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Lukas Razinkovas

Publications and source records attributed to Lukas Razinkovas.

16 recordsLinked to original sources

Impact of strain on electron-phonon coupling of quantum emitters

Defects in semiconductors acting as optically active spin qubits are intriguing objects of fundamental study and future technological developments. These defect-based color centers are of particular interest for detection and response to physical variations such as pressure and strain, or conversely -- as we demonstrate the possibility of herein -- pressure and strain can be utilized to manipulate quantum emitter properties. To investigate how strain can alter the fundamental electron-phonon interaction of quantum defects, we employ the negatively charged silicon vacancy ($\mathrm{V_{Si}^{-}}$) in 4H-SiC as a use-case and study its vibrational structure under applied tensile and compressive uniaxial strain using first-principles calculations. We show that the strain variations of the emission spectrum can be explained by differing responses of bulk-like and quasi-localized vibrational modes. Importantly, the $\mathrm{V_{Si}^{-}}$ defect exhibits a strain-induced enhancement of the Debye-Waller factor under uniaxial tensile strain applied along the $a$-axis of 4H-SiC, thereby improving its performance as a quantum emitter. The strain-dependent changes in the phonon sideband enable distinguishing between compressive and tensile strain, opening up the possibility of magnetic-field-free strain detection using only spin-conserving transitions of solid-state quantum emitters.

cond-mat.mtrl-sci↗

Optical Stability and Photophysics of NV Centers in Diamond up to 120 GPa

The nitrogen vacancy (NV) center has emerged as a powerful quantum sensor in high-pressure research, with the observation of optically detected magnetic resonance at megabar pressures. However, some aspects of NV physics require further investigation to optimize the development of NV-based sensing under pressure. Here, we study both experimentally and theoretically the optical properties of the NV center under hydrostatic pressure. We investigate the evolution of the zero-phonon line (ZPL) position, radiative lifetimes, optical lineshapes, and photoionization thresholds of the NV center under pressures up to ~120 GPa. We also provide spectroscopic guidelines for performing high-pressure optical experiments. Our results confirm that the NV center remains a robust quantum sensor under extreme hydrostatic pressures, especially for magnetic characterization.

quant-ph↗

Unraveling the electronic structure of silicon vacancy centers in 4H-SiC

Point defects in silicon carbide (SiC), particularly the negatively-charged silicon vacancy ($\mathrm{V_{Si}^{-}}$) in 4H-SiC, are leading candidates for scalable quantum technologies due to their favorable spin-optical properties and compatibility with industrial semiconductor fabrication processes. Comprehensive knowledge of a defect's electronic structure is essential for interpreting spin-optical dynamics and for the reliable design and optimization of defect-based quantum devices. Despite extensive study, our knowledge of the electronic structure of $\mathrm{V_{Si}^{-}}$\ is limited since key excited-state manifolds have remained inaccessible to conventional steady-state spectroscopy. In this study, transient absorption spectroscopy is utilized to probe non-equilibrium electronic transitions of $\mathrm{V_{Si}^{-}}$\ and to uncover previously unobserved excited states. The first direct observation of the elusive V2' quartet transition is presented, with its broad spectral signature attributed to nonadiabatic vibronic coupling. Within the spin-doublet manifold, which is central to optically detected magnetic resonance (ODMR) but has remained unresolved spectroscopically, multiple optical transitions are identified. The complete electronic level structure in the relevant energy range is elucidated by combining polarization-resolved spectroscopy, group-theoretical analysis, quantum embedding calculations and first-principles optical lineshape modeling. Collectively, these results provide a microscopic understanding of the $\mathrm{V_{Si}^{-}}$\ electronic structure. Our approach also establishes a general framework for resolving and understanding complex excited-state manifolds in wide-bandgap color centers.

cond-mat.mtrl-sci↗

Charge state equilibration of nitrogen-vacancy center ensembles in diamond: The role of electron tunneling

The charge state stability of nitrogen-vacancy (NV) centers critically affects their application as quantum sensors and qubits. Understanding charge state conversion and equilibration is critical not only for NV centers in diamond but also for defects and impurities in wide-bandgap materials in general. The mechanisms by which these centers change charge state upon optical or electronic excitation without the presence of mobile carriers remain unclear, potentially affecting the performance of applications ranging from phosphors to power electronics. Here, we elucidate this issue for the case of photoionization of NV center ensembles. Using pump-probe spectroscopy, we ionize negatively charged NV centers and monitor the recovery of $\NVm$ on timescales of up to several seconds. We find that the recovery rate depends strongly on the concentration of surrounding nitrogen donors. Remarkably, the equilibration dynamics exhibit no discernible dependence on temperature, ruling out thermally activated processes. The multiphonon-assisted electron tunneling model, supported by density-functional calculations, explains the measurements and identifies tunneling as the equilibration mechanism.

