arXiv subjects

Marcus W. Doherty

Publications and source records attributed to Marcus W. Doherty.

At least 37 records · Page 2Linked to original sources

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↗

arXiv2019

Discovery of ST1 centers in natural diamond

The ST1 center is a point defect in diamond with bright fluorescence and a mechanism for optical spin initialization and readout. The center has impressive potential for applications in diamond quantum computing as a quantum bus to a register of nuclear spins. This is because it has an exceptionally high readout contrast and, unlike the well-known nitrogen-vacancy center, it does not have a ground state electronic spin that decoheres the nuclear spins. However, its chemical structure is unknown and there are large gaps in our understanding of its properties. We present the discovery of ST1 centers in natural diamond. Our experiments identify interesting power dependence of the center's optical dynamics and reveal new electronic structure. We also present a theory of its electron-phonon interactions, which we combine with previous experiments, to shortlist likely candidates for its chemical structure.

quant-ph↗

arXiv2019

Atomic Localization of Quantum Emitters in Multilayer Hexagonal Boron Nitride

The recent discovery of single-photon emitting defects hosted by the two-dimensional wide band gap semiconductor hexagonal boron nitride (hBN) has inspired a great number of experiments. Key characteristics of these quantum emitters are their capability to operate at room temperature with a high luminosity. In spite of large theoretical and experimental research efforts, the exact nature of the emission remains unresolved. In this work we utilize layer-by-layer etching of multilayer hBN to localize the quantum emitters with atomic precision. Our results suggest the position of the emitters correlates with the fabrication method: emitters formed under plasma treatment are always in close proximity to the crystal surface, while emitters created under electron irradiation are distributed randomly throughout the entire crystal. This disparity could be traced back to the lower kinetic energy of the ions in the plasma compared to the kinetic energy of the electrons in the particle accelerator. The emitter distance to the surface also correlates with the excited state lifetime: near-surface emitters have a shorter compared to emitters deep within the crystal. Finite-difference time-domain and density functional theory simulations show that optical and electronic effects are not responsible for this difference, indicating effects such as coupling to surface defects or phonons might cause the reduced lifetime. Our results pave a way toward identification of the defect, as well as engineering the emitter properties.

cond-mat.mes-hall↗

arXiv2019

Diamond nano-pillar arrays for quantum microscopy of neuronal signals

Modern neuroscience is currently limited in its capacity to perform long term, wide-field measurements of neuron electromagnetics with nanoscale resolution. Quantum microscopy using the nitrogen vacancy centre (NV) can provide a potential solution to this problem with electric and magnetic field sensing at nano-scale resolution and good biocompatibility. However, the performance of existing NV sensing technology does not allow for studies of small mammalian neurons yet. In this paper, we propose a solution to this problem by engineering NV quantum sensors in diamond nanopillar arrays. The pillars improve light collection efficiency by guiding excitation/emission light, which improves sensitivity. More importantly, they also improve the size of the signal at the NV by removing screening charges as well as coordinating the neuron growth to the tips of the pillars where the NV is located. Here, we provide a growth study to demonstrate coordinated neuron growth as well as the first simulation of nano-scopic neuron electric and magnetic fields to assess the enhancement provided by the nanopillar geometry.

quant-ph↗

arXiv2018

Radiation tolerance of two-dimensional material-based devices for space applications

Characteristic for devices based on two-dimensional materials are their low size, weight and power requirements. This makes them advantageous for use in space instrumentation, including photovoltaics, batteries, electronics, sensors and light sources for long-distance quantum communication. Here, we present for the first time a comprehensive study on combined radiation effects in earth's atmosphere on various devices based on these nanomaterials. Using theoretical modeling packages, we estimate relevant radiation levels and then expose field-effect transistors, single-photon sources and monolayers as building blocks for future electronics to gamma-rays, protons and electrons. The devices show negligible change in performance after the irradiation, suggesting robust suitability for space use. Under excessive $γ$-radiation, however, monolayer WS$_2$ showed decreased defect densities, identified by an increase in photoluminescence, carrier lifetime and a change in doping ratio proportional to the photon flux. The underlying mechanism was traced back to radiation-induced defect healing, wherein dissociated oxygen passivates sulfur vacancies.

