arXiv subjects

Viktor Ivády

Publications and source records attributed to Viktor Ivády.

At least 19 recordsLinked to original sources

arXiv2026

Accurate description of the electronic states of the V$_{\text{B}}^-$ center in hBN by wavefunction theory

Ensembles of negatively charged boron vacancy (V$_{\text{B}}^-$) centers in hexagonal boron nitride (hBN) have emerged as a two-dimensional spin qubit system interfaced with optics to advance nanoscale quantum sensing. However, a comprehensive description of its optically detected magnetic resonance (ODMR) signal remains challenging due to the strongly correlated nature of the excited electronic states involved in its optical cycle. In this work, we model the energetics, structural relaxation, and transition rates of the V$_{\text{B}}^-$ center using a high-level wave-function-based electron correlation method (CASSCF-NEVPT2). We provide a thorough analysis of the excited state fine structure and pseudo Jahn-Teller effects, singlet-triplet quasi-degeneracies, photoluminescence parameters, intersystem crossing pathways, and stress-dependence of the fine structure and decay parameters. Our findings not only clarify the fundamental behavior of the V$_{\text{B}}^-$ center in hBN but also establish the theoretical foundation for advancing the V$_{\text{B}}^-$ center's readout for integrated 2D quantum sensors.

cond-mat.mtrl-sci↗

arXiv2026

Natural van der Waals silicates as hosts for telecom quantum emitters: the case of erbium-doped talc

Erbium ion is among the most promising solid-state single photon emitters and spin-photon interfaces for quantum networks, emitting directly in the telecom C-band in many host semiconductors. Recently, the search for scalable, low-noise host materials turned toward atomically thin and van der Waals materials that enable efficient integration with nanophotonic architectures. Here, we identify talc, a naturally occurring layered magnesium silicate, as a promising host for telecom-active erbium centers. Using first-principles density functional theory combined with multireference wavefunction calculations, we investigate the thermodynamic stability, electronic structure, crystal-field splitting, and optical transitions of erbium-related defects in talc. We find that substitutional incorporation of Er at Mg sites is energetically favourable over a wide range of Fermi-levels, leading predominantly to telecom C band emitting Er$^{3+}$ configuration. The characteristic ${^4}I_{13/2} \rightarrow {^4}I_{15/2}$ transition of Er$^{3+}$ is preserved in the talc environment and remains centred near 1.55 $μ$m, while crystal-field interactions produce a Stark manifold suitable for spectrally selective optical addressing. The combination of thermodynamic stability, wide band gap, low background emission, and compatibility with van der Waals heterostructures suggests that erbium-doped talc constitutes a promising platform for integrated photonics in the C-band.

cond-mat.mtrl-sci↗

arXiv2026

Color Centers in Cubic Boron Nitride

Cubic boron nitride (c-BN) is a wide-bandgap semiconductor (WBGS) with potential applications in both power electronics and quantum technologies. Color centers in WBGS can be used as single photon emitters and quantum sensors. Several zero phonon lines have been measured in c-BN experiment but not yet identified. To systematically probe the combinatorially complex chemical space of defects, we generate a large-scale point defect data set for c-BN. We apply density functional theory calculation implemented in a high-throughput workflow Automatic Defect Analysis and Qualification (ADAQ) to broadly screen for point defect complexes containing s- or p-elements. More than 8000 defects have been calculated in different charge and spin states. The calculated properties are stored in defect database and are then filtered to find defects with properties similar to the NV-center in diamond. More accurate calculations using hybrid functionals are then performed on a selected set of promising defects to further assess their suitability for quantum technology. In particular, we reexamined the ONVB defect which likely explains the GC-2 line. The hybrid calculations also suggest other defect candidates with bright emission, such as two carbon defects and the NaB- defect.

