arXiv subjects

Adam Gali

Publications and source records attributed to Adam Gali.

At least 19 recordsLinked to original sources

arXiv2026

Solution-phase fluorination of nanodiamond: near-surface NV$^-$ activation and spin relaxation

Nanodiamonds hosting luminescent point defects, known as fluorescent nanodiamonds (FND), are a leading platform for quantum technology. The nitrogen-vacancy (NV) centre is the most intensively studied of these; its negatively charged state (NV$^-$) can serve as a qubit at room temperature, and its stability is governed by surface functional groups. We present two solution-phase fluorination routes for stabilising NV$^-$: direct C-F bond formation by decarboxylation with xenon difluoride via a radical mechanism, and the Balz-Schiemann reaction, which replaces surface amino groups with fluorine. The two routes were compared by infrared, X-ray photoelectron, energy-dispersive X-ray, Raman and photoluminescence spectroscopy. Both gave a high NV$^-$ fraction, up to $\sim$90% on average and approaching 100% in fluorine-rich regions, which to our knowledge is among the highest reported for surface-terminated nanodiamonds of this size and, in particular, for fluorine termination. Frequency-domain relaxometry shows that the fluorinated particles retain a long spin-lattice relaxation time, $733\pm56$ and $712\pm20$ $\mu$s for the XeF$_2$ and Balz-Schiemann routes, several times the values reported for commercial HPHT nanodiamonds, although shorter than the $1173\pm123$ $\mu$s of the as-received material. Charge-state stability and spin lifetime therefore do not improve together: fluorination activates near-surface NV$^-$ centres, which are the most exposed to surface noise but also the ones that dominate relaxometric sensing.

quant-ph↗

arXiv2026

Quantum Relaxometry Under Continuous Wave Excitation

Quantum relaxometry is one of the most successful applications of nitrogen-vacancy (NV) centers in diamond and, more broadly, solid-state spin qubits, enabling ultrasensitive detection of magnetic noise and paramagnetic species via measurements of the spin-lattice relaxation time $T_1$. Conventional pulsed protocols, however, probe $T_1$ efficiently only over a limited temporal range, which restricts the scope and throughput of the technique. Here we introduce a continuous-wave quantum relaxometry protocol that operates in the frequency domain. By measuring the frequency response of the optically detected magnetic resonance signal under low-frequency microwave amplitude modulation, we extract $T_1$ from the characteristic response time of the spin system. The method enables efficient $T_1$ measurements spanning more than three orders of magnitude -- directly demonstrated from 60 $\mu$s to 200 ms in our experiments -- across a broad temperature range and under substantial ensemble inhomogeneity. We further show that this protocol enables quantitative relaxometry-based sensing in nanodiamonds, achieving a substantial speed-up over the pulsed methods and offering a practical approach to optimizing nanodiamond size for enhanced sensitivity.

quant-ph↗

arXiv2026

Dislocation-loop formation is a first-order phase transition

Dislocation loops are the elementary product of radiation damage in crystals, limiting reactor-component lifetimes, power-electronics reliability and the coherence of solid-state qubits. Their nucleation has been simulated for six decades but never reduced to a thermodynamic law. We show that dislocation-loop formation is a \emph{first-order phase transition}, and construct its Ginzburg--Landau free energy, with the loop area as order parameter, entirely from atomistic simulation. In diamond, carbon self-interstitials condense into planar precursors that collapse abruptly into a prismatic $\tfrac{1}{2}\langle110\rangle$ loop across a 3.7-electronvolt barrier, with pressure--volume work supplying only 2\% of the energy released. The reduced free energy proves material-independent: the vacancy platelet-to-loop collapse in body-centred-cubic iron falls on the same one-parameter family, placing loop nucleation on a transferable thermodynamic footing.

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↗

arXiv2026

Enhanced Emission from Boron-Vacancy Center in Rhombohedral Boron Nitride

Boron nitride is a layered crystal whose properties depend on how its atomic sheets are stacked. Its negatively charged boron vacancy is a well-established magnetic defect that can be prepared and read out optically, but in the common hexagonal form it emits very little light, because the symmetry of the surrounding lattice forbids the relevant optical transition. Here we show, using first-principles calculations, that stacking the sheets in the rhombohedral sequence instead removes this restriction and increases the emitted intensity by one to two orders of magnitude, while the magnetic properties remain comparable or improve. We predict that the resulting emission is bright enough for a single defect to be addressed at room temperature, and that a sharp emission line, absent in the hexagonal form, should appear on cooling. Stacking order therefore acts as a design parameter for tailoring the quantum properties of defects embedded in layered materials.