cond-mat.mtrl-sci↗

arXiv2018

NV- - N+ pair centre in 1b diamond

The study establishes that the degree of optically induced spin polarization that can be achieved for NV$^- $in 1b diamond is limited by the concentration of single substitutional nitrogen, N$^0$ . The polarization of the individual NV centres in the diamond is dependent on the separation of the NV$^-$ and the nitrogen donor. When the NV$^-$ - N$^+$ pair separation is large the properties of the pair will be as for single sites and a high degree of spin polarization attainable. When the separation decreases the emission is reduced, the lifetime shortened and the spin polarization downgraded. The deterioration occurs as a consequence of electron tunneling in the excited state from NV$^-$ to N$^+$ and results in an optical cycle that includes NV$^0$. The tunneling process is linear in optical excitation and more prevalent the closer the N$^+$ is to the NV$^-$ centre. However, the separation between the NV$^-$ and its donor N$^+$ can be effected by light through the excitation of NV$^-$ and/or ionization of N$^0$. The optical excitation that creates the spin polarization can also modify the sample properties and during excitation creates charge dynamics. The consequence is that the magnitude of spin polarization, the spin relaxation and coherence times T$_1$ and T$_2$ have a dependence on the nitrogen concentration and on the excitation wavelength. The adjacent N$^+$ gives an electric field that Stark shifts the NV$^-$ transitions and for an ensemble results in line broadening. It is observation of changes of these Stark induced effects that allow the variation in NV$^-$ - N$^+$ separation to be monitored. Spectroscopic measurements including that of the varying line widths are central to the study. They are made at low temperatures and include extensive measurements of the NV$^-$ optical transition at 637 nm, the infrared transition at 1042 nm and ODMR at 2.87 GHz.

cond-mat.mtrl-sci↗

arXiv2018

Spin-Dependent Quantum Emission in Hexagonal Boron Nitride at Room Temperature

Optically addressable spins associated with defects in wide-bandgap semiconductors are versatile platforms for quantum information processing and nanoscale sensing, where spin-dependent inter-system crossing (ISC) transitions facilitate optical spin initialization and readout. Recently, the van der Waals material hexagonal boron nitride (h-BN) has emerged as a robust host for quantum emitters (QEs), but spin-related effects have yet to be observed. Here, we report room-temperature observations of strongly anisotropic photoluminescence (PL) patterns as a function of applied magnetic field for select QEs in h-BN. Field-dependent variations in the steady-state PL and photon emission statistics are consistent with an electronic model featuring a spin-dependent ISC between triplet and singlet manifolds, indicating that optically-addressable spin defects are present in h-BN $-$ a versatile two-dimensional material promising efficient photon extraction, atom-scale engineering, and the realization of spin-based quantum technologies using van der Waals heterostructures.

quant-ph↗

arXiv2017

Nanomechanical sensing using spins in diamond

Nanomechanical sensors and quantum nanosensors are two rapidly developing technologies that have diverse interdisciplinary applications in biological and chemical analysis and microscopy. For example, nanomechanical sensors based upon nanoelectromechanical systems (NEMS) have demonstrated chip-scale mass spectrometry capable of detecting single macromolecules, such as proteins. Quantum nanosensors based upon electron spins of negatively-charged nitrogen-vacancy (NV) centers in diamond have demonstrated diverse modes of nanometrology, including single molecule magnetic resonance spectroscopy. Here, we report the first step towards combining these two complementary technologies in the form of diamond nanomechanical structures containing NV centers. We establish the principles for nanomechanical sensing using such nano-spin-mechanical sensors (NSMS) and assess their potential for mass spectrometry and force microscopy. We predict that NSMS are able to provide unprecedented AC force images of cellular biomechanics and to, not only detect the mass of a single macromolecule, but also image its distribution. When combined with the other nanometrology modes of the NV center, NSMS potentially offer unparalleled analytical power at the nanoscale.

