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M. W. Doherty

Publications and source records attributed to M. W. Doherty.

At least 19 recordsLinked to original sources

NV with nitrogen

The paper highlights the difference the properties the nitrogen vacancy centre in bulk diamond containing nitrogen compared to the properties of single centres. Charge transfer between the negative and neutral charge state can occur with a tunnelling of an electron from an adjacent nitrogen atom without involving conduction or valence electrons. This contrasts with charge transfer of single sites. There are other differences for example with the intersystem crossing.

cond-mat.mtrl-sci

Probing the Evolution of Electron Spin Wavefunction of NV Center in diamond via Pressure Tuning

Understanding the profile of a qubit's wavefunction is key to its quantum applications. Unlike conducting systems, where a scanning tunneling microscope can be used to probe the electron distribution, there is no direct method for solid-state-defect based qubits in wide-bandgap semiconductors. In this work, we use pressure as a tuning method and a nuclear spin as an atomic scale probe to monitor the hyperfine structure of negatively charged nitrogen vacancy (NV) centers in diamonds under pressure. We present a detailed study on the nearest-neighbor $^{13}C$ hyperfine splitting in the optically detected magnetic resonance (ODMR) spectrum of NV centers at different pressures. By examining the $^{13}C$ hyperfine interaction upon pressurizing, we show that the NV hyperfine parameters have prominent changes, resulting in an increase in the NV electron spin density and rehybridization from $sp^3$ to $sp^2$ bonds. The $ab$ $initio$ calculations of strain dependence of the NV center's hyperfine levels are done independently. The theoretical results qualitatively agree well with experimental data without introducing any fitting parameters. Furthermore, this method can be adopted to probe the evolution of wavefunction in other defect systems. This potential capability could play an important role in developing magnetometry and quantum information processing using the defect centers.

cond-mat.mes-hall

Nanoscale vector electric field imaging using a single electron spin

The ability to perform nanoscale electric field imaging of elementary charges at ambient temperatures will have diverse interdisciplinary applications. While the nitrogen-vacancy (NV) center in diamond is capable of high-sensitivity electrometry, demonstrations have so far been limited to macroscopic field features or detection of single charges internal to diamond itself. In this work we greatly extend these capabilities by using a shallow NV center to image the electric field of a charged atomic force microscope tip with nanoscale resolution. This is achieved by measuring Stark shifts in the NV spin-resonance due to AC electric fields. To achieve this feat we employ for the first time, the integration of Qdyne with scanning quantum microscopy. We demonstrate near single charge sensitivity of $η_e = 5.3$ charges/$\sqrt{\text{Hz}}$, and sub-charge detection ($0.68e$). This proof-of-concept experiment provides the motivation for further sensing and imaging of electric fields using NV centers in diamond.

cond-mat.mes-hall

Robust optical readout and characterization of nuclear spin transitions in nitrogen-vacancy ensembles in diamond

Nuclear spin ensembles in diamond are promising candidates for quantum sensing applications, including rotation sensing. Here we perform a characterization of the optically detected nuclear-spin transitions associated with the 14N nuclear spin within diamond nitrogen vacancy (NV) centers. We observe nuclear-spin-dependent fluorescence with the contrast of optically detected 14N nuclear Rabi oscillations comparable to that of the NV electron spin. Using Ramsey spectroscopy, we investigate the temperature and magnetic-field dependence of the nuclear spin transitions in the 77.5-420 K and 350-675 G range, respectively. The nuclear quadrupole coupling constant Q was found to vary with temperature T yielding d|Q|/dT=-35.0(2) Hz/K at T=297 K. The temperature and magnetic field dependencies reported here are important for quantum sensing applications such as rotation sensing and potentially for applications in quantum information processing.

quant-ph

A solid state single photon source with Fourier Transform limited lines at room temperature

