ color center: a ubiquitous visible and near-infrared-II quantum emitter in nitrogen-doped diamond

Photoluminescent defects in diamond, like the nitrogen-vacancy (NV) color center, are at the forefront of emerging optical quantum technologies. Most emit in the visible and near-infrared spectral region below 1000 nm (NIR-I), limiting their applications in photonics, fiber communications, and biology. Here, we show that the nitrogen-vacancy-nitrogen ($N_2V$) center, which emits in the visible and near-infrared-II (NIR-II, 1000-1700 nm), is ubiquitous in as-synthesized and processed nitrogen-doped diamond from bulk samples to nanoparticles. We demonstrate that $N_2V$ is also present in commercially available state-of-the-art NV diamond sensing chips made via chemical vapor deposition (CVD). In high-pressure high-temperature (HPHT) diamonds, the photoluminescence (PL) intensity of both $N_2V$ charge states, $N_2V^0$ in the visible and $N_2V^-$ in the NIR-II, increases with increasing substitutional nitrogen concentration. We determine the PL lifetime of $N_2V^-$ to be 0.3 ns and compare a quantum optical and density functional theory model of the $N_2V^-$ with experimental PL spectra. Finally, we show that detonation nanodiamonds (DND) show stable PL in the NIR-II, which we attribute to the $N_2V$ color center, and use this NIR-II PL to image DNDs inside skin cells. Our results will contribute to the scientific and technological exploration and development of the $N_2V$ color center and inspire more research into its effect on other color centers in diamond.

cond-mat.mes-hall↗

arXiv2024

Extreme Enhancement-Mode Operation Accumulation Channel Hydrogen-Terminated Diamond FETs with $V_{th} < -6V$ and High On-Current

In this work we demonstrate a new Field Effect Transistor device concept based on hydrogen-terminated diamond (H-diamond) that operates in an Accumulation Channel rather than Transfer Doping regime. Our FET devices demonstrate both extreme enhancement-mode operation and high on-current with improved channel charge mobility compared to Transfer-Doped equivalents. Electron-beam evaporated $Al_2O_3$ is used on H-diamond to suppress the Transfer Doping mechanism and produce an extremely high ungated channel resistance. A high-quality H-diamond surface with an unpinned Fermi level is crucially achieved, allowing for formation of a high-density hole accumulation layer by gating the entire device channel which is encapsulated in dual-stacks of $Al_2O_3$. Completed devices with gate/channel length of $1 \mu m$ demonstrate record threshold voltage $< -6 V$ with on-current $> 80 mA/mm$. Carrier density and mobility figures extracted by CV analysis indicate high 2D charge density of $~ 2 \times 10^{12} cm^{-2}$ and increased hole mobility of $110 cm^2 /V \cdot s$ in comparison with more traditional Transfer-Doped H-diamond FETs. These results demonstrate the most negative threshold voltage yet reported for H-diamond FETs and highlight a new strategy for the development of high-performance power devices that better exploit diamond's intrinsic dielectric properties and high hole mobility.

cond-mat.mes-hall↗

arXiv2024

Impact of surface treatments on the electron affinity of nitrogen-doped ultrananocrystalline diamond

In recent years, various forms of nanocrystalline diamond (NCD) have emerged as an attractive group of diamond/graphite mixed-phase materials for a range of applications from electron emission sources to electrodes for neural interfacing. To tailor their properties for different uses, NCD surfaces can be terminated with various chemical functionalities, in particular hydrogen and oxygen, which shift the band edge positions and electron affinity values. While the band edge positions of chemically terminated single crystal diamond are well understood, the same is not true for nanocrystalline diamond, which has uncontrolled crystallographic surfaces with a variety of chemical states as well as graphitic grain boundary regions. In this work, the relative band edge positions of as-grown, hydrogen terminated, and oxygen terminated nitrogen-doped ultrananocrystalline diamond (N-UNCD) are determined using ultraviolet photoelectron spectroscopy (UPS), while the band bending is investigated using photoelectrochemical measurements. In contrast to the widely reported negative electrode affinity of hydrogen terminated single crystal diamond, our work demonstrates that hydrogen terminated N-UNCD exhibits a positive electron affinity owing to the increased surface and bulk defect densities. These findings elucidate the marked differences in electrochemical properties of hydrogen and oxygen terminated N-UNCD, such as the dramatic changes in electrochemical capacitance.

