arXiv subjects

Adam Gali

Publications and source records attributed to Adam Gali.

At least 73 records · Page 4Linked to original sources

arXiv2020

Material Platforms for Defect Qubits and Single Photon Emitters

Quantum technology has grown out of quantum information theory and now provides a valuable tool that researchers from numerous fields can add to their toolbox of research methods. To date, various systems have been exploited to promote the application of quantum information processing. The systems that can be used for quantum technology include superconducting circuits, ultra-cold atoms, trapped ions, semiconductor quantum dots, and solid-state spins and emitters. In this review, we will discuss the state of the art on material platforms for spin-based quantum technology, with a focus on the progress in solid-state spins and emitters in several leading host materials, including diamond, silicon carbide, boron nitride, silicon, two-dimensional semiconductors, and other materials. We will highlight how first-principles calculations can serve as an exceptionally robust tool for finding the novel defect qubits and single photon emitters in solids, through detailed predictions of the electronic, magnetic and optical properties.

cond-mat.mtrl-sci↗

arXiv2020

Stone-Wales defects in hexagonal boron nitride as ultraviolet emitters

Many quantum emitters have been measured close or near the grain boundaries of the two-dimensional hexagonal boron nitride where various Stone-Wales defects appear. We show by means of first principles density functional theory calculations that the pentagon-heptagon Stone-Wales defect is an ultraviolet emitter and its optical properties closely follow the characteristics of a 4.08-eV quantum emitter often observed in polycrystalline hexagonal boron nitride. We also show that the square-octagon Stone-Wales line defects are optically active in the ultraviolet region with varying gaps depending on their density in hexagonal boron nitride. Our results may introduce a paradigm shift in the identification of fluorescent centres in this material.

cond-mat.mtrl-sci↗

arXiv2020

Giant shift upon strain on the fluorescence spectrum of V$_{\rm N}$N$_{\rm B}$ color centers in $h$-BN

We study the effect of strain on the physical properties of the nitrogen antisite-vacancy pair in hexagonal boron nitride ($h$-BN), a color center that may be employed as a quantum bit in a two-dimensional material. With group theory and ab-initio analysis we show that strong electron-phonon coupling plays a key role in the optical activation of this color center. We find a giant shift on the zero-phonon-line (ZPL) emission of the nitrogen antisite-vacancy pair defect upon applying strain that is typical of $h$-BN samples. Our results provide a plausible explanation for the experimental observation of quantum emitters with similar optical properties but widely scattered ZPL wavelengths and the experimentally observed dependence of the ZPL on the strain.

cond-mat.mtrl-sci↗

arXiv2020

Photoluminescence at the ground state level anticrossing of the nitrogen-vacancy center in diamond

The nitrogen-vacancy center (NV center) in diamond at magnetic fields corresponding to the ground state level anticrossing (GSLAC) region gives rise to rich photoluminescence (PL) signals due to the vanishing energy gap between the electron spin states, which enables to have an effect on the NV center's luminescence for a broad variety of environmental couplings. In this article we report on the GSLAC photoluminescence signature of NV ensembles in different spin environments at various external fields. We investigate the effects of transverse electric and magnetic fields, P1 centers, NV centers, and the $^{13}$C nuclear spins, each of which gives rise to a unique PL signature at the GSLAC. The comprehensive analysis of the couplings and related optical signal at the GSLAC provides a solid ground for advancing various microwave-free applications at the GSLAC, including but not limited to magnetometry, spectroscopy, dynamic nuclear polarization (DNP), and nuclear magnetic resonance (NMR) detection. We demonstrate that not only the most abundant $^{14}$NV center but the $^{15}$NV can also be utilized in such applications and that nuclear spins coupled to P1 centers can be polarized directly by the NV center at the GSLAC, through a giant effective nuclear $g$-factor arising from the NV center-P1 center-nuclear spin coupling. We report on new alternative for measuring defect concentration in the vicinity of NV centers and on the optical signatures of interacting, mutually aligned NV centers.

cond-mat.mes-hall↗

arXiv2020

Vibronic states and their effect on the temperature and strain dependence of silicon-vacancy qubits in 4H silicon carbide

