arXiv subjects

Anton Pershin

Publications and source records attributed to Anton Pershin.

At least 19 recordsLinked to original sources

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

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

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↗

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

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↗

arXiv2024

Quantum Emission from Coupled Spin Pairs in Hexagonal Boron Nitride

Optically addressable defect qubits in wide band gap materials are favorable candidates for room temperature quantum information processing. The two-dimensional (2D) hexagonal boron nitride (hBN) is an attractive solid state platform with a great potential for hosting bright quantum emitters with quantum memories with leveraging the potential of 2D materials for realizing scalable preparation of defect qubits. Although, room temperature bright defect qubits have been recently reported in hBN but their microscopic origin, the nature of the optical transition as well as the optically detected magnetic resonance (ODMR) have been remained elusive. Here we connect the variance in the optical spectra, optical lifetimes and spectral stability of quantum emitters to donor-acceptor pairs (DAP) in hBN by means of ab initio calculations. We find that DAPs can exhibit ODMR signal for the acceptor counterpart of the defect pair with S=1/2 ground state at non-zero magnetic fields depending on the donor partner. The donor-acceptor pair model and its transition mechanisms provide a recipe towards defect qubit identification and performance optimization in hBN for quantum applications.

cond-mat.mtrl-sci↗

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

Revealing Polytypism in 2D Boron Nitride with UV Photoluminescence

Boron nitride exhibits diverse crystal structures, predominantly a layered arrangement with strong intraplanar covalent bonds and weak interplanar van der Waals bonds. While commonly referred to as hexagonal BN (hBN), the sp$^2$-bonded BN atomic planes can also arrange in other configurations like Bernal (bBN) or rhombohedral (rBN) stacking orders. Variations in the orientation and translation of successive atomic layers lead to changes in crystal symmetry, potentially resulting in piezoelectric, pyroelectric or ferroelectric effects. However, distinguishing between different polytypes using conventional methods like X-ray diffraction or Raman spectroscopy presents a significant challenge. In this work, we demonstrate that the optical response of the 4.1 eV defect can serve as an indicator of the polytype. To this end, we study BN samples grown by metalorganic vapor phase epitaxy (MOVPE), which contain different polytypes. The identification of the polytypes was achieved by X-ray diffraction and transmission electron microscopy. Photoluminescence and cathodoluminescence measurements with a high spatial resolution allowed for the deconvolution of the signal into two components from which we can extract a zero-phonon line (ZPL) at 4.096 eV (302.6 nm) for hBN and 4.143 eV (299.2 nm) for rBN. We performed calculations that enable us to identify the defect as a carbon dimer CBCN (C2) and show that the ZPL shift reflects differences in the crystal environment for different polytypes. Furthermore, we demonstrate that different polytypic composition ratios of hBN and rBN can be achieved by MOVPE, which could pave the way for future applications in large-area van der Waals heterostructures.

cond-mat.mtrl-sci↗

arXiv2023

Diamond Surface Functionalization via Visible Light-Driven C-H Activation for Nanoscale Quantum Sensing

Nitrogen-vacancy centers in diamond are a promising platform for nanoscale nuclear magnetic resonance sensing. Despite significant progress towards using NV centers to detect and localize nuclear spins down to the single spin level, NV-based spectroscopy of individual, intact, arbitrary target molecules remains elusive. NV molecular sensing requires that target molecules are immobilized within a few nanometers of NV centers with long spin coherence time. The inert nature of diamond typically requires harsh functionalization techniques such as thermal annealing or plasma processing, limiting the scope of functional groups that can be attached to the surface. Solution-phase chemical methods can be more readily generalized to install diverse functional groups, but they have not been widely explored for single-crystal diamond surfaces. Moreover, realizing shallow NV centers with long spin coherence times requires highly ordered single-crystal surfaces, and solution-phase functionalization has not yet been shown to be compatible with such demanding conditions. In this work, we report a versatile strategy to directly functionalize C-H bonds on single-crystal diamond surfaces under ambient conditions using visible light. This functionalization method is compatible with charge stable NV centers within 10 nm of the surface with spin coherence times comparable to the state of the art. As a proof of principle, we use shallow ensembles of NV centers to detect nuclear spins from functional groups attached to the surface. Our approach to surface functionalization based on visible light-driven C-H bond activation opens the door to deploying NV centers as a broad tool for chemical sensing and single-molecule spectroscopy.

cond-mat.mtrl-sci↗

arXiv2023

Exceptionally strong coupling of defect emission in hexagonal boron nitride to stacking sequences

Van der Waals structures present a unique opportunity for tailoring material interfaces and integrating photonic functionalities. By precisely manipulating the twist angle and stacking sequences, it is possible to elegantly tune and functionalize the electronic and optical properties of layered van der Waals structures. Among these materials, two-dimensional hexagonal boron nitride (hBN) stands out for its remarkable optical properties and wide band gap, making it a promising host for solid state single photon emitters at room temperature. Previous investigations have demonstrated the observation of bright single photon emission in hBN across a wide range of wavelengths. In this study, we unveil an application of van der Waals technology in modulating their spectral shapes and brightness by carefully controlling the stacking sequences and polytypes. Our theoretical analysis reveals remarkably large variations in the Huang-Rhys factors-an indicator of the interaction between a defect and its surrounding lattice-reaching up to a factor of 3.3 for the same defect in different stackings. We provide insights into the underlying mechanism behind these variations, shedding light on the design principles necessary to achieve rational and precise control of defect emission. This work paves the way for enhancing defect identification and facilitating the engineering of highly efficient single photon sources and qubits using van der Waals materials.

cond-mat.mes-hall↗

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↗

arXiv2022

Towards large-scale restricted active space calculations inspired by the Schmidt decomposition

We present an alternative, memory-efficient, Schmidt decomposition-based description of the inherently bipartite restricted active space (RAS) scheme, which can be implemented effortlessly within the density matrix renormalization group (DMRG) method via the dynamically extended active space procedure. Benchmark calculations are compared against state-of-the-art results of C$_2$ and Cr$_2$, which are notorious for their multi-reference character. Our results for ground and excited states together with spectroscopic constants demonstrate that the proposed novel approach, dubbed as DMRG-RAS, which is variational and free of uncontrolled method errors, has the potential to outperfom conventional methods for strongly correlated molecules.

physics.chem-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

Can neural networks predict dynamics they have never seen?

