arXiv subjects

Ádám Gali

Publications and source records attributed to Ádám Gali.

17 recordsLinked to original sources

arXiv2026

Machine-learning-driven kinetic discovery of carbon interstitial color centers in diamond

Diamond hosts optically active point defects central to quantum technologies, yet the carbon self-interstitials introduced during growth and irradiation compete with them and form new defects whose configurational landscape is poorly charted, as subtle energy differences govern the competing minima and pathways. Here we build an interstitial-focused dataset by active learning and benchmark three machine-learning interatomic potentials -- GAP, NEP and the equivariant MACE -- against density functional theory for energies, forces and migration barriers. MACE reproduces the reference energetics and relative stabilities, whereas the others can misorder the ground states. Annealing molecular dynamics with the validated potentials uncovers a series of previously unreported carbon interstitial clusters, from di- to octa-interstitials -- several introducing in-gap states of interest as colour centres -- and shows that their metastability is governed by kinetically accessible pathways rather than energetic ordering. These results chart the interstitial defect landscape and accelerate defect discovery for quantum technologies.

physics.comp-ph↗

arXiv2026

Increased cyclicity of atomic transitions via coherent interference of decay paths

Optical readout is a fundamental tool in atomic state measurement, yet the fidelity of optical readout is frequently limited by imperfect photon collection. This can be mitigated when readout occurs on a cycling transition which continuously fluoresces under resonant excitation, thus increasing signal and enabling single-shot readout. We present a method to extend the cyclicity of atomic transitions via coherent destructive interference between spurious decay paths. We describe the characteristics of atomic systems in which this method can be implemented and model several examples in which the number of emitted photons is increased by multiple orders of magnitude.

quant-ph↗

arXiv2026

From Mono- to Hexa-Interstitials: Computational Insights into Carbon Defects in Diamond

We present a comprehensive first-principles investigation of carbon self-interstitial defects in diamond, ranging from mono- to hexa-interstitial complexes. By quantum mechanical density functional theory, empowered by interatomic potential models, we efficiently sample the complex configurational landscape and identify both known and previously unreported defect geometries. Our results reveal a pronounced energetic driving force for aggregation: the formation energy per interstitial decreases systematically from isolated split interstitials to compact multi-interstitial clusters, with the tetra-interstitial platelet emerging as a particularly stable structural motif. Additionally, charge analysis indicates that the predominantly covalent bonding in diamond becomes more polar within the defect centers. Analysis of defect energy levels shows that only the investigated mono-, di-, penta-, and hexa-interstitial complexes introduce in-gap electronic states, whereas the tri- and tetra-interstitial clusters are electronically inert. Vibrational spectroscopies further reveal that self-interstitials generate characteristic signatures. Short carbon-carbon bonds inside the defect cores give rise to high-frequency vibrational modes between 1375 and 1925 cm$^{-1}$, which are strongly IR-active but exhibit weak Raman activity. Through a systematic analysis of metastable configurations, we identify the 3H defect center as a neutral di-interstitial defect. Based on this identification, we further suggest that the TR12 center may arise from a 3H-containing defect like a metastable hexa-interstitial configuration. Taken together, these findings provide a coherent picture of the structural, electronic, and vibrational characteristics of carbon self-interstitials and establish a robust framework for their experimental identification.

cond-mat.mtrl-sci↗

arXiv2026

Optically Addressable Molecular Spins at 2D Surfaces

Optically addressable spins at material surfaces have represented a long-standing ambition in quantum sensing, providing atomic resolution and quantum-limited sensitivity. However, they are constrained by a finite depth at which the quantum spins can be stabilized. Here, we demonstrate a hybrid molecular-2D architecture that realizes quantum spin sensors directly on top of the surface. By anchoring spin-active molecules onto hexagonal boron nitride (hBN), we eliminate the depth of the quantum sensor while also exhibiting robust spin properties from 4~K to room temperature (RT). The Hahn-echo spin coherence time exceeds $T_2 = 3.4~\upmu\text{s}$ at 4~K, outperforming values in bulk organic crystals and overturning the prevailing expectation that spin inevitably deteriorates upon approaching the surface. By chemically tuning the molecule through deuteration, $T_2$ improves by more than 10-fold, and under dynamic decoupling, coherence is prolonged to the intrinsic lifetime limit, exceeding 300~$\upmu\text{s}$. Proximal proton spins and the magnetic response of two-dimensional magnets beneath the hBN layer have been detected at RT. These molecular spins form surface quantum sensors with long coherence, optical addressability, and interfacial versatility, enabling a scalable, adaptable architecture beyond what conventional solid-state platforms offer.