physics.app-ph↗

arXiv2024

Towards optical neuromodulation using nitrogen-doped ultrananocrystalline diamond photoelectrodes

Nitrogen-doped ultrananocrystalline diamond (N-UNCD) is a form of diamond electrode with near-infrared photoresponsivity, making it well suited for physiological applications. N-UNCD's photoresponsivity is strongly influenced by its surface. While it is known that oxygen treatment provides a higher photoresponsivity, a better understanding of its surface processes is needed to tailor the material for optical neuromodulation. This work examines the impact of various oxygen treatment methods, with aim of creating oxygen rich surfaces with different chemical and structural properties. Surface characterisation methods along with electrochemical and photoelectrochemical measurements and modelling were used to investigate the films. It was found that oxygen furnace annealing resulted in orders of magnitude improvement in the near-infrared photoresponsivity, to 3.75 +/- 0.05 uA/W. This translates to an approximate 200 times increase in the photocurrent compared to the untreated surface. This enhancement in photocurrent is largely due to the changes in the chemical species present at the surface. The photocurrent is estimated to be sufficient for extra-cellular stimulation of brain neurons within the safe optical exposure limit, positioning N-UNCD as an excellent candidate to be used in next-generation photoelectrodes for photobiomodulation.

physics.app-ph↗

arXiv2024

Miniature fluorescence sensor for quantitative detection of brain tumour

Fluorescence-guided surgery has emerged as a vital tool for tumour resection procedures. As well as intraoperative tumour visualisation, 5-ALA-induced PpIX provides an avenue for quantitative tumour identification based on ratiometric fluorescence measurement. To this end, fluorescence imaging and fibre-based probes have enabled more precise demarcation between the cancerous and healthy tissues. These sensing approaches, which rely on collecting the fluorescence light from the tumour resection site and its remote spectral sensing, introduce challenges associated with optical losses. In this work, we demonstrate the viability of tumour detection at the resection site using a miniature fluorescence measurement system. Unlike the current bulky systems, which necessitate remote measurement, we have adopted a millimetre-sized spectral sensor chip for quantitative fluorescence measurements. A reliable measurement at the resection site requires a stable optical window between the tissue and the optoelectronic system. This is achieved using an antifouling diamond window, which provides stable optical transparency. The system achieved a sensitivity of 92.3% and specificity of 98.3% in detecting a surrogate tumour at a resolution of 1 x 1 mm2. As well as addressing losses associated with collecting and coupling fluorescence light in the current remote sensing approaches, the small size of the system introduced in this work paves the way for its direct integration with the tumour resection tools with the aim of more accurate interoperative tumour identification.

eess.SY↗

arXiv2024

Methods for color center preserving hydrogen-termination of diamond

Chemical functionalization of diamond surfaces by hydrogen is an important method for controlling the charge state of near-surface fluorescent color centers, an essential process in fabricating devices such as diamond field-effect transistors and chemical sensors, and a required first step for realizing families of more complex terminations through subsequent chemical processing. In all these cases, termination is typically achieved using hydrogen plasma sources which can etch or damage the diamond as well as deposited materials or embedded colour centers. This work explores alternative methods for lower-damage hydrogenation of diamond surfaces, specifically the annealing of diamond samples in high-purity, non-explosive mixtures of nitrogen and hydrogen gas, and the exposure of samples to microwave hydrogen plasmas in the absence of intentional stage heating. The effectiveness of these methods are characterized by x-ray photoelectron spectroscopy, and comparison of the results to density-functional modelling of the surface hydrogenation energetics implicates surface oxygen ligands as the primary factor limiting the termination quality of annealed samples. Finally, photoluminescence spectroscopy is used to verify that both the annealing and reduced sample temperature plasma methods are non-destructive to near-surface ensembles of nitrogen-vacancy centers, in stark contrast to plasma treatments which use heated sample stages.

