arXiv subjects

Adam Gali

Publications and source records attributed to Adam Gali.

At least 55 records · Page 3Linked to original sources

arXiv2023

\emph{Ab initio} study of (100) diamond surface spins

Unpaired electronic spins at diamond surfaces are ubiquitous and can lead to excess magnetic noise. They have been observed in several studies to date, but their exact chemical nature is still unknown. We propose a simple model to explain the existence and chemical stability of surface spins associated with the $sp^3$ dangling bond on the (100) diamond surface using density functional theory. We find that the (111) facet, which is naturally generated at a step edge of (100) crystalline diamond surface, can sterically protect a spinful defect. Our study reveals a mechanism for annihilation of these surface spins upon annealing, consistent with recent experimental results. We also demonstrate that the Fermi-contact term in the hyperfine coupling is not negligible between the surface spins and the surrounding nuclear spins, and thus \textit{ab initio} simulation can be used to devise a sensing protocol where the surface spins act as reporter spins to sense nuclear spins on the surface.

quant-ph↗

arXiv2023

The positively charged carbon vacancy defect as a near-infrared emitter in 4H-SiC

Certain intrinsic point defects in silicon carbide are promising quantum systems with efficient spin-photon interface. Despite carbon vacancy in silicon carbide is an elementary and relatively abundant intrinsic defect, no optical signal has been reported associated with it. Here, we revisit the positively charged carbon vacancy defects in the 4H polytype of silicon carbide (4H-SiC) by means of \textit{ab initio} calculations. We find that the excited state is optically active for the so-called h-site configuration of carbon vacancy in 4H-SiC, with zero-phonon line at $0.65~\mathrm{eV}$. We propose this defect as an exotic paramagnetic near-infrared emitter in the IR-B region.

quant-ph↗

arXiv2023

The Role of Electrolytes in the Relaxation of Near-Surface Spin Defects in Diamond

Quantum sensing with spin defects in diamond, such as the nitrogen-vacancy (NV) center, enables the detection of various chemical species on the nanoscale. Molecules or ions with unpaired electronic spins are typically probed by their influence on the NV center's spin relaxation. Whereas it is well-known that paramagnetic ions reduce the NV center's relaxation time ($T_1$), here we report on the opposite effect for diamagnetic ions. We demonstrate that millimolar concentrations of aqueous diamagnetic electrolyte solutions increase the $T_1$ time of near-surface NV center ensembles compared to pure water. To elucidate the underlying mechanism of this surprising effect, single and double quantum NV experiments are performed, which indicate a reduction of magnetic and electric noise in the presence of diamagnetic electrolytes. In combination with ab initio simulations, we propose that a change in the interfacial band bending due to the formation of an electric double layer leads to a stabilization of fluctuating charges at the interface of an oxidized diamond. This work not only helps to understand noise sources in quantum systems but could also broaden the application space of quantum sensors towards electrolyte sensing in cell biology, neuroscience and electrochemistry.

physics.app-ph↗

arXiv2023

Coherent control of an ultrabright single spin in hexagonal boron nitride at room temperature

Hexagonal boron nitride (hBN) is a remarkable two-dimensional (2D) material that hosts solid-state spins and has great potential to be used in quantum information applications, including quantum networks. However, in this application, both the optical and spin properties are crucial for single spins but have not yet been discovered simultaneously for hBN spins. Here, we realize an efficient method for arraying and isolating the single defects of hBN and use this method to discover a new spin defect with a high probability of 85%. This single defect exhibits outstanding optical properties and an optically controllable spin, as indicated by the observed significant Rabi oscillation and Hahn echo experiments at room temperature. First principles calculations indicate that complexes of carbon and oxygen dopants may be the origin of the single spin defects. This provides a possibility for further addressing spins that can be optically controlled.

physics.optics↗

arXiv2022

Optical properties of SiV and GeV color centers in nanodiamonds under hydrostatic pressures up to 180 GPa

We investigate the optical properties of silicon-vacancy (SiV) and germanium-vacancy (GeV) color centers in nanodiamonds under hydrostatic pressure up to 180 GPa. The nanodiamonds were synthetized by Si or Ge-doped plasma assisted chemical vapor deposition and, for our experiment, pressurized in a diamond anvil cell. Under hydrostatic pressure we observe blue-shifts of the SiV and GeV zero-phonon lines by 17 THz (70 meV) and 78 THz (320 meV), respectively. These measured pressure induced shifts are in good agreement with ab initio calculations that take into account the lattice compression based on the equation of state of diamond and that are extended to the case of the tin-vacancy (SnV) center. This work provides guidance on the use of group-IV-vacancy centers as quantum sensors under extreme pressures that will exploit their specific optical and spin properties induced by their intrinsic inversion-symmetric structure.