Solid state single photon sources with Fourier Transform (FT) limited lines are among the most crucial constituents of photonic quantum technologies and have been accordingly the focus of intensive research over the last several decades. However, so far, solid state systems have only exhibited FT limited lines at cryogenic temperatures due to strong interactions with the thermal bath of lattice phonons. In this work, we report a solid state source that exhibits FT limited lines measured in photo luminescence excitation (sub 100 MHz linewidths) from 3K-300K. The studied source is a color center in the two-dimensional hexagonal boron nitride and we propose that the center's decoupling from phonons is a fundamental consequence of material's low dimensionality. While the center's luminescence lines exhibit spectral diffusion, we identify the likely source of the dffusion and propose to mitigate it via dynamic spectral tuning. The discovery of FT-limited lines at room temperature, which once the spectral diffusion is controlled, will also yield FT-limited emission. Our work motivates a significant advance towards room temperature photonic quantum technologies and a new research direction in the remarkable fundamental properties of two-dimensional materials.

cond-mat.mes-hall

The fine structure of the neutral nitrogen-vacancy center in diamond

The nitrogen-vacancy (NV) center in diamond is a widely-utilized system due to its useful quantum properties. Almost all research focuses on the negative charge state (NV$^-$) and comparatively little is understood about the neutral charge state (NV$^0$). This is surprising as the charge state often fluctuates between NV$^0$, and NV$^-$, during measurements. There are potentially under utilized technical applications that could take advantage of NV$^0$, either by improving the performance of NV$^-$, or utilizing NV$^0$, directly. However, the fine-structure of NV$^0$, has not been observed. Here, we rectify this lack of knowledge by performing magnetic circular dichroism (MCD) measurements that quantitatively determine the fine-structure of NV$^0$. The observed behavior is accurately described by spin-Hamiltonians in the ground and excited states with the ground state yielding a spin-orbit coupling of $λ= 2.24 \pm 0.05$ GHz and a orbital $g-$factor of $0.0186 \pm 0.0005$. The reasons why this fine-structure has not been previously measured are discussed and strain-broadening is concluded to be the likely reason

cond-mat.mes-hall

Temperature dependence of the $^{13}$C hyperfine structure of the negatively-charged nitrogen-vacancy center in diamond

The nitrogen-vacancy (NV) center is a well utilized system for quantum technology, in particular quantum sensing and microscopy. Fully employing the NV center's capabilities for metrology requires a strong understanding of the behavior of the NV center with respect to changing temperature. Here, we probe the NV electronic spin density as the surrounding crystal temperature changes from 10 K to 700 K by examining its $^{13}$C hyperfine interactions. These results are corroborated with \textit{ab initio} calculations and demonstrate that the change in hyperfine interaction is small and dominated by a change in the hybridization of the orbitals constituting the spin density. Thus indicating that the defect and local crystal geometry is returning towards an undistorted structure at higher temperature.

cond-mat.mes-hall

Microscopic imaging of elastic deformation in diamond via in-situ stress tensor sensors

The precise measurement of mechanical stress at the nanoscale is of fundamental and technological importance. In principle, all six independent variables of the stress tensor, which describe the direction and magnitude of compression/tension and shear stress in a solid, can be exploited to tune or enhance the properties of materials and devices. However, existing techniques to probe the local stress are generally incapable of measuring the entire stress tensor. Here, we make use of an ensemble of atomic-sized in-situ strain sensors in diamond (nitrogen-vacancy defects) to achieve spatial mapping of the full stress tensor, with a sub-micrometer spatial resolution and a sensitivity of the order of 1 MPa (corresponding to a strain of less than $10^{-6}$). To illustrate the effectiveness and versatility of the technique, we apply it to a broad range of experimental situations, including mapping the elastic stress induced by localized implantation damage, nano-indents and scratches. In addition, we observe surprisingly large stress contributions from functional electronic devices fabricated on the diamond, and also demonstrate sensitivity to deformations of materials in contact with the diamond. Our technique could enable in-situ measurements of the mechanical response of diamond nanostructures under various stimuli, with potential applications in strain engineering for diamond-based quantum technologies and in nanomechanical sensing for on-chip mass spectroscopy.

cond-mat.mtrl-sci

Spin polarization through Intersystem Crossing in the silicon vacancy of silicon carbide

Silicon carbide (SiC)-based defects are promising for quantum communications, quantum information processing, and for the next generation of quantum sensors, as they feature long coherence times, frequencies near the telecom, and optical and microwave transitions. For such applications, the efficient initialization of the spin state is necessary. We develop a theoretical description of the spin polarization process by using the intersystem crossing of the silicon vacancy defect, which is enabled by a combination of optical driving, spin-orbit coupling, and interaction with vibrational modes. By using distinct optical drives, we analyze two spin polarization channels. Interestingly, we find that different spin projections of the ground state manifold can be polarized. This work helps to understand initialization and readout of the silicon vacancy and explains some existing experiments with the silicon vacancy center in SiC.