quant-ph↗

arXiv2026

Single-photon emitters and spin-photon interfaces in silicon

Single photons enable the distribution of quantum information over large distances and thus play a major role in quantum technologies such as communication and computing. Solid-state emitters are practical and efficient sources of single photons that can be manufactured in large numbers. When combined with a spin, the resulting spin-photon interfaces can store quantum states for extended periods and serve as the basis for quantum networks and repeaters. Among the many host materials explored over the past few decades, silicon stands out for its advanced nanofabrication, the maturity of its integrated photonics and microelectronics, and its high isotopic purity, which leads to exceptionally long spin coherence. These properties position silicon single-photon emitters and spin-photon interfaces among the most promising hardware platforms for implementing quantum networks and distributed quantum information processors. This review summarizes the current state of the art and open challenges towards coherent single-photon sources and scalable spin-photon interfaces based on color centers and erbium dopants in nanophotonic silicon structures.

quant-ph↗

arXiv2026

Magneto-optical properties of the neutral silicon-vacancy center in diamond under extreme isotropic strain fields

The neutral silicon--vacancy (SiV$^{0}$) center in diamond combines inversion symmetry with optical emission, making it a robust quantum emitter resilient to stray electric fields. Using first-principles density-functional theory, we quantify its response to isotropic strain spanning strong compression and tensile regimes (effective hydrostatic pressures of approximately $-80$ to $180$~GPa). The coexistence of doubly degenerate $e_g$ and $e_u$ levels produces a structural instability captured by a quadratic product Jahn--Teller model. Under isotropic compression, the zero-phonon line blue-shifts nearly linearly while the $E_g$ phonon stiffens, suppressing vibronic instabilities and reducing Jahn--Teller quenching. Consequently, the Ham-reduced excited-state spin--orbit splitting increases substantially and the dark--bright vibronic gap widens. In contrast, isotropic tensile strain enhances vibronic effects and induces symmetry breaking beyond a critical strain, with tunneling-mediated dynamical averaging at the onset. Throughout the symmetry-preserving regime, parity remains well defined, so isotropic strain alone does not activate the dark transition. Charge-transition levels indicate photostability of the emission deep into the compressive regime, and near the highest photostable deformation ($\sim 100$~GPa), the radiative lifetime increases due to a reduced transition dipole moment despite the increasing optical energy. These trends yield compact calibration relations linking optical and spin observables to isotropic strain and establish SiV$^{0}$ as a symmetry-protected, strain-tunable quantum emitter operating into the multi-megabar-equivalent regime.

quant-ph↗

arXiv2026

Coherent Spin-Photon Interface of single PL6 Color Centers in Silicon Carbide

The PL6 color center in silicon carbide has recently emerged as a promising platform for quantum information processing, yet its coherent spin--photon interface has remained largely unexplored. Here we present a comprehensive investigation of single PL6 centers, combining spectroscopy with theoretical analysis. The excited-state fine structure is fully resolved using group-theoretical modeling and strain-dependent measurements. Under resonant excitation, we achieve a spin initialization fidelity of $99.69 \pm 0.03\%$ and a readout contrast of $98.31 \pm 1.03\%$. The spin--photon--entangled $A_2$ transition exhibits narrow optical linewidths ($\sim 180$~MHz) and a polarization visibility of $\sim 82\%$. Coherent optical driving enables Rabi frequencies up to $2.895$~GHz, while dynamical decoupling extends the spin coherence time from $0.5$~ms to $5.70$~ms. Our results establish PL6 as a competitive solid-state spin--photon interface hosted in a commercially available semiconductor platform.

quant-ph↗

arXiv2025

Roadmap: 2D Materials for Quantum Technologies

Two-dimensional (2D) materials have emerged as a versatile and powerful platform for quantum technologies, offering atomic-scale control, strong quantum confinement, and seamless integration into heterogeneous device architectures. Their reduced dimensionality enables unique quantum phenomena, including optically addressable spin defects, tunable single-photon emitters, low-dimensional magnetism, gate-controlled superconductivity, and correlated states in Moir\'e superlattices. This Roadmap provides a comprehensive overview of recent progress and future directions in exploiting 2D materials for quantum sensing, computation, communication, and simulation. We survey advances spanning spin defects and quantum sensing, quantum emitters and nonlinear photonics, computational theory and data-driven discovery of quantum defects, spintronic and magnonic devices, cavity-engineered quantum materials, superconducting and hybrid quantum circuits, quantum dots, Moir\'e quantum simulators, and quantum communication platforms. Across these themes, we identify common challenges in defect control, coherence preservation, interfacial engineering, and scalable integration, alongside emerging opportunities driven by machine$-$learning$-$assisted design and integrated experiment$-$theory feedback loops. By connecting microscopic quantum states to mesoscopic excitations and macroscopic device architectures, this Roadmap outlines a materials-centric framework for integrating coherent quantum functionalities and positions 2D materials as foundational building blocks for next-generation quantum technologies.