cond-mat.mtrl-sci↗

Magneto-optical properties of Group-IV--vacancy centers in diamond upon hydrostatic pressure

In recent years, the negatively charged group-IV--vacancy defects in diamond, labeled as G4V(-) or G4V centers, have attracted significant attention in quantum information processing. In this study, we investigate the magneto-optical properties of G4V centers under high compressive hydrostatic pressures up to 180 GPa. The spin-orbit splitting of the electronic ground and excited states, as well as the hyperfine tensors, are calculated using plane-wave supercell density functional theory, providing distinctive fingerprints that uniquely characterize these defects. To this end, we develop a theory for calculating the hyperfine tensors when the electronic states are subject to the Jahn--Teller effect. We find that the zero-phonon-line energy increases with hydrostatic pressure, with the deformation potential increasing from SiV(-) to PbV(-). On the other hand, our calculated photoionization threshold energies indicate that PbV(-)-based quantum sensors can operate only up to 32 GPa, whereas SnV(-), GeV(-), and SiV(-) remain photostable up to 180 GPa. We also find that the spin-orbit splitting increases in both the electronic ground and excited states with increasing pressure. The optical transitions associated with the hyperfine fine structure of the dopant atoms are interpreted using our theoretical framework, which reproduces existing experimental data at zero strain. We show that the hyperfine levels are weakly dependent on magnetic field, and increasing pressure leads to optical transitions at longer wavelengths. Finally, we estimate the spin coherence times of the G4V centers under increasing hydrostatic pressure across different temperature regimes.

quant-ph↗

Characterization of Chromium Impurities in $β$-Ga$_2$O$_3$

Chromium is a common transition-metal impurity that is easily incorporated during crystal growth. It is perhaps best known for giving rise to the 694.3 nm (1.786 eV) emission in Cr-doped Al$_2$O$_3$, exploited in ruby lasers. Chromium has also been found in monoclinic gallium oxide, a wide-bandgap semiconductor being pursued for power electronics. In this work, we thoroughly characterize the behavior of Cr in Ga$_2$O$_3$ through theoretical and experimental techniques. $β$-Ga$_2$O$_3$ samples are grown with the floating zone method and show evidence of a sharp photoluminescence signal, reminiscent of ruby. We calculate the energetics of formation of Cr from first principles, demonstrating that Cr preferentially incorporates as a neutral impurity on the octahedral site. Cr possesses a quartet ground-state spin and has an internal transition with a zero-phonon line near 1.8 eV. By comparing the calculated and experimentally measured luminescence lineshape function, we elucidate the role of coupling to phonons and uncover features beyond the Franck-Condon approximation. The combination of strong emission with a small Huang-Rhys factor of 0.05 and a technologically relevant host material render Cr in Ga$_2$O$_3$ attractive as a quantum defect.

cond-mat.mtrl-sci↗

Theory of the divacancy in 4H-SiC: Impact of Jahn-Teller effect on optical properties

Understanding the optical properties of color centers in silicon carbide is essential for their use in quantum technologies, such as single-photon emission and spin-based qubits. In this work, first-principles calculations were employed using the r2SCAN density functional to investigate the electronic and vibrational properties of neutral divacancy configurations in 4H-SiC. Our approach addresses the dynamical Jahn-Teller effect in the excited states of axial divacancies. By explicitly solving the multimode dynamical Jahn-Teller problem, we compute emission and absorption lineshapes for axial divacancy configurations, providing insights into the complex interplay between electronic and vibrational degrees of freedom. The results show strong alignment with experimental data, underscoring the predictive power of the methodologies. Our calculations predict spontaneous symmetry breaking due to the pseudo Jahn-Teller effect in the excited state of the $kh$ divacancy, accompanied by the lowest electron-phonon coupling among the four configurations and distinct polarizability. These unique properties facilitate its selective excitation, setting it apart from other divacancy configurations, and highlight its potential utility in quantum technology applications. These findings underscore the critical role of electron-phonon interactions and optical properties in spin defects with pronounced Jahn-Teller effects, offering valuable insights for the design and integration of quantum emitters for quantum technologies.

cond-mat.mtrl-sci↗

Optical lineshapes of the C-center in silicon from ab initio calculations: Interplay of localized modes and bulk phonons

