Level Anticrossings Research Articles

Robust Nuclear Spin Polarization via Ground-State Level Anticrossing of Boron Vacancy Defects in Hexagonal Boron Nitride.

Nuclear spin polarization plays a crucial role in quantum information processing and quantum sensing. In this work, we demonstrate a robust and efficient method for nuclear spin polarization with boron vacancy (V_{B}^{-}) defects in hexagonal boron nitride (h-BN) using ground-state level anticrossing (GSLAC). We show that GSLAC-assisted nuclear polarization can be achieved with significantly lower laser power than excited-state level anticrossing, making the process experimentally more viable. Furthermore, we have demonstrated direct optical readout of nuclear spins for V_{B}^{-} in h-BN. Our findings suggest that GSLAC is a promising technique for the precise control and manipulation of nuclear spins in V_{B}^{-} defects in h-BN.

Anomalous variations of optical properties in the vicinity of level anti-crossing in InAs/GaAs conical quantum dot nanowire

The present study focuses on the investigation of the linear and nonlinear optical properties corresponding to electronic transitions in the vicinity of Level Anti-Crossing (LAC) points from a theoretical perspective. The system under consideration is an InAs conical quantum dot embedded in an infinite GaAs nanowire. The special configuration of the system leads to repeatedly LAC points in the energy spectrum of the system, three of which are considered here. The findings indicate a forward-backward shift in the energy location of the linear and non-linear Absorption Coefficient (AC) around the LAC. On the other hand, it is demonstrated that in this vicinity, AC for the transition to one of the crossing levels vanishes while that of the other maximizes. It is also found that, save for the lowest transition, the nonlinear component has essentially little share of the total AC, nearly for all incident photon energies, due to the limited and low values of the transition dipole moment.

Qudit-Based Spectroscopy for Measurement and Control of Nuclear-Spin Qubits in Silicon Carbide.

Nuclear spins with hyperfine coupling to single electron spins are highly valuable quantum bits. Here we probe and characterize the particularly rich nuclear-spin environment around single silicon vacancy color centers (V2) in 4H-SiC. By using the electron spin-3/2 qudit as a four level sensor, we identify several sets of ^{29}Si and ^{13}C nuclear spins through their hyperfine interaction. We extract the major components of their hyperfine coupling via optical detected nuclear magnetic resonance, and assign them to shells in the crystal via the density function theory simulations. We utilize the ground-state level anticrossing of the electron spin for dynamic nuclear polarization and achieve a nuclear-spin polarization of up to 98±6%. We show that this scheme can be used to detect the nuclear magnetic resonance signal of individual spins and demonstrate their coherent control. Our work provides a detailed set of parameters and first steps for future use of SiC as a multiqubit memory and quantum computing platform.

Fully Optical Scanning Spectroscopy of the Anticrossing of Electron and Nuclear Spin Levels in a 4H-SiC Crystal

Transitions in a system of interacting electron and nuclear spins in color centers with S = 3/2 in a 4H-SiC crystal with the natural isotopic composition have been detected by fully optical methods at room temperature. Giant changes in the photoluminescence in a volume of about 1 μm3 under cw and pulsed laser excitation occur in the region of the anticrossing of electron and nuclear spin levels. An optical manifestation of the flip of the nuclear spin of the 29Si isotope with the conservation of the projection of the electron spin has been detected. All anticrossing points of the spin sublevels coupled by hyperfine interactions have been identified. This identification enables the observation of such effects in the family of quarter spin centers in other SiC polytypes.

Excitation of long-lived nuclear spin order using spin-locking: a geometrical formalism.

Over the last two decades, numerous pulse sequences have been introduced for the excitation of long-lived spin order (LLS) in high fields. The long continuous wave (CW) or adiabatic pulses used in the SLIC and APSOC sequences should remind one of the spin-locking pulses that are used to induce cross-polarization (CP). Dynamics during these spin-lockings in CP experiments are explained through a geometrical formalism. However, the SLIC and APSOC sequences are described in terms of the energy-level picture or in the language of level anti-crossings. Motivated by this analogy, this work presents here a geometrical formalism for the LLS excitation by spin-locking pulses in weakly coupled systems. The formalism is similar to the one used for CP dynamics and reveals new pulse sequences involving CW or adiabatic locking. A similar formalism for the sustaining period of LLS is also provided, which reveals new features of the dynamics and suggests the usage of modulated spin-lockings for proper LLS sustaining. For strong and intermediate regimes, although a simple geometrical formalism seems infeasible, a new pulse sequence that employs a ramp-down adiabatic pulse for both LLS excitation and reconversion to observables in both these regimes is presented here. Given the similarities between LLS excitation and well-developed CP, it may be anticipated that this work would initiate the search for new LLS excitation methods and applications.