quant-ph↗

arXiv2025

Exe.py: Ab initio fine structure parameters for trigonal defect qubits within the E$\otimes$e Jahn-Teller case

Trigonal solid-state defects are often subjects of spontaneous symmetry breaking driven by the $E\otimes e$ Jahn-Teller effect, reflecting strong electron-phonon coupling. These systems, particularly paramagnetic defect qubits in solids are central for quantum technology applications, where accurate knowledge of their fine-structure parameters $-$ shaped by the complex interplay of spin-orbit and electron-phonon interactions $-$ is essential. We introduce the Exe.py code part of the jahn-teller-dynamics package, a Python code that implements the first-principles approach of [Phys. Rev. X 8, 021063 (2018)] to accurately compute the spin-orbit-phonon entanglement in trigonal defects utilizing the output from density functional theory calculations (DFT). By employing $\Delta$SCF calculations, the method extends naturally to excited states and predicts fine-structure parameters of zero-phonon lines (ZPLs), including Zeeman shifts under external magnetic fields. The approach is applicable not only to solid-state defects but also to Jahn-Teller active trigonal molecules such as the $X$CH$_3$ family. We demonstrate the capabilities of Exe.py through applications to negatively charged Group-IV$-$vacancy (G4V) defects in diamond: SiV$^-$, GeV$^-$, SnV$^-$, PbV$^-$ and the neutral N$_3$V$^0$ defect in diamond, and the CH$_3$O methoxy radical.

cond-mat.mtrl-sci↗

arXiv2025

High-yield engineering and identification of oxygen-related modified divacancies in 4H-SiC

Modified divacancies in the 4H polytype of silicon carbide (SiC) exhibit enhanced charge stability and spin addressability at room temperature, making them attractive for quantum applications. However, their low formation yield and lack of direct structural identification have hindered progress. Here, we demonstrate a controllable method for high-yield engineering and identification of oxygen-related modified divacancy color centers in 4H-SiC via oxygen-ion implantation. Based on their distinct optical and spin-resonance characteristics, we experimentally resolve four types of modified divacancies. Furthermore, by measuring isotope-resolved 17O hyperfine interactions, we identify them as the four crystallographic configurations of oxygen-vacancy (OV) complexes. Remarkably, single OV centers account for over 90% of the total defect population and exhibit superior optical properties and spin coherence compared with defects created by conventional carbon or nitrogen implantation. We characterize the zero-phonon lines of these OV centers and reveal distinct temperature-dependent behavior in spin-readout contrast. By optimizing implantation dose and annealing temperature, we achieve high-density ensembles and observe Rabi-oscillation beating patterns associated with different orientations of basal-type defects. These results establish a high-yield route for scalable engineering of these four oxygen-related modified divacancies in 4H-SiC and clarify their atomic structure, opening new opportunities for solid-state quantum technologies.

quant-ph↗

arXiv2025

Strain Enhanced Spin Readout Contrast in Silicon Carbide Membranes

Quantum defects in solids have emerged as a transformative platform for advancing quantum technologies. A key requirement for these applications is achieving high-fidelity single-spin readout, particularly at room temperature for quantum biosensing. Here, we demonstrate through ab initio simulations of a primary quantum defect in 4H silicon carbide that strain is an effective control parameter for significantly enhancing readout contrast. We validate this principle experimentally by inducing local strain in silicon carbide-on-insulator membranes, achieving a readout contrast exceeding 60% while preserving the favorable coherence properties of single spins. Our findings establish strain engineering as a powerful and versatile strategy for optimizing coherent spin-photon interfaces in solid-state quantum systems.

quant-ph↗

arXiv2025

Spin-Phonon Relaxation of Boron-Vacancy Centers in Two-Dimensional Boron Nitride Polytypes

Two-dimensional (2D) materials hosting color centers and spin defects are emerging as key platforms for quantum technologies. However, the impact of reduced dimensionality on the spin-lattice relaxation time ($T_1$) of embedded defect spins -- critical for quantum applications -- remains largely unexplored. In this study, we present a systematic first-principles investigation of the negatively charged boron-vacancy (V$_{\text{B}}^-$) defect in monolayer boron nitride (BN), as well as in AA$^\prime$-stacked hexagonal BN (hBN) and ABC-stacked rhombohedral BN (rBN). Our results reveal that the $T_1$ times of V$_{\text{B}}^-$ in monolayer BN and hBN are nearly identical at room temperature. Surprisingly, despite the symmetry reduction in rBN opening additional spin relaxation channels, V$_{\text{B}}^-$ exhibits a longer $T_1$ compared to hBN. We attribute this effect to the stiffer out-of-plane phonon modes in rBN, which activate spin-phonon relaxation at reduced strength. These findings suggest that V$_{\text{B}}^-$ in rBN offers enhanced spin coherence properties, making it a promising candidate for quantum technology applications.