cond-mat.mtrl-sci↗

arXiv2026

Proximity-Induced Spin Reorientation in Monolayer CrI$_3$ on Hexagonal WTe$_2$

Magnetic anisotropy controls the orientation and thermal stability of two-dimensional magnetic order. Predicting proximity-induced changes in anisotropy requires linking the electronic structure to microscopic magnetic interactions and finite-temperature behavior. Here we study monolayer CrI$_3$ on hexagonal WTe$_2$ using a first-principles-to-finite-temperature workflow centered on relativistic spin-Hamiltonian mapping. We find that WTe$_2$ reorients the CrI$_3$ magnetization from out-of-plane to in-plane and substantially enhances the magnetic ordering scale within the extracted spin models. Analysis of the extracted spin Hamiltonians shows that the reorientation is driven by a substrate-induced change in the balance between symmetric anisotropic exchange and onsite anisotropy. We establish a transferable workflow for proximity-controlled magnetism in two-dimensional van der Waals heterostructures.

cond-mat.mtrl-sci↗

arXiv2026

Exploiting ionization dynamics in the nitrogen vacancy center for rapid, high-contrast spin and charge state initialization

We propose and experimentally demonstrate a method to strongly increase the sensitivity of spin measurements on nitrogen-vacancy (NV) centers in diamond, which can be readily implemented in existing quantum sensing experiments. While charge state transitions of this defect are generally considered a parasitic effect to be avoided, we show here that these can be used to significantly increase the NV center's spin contrast, a key quantity for high sensitivity magnetometry and high fidelity state readout. The protocol consists of a two-step procedure, in which the charge state of the defect is first purified by a strong laser pulse, followed by weak illumination to obtain high spin polarization. We observe a relative improvement of the readout contrast by 17 %, and infer a reduction of the initialization error of more than 50 %. The contrast enhancement is accompanied by a beneficial increase of the readout signal. For long sequence durations, typically encountered in high-resolution magnetometry, a measurement speedup by a factor of >1.5 is extracted, and we find that the technique is beneficial for sequences of any duration. Additionally, our findings give detailed insight into the charge and spin polarization dynamics of the NV center, and provide actionable insights for direct optical, spin-to-charge, and electrical readout of solid-state spin centres.

quant-ph↗

arXiv2025

Localization and coherent control of 25 nuclear spins in Silicon Carbide

Optically addressable spin defects are excellent candidate platform for quantum sensing and quantum network. Nuclear spins coupled to color centers naturally enable long lived quantum memories and local qubits registers. To fully leverage this potential precise characterization of the surrounding nuclear-spin environment augmented with refined DFT models is required. In this work, we report angstrom-level 3D localization of 25 nuclear spins around a single V2 center in 4H Silicon Carbide. Utilizing specially placed robust nuclear memory as a highly efficient readout ancilla for readout, we apply correlation based spectroscopy and by selecting multi-spin chains up to length four, we access and characterize extended nuclear spin cluster. Using the coupling map we reconstruct their couplings to the central electron spin and neighboring nuclei. This work paves the way towards advanced quantum register applications on Silicon Carbide platform.

quant-ph↗

arXiv2025

Demonstration of the ODMR activity of the telecom range ClV center in SiC: a wavefunction theory analysis

Recently, density functional theory-based high-throughput screening of point defects in 4H-SiC revealed the positively charged chlorine-vacancy (ClV) defect to be a promising quantum bit candidate emitting at telecom wavelengths, with an electronic structure analogous to the well-known NV center in diamond. Furthermore, recent infrared photoluminescence (PL) measurements on chlorine-implanted 4H-SiC have revealed new PL lines associated with the ClV defect. While the defect possesses a high-spin ground state, there is a lack of evidence of optically detected magnetic resonance (ODMR), a key ingredient for optical spin initialization and readout. In this Letter, we employ a multireference wavefunction-based quantum chemistry method, specifically, second-order perturbation theory (NEVPT2) on top of a defect-localized many-body wavefunction (CASSCF), to explore the many-body electronic structure of the ClV center. We estimate photoluminescence, internal conversion, and intersystem crossing rates to investigate the possibility of spin polarization and ODMR activity. Our findings establish the ClV center in 4H-SiC as an optically addressable spin qubit with fiber optics compatibility in the technologically mature 4H-SiC host material, enabling the development of large-scale quantum networks.