quant-ph↗

arXiv2022

Bistable carbon-vacancy defects in $h$-BN

Single photon emitters in hexagonal boron nitride have been extensively studied recently. Although unambiguous identification of the emitters is still under intense research, carbon related defects are believed to play a vital role for the emitter producing zero-phonon-lines in the range of $1.6$ to $2.2$~eV. In this study, we systematically investigate two configurations of carbon-vacancy defects, VNCB and CNVB, by means of density functional theory calculations. We calculated the reaction barrier energies from one defect to the other to determine relative stability. We find the barrier energies are charge dependent and CNVB could easily transform to VNCB in neutral and positive charge states while it is stable when negatively charged. Formation energy calculations show that the VNCB is the dominant defect over CNVB. However, neither VNCB nor CNVB has suitable fluorescence spectra that could reproduce the observed ones. Our results indicate that the origin of the $1.6$-to-$2.2$-eV emitters should be other carbon-related configurations.

cond-mat.mtrl-sci↗

arXiv2022

Detection of single W-centers in silicon

Controlling the quantum properties of individual fluorescent defects in silicon is a key challenge towards advanced quantum photonic devices prone to scalability. Research efforts have so far focused on extrinsic defects based on impurities incorporated inside the silicon lattice. Here we demonstrate the detection of single intrinsic defects in silicon, which are linked to a tri-interstitial complex called W-center, with a zero-phonon line at 1.218$μ$m. Investigating their single-photon emission properties reveals new information about this common radiation damage center, such as its dipolar orientation and its photophysics. We also identify its microscopic structure and show that although this defect does not feature electronic states in the bandgap, Coulomb interactions lead to excitonic radiative recombination below the silicon bandgap. These results could set the stage for numerous quantum perspectives based on intrinsic luminescent defects in silicon, such as quantum integrated photonics, quantum communications and quantum sensing.

quant-ph↗

arXiv2021

Quantum sensor in a single layer van der Waals material

Point defect qubits in semiconductors have demonstrated their outstanding high spatial resolution sensing capabilities of broad multidisciplinary interest. Two-dimensional (2D) semiconductors hosting such sensors have recently opened up new horizons for sensing in the subnanometer scales in 2D heterostructures. However, controlled creation of quantum sensor in a single layer 2D materials with high sensitivity has been elusive so far. Here, we report on a novel 2D quantum sensor, the VB2 centre in hexagonal boron nitride (hBN), with superior sensing capabilities. The centre's inherently low symmetry configuration gives rise to unique electronic and spin properties that implement a qubit in a 2D material with unprecedented sensitivity. The qubit is decoupled from its dense spin environment at low magnetic fields that gives rise to the reduction of the spin resonance linewidth and elongation of the coherence time. The VB2 centre is also equipped with a classical memory that can be utilized in storing population information. Using scanning transmission electron microscopy imaging, we confirm the presence of the point defect structure in free standing monolayer hBN created by electron beam irradiation. Our results provide a new material solution towards atomic-scale sensing in low dimensions.

cond-mat.mes-hall↗

arXiv2021

Ultraviolet quantum emitters in $h$-BN from carbon clusters

Ultraviolet (UV) quantum emitters in hexagonal boron nitride (hBN) have generated considerable interest due to their outstanding optical response. Recent experiments have identified a carbon impurity as a possible source of UV single photon emission. Here, based on the first principles calculations, we systematically evaluate the ability of substitutional carbon defects to develop the UV colour centres in hBN. Of seventeen defect configurations under consideration, we particularly emphasize the carbon ring defect (6C), for which the calculated zero-phonon line (ZPL) agrees well the experimental 4.1-eV emission signal. We also compare the optical properties of 6C with those of other relevant defects, thereby outlining the key differences in the emission mechanism. Our findings provide new insights about the large response from this colour centre to external perturbations and pave the way to a robust identification of the particular carbon substitutional defects by spectroscopic methods.