quant-ph↗

arXiv2025

Sulfur in diamond and its effect on the creation of nitrogen-vacancy defect from \textit{ab initio} simulations

The negatively charged nitrogen-vacancy (NV) center is one of the most significant and widely studied defects in diamond that plays a prominent role in quantum technologies. The precise engineering of the location and concentration of NV centers is of great importance in quantum technology applications. To this end, irradiation techniques such as nitrogen-molecule ion implantation are applied. Recent studies have reported enhanced NV center creation and activation efficiencies introduced by nitrogen molecule ion implantation in doped diamond layers, where the maximum creation efficiency at $\sim75$\% has been achieved in sulfur-doped layers. However, the microscopic mechanisms behind these observations and the limits of the efficiencies are far from understood. In this study, we employ hybrid density functional theory calculations to compute the formation energies, charge transition levels, and the magneto-optical properties of various sulfur defects in diamond where we also consider the interaction of sulfur and hydrogen in chemical vapor-deposited diamond layers. Our results imply that the competition between the donor substitutional sulfur and the hyper-deep acceptor sulfur-vacancy complex is an important limiting factor on the creation efficiency of the NV center in diamond. However, both species are able to trap interstitial hydrogen from diamond, which favorably mediates the creation of NV centers in chemical vapor-deposited diamond layers.

cond-mat.mtrl-sci↗

arXiv2025

Theory of optical spin polarization of axial divacancy and nitrogen-vacancy defects in 4H-SiC

The neutral divacancy and the negatively charged nitrogen-vacancy defects in 4H-silicon carbide (SiC) are two of the most prominent candidates for functioning as room-temperature quantum bits (qubits) with telecommunication-wavelength emission. Nonetheless, the pivotal role of electron-phonon coupling in the spin polarization loop is still unrevealed. In this work, we theoretically investigate the microscopic magneto-optical properties and spin-dependent optical loops utilizing the first-principles calculations. First, we quantitatively demonstrate the electronic level structure, assisted by symmetry analysis. Moreover, the fine interactions, including spin-orbit coupling and spin-spin interaction, are fully characterized to provide versatile qubit functional parameters. Subsequently, we explore the electron-phonon coupling, encompassing dynamics- and pseudo-Jahn--Teller effects in the intersystem crossing transition. In addition, we analyze the photoluminescence PL lifetime based on the major transition rates in the optical spin polarization loop. We compare two promising qubits with similar electronic properties, but their respective rates differ substantially. Finally, we detail the threshold of ODMR contrast for further optimization of the qubit operation. This work not only reveals the mechanism underlying the optical spin polarization but also proposes productive avenues for optimizing quantum information processing tasks based on the ODMR protocol.

quant-ph↗

arXiv2024

Telecom light-emitting diodes based on nanoconfined self-assembled silicon-based color centers

Silicon color centers (SiCCs) have recently emerged as potential building blocks for light emitters in Si photonics, quantum emitters with spin storage capabilities, and Si-based quantum repeaters. We have recently developed a non-invasive method to engineer carbon-related SiCCs confined to ultra-thin nanolayers within a pristine crystalline environment, which is of utmost importance for the photostability of SiCCs. Here, we demonstrate embedding these C-doping-based SiCCs into the only 9 nm wide intrinsic region of a p-i-n diode using the epitaxial self-assembly of color centers. We report electrically-pumped light emission with an exponential increase in the intensity as a function of the driving current until saturation. We associate this property with the shift of quasi-Fermi-level position upon electrical driving, which simultaneously improves the spectral homogeneity of the engineered SiCCs. Our study demonstrates the electrical control and driving of near-infrared emitters in high-quality silicon diodes, an essential milestone for advancing classical and quantum optoelectronics.