quant-ph↗

arXiv2016

Optical patterning of trapped charge in nitrogen-doped diamond

The nitrogen-vacancy (NV) centre in diamond is emerging as a promising platform for solid-state quantum information processing and nanoscale metrology. Of interest in these applications is the manipulation of the NV charge, which can be attained by optical excitation. Here we use two-color optical microscopy to investigate the dynamics of NV photo-ionization, charge diffusion, and trapping in type-1b diamond. We combine fixed-point laser excitation and scanning fluorescence imaging to locally alter the concentration of negatively charged NVs, and to subsequently probe the corresponding redistribution of charge. We uncover the formation of spatial patterns of trapped charge, which we qualitatively reproduce via a model of the interplay between photo-excited carriers and atomic defects. Further, by using the NV as a probe, we map the relative fraction of positively charged nitrogen upon localized optical excitation. These observations may prove important to transporting quantum information between NVs or to developing three-dimensional, charge-based memories.

cond-mat.mes-hall↗

arXiv2016

Development of a high quality thin diamond membrane with embedded nitrogen-vacancy centers for hybrid spin-mechanical quantum systems

Hybrid quantum systems (HQSs) have attracted several research interests in the last years. In this Letter, we report on the design, fabrication, and characterization of a novel diamond architecture for HQSs that consists of a high quality thin circular diamond membrane with embedded near-surface nitrogen-vacancy centers (NVCs). To demonstrate this architecture, we employed the NVCs by means of their optical and spin interfaces as nanosensors of the motion of the membrane under static pressure and in-resonance vibration, as well as the residual stress of the membrane. Driving the membrane at its fundamental resonance mode, we observed coupling of this vibrational mode to the spin of the NVCs by Hahn echo signal. Our realization of this architecture will enable futuristic HQS-based applications in diamond piezometry and vibrometry, as well as spin-mechanical and mechanically mediated spin-spin coupling in quantum information science.

cond-mat.mes-hall↗

arXiv2015

Towards a room-temperature spin quantum bus in diamond via optical spin injection, transport and detection

Diamond is a proven solid-state platform for spin-based quantum technology. The nitrogen-vacancy (NV) center in diamond has been used to realize small-scale quantum information processing (QIP) and quantum sensing under ambient conditions. A major barrier in the development of large-scale QIP in diamond is the connection of NV spin registers by a quantum bus at room temperature. Given that diamond is expected to be an ideal spin transport material, the coherent transport of spin directly between the spin registers offers a potential solution. Yet, there has been no demonstration of spin transport in diamond due to difficulties in achieving spin injection and detection via conventional methods. Here, we exploit detailed knowledge of the paramagnetic defects in diamond to identify novel mechanisms to achieve spin injection, transport and detection in diamond at room temperature. Having identified these mechanisms, we explore how they may be combined to realise an on-chip spin quantum bus.

quant-ph↗

arXiv2015

The electron-phonon processes of the nitrogen-vacancy center in diamond

Applications of negatively charged nitrogen-vacancy center in diamond exploit the center's unique optical and spin properties, which at ambient temperature, are predominately governed by electron-phonon interactions. Here, we investigate these interactions at ambient and elevated temperatures by observing the motional narrowing of the center's excited state spin resonances. We determine that the center's Jahn-Teller dynamics are much slower than currently believed and identify the vital role of symmetric phonon modes. Our results have pronounced implications for center's diverse applications (including quantum technology) and for understanding its fundamental properties.

quant-ph↗

arXiv2015

All-optical thermometry and the thermal properties of the optically detected spin resonances of the NV center in nano-diamond

The negatively-charged nitrogen-vacancy (NV) center in diamond is at the frontier of quantum nano-metrology and bio-sensing. Recent attention has focused on the application of high-sensitivity thermometry using the spin resonances of NV centers in nano-diamond to sub-cellular biological and biomedical research. Here, we report a comprehensive investigation of the thermal properties of the center's spin resonances and demonstrate an alternate all-optical NV thermometry technique that exploits the temperature dependence of the center's optical Debye-Waller factor.