Neural networks have proven to be remarkably successful for a wide range of complicated tasks, from image recognition and object detection to speech recognition and machine translation. One of their successes is the skill in prediction of future dynamics given a suitable training set of data. Previous studies have shown how Echo State Networks (ESNs), a subset of Recurrent Neural Networks, can successfully predict even chaotic systems for times longer than the Lyapunov time. This study shows that, remarkably, ESNs can successfully predict dynamical behavior that is qualitatively different from any behavior contained in the training set. Evidence is provided for a fluid dynamics problem where the flow can transition between laminar (ordered) and turbulent (disordered) regimes. Despite being trained on the turbulent regime only, ESNs are found to predict laminar behavior. Moreover, the statistics of turbulent-to-laminar and laminar-to-turbulent transitions are also predicted successfully, and the utility of ESNs in acting as an early-warning system for transition is discussed. These results are expected to be widely applicable to data-driven modelling of temporal behaviour in a range of physical, climate, biological, ecological and finance models characterized by the presence of tipping points and sudden transitions between several competing states.

cs.LG↗

arXiv2021

Dielectric control of reverse intersystem crossing in thermally-activated delayed fluorescence emitters

Thermally-activated delayed fluorescence (TADF) enables organic semiconductors with charge transfer (CT)-type excitons to convert dark triplet states into bright singlets via a reverse intersystem crossing (rISC) process. Here, we consider the role of the dielectric environment in a range of TADF materials with varying changes in dipole moment upon optical excitation. In a dipolar reference emitter, TXO-TPA, environmental reorganisation after excitation in both solution and doped films triggers the formation of the full CT product state. This lowers the singlet excitation energy by 0.3 eV and minimises the singlet-triplet energy gap (ΔEST). Using impulsive Raman measurements, we observe the emergence of two (reactant-inactive) modes at 412 and 813 cm-1 as a vibrational fingerprint of the CT product. In contrast, the dielectric environment plays a smaller role in the electronic excitations of a less dipolar material, 4CzIPN. Quantum-chemical calculations corroborate the appearance of these new product modes in TXO-TPA and show that the dynamic environment fluctuations are large compared to ΔEST. The analysis of the energy-time trajectories and the corresponding free energy functions reveals that the dielectric environment significantly reduces the activation energy for rISC, thus increasing the rISC rate by up to three orders of magnitude when compared to a vacuum environment.

physics.app-ph↗

arXiv2021

Optimizing the control of transition to turbulence using a Bayesian method

The nonlinear robustness of laminar plane Couette flow is considered under the action of in-phase spanwise wall oscillations by computing properties of the edge of chaos, i.e., the boundary of its basin of attraction. Three measures are used to quantify the chosen control strategy on laminar-to-turbulent transition: the kinetic energy of edge states (local attractors on the edge of chaos), the form of the minimal seed (least energetic perturbation on the edge of chaos), and the laminarization probability (the probability that a random perturbation from the laminar flow of given kinetic energy will laminarize). A novel Bayesian approach is introduced to enable the accurate computation of the laminarization probability at a fraction of the cost of previous methods. While the edge state and the minimal seed provide useful information about the dynamics of transition to turbulence, neither measure is particularly useful to judge the effectiveness of the control strategy since they are not representative of the global geometry of the edge. In contrast, the laminarization probability provides global information about the edge and can be used to evaluate the control effectiveness by computing a laminarization score (the expected laminarization probability) and the associated expected dissipation rate of the controlled flow. These two quantities allow for the determination of optimal control parameter values subject to desired constraints. The results discussed in the paper are expected to be applied to a wide range of transitional flows and control strategies aimed at suppressing or triggering transition to turbulence.

physics.flu-dyn↗

arXiv2020

The role of charge recombination to spin-triplet excitons in non-fullerene acceptor organic solar cells

The power conversion efficiencies (PCEs) of organic solar cells (OSCs) using non-fullerene acceptors (NFAs) have now reached 18%. However, this is still lower than inorganic solar cells, for which PCEs >20% are commonplace. A key reason is that OSCs still show low open-circuit voltages (Voc) relative to their optical band gaps, attributed to non-radiative recombination. For OSCs to compete with inorganics in efficiency, all non-radiative loss pathways must be identified and where possible, removed. Here, we show that in most NFA OSCs, the majority of charge recombination at open-circuit proceeds via formation of non-emissive NFA triplet excitons (T1); in the benchmark PM6:Y6 blend, this fraction reaches 90%, contributing 60 mV to the reduction of Voc. We develop a new design to prevent recombination via this non-radiative channel through the engineering of significant hybridisation between the NFA T1 and the spin-triplet charge transfer exciton (3CTE). We model that the rate of the back charge transfer from 3CTE to T1 can be reduced by an order of magnitude, allowing re-dissociation of the 3CTE. We then demonstrate NFA systems where T1 formation is suppressed. This work therefore provides a clear design pathway for improved OSC performance to 20% PCE and beyond.

physics.app-ph↗