cond-mat.mtrl-sci↗

arXiv2025

Nuclear Spin-Mediated Relaxation Mechanisms of the V$_{B}^-$ Center in hBN

The negatively charged boron vacancy $V_B^-$ defect in hexagonal boron nitride (hBN) has recently emerged as a promising spin qubit for sensing due to its high-temperature spin control and versatile integration into van der Waals structures. While extensive experiments have explored their coherence properties, much less is known about the spin relaxation time $T_1$ and its control-parameter dependence. In this work, we develop a parameter-free spin dynamics model based on the cluster-expansion technique to investigate $T_1$ relaxation mechanisms at low temperature. Our results reveal that the $V_B^-$ center constitutes a strongly coupled electron spin-nuclear spin core, which necessitates the inclusion of the coherent dynamics and derived memory effects of the three nearest-neighbor nitrogen nuclear spins. Using this framework, this work closely reproduces the experimentally observed $T_1$ time at $B = 90\,\mathrm{G}$ and further predicts the $T_1$ dependence on external magnetic field in the $0 \le B \le 2000\,\mathrm{G}$ interval, when the spin relaxation is predominantly driven by electron-nuclear and nuclear-nuclear flip-flop processes mediated by hyperfine and dipolar interactions. This study establishes a reliable and scalable approach for describing $T_1$ relaxation in $V_B^-$ centers and offers microscopic insights to support future developments in nuclear-spin-based quantum technologies.

quant-ph↗

arXiv2025

Defects in hexagonal boron nitride for quantum technologies

Atomic defects in solid-state materials are building blocks for future quantum technologies, such as quantum communication networks, computers, and sensors. Until recently, a handful of defects in a small selection of host materials have been possible candidates. Recent developments have revealed that hexagonal boron nitride, a wide-bandgap two-dimensional material, hosts single-photon-emitting atomic defects with access to optically addressable electronic and nuclear spins at room temperature. Now, atomically thin quantum devices that operate at ambient conditions are a possibility. In this perspective, we discuss the recent progress, and challenges, in understanding the fundamental photophysics of defects in hBN, as well as specific opportunities they present for the development of quantum technologies.

cond-mat.mes-hall↗

arXiv2025

Coherent control of nitrogen nuclear spins via the V$_B^-$-center in hexagonal boron nitride

Charged boron vacancies (V$_\text{B}^-$) in hexagonal boron nitride (hBN) have emerged as a promising platform for quantum nanoscale sensing and imaging. While these primarily involve electron spins, nuclear spins provide an additional resource for quantum operations. This work presents a comprehensive experimental and theoretical study of the properties and coherent control of the nearest-neighbor $^{15}$N nuclear spins of V$_\text{B}^-$-ensembles in isotope-enriched h$^{10}$B$^{15}$N. Multi-nuclear spin states are selectively addressed, enabled by state-specific nuclear spin transitions arising from spin-state mixing. We perform Rabi driving between selected state pairs, define elementary quantum gates, and measure longer than 10~$μ$s nuclear Rabi coherence times. We observe a two orders of magnitude nuclear g-factor enhancement that underpins fast nuclear spin gates. Accompanying numerical simulations provide a deep insight into the underlying mechanisms. These results establish the foundations for leveraging nuclear spins in V$_\text{B}^-$ center-based quantum applications, particularly for extending coherence times and enhancing the sensitivity of 2D quantum sensing foils.

cond-mat.mtrl-sci↗

arXiv2025

Native defects and impurities in talcum quasi-2D layers

Layered semiconductors have recently emerged as capable host materials for novel quantum applications ranging from phonics to sensing. Most studies have focused on artificial layered materials, while natural layered materials, such as talc and other silicates, have remained largely unexplored despite their desirable properties, e.g, wide direct bandgap, low concentration of optically active defects, and low abundance of nuclear spins. In this article, we carry out a comprehensive computational study of pristine and defective talc layers and discuss their potential applications. After investigating bulk properties, such as lattice parameters, band structure, and dielectric constant, we study the electronic structure, charge states, spin and optical properties of vacancy defects, metal, metalloid, and non-metallic impurities. Our results establish the basis for identifying color centers, electron paramagnetic resonance centers, potential spin quantum bits, and p and n-type dopants. These findings mature the theory of talc and point toward potential applications in quantum technologies.