Silicon-vacancy qubits in silicon carbide (SiC) are emerging tools in quantum technology applications due to their excellent optical and spin properties. In this paper, we explore the effect of temperature and strain on these properties by focusing on the two silicon-vacancy qubits, V1 and V2, in 4H SiC. We apply density functional theory beyond the Born-Oppenheimer approximation to describe the temperature dependent mixing of electronic excited states assisted by phonons. We obtain polaronic gap around 5 and 22~meV for V1 and V2 centers, respectively, that results in significant difference in the temperature dependent dephasing and zero-field splitting of the excited states, which explains recent experimental findings. We also compute how crystal deformations affect the zero-phonon-line of these emitters. Our predictions are important ingredients in any quantum applications of these qubits sensitive to these effects.

quant-ph↗

arXiv2020

Room-temperature coherent control of implanted defect spins in silicon carbide

Recently, vacancy-related spin defects in silicon carbide (SiC) have been demonstrated to be potentially suitable for versatile quantum interface building and scalable quantum network construction. Significant efforts have been undertaken to identify spin systems in SiC and to extend their quantum capabilities using large-scale growth and advanced nanofabrication methods. Here we demonstrated a type of spin defect in the 4H polytype of SiC generated via hydrogen ion implantation with high-temperature post-annealing, which is different from any known defects. These spin defects can be optically addressed and coherently controlled even at room temperature, and their fluorescence spectrum and optically detected magnetic resonance spectra are different from those of any previously discovered defects. Moreover, the generation of these defects can be well controlled by optimizing the annealing temperature after implantation. These defects demonstrate high thermal stability with coherently controlled electron spins, facilitating their application in quantum sensing and masers under harsh conditions.

physics.app-ph↗

arXiv2020

Spectroscopic Investigations of Negatively Charged Tin-Vacancy Centres in Diamond

The recently discovered negatively charged tin-vacancy centre in diamond is a promising candidate for applications in quantum information processing (QIP). We here present a detailed spectroscopic study encompassing single photon emission and polarisation properties, the temperature dependence of emission spectra as well as a detailed analysis of the phonon sideband and Debye-Waller factor. Using photoluminescence excitation spectroscopy (PLE) we probe an energetically higher lying excited state and prove fully lifetime limited linewidths of single emitters at cryogenic temperatures. For these emitters we also investigate the stability of the charge state under resonant excitation. These results provide a detailed insight into the spectroscopic properties of the $\text{SnV}^-$ centre and lay the foundation for further studies regarding its suitability in QIP.

quant-ph↗

arXiv2020

Spin-controlled generation of indistinguishable and distinguishable photons from silicon vacancy centres in silicon carbide

Quantum systems combining indistinguishable photon generation and spin-based quantum information processing are essential for remote quantum applications and networking. However, identification of suitable systems in scalable platforms remains a challenge. Here, we investigate the silicon vacancy centre in silicon carbide and demonstrate controlled emission of indistinguishable and distinguishable photons via coherent spin manipulation. Using strong off-resonant excitation and collecting photons from the ultra-stable zero-phonon line optical transitions, we show a two-photon interference contrast close to 90% in Hong-Ou-Mandel type experiments. Further, we exploit the system's intimate spin-photon relation to spin-control the colour and indistinguishability of consecutively emitted photons. Our results provide a deep insight into the system's spin-phonon-photon physics and underline the potential of the industrially compatible silicon carbide platform for measurement-based entanglement distribution and photonic cluster state generation. Additional coupling to quantum registers based on recently demonstrated coupled individual nuclear spins would further allow for high-level network-relevant quantum information processing, such as error correction and entanglement purification.

quant-ph↗

arXiv2019

Ab initio theory of negatively charged boron vacancy qubit in hBN

Highly correlated orbitals coupled with phonons in two-dimension are identified for paramagnetic and optically active boron vacancy in hexagonal boron nitride by first principles methods which are responsible for recently observed optically detected magnetic resonance signal. We report ab initio analysis of the correlated electronic structure of this center by density matrix renormalization group and Kohn-Sham density functional theory methods. By establishing the nature of the bright and dark states as well as the position of the energy levels, we provide a complete description of the magneto-optical properties and corresponding radiative and non-radiative routes which are responsible for the optical spin polarization and spin dependent luminescence of the defect. Our findings pave the way toward advancing the identification and characterization of room temperature quantum bits in two-dimensional solids.

cond-mat.mes-hall↗

arXiv2019

\emph{Ab initio} theory of nitrogen-vacancy center in diamond

Nitrogen-vacancy center in diamond is a solid state defect qubit with favorable coherence time up to room temperature which could be harnessed in several quantum enhanced sensor and quantum communication applications, and has a potential in quantum simulation and computing. The quantum control largely depends on the intricate details about the electronic structure and states of the nitrogen-vacancy center, radiative and non-radiative rates between these states and the coupling of these states to external spins, electrical, magnetic and strain fields and temperature. In this review paper it is shown how first principles calculations contributed to understanding the properties of nitrogen-vacancy center, and will be briefly discussed the issues to be solved towards full \emph{ab initio} description of solid state defect qubits.

