arXiv subjects

Marcus W. Doherty

Publications and source records attributed to Marcus W. Doherty.

At least 19 recordsLinked to original sources

arXiv2026

Spin-Dependent Charge-State Conversion in NV Ensembles Mediated by Electron Tunneling

The nitrogen-vacancy (NV) center in diamond enables optical initialization and readout of its electronic spin, forming the basis of a wide range of quantum sensing and metrology applications. A central challenge in such measurements is the coexistence of two charge states, NV- and NV0: While detection protocols rely on the spin-dependent properties of NV-, fluorescence from NV0 does not carry useful contrast and is typically removed as background, reducing the available signal. Here, we show that the origin of NV0 emission depends strongly on the excitation wavelength in nitrogen-containing diamond. Using ensembles of NV centers with varying nitrogen concentrations, we compare excitation at the NV0 zero-phonon line (ZPL) at 575 nm with the commonly used 532 nm. We find that excitation at 575 nm generates NV0 predominantly through spin-selective tunneling from the excited state of NV- to nearby nitrogen donors, such that the NV0 emission follows the spin polarization of NV-. As a result, the NV0 fluorescence contributes to the measurable spin contrast, allowing the full fluorescence signal to be used for detection. This result opens opportunities for improved sensitivity in NV-based sensing applications.

cond-mat.mes-hall↗

arXiv2026

Tunneling probe-based identification of the sp${}^3$ dangling bond on the H-C(100):$2\times1$ surface

The sp${}^3$ dangling bond on the diamond surface plays a critical role in the performance and fabrication of diamond quantum technologies. For the former, the magnetic and electric properties of this defect can impede the performance of quantum sensors and computers. For the latter, the chemical properties of the dangling bond are integral to proposed methods for bottom-up fabrication of scalable diamond quantum devices. In pursuit of high performance and scalable diamond quantum technology, tunneling probe-based techniques offers the ability to create and modify the sp${}^3$ dangling bond with atomic-scale precision. However, these capabilities cannot be realised either deterministically or at scale without a means for identifying the sp${}^3$ dangling bond amidst the myriad of other defects on the diamond surface. Consequently, in this work we provide a comprehensive experimental and theoretical framework for STS-based characterisation of the sp${}^3$ defect on the H-terminated (100) diamond surface. This capability provides the foundation for future tunneling probe studies in the modification of dangling bonds.

cond-mat.mes-hall↗

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↗

arXiv2023

First quantum machine learning applications on an on-site room-temperature quantum computer

We demonstrate - for the first time - the application of a quantum machine learning (QML) algorithm on an on-site room-temperature quantum computer. A two-qubit quantum computer installed at the Pawsey Supercomputing Centre in Perth, Australia, is used to solve multi-class classification problems on unseen, i.e. untrained, 2D data points. The underlying 1-qubit model is based on the data re-uploading framework of the universal quantum classifier and was trained on an ideal quantum simulator using the Adam optimiser. No noise models or device-specific insights were used in the training process. The optimised model was deployed to the quantum device by means of a single XYX decomposition leading to three parameterised single qubit rotations. The results for different classification problems are compared to the optimal results of an ideal simulator. The room-temperature quantum computer achieves very high classification accuracies, on par with ideal state vector simulations.

quant-ph↗

arXiv2023

Semiempirical $\textit{ab initio}$ modeling of bound states of deep defects in semiconductor quantum technologies

A significant hurdle in developing high-performance semiconductor quantum technologies utilizing deep defects is related to charge dynamics. Unfortunately, progress in modeling their charge dynamics has been hindered over recent decades due to the absence of appropriate multiscale models capable of accurately representing the atomic properties of these defects and their impact on device performance. Here, we present a semi-\textit{ab initio} method for modeling the bound states of deep defects in semiconductor quantum technologies, applied to the negatively charged nitrogen vacancy (NV$^-$) center in diamond. We employ density functional theory calculations to construct accurate potentials for an effective mass model, which allow us to unveil the structure of the bound hole states. We develop a model to calculate the nonradiative capture cross sections, which agrees with experiment within one order of magnitude. Finally, we present our attempt at constructing the photoionization spectrum of NV$^0\rightarrow$ NV$^-$ + bound hole, showing that the electronic transitions of the bound holes can be distinguished from phonon sidebands. This paper offers a practical and efficient solution to a long-standing challenge in understanding the charge dynamics of deep defects.