quant-ph↗

arXiv2021

Identification of a telecom wavelength single photon emitter in silicon

We identify the exact microscopic structure of the G photoluminescence center in silicon by first principles calculations with including a self-consistent many-body perturbation method, which is a telecommunication wavelength single photon source. The defect constitutes of $\text{C}_\text{s}\text{C}_\text{i}$ carbon impurities in its $\text{C}_\text{s}-\text{Si}_\text{i}-\text{C}_\text{s}$ configuration in the neutral charge state, where $s$ and $i$ stand for the respective substitutional and interstitial positions in the Si lattice. We reveal that the observed fine structure of its optical signals originates from the athermal rotational reorientation of the defect. We attribute the monoclinic symmetry reported in optically detected magnetic resonance measurements to the reduced tunneling rate at very low temperatures. We discuss the thermally activated motional averaging of the defect properties and the nature of the qubit state.

quant-ph↗

arXiv2021

Vibrational modes of negatively charged silicon-vacancy centers in diamond from ab initio calculations

Silicon-vacancy (SiV) center in diamond is a photoluminescence (PL) center with a characteristic zero-phonon line energy at 1.681 eV that acts as a solid-state single photon source and, potentially, as a quantum bit. The majority of the luminescence intensity appears in the zero-phonon line; nevertheless, about 30\% of the intensity manifests in the phonon sideband. Since phonons play an essential role in the operation of this system, it is of importance to understand the vibrational properties of the SiV center in detail. To this end, we carry out density functional theory calculations of dilute SiV centers by embedding the defect in supercells of a size of a few thousand atoms. We find that there exist two well-pronounced quasi-local vibrational modes (resonances) with $A_{2u}$ and $E_u$ symmetries, corresponding to the vibration of the Si atom along and perpendicular to the defect symmetry axis, respectively. Isotopic shifts of these modes explain the isotopic shifts of prominent vibronic features in the experimental SiV PL spectrum. Moreover, calculations show that the vibrational frequency of the $A_{2u}$ mode increases by about 30\% in the excited state with respect to the ground state, while the frequency of the $E_u$ mode increases by about 5\%. These changes explain experimentally observed isotopic shifts of the zero-phonon line energy. We also emphasize possible dangers of extracting isotopic shifts of vibrational resonances from finite-size supercell calculations, and instead propose a method to do this correctly.

quant-ph↗

arXiv2021

Towards $\textit{ab initio}$ identification of paramagnetic substitutional carbon defects in hexagonal boron nitride acting as quantum bits

Paramagnetic substitutional carbon (C$_\text{B}$, C$_\text{N}$) defects in hexagonal boron nitride (hBN) are discussed as candidates for quantum bits. Their identification and suitability are approached by means of photoluminescence (PL), charge transitions, electron paramagnetic resonance, and optically detected magnetic resonance (ODMR) spectra. Several clear trends in these are revealed by means of an efficient plane wave periodic supercell \textit{ab initio} density functional theory approach. In particular, this yields insight into the role of the separation between C$_\text{B}$ and C$_\text{N}$. In most of the cases the charge transition between the neutral and a singly charged ground state of a defect is predicted to be experimentally accessible, since the charge transition level (CTL) position lies within the band gap. \textit{A posteriori} charge corrections are also discussed. A near-identification of an experimentally isolated single spin center as the neutral C$_\text{B}$ point defect was found via comparison of results to recently observed PL and ODMR spectra.

quant-ph↗

arXiv2021

Room temperature coherent manipulation of single-spin qubits in silicon carbide with a high readout contrast

Spin defects in silicon carbide (SiC) with mature wafer-scale fabrication and micro/nano-processing technologies have recently drawn considerable attention. Although room temperature single-spin manipulation of colour centres in SiC has been demonstrated, the typically detected contrast is less than 2%, and the photon count rate is also low. Here, we present the coherent manipulation of single divacancy spins in 4H-SiC with a high readout contrast (-30%) and a high photon count rate (150 kilo counts per second) under ambient conditions, which are competitive with the nitrogen-vacancy (NV) centres in diamond. Coupling between a single defect spin and a nearby nuclear spin is also observed. We further provide a theoretical explanation for the high readout contrast by analysing the defect levels and decay paths. Since the high readout contrast is of utmost importance in many applications of quantum technologies, this work might open a new territory for SiC-based quantum devices with many advanced properties of the host material.