cond-mat.mes-hall↗

arXiv2024

Terahertz Emission From Diamond Nitrogen-Vacancy Centers

Coherent light sources emitting in the terahertz range are highly sought after for fundamental research and applications. THz lasers rely on achieving population inversion. We demonstrate the generation of THz radiation using nitrogen-vacancy (NV) centers in a diamond single crystal. Population inversion is achieved through the Zeeman splitting of the $S=1$ state in $15\ \text{T}$, resulting in a splitting of $0.42\ \text{THz}$, where the middle $S_z=0$ sublevel is selectively pumped by visible light. To detect the THz radiation, we utilize a phase-sensitive THz setup, optimized for electron spin resonance measurements (ESR). We determine the spin-lattice relaxation time up to $15\ \text{T}$ using the light-induced ESR measurement, which shows the dominance of phonon-mediated relaxation and the high efficacy of the population inversion. The THz radiation is tunable by the magnetic field, thus these findings may lead to the next generation of tunable coherent THz sources.

physics.optics↗

arXiv2024

All epitaxial self-assembly of vertically-confined silicon color centers using ultra-low temperature epitaxy

Silicon-based color-centers (SiCCs) have recently emerged as quantum-light sources that can be combined with telecom-range Si Photonics platforms. Unfortunately, using current SiCC fabrication, deterministic control over the vertical emitter position is impossible due to ion-implantation's stochastic nature. To overcome this bottleneck towards high-yield integration, we demonstrate a radically innovative creation method for various SiCCs, solely relying on epitaxial growth of Si and C-doped Si at atypically-low temperatures in a ultra-clean growth environment. These telecom emitters can be confined within sub-1nm thick layers embedded at arbitrary vertical positions within a highly crystalline Si matrix. Tuning growth conditions and doping, different SiCC types, e.g., W-centers, T-centers, G-centers, or derivatives like G'-centers can be created, which are particularly promising as Si-based single-photon sources and spin-photon interfaces. The zero-phonon emission from G'-centers can be conveniently tuned by the C-concentration, leading to a systematic wavelength shift and linewidth narrowing towards low emitter densities.

cond-mat.mes-hall↗

arXiv2023

Resonant versus non-resonant spin readout of a nitrogen-vacancy center in diamond under cryogenic conditions

The last decade has seen an explosive growth in the use of color centers for metrology applications, the paradigm example arguably being the nitrogen-vacancy (NV) center in diamond. Here, we focus on the regime of cryogenic temperatures and examine the impact of spin-selective, narrow-band laser excitation on NV readout. Specifically, we demonstrate a more than four-fold improvement in sensitivity compared to that possible with non-resonant (green) illumination, largely due to a boost in readout contrast and integrated photon count. We also leverage nuclear spin relaxation under resonant excitation to polarize the 14N host, which we then prove beneficial for spin magnetometry. These results open opportunities in the application of NV sensing to the investigation of condensed matter systems, particularly those exhibiting superconducting, magnetic, or topological phases selectively present at low temperatures.

cond-mat.mes-hall↗

arXiv2023

Investigation of oxygen-vacancy complexes in diamond by means of \textit{ab initio} calculations

Point defects in diamond may act as quantum bits. Recently, oxygen-vacancy related defects have been proposed to the origin of the so-called ST1 color center in diamond that can realize a long-living solid-state quantum memory. Motivated by this proposal we systematically investigate oxygen-vacancy complexes in diamond by means of first principles density functional theory calculations. We find that all the considered oxygen-vacancy defects have a high-spin ground state in their neutral charge state, which disregards them as an origin for the ST1 color center. We identify a high-spin metastable oxygen-vacancy complex and characterize their magnetooptical properties for identification in future experiments.

cond-mat.mtrl-sci↗

arXiv2022

A telecom O-band emitter in diamond

Color centers in diamond are promising platforms for quantum technologies. Most color centers in diamond discovered thus far emit in the visible or near-infrared wavelength range, which are incompatible with long-distance fiber communication and unfavorable for imaging in biological tissues. Here, we report the experimental observation of a new color center that emits in the telecom O-band, which we observe in silicon-doped bulk single crystal diamonds and microdiamonds. Combining absorption and photoluminescence measurements, we identify a zero-phonon line at 1221 nm and phonon replicas separated by 42 meV. Using transient absorption spectroscopy, we measure an excited state lifetime of around 270 ps and observe a long-lived baseline that may arise from intersystem crossing to another spin manifold.

cond-mat.mtrl-sci↗

arXiv2020

DMRG on top of plane-wave Kohn-Sham orbitals: case study of defected boron nitride