cond-mat.mes-hall↗

arXiv2023

Detection and modeling of hole capture by single point defects under variable electric fields

Understanding carrier trapping in solids has proven key to semiconductor technologies but observations thus far have relied on ensembles of point defects, where the impact of neighboring traps or carrier screening is often important. Here, we investigate the capture of photo-generated holes by an individual negatively-charged nitrogen-vacancy (NV) center in diamond at room temperature. Using an externally gated potential to minimize space-charge effects, we find the capture probability under electric fields of variable sign and amplitude shows an asymmetric-bell-shaped response with maximum at zero voltage. To interpret these observations, we run semi-classical Monte Carlo simulations modeling carrier trapping through a cascade process of phonon emission, and obtain electric-field-dependent capture probabilities in good agreement with experiment. Since the mechanisms at play are insensitive to the trap characteristics, the capture cross sections we observe - largely exceeding those derived from ensemble measurements - should also be present in materials platforms other than diamond.

cond-mat.mes-hall↗

arXiv2023

Quantum utility -- definition and assessment of a practical quantum advantage

Several benchmarks have been proposed to holistically measure quantum computing performance. While some have focused on the end user's perspective (e.g., in application-oriented benchmarks), the real industrial value taking into account the physical footprint of the quantum processor are not discussed. Different use-cases come with different requirements for size, weight, power consumption, or data privacy while demanding to surpass certain thresholds of fidelity, speed, problem size, or precision. This paper aims to incorporate these characteristics into a concept coined quantum utility, which demonstrates the effectiveness and practicality of quantum computers for various applications where quantum advantage -- defined as either being faster, more accurate, or demanding less energy -- is achieved over a classical machine of similar size, weight, and cost. To successively pursue quantum utility, a level-based classification scheme -- constituted as application readiness levels (ARLs) -- as well as extended classification labels are introduced. These are demonstratively applied to different quantum applications from the fields of quantum chemistry, quantum simulation, quantum machine learning, and data analysis followed by a brief discussion.

quant-ph↗

arXiv2022

Temperature Sensitivity of $^{14}\mathrm{NV}$ and $^{15}\mathrm{NV}$ Ground State Manifolds

We measure electron and nuclear spin transition frequencies in the ground state of nitrogen-vacancy (NV) centers in diamond for two nitrogen isotopes ($^{14}\mathrm{NV}$ and $^{15}\mathrm{NV}$) over temperatures ranging from 77 K to 400 K. Measurements are performed using Ramsey interferometry and direct optical readout of the nuclear and electron spins. We extract coupling parameters $Q$ (for $^{14}\mathrm{NV}$), $D$, $A_{||}$, $A_{\perp}$, $γ_e/γ_n$, and their temperature dependences for both isotopes. The temperature dependences of the nuclear-spin transitions within the $m_s = 0$ spin manifold near room temperature are found to be +0.52(1) ppm/K for $^{14}\mathrm{NV}$ ($|m_I=-1> \leftrightarrow |m_I=+1>$) and -1.1(1) ppm/K for $^{15}\mathrm{NV}$ ($|m_I=-1/2> \leftrightarrow |m_I=+1/2>$). An isotopic shift in the zero-field splitting parameter $D$ between $^{14}\mathrm{NV}$ and $^{15}\mathrm{NV}$ is measured to be $\sim$ 120 kHz. Residual transverse magnetic fields are observed to shift the nuclear spin transition frequencies, especially for $^{15}\mathrm{NV}$. We have precisely determined the set of parameters relevant for the development of nuclear-spin-based diamond quantum sensors with greatly reduced sensitivity to environmental factors.

quant-ph↗

arXiv2021

Optical activation and detection of charge transport between individual color centers in room-temperature diamond

Charge control of color centers in semiconductors promises opportunities for novel forms of sensing and quantum information processing. Here, we articulate confocal fluorescence microscopy and magnetic resonance protocols to induce and probe charge transport between discrete sets of engineered nitrogen-vacancy (NV) centers in diamond, down to the level of individual defects. In our experiments, a "source" NV undergoes optically-driven cycles of ionization and recombination to produce a stream of photo-generated carriers, one of which we subsequently capture via a "target" NV several micrometers away. We use a spin-to-charge conversion scheme to encode the spin state of the source color center into the charge state of the target, in the process allowing us to set an upper bound to carrier injection from other background defects. We attribute our observations to the action of unscreened Coulomb potentials producing giant carrier capture cross-sections, orders of magnitude greater than those typically attained in ensemble measurements. Besides their fundamental interest, these results open intriguing prospects in the use of free carriers as a quantum bus to mediate effective interactions between paramagnetic defects in a solid-state chip.