cond-mat.mtrl-sci↗

arXiv2024

Identification of defects and the origins of surface noise on hydrogen-terminated (100) diamond

Near-surface nitrogen-vacancy centres are critical to many diamond-based quantum technologies such as information processors and nanosensors. Surface defects play an important role in the design and performance of these devices. The targeted creation of defects is central to proposed bottom-up approaches to nanofabrication of quantum diamond processors, and uncontrolled surface defects may generate noise and charge trapping which degrade shallow NV device performance. Surface preparation protocols may be able to control the production of desired defects and eliminate unwanted defects, but only if their atomic structure can first be conclusively identified. This work uses a combination of scanning tunnelling microscopy (STM) imaging and first-principles simulations to identify several surface defects on H:C(100)-2x1 surfaces prepared using chemical vapour deposition (CVD). The atomic structure of these defects is elucidated, from which the microscopic origins of magnetic noise and charge trapping is determined based on modelling of their paramagnetic properties and acceptor states. Rudimentary control of these deleterious properties is demonstrated through STM tip-induced manipulation of the defect structure. Furthermore, the results validate accepted models for CVD diamond growth by identifying key adsorbates responsible for nucleation of new layers.

cond-mat.mes-hall↗

arXiv2024

Pick-and-place transfer of arbitrary-metal electrodes for van der Waals device fabrication

Van der Waals electrode integration is a promising strategy to create near-perfect interfaces between metals and two-dimensional materials, with advantages such as eliminating Fermi-level pinning and reducing contact resistance. However, the lack of a simple, generalizable pick-and-place transfer technology has greatly hampered the wide use of this technique. We demonstrate the pick-and-place transfer of pre-fabricated electrodes from reusable polished hydrogenated diamond substrates without the use of any surface treatments or sacrificial layers. The technique enables transfer of large-scale arbitrary metal electrodes, as demonstrated by successful transfer of eight different elemental metals with work functions ranging from 4.22 to 5.65 eV. The mechanical transfer of metal electrodes from diamond onto van der Waals materials creates atomically smooth interfaces with no interstitial impurities or disorder, as observed with cross-sectional high-resolution transmission electron microscopy and energy-dispersive X-ray spectroscopy. As a demonstration of its device application, we use the diamond-transfer technique to create metal contacts to monolayer transition metal dichalcogenide semiconductors with high-work-function Pd, low-work-function Ti, and semi metal Bi to create n- and p-type field-effect transistors with low Schottky barrier heights. We also extend this technology to other applications such as ambipolar transistor and optoelectronics, paving the way for new device architectures and high-performance devices.

physics.app-ph↗

arXiv2024

Formation of a boron-oxide termination for the (100) diamond surface

A boron-oxide termination of the diamond (100) surface has been formed by depositing molecular boron oxide $\rm{B_2O_3}$ onto the hydrogen-terminated (100) diamond surface under ultrahigh vacuum conditions and annealing to $\rm{950^{\circ} C}$. The resulting termination was highly oriented and chemically homogeneous, although further optimisation is required to increase the surface coverage beyond the 0.4 ML achieved here. This work demonstrates the possibility of using molecular deposition under ultrahigh vacuum conditions for complex surface engineering of the diamond surface, and may be a first step in an alternative approach to fabricating boron doped delta layers in diamond.

cond-mat.mtrl-sci↗

arXiv2023

Diamond Surface Functionalization via Visible Light-Driven C-H Activation for Nanoscale Quantum Sensing