cond-mat.mtrl-sci↗

arXiv2025

Understanding Decoherence of the Boron Vacancy Center in Hexagonal Boron Nitride

Hexagonal boron nitride (hBN) has emerged as a significant material for quantum sensing, particularly due to its ability to host spin active defects, such as the negatively charged boron vacancy (V$_\mathrm{B}^-$ center). The optical addressability of the V$_\mathrm{B}^-$ center and hBN's 2D structure enable high spatial resolution and integration into various platforms. However, decoherence due to the strong magnetic noise in hBN imposes fundamental limitations on the sensitivity of V$_\mathrm{B}^-$ center-based applications. Understanding the phenomena behind decoherence and identifying parameter settings that provide the highest performance are essential for advancing V$_\mathrm{B}^-$ sensors. This study employs state-of-the-art computational methods to investigate the decoherence of the V$_\mathrm{B}^-$ center in hexagonal boron nitride across a wide range of magnetic field values from 0 T up to 3 T. The provided in-depth numerical and analytical analysis reveals an intricate interplay of various decoherence mechanisms. This study identifies five distinct magnetic field regions governed by different types of magnetic interactions with and within the abundant nuclear spin bath. In addition to magnetic field, the effects of zero-field splitting, nuclear polarization, and different hyperfine coupling terms are studied, representing an important step forward in utilizing V$_\mathrm{B}^-$ ensembles in sensing. In particular, this study proposes operation in the moderate $180-350$ mT magnetic field range in chemically pure h$^{11}$B$^{15}$N samples, where the coherence time can reach $1-20$ $μ$s, significantly exceeding the $\mathcal{O}( 100~\text{ns})$ low-field $T_2$ values.

quant-ph↗

arXiv2025

A charge transfer mechanism for optically addressable solid-state spin pairs

Optically detected magnetic resonance (ODMR) with no resolvable zero-field splitting has been observed from emitters in hexagonal boron nitride across a broad range of wavelengths, but so far an understanding of their microscopic structure and the physical origin of ODMR has been lacking. Here we perform comprehensive measurements and modelling of the spin-resolved photodynamics of ensembles and single emitters, and uncover a universal model that accounts, and provides an intuitive physical explanation, for all key experimental features. The model, inspired by the radical-pair mechanism from spin chemistry, assumes a pair of nearby point defects -- a primary optically active defect and a secondary defect. Charge transfer between the two defects creates a metastable weakly coupled spin pair with ODMR naturally arising from selection rules. Using first-principle calculations, we show that simple defect pairs made of common carbon defects provide a plausible microscopic explanation. Our optical-spin defect pair (OSDP) model resolves several previously open questions including the asymmetric envelope of the Rabi oscillations, the large variability in ODMR contrast amplitude and sign, and the wide spread in emission wavelength. It may also explain similar phenomena observed in other wide bandgap semiconductors such as GaN. The presented framework will be instrumental in guiding future theoretical and experimental efforts to study and engineer solid-state spin pairs.

cond-mat.mes-hall↗

arXiv2025

Identifying high-energy electronic states of NV$^-$ centers in diamond

The negatively charged nitrogen-vacancy center in diamond is a prototype photoluminescent point defect spin qubit with promising quantum technology applications, enabled by its efficient optical spin polarization and readout. Its low-lying electronic states and optical spin polarization cycle have been well characterized over decades, establishing it as a benchmark system for state-of-the-art computational methods in point defect research. While the optical cycle is well understood, a comprehensive energetic analysis of higher-lying states has received less attention until recently. In this joint experimental theoretical study, we identify and characterize five high-energy states beyond those involved in the optical cycle. Using transient absorption spectroscopy, we determine their transition energies and relative oscillator strengths. Additionally, we perform two independent numerical studies employing two state-of-the-art post-DFT methods to support the experimental findings and assign energy levels. These results enhance our understanding of the NV center's energy spectrum and providing a broader reference for benchmarking high-level first-principles methods.

cond-mat.mtrl-sci↗

arXiv2025

Generation of narrowband quantum emitters in hBN with optically addressable spins