quant-ph

Spatial mapping of band bending in semiconductor devices using in-situ quantum sensors

Band bending is a central concept in solid-state physics that arises from local variations in charge distribution especially near semiconductor interfaces and surfaces. Its precision measurement is vital in a variety of contexts from the optimisation of field effect transistors to the engineering of qubit devices with enhanced stability and coherence. Existing methods are surface sensitive and are unable to probe band bending at depth from surface or bulk charges related to crystal defects. Here we propose an in-situ method for probing band bending in a semiconductor device by imaging an array of atomic-sized quantum sensing defects to report on the local electric field. We implement the concept using the nitrogen-vacancy centre in diamond, and map the electric field at different depths under various surface terminations. We then fabricate a two-terminal device based on the conductive two-dimensional hole gas formed at a hydrogen-terminated diamond surface, and observe an unexpected spatial modulation of the electric field attributed to a complex interplay between charge injection and photo-ionisation effects. Our method opens the way to three-dimensional mapping of band bending in diamond and other semiconductors hosting suitable quantum sensors, combined with simultaneous imaging of charge transport in complex operating devices.

cond-mat.mtrl-sci

Electronic structure of the neutral silicon-vacancy center in diamond

The neutrally-charged silicon vacancy in diamond is a promising system for quantum technologies that combines high-efficiency, broadband optical spin polarization with long spin lifetimes (T2 ~ 1 ms at 4 K) and up to 90% of optical emission into its 946 nm zero-phonon line. However, the electronic structure of SiV0 is poorly understood, making further exploitation difficult. Performing photoluminescence spectroscopy of SiV0 under uniaxial stress, we find the previous excited electronic structure of a single 3A1u state is incorrect, and identify instead a coupled 3Eu - 3A2u system, the lower state of which has forbidden optical emission at zero stress and so efficiently decreases the total emission of the defect: we propose a solution employing finite strain to form the basis of a spin-photon interface. Isotopic enrichment definitively assigns the 976 nm transition associated with the defect to a local mode of the silicon atom.

cond-mat.mtrl-sci

The neutral silicon-vacancy center in diamond: spin polarization and lifetimes

We demonstrate optical spin polarization of the neutrally-charged silicon-vacancy defect in diamond ($\mathrm{SiV^{0}}$), an $S=1$ defect which emits with a zero-phonon line at 946 nm. The spin polarization is found to be most efficient under resonant excitation, but non-zero at below-resonant energies. We measure an ensemble spin coherence time $T_2>100~\mathrm{μs}$ at low-temperature, and a spin relaxation limit of $T_1>25~\mathrm{s}$. Optical spin state initialization around 946 nm allows independent initialization of $\mathrm{SiV^{0}}$ and $\mathrm{NV^{-}}$ within the same optically-addressed volume, and $\mathrm{SiV^{0}}$ emits within the telecoms downconversion band to 1550 nm: when combined with its high Debye-Waller factor, our initial results suggest that $\mathrm{SiV^{0}}$ is a promising candidate for a long-range quantum communication technology.

quant-ph

Magnetic field-induced enhancement of the nitrogen-vacancy fluorescence quantum yield

The nitrogen-vacancy (NV) centre in diamond is a unique optical defect that is used in many applications today and methods to enhance its fluorescence brightness are highly sought after. We observed experimentally an enhancement of the NV quantum yield by up to 7% in bulk diamond caused by an external magnetic field relative to the field-free case. This observation is rationalised phenomenologically in terms of a magnetic field dependence of the NV excited state triplet-to-singlet transition rate. The theoretical model is in good qualitative agreement with the experimental results at low excitation intensities. Our results significantly contribute to our fundamental understanding of the photophysical properties of the NV defect in diamond and may enable novel NV centre-based magnetometry techniques.

cond-mat.mes-hall

Strain broadening of the 1042-nm zero-phonon line of the NV- center in diamond: a promising spectroscopic tool for defect tomography