Nitrogen-vacancy centers in diamond are a promising platform for nanoscale nuclear magnetic resonance sensing. Despite significant progress towards using NV centers to detect and localize nuclear spins down to the single spin level, NV-based spectroscopy of individual, intact, arbitrary target molecules remains elusive. NV molecular sensing requires that target molecules are immobilized within a few nanometers of NV centers with long spin coherence time. The inert nature of diamond typically requires harsh functionalization techniques such as thermal annealing or plasma processing, limiting the scope of functional groups that can be attached to the surface. Solution-phase chemical methods can be more readily generalized to install diverse functional groups, but they have not been widely explored for single-crystal diamond surfaces. Moreover, realizing shallow NV centers with long spin coherence times requires highly ordered single-crystal surfaces, and solution-phase functionalization has not yet been shown to be compatible with such demanding conditions. In this work, we report a versatile strategy to directly functionalize C-H bonds on single-crystal diamond surfaces under ambient conditions using visible light. This functionalization method is compatible with charge stable NV centers within 10 nm of the surface with spin coherence times comparable to the state of the art. As a proof of principle, we use shallow ensembles of NV centers to detect nuclear spins from functional groups attached to the surface. Our approach to surface functionalization based on visible light-driven C-H bond activation opens the door to deploying NV centers as a broad tool for chemical sensing and single-molecule spectroscopy.

cond-mat.mtrl-sci↗

arXiv2022

A telecom O-band emitter in diamond

Color centers in diamond are promising platforms for quantum technologies. Most color centers in diamond discovered thus far emit in the visible or near-infrared wavelength range, which are incompatible with long-distance fiber communication and unfavorable for imaging in biological tissues. Here, we report the experimental observation of a new color center that emits in the telecom O-band, which we observe in silicon-doped bulk single crystal diamonds and microdiamonds. Combining absorption and photoluminescence measurements, we identify a zero-phonon line at 1221 nm and phonon replicas separated by 42 meV. Using transient absorption spectroscopy, we measure an excited state lifetime of around 270 ps and observe a long-lived baseline that may arise from intersystem crossing to another spin manifold.

cond-mat.mtrl-sci↗

arXiv2022

DC Quantum Magnetometry Below the Ramsey Limit

We demonstrate quantum sensing of dc magnetic fields that exceeds the sensitivity of conventional $T_2^\ast$-limited dc magnetometry by more than an order of magnitude. We used nitrogen-vacancy centers in a diamond rotating at periods comparable to the spin coherence time, and characterize the dependence of magnetic sensitivity on measurement time and rotation speed. Our method up-converts only the dc field of interest and preserves the quantum coherence of the sensor. These results definitively improve the sensitivity of a quantum magnetometer to dc fields, an important and useful addition to the quantum sensing toolbox.

quant-ph↗

arXiv2021

Proximal nitrogen reduces the fluorescence quantum yield of nitrogen-vacancy centres in diamond

The nitrogen-vacancy colour centre in diamond is emerging as one of the most important solid-state quantum systems. It has applications to fields including high-precision sensing, quantum computing, single photon communication, metrology, nanoscale magnetic imaging and biosensing. For all of these applications, a high quantum yield of emitted photons is desirable. However, diamond samples engineered to have high densities of nitrogen-vacancy centres show levels of brightness varying significantly within single batches, or even within the same sample. Here we show that nearby nitrogen impurities quench emission of nitrogen-vacancy centres via non-radiative transitions, resulting in a reduced fluorescence quantum yield. We monitored the emission properties of nitrogen-vacancy centre ensembles from synthetic diamond samples with different concentrations of nitrogen impurities. While at low nitrogen densities of 1.81 ppm we measured a lifetime of 13.9 ns, we observed a strong reduction in lifetime with increasing nitrogen density. We measure a lifetime as low as 4.4 ns at a nitrogen density of 380 ppm. The change in lifetime matches a reduction in relative fluorescence quantum yield from 77.4 % to 32 % with an increase in nitrogen density from 88 ppm to 380 ppm, respectively. These results will inform the conditions required to optimise the properties of diamond crystals devices based on the fluorescence of nitrogen-vacancy centres. Furthermore, this work provides insights into the origin of inhomogeneities observed in high-density nitrogen-vacancy ensembles within diamonds and nanodiamonds.

quant-ph↗