In this work, we present a first-principles density functional theory (DFT) computational investigation of the luminescence and absorption lineshapes associated with the neutral carbon-oxygen interstitial pair (CiOi) defect in silicon. We obtain the lineshapes of the defect in the dilute limit using a computational methodology that constructs dynamical matrices of supercells containing tens of thousands of atoms, utilizing systems directly accessible through DFT. Both perturbed bulk phonons and localized vibrations contribute to the phonon sideband. We achieve excellent agreement with experimental luminescence data. Our findings further reinforce the attribution of the well-known C-line in silicon to the neutral CiOi complex.

cond-mat.mtrl-sci↗

Optical lineshapes for orbital singlet to doublet transitions in a dynamical Jahn-Teller system: the NiV$^{-}$ center in diamond

We apply density functional theory to investigate interactions between electronic and vibrational states in crystal defects with multi-mode dynamical Jahn-Teller (JT) systems. Our focus is on transitions between orbital singlet and degenerate orbital doublet characterized by $E \otimes (e \oplus e \oplus \cdots)$ JT coupling, which frequently occurs in crystal defects that are investigated for applications in quantum information science. We utilize a recently developed methodology to model the photoluminescence (PL) spectrum of the negatively charged split nickel-vacancy center (NiV$^{-}$) in diamond, where JT-active modes significantly influence electron-phonon interactions. Our results validate the effectiveness of the methodology in accurately reproducing the observed 1.4 eV PL lineshape. The strong agreement between our theoretical predictions and experimental observations reinforces the identification of the 1.4 eV PL center with the NiV$^{-}$ complex. This study highlights the critical role of JT-active modes in affecting optical lineshapes and demonstrates the power of advanced techniques for modeling optical properties in complex systems with multiple JT-active frequencies.

cond-mat.mtrl-sci↗

Blue quantum emitter in hexagonal boron nitride and carbon chain tetramer: proposition of identification

Single photon emitters in hexagonal boron nitride offer a gateway to the future of quantum technologies, yet their identification remains challenging and subject to ongoing debate. We demonstrate through ab initio calculations that the optical properties of a carbon chain tetramer are in excellent agreement with the characteristics of a blue quantum emitter in hexagonal boron nitride emitting at 435 nm. Its calculated zero-phonon line energy (2.77 eV) and radiative lifetime (1.6 ns) perfectly align with experimental observations. The relatively weak electron--phonon coupling (Huang-Rhys factor of 1.5) indicates intense emission at the zero-phonon line. Despite the absence of an inversion center in the carbon tetramer, we demonstrate that it exhibits a negligible linear Stark effect, consistent with experimental findings. Additionally, our hypothesis explains the experimental observation that the formation of blue emitters is only possible in samples containing numerous ultraviolet emitters, which are likely identical to carbon dimers.

cond-mat.mtrl-sci↗

Optical properties of SiV and GeV color centers in nanodiamonds under hydrostatic pressures up to 180 GPa

We investigate the optical properties of silicon-vacancy (SiV) and germanium-vacancy (GeV) color centers in nanodiamonds under hydrostatic pressure up to 180 GPa. The nanodiamonds were synthetized by Si or Ge-doped plasma assisted chemical vapor deposition and, for our experiment, pressurized in a diamond anvil cell. Under hydrostatic pressure we observe blue-shifts of the SiV and GeV zero-phonon lines by 17 THz (70 meV) and 78 THz (320 meV), respectively. These measured pressure induced shifts are in good agreement with ab initio calculations that take into account the lattice compression based on the equation of state of diamond and that are extended to the case of the tin-vacancy (SnV) center. This work provides guidance on the use of group-IV-vacancy centers as quantum sensors under extreme pressures that will exploit their specific optical and spin properties induced by their intrinsic inversion-symmetric structure.

quant-ph↗

Enhancement of spin-to-charge conversion of diamond NV centers at ambient conditions using surface electrodes

The nitrogen-vacancy (NV) center in diamond is a heavily studied defect due to its potential applications to quantum metrology and computation, particularly in ambient conditions. The key mechanism to using the NV in any application lies in the ability to read out the spin state of the defect which is typically done optically. The optical contrast is then the key metric for electron spin readout fidelity and one of the key limiting factors in the NV's overall performance. We present a new mechanism for high contrast readout using the spin-to-charge conversion (SCC) mechanism in conjunction with an electrode to improve the spin contrast by altering the NV energy levels relative to the diamond conduction band. Theoretical modelling predicts an optical spin contrast at 42% which would be the highest optical contrast for the NV at room temperature and the technique opens up a range of alternative research pathways for the NV which are discussed.