cond-mat.mes-hall↗

arXiv2021

Spin-to-Charge conversion with electrode confinement in diamond

The nitrogen-vacancy (NV) center in diamond has a wide range of potential applications in quantum metrology, communications and computation. The key to its use lies in how large the optical spin contrast is and the associated fidelity of spin state readout. In this paper we propose a new mechanism for improving contrast with a spin-to-charge protocol that relies on the use of an external electrode and cryogenic temperatures to discretize the diamond conduction band for spin-selective resonant photoionization. We use effective mass theory to calculate the discrete eigenenergies in this new system and use them to formulate a new spin-to-charge protocol that involves resonant photoionization out the NV ground state into the diamond conduction band. The major sources of broadening are also addressed which guide the design of the experiment. With this mechanism we theorise an optical spin contrast that and an associated spin readout fidelity of 85%. This significant improvement can be applied to a number of cryogenic quantum technologies.

quant-ph↗

arXiv2021

Vibrational and vibronic structure of isolated point defects: the nitrogen-vacancy center in diamond

We present a theoretical study of vibrational and vibronic properties of a point defect in the dilute limit by means of first-principles density functional theory calculations. As an exemplar we choose the negatively charged nitrogen-vacancy center, a solid-state system that has served as a testbed for many protocols of quantum technology. We achieve low effective concentrations of defects by constructing dynamical matrices of large supercells containing tens of thousands of atoms. The main goal of the paper is to calculate luminescence and absorption lineshapes due to coupling to vibrational degrees of freedom. The coupling to symmetric $a_1$ modes is computed via the Huang-Rhys theory. Importantly, to include a nontrivial contribution of $e$ modes we develop an effective methodology to solve the multi-mode $E \otimes e$ Jahn-Teller problem. Our results show that for NV centers in diamond a proper treatment of $e$ modes is particularly important for absorption. We obtain good agreement with experiment for both luminescence and absorption. Finally, the remaining shortcomings of the theoretical approach are critically reviewed. The presented theoretical approach will benefit identification and future studies of point defects in solids.

cond-mat.mtrl-sci↗

arXiv2021

Prolonged orbital relaxation by locally modified phonon density of states for SiV$^-$ center in nanodiamonds

Coherent quantum systems are a key resource for emerging quantum technology. Solid-state spin systems are of particular importance for compact and scalable devices. However, interaction with the solid-state host degrades the coherence properties. The negatively-charged silicon vacancy center in diamond is such an example. While spectral properties are outstanding, with optical coherence protected by the defects symmetry, the spin coherence is susceptible to rapid orbital relaxation limiting the spin dephasing time. A prolongation of the orbital relaxation time is therefore of utmost urgency and has been tackled by operating at very low temperatures or by introducing large strain. However, both methods have significant drawbacks, the former requires use of dilution refrigerators and the latter affects intrinsic symmetries. Here, a novel method is presented to prolong the orbital relaxation with a locally modified phonon density of states in the relevant frequency range, by restricting the diamond host to below 100 nm. The method works at liquid Helium temperatures of few Kelvin and in the low-strain regime.

quant-ph↗

arXiv2021

Photoionization of negatively charged NV centers in diamond: theory and ab initio calculations

We present ab-initio calculations of photoionization thresholds and cross sections of the negatively charged nitrogen-vacancy (NV) center in diamond from the ground $^{3}\!A_2$ and the excited $^{3}\!E$ states. We show that after the ionization from the $^{3}\!E$ level the NV center transitions into the metastable $^{4}\!A_2$ electronic state of the neutral defect. We reveal how spin polarization of $\mathrm{NV}^{-}$ gives rise to spin polarization of the $^{4}\!A_2$ state, providing an explanation of electron spin resonance experiments. We obtain smooth photoionization cross sections by employing dense $k$-point meshes for the Brillouin zone integration together with the band unfolding technique to rectify the distortions of the band structure induced by artificial periodicity of the supercell approach. Our calculations provide a comprehensive picture of photoionization mechanisms of $\mathrm{NV}^{-}$. They will be useful in interpreting and designing experiments on charge-state dynamics at NV centers. In particular, we offer a consistent explanation of recent results of spin-to-charge conversion of NV centers.