quant-ph↗

arXiv2014

Electron-phonon processes of the silicon-vacancy centre in diamond

We investigate phonon induced electronic dynamics in the ground and excited states of the negatively charged silicon-vacancy ($\mathrm{SiV}^-$) centre in diamond. Optical transition line widths, transition wavelength and excited state lifetimes are measured for the temperature range 4-350 K. The ground state orbital relaxation rates are measured using time-resolved fluorescence techniques. A microscopic model of the thermal broadening in the excited and ground states of the $\mathrm{SiV}^-$ centre is developed. A vibronic process involving single-phonon transitions is found to determine orbital relaxation rates for both the ground and the excited states at cryogenic temperatures. We discuss the implications of our findings for coherence of qubit states in the ground states and propose methods to extend coherence times of $\mathrm{SiV}^-$ qubits.

quant-ph↗

arXiv2014

Singlet levels of the NV$^{-}$ centre in diamond

The characteristic transition of the NV- centre at 637 nm is between ${}^3\mathrm{A}_2$ and ${}^3\mathrm{E}$ triplet states. There are also intermediate ${}^1\mathrm{A}_1$ and ${}^1\mathrm{E}$ singlet states, and the infrared transition at 1042 nm between these singlets is studied here using uniaxial stress. The stress shift and splitting parameters are determined, and the physical interaction giving rise to the parameters is considered within the accepted electronic model of the centre. It is established that this interaction for the infrared transition is due to a modification of electron-electron Coulomb repulsion interaction. This is in contrast to the visible 637 nm transition where shifts and splittings arise from modification to the one-electron Coulomb interaction. It is also established that a dynamic Jahn-Teller interaction is associated with the singlet ${}^1\mathrm{E}$ state, which gives rise to a vibronic level 115 $\mathrm{cm}^{-1}$ above the ${}^1\mathrm{E}$ electronic state. Arguments associated with this level are used to provide experimental confirmation that the ${}^1\mathrm{A}_1$ is the upper singlet level and ${}^1\mathrm{E}$ is the lower singlet level.

cond-mat.mtrl-sci↗

arXiv2014

Generation of spin-polarized currents via cross-relaxation with dynamically pumped paramagnetic impurities

Key to future spintronics and spin-based information processing technologies is the generation, manipulation, and detection of spin polarization in a solid state platform. Here, we theoretically explore an alternative route to spin injection via the use of dynamically polarized nitrogen-vacancy (NV) centers in diamond. We focus on the geometry where carriers and NV centers are confined to proximate, parallel layers and use a 'trap-and-release' model to calculate the spin cross-relaxation probabilities between the charge carriers and neighboring NV centers. We identify near-unity regimes of carrier polarization depending on the NV spin state, applied magnetic field, and carrier g-factor. In particular, we find that unlike holes, electron spins are distinctively robust against spin-lattice relaxation by other, unpolarized paramagnetic centers. Further, the polarization process is only weakly dependent on the carrier hopping dynamics, which makes this approach potentially applicable over a broad range of temperatures.

cond-mat.mes-hall↗

arXiv2014

Measuring the defect structure orientation of a single NV- centre in diamond

The negatively charged nitrogen-vacancy (NV-) centre in diamond has many exciting applications in quantum nano-metrology, including magnetometry, electrometry, thermometry and piezometry. Indeed, it is possible for a single NV- centre to measure the complete three-dimensional vector of the local electric field or the position of a single fundamental charge in ambient conditions. However, in order to achieve such vector measurements, near complete knowledge of the orientation of the centre's defect structure is required. Here, we demonstrate an optically detected magnetic resonance (ODMR) technique employing rotations of static electric and magnetic fields that precisely determines the orientation of the centre's major and minor trigonal symmetry axes. Thus, our technique is an enabler of the centre's existing vector sensing applications and also motivates new applications in multi-axis rotation sensing, NV growth characterization and diamond crystallography.

quant-ph↗

arXiv2014

Electronic structure of the negatively-charged silicon-vacancy center in diamond

The negatively-charged silicon-vacancy (SiV$^-$) center in diamond is a promising single photon source for quantum communications and information processing. However, the center's implementation in such quantum technologies is hindered by contention surrounding its fundamental properties. Here we present optical polarization measurements of single centers in bulk diamond that resolve this state of contention and establish that the center has a $\langle111\rangle$ aligned split-vacancy structure with $D_{3d}$ symmetry. Furthermore, we identify an additional electronic level and evidence for the presence of dynamic Jahn-Teller effects in the center's 738 nm optical resonance.

cond-mat.mtrl-sci↗