Electron spins coupled with optical transitions in solids stand out as a promising platform for developing spin-based quantum technologies. Recently, hexagonal boron nitride (hBN) - a layered Van der Waals (vdW) crystal, has emerged as a promising host for optically addressable spin systems. However, to date, on-demand generation of isolated single photon emitters with pre-determined spin transitions has remained elusive. Here, we report on a single step, thermal processing of hBN flakes that produces high density, narrowband, quantum emitters with optically active spin transitions. Remarkably, over 25% of the emitters exhibit a clear signature of an optical spin readout at room temperature, surpassing all previously reported results by an order of magnitude. The generated spin defect complexes exhibit both S = 1 and S = 1/2 transitions, which are explained by charge transfer from strongly to weakly coupled spin pairs. Our work advances the understanding of spin complexes in hBN and paves the way for single spin - photon interfaces in layered vdW materials with applications in quantum sensing and information processing.

quant-ph↗

arXiv2025

A Coherence-Protection Scheme for Quantum Sensors Based on Ultra-Shallow Single Nitrogen-Vacancy Centers in Diamond

Recent advances in the engineering of diamond surfaces make it possible to stabilize the charge state of 7-30 nanometers deep nitrogen-vacancy (NV) quantum sensors in diamond and to remove the charge noise at the surface principally. However, it is still a challenge to simultaneously increase the action volume of the quantum sensor by placing NV centers 0.5-2 nanometers deep and to maintain their favorable spin coherence properties which are limited by the magnetic noise from the fluctuating nuclear spins of the surface termination of diamond. Here we show by means of first principles simulations that leveraging the interplay of the surface-induced strain and small constant magnetic fields, the spin coherence times of the ultra-shallow 1-nanometer deep NV center can be significantly enhanced near the spin-phonon limited regime at room temperature in $^{12}$C enriched diamonds. We demonstrate that our protocol is beneficial to $\sim$10-nanometers deep NV centers in natural diamond too where the variable coherence properties of the center to the direction of the small constant magnetic fields establish vector magnetometry at the nanoscale.

quant-ph↗

arXiv2024

Accurate and convergent energetics of color centers by wavefunction theory

Ab initio description of point defects in semiconductors, characterized by in-gap states of significant multideterminant character, presents a longstanding theoretical challenge for density functional theory (DFT) methods. In this study, we devise a wavefunction theory (WFT) based ab initio methodology as a competing alternative approach. Specifically, we apply perturbation theory (NEVPT2 level) on top of a defect-localized many-body wavefunction (CASSCF level), which provides a balanced description of dynamic and static correlation effects, respectively. This quantum chemical methodology, exemplified for the NV$^-$ center in diamond in this study, is not only used for the calculation of energies and properties, but also for geometry optimization, performed for each electronic state individually. By relaxing cluster models of increasing size and investigating convergence behavior, we quantitatively reproduce (i) the full energy spectrum of NV$^-$ including the recently characterized high-energy states, (ii) the effect of Jahn-Teller distortion on measurable properties, (iii) the fine structure of ground and excited states, (iv) the pressure dependence of zero-phonon lines. Our findings showcase that applying conventional wave-function-based quantum chemistry on carefully crafted clusters can be a robust routine tool for discussing defect-state energetics.

cond-mat.mtrl-sci↗

arXiv2024

First-principles computational methods for quantum defects in two-dimensional materials: A perspective

Quantum defects are atomic defects in materials that provide resources to construct quantum information devices such as single-photon emitters (SPEs) and spin qubits. Recently, two-dimensional (2D) materials gained prominence as a host of quantum defects with many attractive features derived from their atomically thin and layered material formfactor. In this perspective, we discuss first-principles computational methods and challenges to predict the spin and electronic properties of quantum defects in 2D materials. We focus on the open quantum system nature of the defects and their interaction with external parameters such as electric field, magnetic field, and lattice strain. We also discuss how such prediction and understanding can be used to guide experimental studies, ranging from defect identification to tuning of their spin and optical properties. This perspective provides significant insights into the interplay between the defect, the host material, and the environment, which will be essential in the pursuit of ideal two-dimensional quantum defect platforms.

physics.comp-ph↗