cond-mat.mtrl-sci↗

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↗

arXiv2020

Optimisation of diamond quantum processors

Diamond quantum processors consisting of a nitrogen-vacancy (NV) centre and surrounding nuclear spins have been the key to significant advancements in room-temperature quantum computing, quantum sensing and microscopy. The optimisation of these processors is crucial for the development of large-scale diamond quantum computers and the next generation of enhanced quantum sensors and microscopes. Here, we present a full model of multi-qubit diamond quantum processors and develop a semi-analytical method for designing gate pulses. This method optimises gate speed and fidelity in the presence of random control errors and is readily compatible with feedback optimisation routines. We theoretically demonstrate infidelities approaching $\sim 10^{-5}$ for single-qubit gates and established evidence that this can also be achieved for a two-qubit CZ gate. Consequently, our method reduces the effects of control errors below the errors introduced by hyperfine field misalignment and the unavoidable decoherence that is intrinsic to the processors. Having developed this optimal control, we simulated the performance of a diamond quantum processor by computing quantum Fourier transforms. We find that the simulated diamond quantum processor is able to achieve fast operations with low error probability.

quant-ph↗

arXiv2020

Mechanical Decoupling of Quantum Emitters in Hexagonal Boron Nitride from Low-Energy Phonon Modes

Quantum emitters in hexagonal Boron Nitride (hBN) were recently reported to hol a homogeneous linewidth according to the Fourier-Transform limit up to room temperature. This unusual observation was traced back to decoupling from in-plane phonon modes which can arise if the emitter is located between two planes of the hBN host material. In this work, we investigate the origins for the mechanical decoupling. Improved sample preparation enabled a reduced background and a 70-fold decrease of spectral diffusion which was so far the major drawback of defect center in hBN and allowed us to reveal a gap in the electron-phonon spectral density for low phonon frequencies. This decoupling from phonons persists at room temperature and explains the observed Fourier Transform limited lines up to 300K. Furthermore, we investigate the dipole emission directionality and show a preferred photon emission through the side of the hBN flakes supporting the claim for an out-of-plane distortion of the defect center. Our work lays the foundation to a deeper understanding of the underlying physics for the persistence of Fourier-Transform limit lines up to room temperature. It furthermore provides a description on how to identify the mechanically isolated emitter within the large number of defect centers in hBN. Therefore, it paves the way for quantum optics applications with defect centers in hBN at room temperature.

cond-mat.mes-hall↗

arXiv2019

A solution to electric-field screening in diamond quantum electrometers

There are diverse interdisciplinary applications for nanoscale resolution electrometry of elementary charges under ambient conditions. These include characterization of 2D electronics, charge transfer in biological systems, and measurement of fundamental physical phenomena. The nitrogen-vacancy center in diamond is uniquely capable of such measurements, however electrometry thus far has been limited to charges within the same diamond lattice. It has been hypothesized that the failure to detect charges external to diamond is due to quenching and surface screening, but no proof, model, or design to overcome this has yet been proposed. In this work we affirm this hypothesis through a comprehensive theoretical model of screening and quenching within a diamond electrometer and propose a solution using controlled nitrogen doping and a fluorine-terminated surface. We conclude that successful implementation requires further work to engineer diamond surfaces with lower surface defect concentrations.

physics.app-ph↗

arXiv2019

Mechanical rotation via optical pumping of paramagnetic impurities

Hybrid quantum systems exhibiting coupled optical, spin, and mechanical degrees of freedom can serve as a platform for sensing, or as a bus to mediate interactions between qubits with disparate energy scales. These systems are also creating opportunities to test foundational ideas in quantum mechanics, including direct observations of the quantum regime in macroscopic objects. Here, we make use of angular momentum conservation to study the dynamics of a pair of paramagnetic centers featuring different spin numbers in the presence of a properly tuned external magnetic field. We examine the interplay between optical excitation, spin evolution, and mechanical motion, and theoretically show that in the presence of continuous optical illumination, inter-spin cross-relaxation must induce rigid rotation of the host crystal. The system dynamics is robust to scattering of spin-polarized phonons, a result we build on to show this form of angular momentum transfer should be observable using state-of-the-art torsional oscillators or trapped nanoparticles.

quant-ph↗