quant-ph↗

Thermodynamics of carbon point defects in hexagonal boron nitride

We present a first-principles computational study of the thermodynamics of carbon defects in hexagonal boron nitride (hBN). The defects considered are carbon monomers, dimers, trimers, and larger carbon clusters, as well as complexes of carbon with vacancies, antisites, and substitutional oxygen. Our calculations show that monomers ($\text{C}_{\text{B}}$, $\text{C}_{\text{B}}$), dimers, trimers, and $\text{C}_{\text{N}}\text{O}_{\text{N}}$ pairs are the most prevalent species under most growth conditions. Compared to these defects, larger carbon clusters, as well as complexes of carbon with vacancies and antisites, occur at much smaller concentrations. Our results are discussed in view of the relevance of carbon defects in single-photon emission in hBN.

cond-mat.mtrl-sci↗

Vibrational and vibronic structure of isolated point defects: the nitrogen-vacancy center in diamond

We present a theoretical study of vibrational and vibronic properties of a point defect in the dilute limit by means of first-principles density functional theory calculations. As an exemplar we choose the negatively charged nitrogen-vacancy center, a solid-state system that has served as a testbed for many protocols of quantum technology. We achieve low effective concentrations of defects by constructing dynamical matrices of large supercells containing tens of thousands of atoms. The main goal of the paper is to calculate luminescence and absorption lineshapes due to coupling to vibrational degrees of freedom. The coupling to symmetric $a_1$ modes is computed via the Huang-Rhys theory. Importantly, to include a nontrivial contribution of $e$ modes we develop an effective methodology to solve the multi-mode $E \otimes e$ Jahn-Teller problem. Our results show that for NV centers in diamond a proper treatment of $e$ modes is particularly important for absorption. We obtain good agreement with experiment for both luminescence and absorption. Finally, the remaining shortcomings of the theoretical approach are critically reviewed. The presented theoretical approach will benefit identification and future studies of point defects in solids.

cond-mat.mtrl-sci↗

Vibrational modes of negatively charged silicon-vacancy centers in diamond from ab initio calculations

Silicon-vacancy (SiV) center in diamond is a photoluminescence (PL) center with a characteristic zero-phonon line energy at 1.681 eV that acts as a solid-state single photon source and, potentially, as a quantum bit. The majority of the luminescence intensity appears in the zero-phonon line; nevertheless, about 30\% of the intensity manifests in the phonon sideband. Since phonons play an essential role in the operation of this system, it is of importance to understand the vibrational properties of the SiV center in detail. To this end, we carry out density functional theory calculations of dilute SiV centers by embedding the defect in supercells of a size of a few thousand atoms. We find that there exist two well-pronounced quasi-local vibrational modes (resonances) with $A_{2u}$ and $E_u$ symmetries, corresponding to the vibration of the Si atom along and perpendicular to the defect symmetry axis, respectively. Isotopic shifts of these modes explain the isotopic shifts of prominent vibronic features in the experimental SiV PL spectrum. Moreover, calculations show that the vibrational frequency of the $A_{2u}$ mode increases by about 30\% in the excited state with respect to the ground state, while the frequency of the $E_u$ mode increases by about 5\%. These changes explain experimentally observed isotopic shifts of the zero-phonon line energy. We also emphasize possible dangers of extracting isotopic shifts of vibrational resonances from finite-size supercell calculations, and instead propose a method to do this correctly.

quant-ph↗

Photoionization of negatively charged NV centers in diamond: theory and ab initio calculations

We present ab-initio calculations of photoionization thresholds and cross sections of the negatively charged nitrogen-vacancy (NV) center in diamond from the ground $^{3}\!A_2$ and the excited $^{3}\!E$ states. We show that after the ionization from the $^{3}\!E$ level the NV center transitions into the metastable $^{4}\!A_2$ electronic state of the neutral defect. We reveal how spin polarization of $\mathrm{NV}^{-}$ gives rise to spin polarization of the $^{4}\!A_2$ state, providing an explanation of electron spin resonance experiments. We obtain smooth photoionization cross sections by employing dense $k$-point meshes for the Brillouin zone integration together with the band unfolding technique to rectify the distortions of the band structure induced by artificial periodicity of the supercell approach. Our calculations provide a comprehensive picture of photoionization mechanisms of $\mathrm{NV}^{-}$. They will be useful in interpreting and designing experiments on charge-state dynamics at NV centers. In particular, we offer a consistent explanation of recent results of spin-to-charge conversion of NV centers.

cond-mat.mtrl-sci↗