quant-ph↗

arXiv2019

Electrical charge state manipulation of single silicon vacancies in a silicon carbide quantum optoelectronic device

Colour centres with long-lived spins are established platforms for quantum sensing and quantum information applications. Colour centres exist in different charge states, each of them with distinct optical and spin properties. Application to quantum technology requires the capability to access and stabilize charge states for each specific task. Here, we investigate charge state manipulation of individual silicon vacancies in silicon carbide, a system which has recently shown a unique combination of long spin coherence time and ultrastable spin-selective optical transitions. In particular, we demonstrate charge state switching through the bias applied to the colour centre in an integrated silicon carbide opto-electronic device. We show that the electronic environment defined by the doping profile and the distribution of other defects in the device plays a key role for charge state control. Our experimental results and numerical modeling evidence that control of these complex interactions can, under certain conditions, enhance the photon emission rate. These findings open the way for deterministic control over the charge state of spin-active colour centres for quantum technology and provide novel techniques for monitoring doping profiles and voltage sensing in microscopic devices.

cond-mat.mes-hall↗

arXiv2019

Electrically driven optical interferometry with spins in silicon carbide

Interfacing solid-state defect electron spins to other quantum systems is an ongoing challenge. The ground-state spin's weak coupling to its environment bestows excellent coherence properties, but also limits desired drive fields. The excited-state orbitals of these electrons, however, can exhibit stronger coupling to phononic and electric fields. Here, we demonstrate electrically driven coherent quantum interference in the optical transition of single, basally oriented divacancies in commercially available 4H silicon carbide. By applying microwave frequency electric fields, we coherently drive the divacancy's excited-state orbitals and induce Landau-Zener-Stuckelberg interference fringes in the resonant optical absorption spectrum. Additionally, we find remarkably coherent optical and spin subsystems enabled by the basal divacancy's symmetry. These properties establish divacancies as strong candidates for quantum communication and hybrid system applications, where simultaneous control over optical and spin degrees of freedom is paramount.

quant-ph↗

arXiv2019

Oxygenated (113) diamond surface for nitrogen-vacancy quantum sensors with preferential alignment and long coherence time from first principles

Shallow nitrogen-vacancy (NV) center in diamond is promising in quantum sensing applications however its sensitivity has been limited by surface terminators and defects. There is an immediate quest to find suitable diamond surfaces for NV sensors. In this work, the surface terminators of (113) diamond to host shallow NV centers are studied by means of first principles calculations. Results indicate that complete oxygen termination of (113) diamond creates positive electron affinity with neither strain on the surface nor in-gap levels. This is a very surprising result as the commonly employed oxygenated (001) diamond surface is often defective due to the disorder created by the strain of ether groups at the surface that seriously undermine the coherence properties of the shallow NV centers. The special atomic configurations on (113) diamond surface are favorable for oxygen bonding, in contrast to (001) and (111) diamond surfaces. These simulations imply that oxygenated diamond (113) surface can be produced by conventional diamond chemical vapor deposition growth. Combining this with the ~73% preferential alignment of as-grown NV centers in (113) oriented diamond, oxygenated (113) diamond is presently supposed to be the most prospective host for NV quantum sensors.

cond-mat.mes-hall↗

arXiv2019

The $(e_g \otimes e_u) \otimes E_g$ product Jahn-Teller effect in the neutral group-IV--vacancy quantum bits in diamond

The product Jahn-Teller (pJT) effect may occur for such coupled electron-phonon systems in solids where single electrons occupy double degenerate orbitals. We propose that the excited state of the neutral $X$V split-vacancy complex in diamond, where $X$ and V labels a group-IV impurity atom of $X$=Si, Ge, Sn, Pb and the vacancy, respectively, is such a system with $e_g$ and $e_u$ double degenerate orbitals and $E_g$ quasi-localized phonons. We develop and apply \emph{ab initio} theory to quantify the strength of electron-phonon coupling for neutral $X$V complexes in diamond, and find a significant impact on the corresponding optical properties of these centers. Our results show good agreement with recent experimental data on the prospective SiV($0$) quantum bit, and reveals the complex nature of the excited states of neutral $X$V color centers in diamond.