The negatively charged nitrogen-vacancy (NV-) center in diamond is a promising candidate for many quantum applications. Here, we examine the splitting and broadening of the center's infrared (IR) zero-phonon line (ZPL). We develop a model for these effects that accounts for the strain induced by photo-dependent microscopic distributions of defects. We apply this model to interpret observed variations of the IR ZPL shape with temperature and photoexcitation conditions. We identify an anomalous temperature dependent broadening mechanism and that defects other than the substitutional nitrogen center significantly contribute to strain broadening. The former conclusion suggests the presence of a strong Jahn-Teller effect in the center's singlet levels and the latter indicates that major sources of broadening are yet to be identified. These conclusions have important implications for the understanding of the center and the engineering of diamond quantum devices. Finally, we propose that the IR ZPL can be used as a sensitive spectroscopic tool for probing microscopic strain fields and performing defect tomography.

cond-mat.mtrl-sci

State-selective intersystem crossing in nitrogen-vacancy centers

The intersystem crossing (ISC) is an important process in many solid-state atomlike impurities. For example, it allows the electronic spin state of the nitrogen-vacancy (NV) center in diamond to be initialized and read out using optical fields at ambient temperatures. This capability has enabled a wide array of applications in metrology and quantum information science. Here, we develop a microscopic model of the state-selective ISC from the optical excited state manifold of the NV center. By correlating the electron-phonon interactions that mediate the ISC with those that induce population dynamics within the NV center's excited state manifold and those that produce the phonon sidebands of its optical transitions, we quantitatively demonstrate that our model is consistent with recent ISC measurements. Furthermore, our model constrains the unknown energy spacings between the center's spin-singlet and spin-triplet levels. Finally, we discuss prospects to engineer the ISC in order to improve the spin initialization and readout fidelities of NV centers.

quant-ph

Phonon-Induced Population Dynamics and Intersystem Crossing in Nitrogen-Vacancy Centers

We report direct measurement of population dynamics in the excited state manifold of a nitrogen-vacancy (NV) center in diamond. We quantify the phonon-induced mixing rate and demonstrate that it can be completely suppressed at low temperatures. Further, we measure the intersystem crossing (ISC) rate for different excited states and develop a theoretical model that unifies the phonon-induced mixing and ISC mechanisms. We find that our model is in excellent agreement with experiment and that it can be used to predict unknown elements of the NV center's electronic structure. We discuss the model's implications for enhancing the NV center's performance as a room-temperature sensor.

quant-ph

The Infrared Absorption Band and Vibronic Structure of the Nitrogen-Vacancy Center in Diamond

Negatively-charged nitrogen-vacancy (NV$^-$) color centers in diamond have generated much interest for use in quantum technology. Despite the progress made in developing their applications, many questions about the basic properties of NV$^-$ centers remain unresolved. Understanding these properties can validate theoretical models of NV$^-$, improve their use in applications, and support their development into competitive quantum devices. In particular, knowledge of the phonon modes of the $^1A_1$ electronic state is key for understanding the optical pumping process. Using pump-probe spectroscopy, we measured the phonon sideband of the ${^1}E\rightarrow{^1}A_1$ electronic transition in the NV$^-$ center. From this we calculated the ${^1}E\rightarrow{^1}A_1$ one-phonon absorption spectrum and found it to differ from that of the ${^3}E\rightarrow{^3}A_2$ transition, a result which is not anticipated by previous group-theoretical models of the NV$^-$ electronic states. We identified a high-energy 169 meV localized phonon mode of the $^1A_1$ level.

physics.atom-ph

Assignment of the NV0 575 nm zero-phonon line in diamond to a 2E-2A2 transition

The time-averaged emission spectrum of single nitrogen-vacancy defects in diamond gives zero-phonon lines of both the negative charge state at 637 nm (1.945 eV) and the neutral charge state at 575 nm (2.156 eV). This occurs through photo-conversion between the two charge states. Due to strain in the diamond the zero-phonon lines are split and it is found that the splitting and polarization of the two zero-phonon lines are the same. From this observation and consideration of the electronic structure of the nitrogen-vacancy center it is concluded that the excited state of the neutral center has A2 orbital symmetry. The assignment of the 575 nm transition to a 2E - 2A2 transition has not been established previously.

cond-mat.mtrl-sci