cond-mat.mes-hall↗

arXiv2021

Probing spin dynamics on diamond surfaces using a single quantum sensor

Understanding the dynamics of a quantum bit's environment is essential for the realization of practical systems for quantum information processing and metrology. We use single nitrogen-vacancy (NV) centers in diamond to study the dynamics of a disordered spin ensemble at the diamond surface. Specifically, we tune the density of "dark" surface spins to interrogate their contribution to the decoherence of shallow NV center spin qubits. When the average surface spin spacing exceeds the NV center depth, we find that the surface spin contribution to the NV center free induction decay can be described by a stretched exponential with variable power n. We show that these observations are consistent with a model in which the spatial positions of the surface spins are fixed for each measurement, but some of them reconfigure between measurements. In particular, we observe a depth-dependent critical time associated with a dynamical transition from Gaussian (n=2) decay to n=2/3, and show that this transition arises from the competition between the small decay contributions of many distant spins and strong coupling to a few proximal spins at the surface. These observations demonstrate the potential of a local sensor for understanding complex systems and elucidate pathways for improving and controlling spin qubits at the surface.

quant-ph↗

arXiv2021

Room-temperature control and electrical readout of individual nitrogen-vacancy nuclear spins

Nuclear spins in semiconductors are leading candidates for quantum technologies, including quantum computation, communication, and sensing. Nuclear spins in diamond are particularly attractive due to their extremely long coherence lifetime. With the nitrogen-vacancy (NV) centre, such nuclear qubits benefit from an auxiliary electronic qubit, which has enabled entanglement mediated by photonic links. The transport of quantum information by the electron itself, via controlled transfer to an adjacent centre or via the dipolar interaction, would enable even faster and smaller processors, but optical readout of arrays of such nodes presents daunting challenges due to the required sub-diffraction inter-site distances. Here, we demonstrate the electrical readout of a basic unit of such systems - a single 14N nuclear spin coupled to the NV electron. Our results provide the key ingredients for quantum gate operations and electrical readout of nuclear qubit registers, in a manner compatible with nanoscale electrode structures. This demonstration is therefore a milestone towards large-scale diamond quantum devices with semiconductor scalability.

cond-mat.mes-hall↗

arXiv2020

Optically detected magnetic resonance in neutral silicon vacancy centers in diamond via bound exciton states

Neutral silicon vacancy (SiV0) centers in diamond are promising candidates for quantum networks because of their excellent optical properties and long spin coherence times. However, spin-dependent fluorescence in such defects has been elusive due to poor understanding of the excited state fine structure and limited off-resonant spin polarization. Here we report the realization of optically detected magnetic resonance and coherent control of SiV0 centers at cryogenic temperatures, enabled by efficient optical spin polarization via previously unreported higher-lying excited states. We assign these states as bound exciton states using group theory and density functional theory. These bound exciton states enable new control schemes for SiV0 as well as other emerging defect systems.

cond-mat.mes-hall↗

arXiv2020

{\textit{Ab initio} determination of pseudospin for paramagnetic defects in SiC

Paramagnetic point defects in solids may exhibit a rich set of interesting and not yet fully resolved physics. In particular, character of wavefunctions and electron-phonon coupling in these defects may highly influence their interaction with external magnetic fields. Complex interplay between the electronic orbitals, phonons and electron spin determines the effective pseudospin of the system that we demonstrate on vanadium and molybdenum defects in hexagonal silicon carbide (SiC) by means of \textit{ab initio} calculations. In this Rapid Communication, we find a giant anisotropy in the $g$-tensor of these defects with Kramers doublet spin ground state, resulting in reduced and vanishing interaction with the magnetic field in parallel and transverse directions, respectively. The consequences of our finding in the application of these defects for quantum information processing are briefly discussed.

quant-ph↗

arXiv2020

Qubit guidelines for solid-state spin defects

Defects with associated electron and nuclear spins in solid-state materials have a long history relevant to quantum information science going back to the first spin echo experiments with silicon dopants in the 1950s. Since the turn of the century, the field has rapidly spread to a vast array of defects and host crystals applicable to quantum communication, sensing, and computing. From simple spin resonance to long-distance remote entanglement, the complexity of working with spin defects is fast advancing, and requires an in-depth understanding of their spin, optical, charge, and material properties in this modern context. This is especially critical for discovering new relevant systems dedicated to specific quantum applications. In this review, we therefore expand upon all the key components with an emphasis on the properties of defects and the host material, on engineering opportunities and other pathways for improvement. Finally, this review aims to be as defect and material agnostic as possible, with some emphasis on optical emitters, providing a broad guideline for the field of solid-state spin defects for quantum information.

quant-ph↗