quant-ph↗

arXiv2019

Spectrally stable defect qubits with no inversion symmetry for robust spin-to-photon interface

Scalable spin-to-photon interfaces require quantum emitters with strong optical transition dipole moment and low coupling to phonons and stray electric fields. It is known that particularly for coupling to stray electric fields, these conditions can be simultaneously satisfied for emitters that show inversion symmetry. Here, we show that inversion symmetry is not a prerequisite criterion for a spectrally stable quantum emitter. We find that identical electron density in ground and excited states can eliminate the coupling to the stray electric fields. Further, a strong optical transition dipole moment is achieved in systems with altering sign of the ground and excited wavefunctions. We use density functional perturbation theory to investigate an optical center that lacks of inversion symmetry. Our results show that this system close to ideally satisfies the criteria for an ideal quantum emitter. Our study opens a novel rationale in seeking promising materials and point defects towards the realisation of robust spin-to-photon interfaces.

quant-ph↗

arXiv2018

Excitation properties of the divacancy in 4H-SiC

We investigate the quenching of the photoluminescence (PL) from the divacancy defect in 4H-SiC consisting of a nearest-neighbour silicon and carbon vacancies. The quenching occurs only when the PL is excited below certain photon energies (thresholds), which differ for the four different inequivalent divacancy configurations in 4H-SiC. Refined theoretical ab initio calculation for the charge-transfer levels of the divacancy show very good agreement between the position of the (0/-) level with respect to the conduction band for each divacancy configurations and the corresponding experimentally observed threshold, allowing us to associate the PL decay with conversion of the divacancy from neutral to negative charge state due to capture of electrons photoionized from other defects (traps) by the excitation. Electron paramagnetic resonance measurements are conducted in dark and under excitation similar to that used in the PL experiments and shed light on the possible origin of traps in the different samples. A simple model built on this concept agrees well with the experimentally-observed decay curves.

cond-mat.mtrl-sci↗

arXiv2018

Strongly inhomogeneous distribution of spectral properties of silicon-vacancy color centers in nanodiamonds

The silicon-vacancy (SiV) color center in diamond is a solid-state single photon emitter and spin quantum bit suited as a component in quantum devices. Here, we show that the SiV center in nanodiamond exhibits a strongly inhomogeneous distribution with regard to the center wavelengths and linewidths of the zero-phonon-line (ZPL) emission at room temperature. We find that the SiV centers separate in two clusters: one group exhibits ZPLs with center wavelengths within a narrow range of approximatly 730 nm to 742 nm and broad linewidths between 5 nm and 17 nm, whereas the second group comprises a very broad distribution of center wavelengths between 715 nm and 835 nm, but narrow linewidths from below 1 nm up to 4 nm. Supported by ab initio Kohn-Sham density functional theory calculations we show that the ZPL shifts of the first group are consistently explained by strain in the diamond lattice. Further, we suggest, that the second group showing the strongly inhomogeneous distribution of center wavelengths might be comprised of modified SiV centers. Whereas single photon emission is demonstrated for SiV centers of both clusters, we show that emitters from different clusters show different spectroscopic features such as variations of the phonon sideband spectra and different blinking dynamics.

quant-ph↗

arXiv2018

Evidence for Primal sp2 Defects at the Diamond Surface: Candidates for Electron Trapping and Noise Sources

Diamond materials are central to an increasing range of advanced technological demonstrations, from high power electronics, to nano-scale quantum bio-imaging with unprecedented sensitivity. However, the full exploitation of diamond for these applications is often limited by the uncontrolled nature of the diamond material surface, which suffers from Fermi-level pinning and hosts a significant density of electro-magnetic noise sources. These issues occur despite the oxide-free and air-stable nature of the diamond crystal surface, which should be an ideal candidate for functionalization and chemical-engineering. In this work we reveal a family of previously unidentified and near-ubiquitous primal surface defects which we assign to differently reconstructed surface vacancies. The density of these defects is quantified with X-ray absorption spectroscopy, their energy structures are elucidated by ab initio calculations, and their effect on near-surface quantum probes is measured directly. Subsequent ab-initio calculation of band-bending from these defects suggest they are the source of Fermi-level pinning at most diamond surfaces. Finally, an investigation is conducted on a broad range of post-growth surface treatments and concludes that none of them can reproducibly reduce this defect density below the Fermi-pinning threshold, making this defect a prime candidate as the source for decoherence-limiting noise in near-surface quantum probes.

cond-mat.mes-hall↗