quant-ph↗

arXiv2025

Thiolation and PEGylation of silicon carbide nanoparticle

In this study, we implement thiol termination on the surface of few-nanometer-sized silicon carbide (SiC) nanoparticles (NPs) to enable further applications, such as fluorescent biomarkers. Various spectroscopic techniques are employed to monitor the effectiveness of the surface treatment. A thiol-Michael addition reaction is performed by conjugating 4-arm PEGmaleimide molecules to the thiol groups of SiC NPs, further demonstrating the reactivity of thiol-terminated SiC NPs, which also acts as a protection layer against oxidation. These fluorescent thiolated SiC NPs, both with and without conjugated molecules, are directly applicable as bioinert probes. Since SiC NPs can potentially host room-temperature fluorescent defect quantum bits, our results are an important step to realize a bioinert, ultrasmall quantum sensor bioagents, which may open new avenues in biotechnology.

cond-mat.mtrl-sci↗

arXiv2025

Materials and Spin Characteristics of Nanodiamonds Partially Covered with Amino Groups and Embedded with Nitrogen-Vacancy Color Centers

Fluorescent nanodiamonds (FNDs) with optically read qubits hold great potential for detecting electric and magnetic fields, temperature, and other nanoscale physicochemical quantities relevant to chemistry and biology. Proper surface functionalization is essential for their application as probes, but surface modifications can impact qubit sensor properties. We systematically study nitrogen-vacancy (NV) color centers in FNDs as a function of size and surface termination. FNDs were produced from high-pressure, high-temperature diamonds, with NV centers introduced via electron irradiation and annealing. The initial oxygen-covered FNDs were homogenized with hydroxyl (-OH) groups as reference samples, while the noninvasive Hofmann degradation introduced amino (-NH2) groups for potential direct biomolecule attachment. Amino groups may not cover the nanodiamonds homogeneously, but we label them as -NH2 terminated throughout. We monitored charge state stability and the zero-field splitting parameters of the embedded NV centers. First, we resolve the size dependence of the NV(-) zero-field splitting parameters across the 10-140 nm range and show that the symmetry-breaking E parameter decreases monotonically from about 8 to about 5 MHz with increasing size while the axial D parameter is shifted only in the smallest (<= 30 nm) particles, thereby disentangling the static-strain and fluctuating electric-field contributions to the spin levels. Second, while NV charge state stabilization was observed in both -OH- and -NH2-terminated FNDs above a certain size, we demonstrate that a remarkably high and laser-power-independent NV(-) content (f_NV(-) of about 0.8) is achieved by wet-chemical Hofmann amino termination only in 140 nm particles, an effect we link through electron spin resonance to the degradation of surface paramagnetic defects rather than to the introduction of new ones.

quant-ph↗

arXiv2025

Native antisite defects in h-BN

Hexagonal boron nitride (hBN) is an excellent host for solid-state single phonon emitters. Experimental observed emission ranges from infrared to ultraviolet. The emission centers are generally attributed to either intrinsic or extrinsic point defects embedded into hBN. Nevertheless, the microscopic structure of most of these defect emitters is uncertain. Here, through density-functional theory calculations we studied the native antisite defects in hBN. We find that the neutral boron antisite might be a nonmagnetic single photon source with zero-phonon-line (ZPL) at 1.58 eV and such a lineshape that is often observed in experiments. Furthermore, the positively charged nitrogen antisite might be associated with a dim color center recently observed as a blue emitter with ZPL at 2.63 eV. These simple single substitution defects indicate the existence of out-of-plane phonon mode which significantly affects the optical properties. Our results could provide useful information for identification of quantum emitters in hBN.

cond-mat.mtrl-sci↗

arXiv2024

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

Single V2 defect in 4H Silicon Carbide Schottky diode at low temperature

Nanoelectrical and photonic integration of quantum optical components is crucial for scalable solid-state quantum technologies. Silicon carbide stands out as a material with mature quantum defects and a wide variety of applications in semiconductor industry. Here, we study the behaviour of single silicon vacancy (V2) colour centres in a metal-semiconductor (Au/Ti/4H-SiC) epitaxial wafer device, operating in a Schottky diode configuration. We explore the depletion of free carriers in the vicinity of the defect, as well as electrical tuning of the defect optical transition lines. By detecting single charge traps, we investigate their impact on V2 optical line width. Additionally, we investigate the charge-photon-dynamics of the V2 centre and find its dominating photon-ionisation processes characteristic rate and wavelength dependence. Finally, we probe the spin coherence properties of the V2 system in the junction and demonstrate several key protocols for quantum network applications. Our work shows the first demonstration of low temperature integration of a Schottky device with optical microstructures for quantum applications and paves the way towards fundamentally scalable and reproducible optical spin defect centres in solids.

quant-ph↗