In this paper, we analyze the numerical aspects of the inherently multi-reference density matrix renormalization group (DMRG) calculations on top of the periodic Kohn-Sham density functional theory (DFT) using the complete active space (CAS) approach. Following the technical outline related to the computation of the Hamiltonian matrix elements and to the construction of the active space, we illustrate the potential of the framework by studying the vertical many-body energy spectrum of hexagonal boron nitride (hBN) nano-flakes embedding a single boron vacancy point defect with prominent multi-reference character. We investigate the consistency of the DMRG energy spectrum from the perspective of sample size, basis size, and active space selection protocol. Results obtained from standard quantum chemical atom-centered basis calculations and plane-wave based counterparts show excellent agreement. Furthermore, we also discuss the spectrum of the periodic sheet which is in good agreement with extrapolated data of finite clusters. These results pave the way toward applying DMRG method in extended correlated solid state systems, such as point qubit in wide band gap semiconductors.

cond-mat.str-el↗

arXiv2018

High-fidelity spin and optical control of single silicon vacancy centres in silicon carbide

Optically interfaced spins in the solid promise scalable quantum networks. Robust and reliable optical properties have so far been restricted to systems with inversion symmetry. Here, we release this stringent constraint by demonstrating outstanding optical and spin properties of single silicon vacancy centres in silicon carbide. Despite the lack of inversion symmetry, the system's particular wave function symmetry decouples its optical properties from magnetic and electric fields, as well as from local strain. This provides a high-fidelity spin-to-photon interface with exceptionally stable and narrow optical transitions, low inhomogeneous broadening, and a large fraction of resonantly emitted photons. Further, the weak spin-phonon coupling results in electron spin coherence times comparable with nitrogen-vacancy centres in diamond. This allows us to demonstrate coherent hyperfine coupling to single nuclear spins, which can be exploited as qubit memories. Our findings promise quantum network applications using integrated semiconductor-based spin-to-photon interfaces.

quant-ph↗

arXiv2017

Isolated spin qubits in SiC with a high-fidelity infrared spin-to-photon interface

The divacancies in SiC are a family of paramagnetic defects that show promise for quantum communication technologies due to their long-lived electron spin coherence and their optical addressability at near-telecom wavelengths. Nonetheless, a mechanism for high-fidelity spin-to-photon conversion, which is a crucial prerequisite for such technologies, has not yet been demonstrated. Here we demonstrate a high-fidelity spin-to-photon interface in isolated divacancies in epitaxial films of 3C-SiC and 4H-SiC. Our data show that divacancies in 4H-SiC have minimal undesirable spin-mixing, and that the optical linewidths in our current sample are already similar to those of recent remote entanglement demonstrations in other systems. Moreover, we find that 3C-SiC divacancies have millisecond Hahn-echo spin coherence time, which is among the longest measured in a naturally isotopic solid. The presence of defects with these properties in a commercial semiconductor that can be heteroepitaxially grown as a thin film on shows promise for future quantum networks based on SiC defects.

quant-ph↗

arXiv2015

Optical polarization of nuclear spins in silicon carbide

We demonstrate optically pumped dynamic nuclear polarization of 29-Si nuclear spins that are strongly coupled to paramagnetic color centers in 4H- and 6H-SiC. The 99 +/- 1% degree of polarization at room temperature corresponds to an effective nuclear temperature of 5 microKelvin. By combining ab initio theory with the experimental identification of the color centers' optically excited states, we quantitatively model how the polarization derives from hyperfine-mediated level anticrossings. These results lay a foundation for SiC-based quantum memories, nuclear gyroscopes, and hyperpolarized probes for magnetic resonance imaging.

cond-mat.mes-hall↗

arXiv2013

Electrically and mechanically tunable electron spins in silicon carbide color centers

The electron spins of semiconductor defects can have complex interactions with their host, particularly in polar materials like SiC where electrical and mechanical variables are intertwined. By combining pulsed spin resonance with ab-initio simulations, we show that spin-spin interactions within SiC neutral divacancies give rise to spin states with an enhanced Stark effect, sub-10**-6 strain sensitivity, and highly spin-dependent photoluminescence with intensity contrasts of 15-36%. These results establish SiC color centers as compelling systems for sensing nanoscale fields.

cond-mat.mes-hall↗