Nodes and Spin Windings for Topological Transitions in Light–Matter Interactions

AbstractThe anisotropic quantum Rabi model (QRM) is the fundamental model of light–matter interactions with indispensable counter‐rotating terms in ultra‐strong couplings. By extracting different levels of topological information a new light is shed on the energy spectrum of the anisotropic QRM. Besides conventional topological transitions (TTs) at gap closing, abundant unconventional TTs are unveiled underlying level anticrossings without gap closing by tracking the wave‐function nodes, including a particular unconventional TT which turns out to be universal for different energy levels. On the other hand, it is found that the nodes have a correspondence to spin windings, which not only endows the nodes a more explicit topological character in supporting single‐qubit TTs but also turns the topological information physically detectable. Furthermore, hidden small‐spin‐knot transitions are exposed for the ground state, while more kinds of spin‐knot transitions emerge in excited states including unmatched node numbers and spin winding numbers. Based on node sorting, algebraic formulation is established to decode the topological information encoded geometrically in the wave functions and spin windings.

Electron and nuclear magnetic properties near ZEFOZ region

In the vicinity of spin level anti-crossings, electron-nuclear spin systems reveal characteristic features that have been investigated by electron paramagnetic resonance (EPR) methods, including electron spin echo envelope modulation (ESEEM). The spectral properties depend considerably on the difference, ΔB, between the magnetic field and the critical field at which the zero first-order Zeeman shift (ZEFOZ) occurs. To analyze the characteristic features near the ZEFOZ point, analytical expressions for the behavior of EPR spectra and ESEEM traces as a function of ΔB are obtained. It is shown that the influence of hyperfine interactions (HFI) decreases linearly when approaching the ZEFOZ point. The HFI splitting of the EPR lines is essentially independent of ΔB near the ZEFOZ point, while the depth of the ESEEM signal has an approximately quadratic dependence on ΔB with a small cubic asymmetry due to the Zeeman interaction of the nuclear spin.

High-resolution spectroscopy of a single nitrogen-vacancy defect at zero magnetic field

We report a study of high-resolution microwave spectroscopy of nitrogen-vacancy (NV) centers in diamond crystals at and around zero magnetic field. We observe characteristic splitting and transition imbalance of the hyperfine transitions, which originate from level anti-crossings (LACs) in the presence of a transverse effective field. We use pulsed electron spin resonance spectroscopy to measure the zero-field spectral features of single NV centers for clearly resolving such LACs. To quantitatively analyze the magnetic resonance behavior of the hyperfine spin transitions in the presence of the effective field, we present a theoretical model, which describes the transition strengths under the action of an arbitrarily polarized microwave magnetic field. Our results are of importance for the optimization of the experimental conditions for the polarization-selective microwave excitation of spin-1 systems in zero or weak magnetic fields.

Adiabatic Passage through Level Anticrossings in Systems of Chemically Inequivalent Protons Incorporating Parahydrogen: Theory, Experiment, and Prospective Applications.

Level anticrossings (LACs) are ubiquitous in quantum systems and have been exploited for spin-order transfer in hyperpolarized nuclear magnetic resonance spectroscopy. This paper examines the manifestations of adiabatic passage through a specific type of LAC found in homonuclear systems of chemically inequivalent coupled protons incorporating parahydrogen (pH2). Adiabatic passage through such a LAC is shown to elicit translation of the pH2 spin order. As an example, with prospective applications in biomedicine, proton spin polarizations of at least 19.8 ± 2.6% on the methylene protons and 68.7 ± 0.5% on the vinylic protons of selectively deuterated allyl pyruvate ester are demonstrated experimentally. After ultrasonic spray injection of a precursor solution containing propargyl pyruvate and a dissolved Rh catalyst into a chamber pressurized with 99% para-enriched H2, the products are collected and transported to a high magnetic field for NMR detection. The LAC-mediated hyperpolarization of the methylene protons is significant because of the stronger spin coupling to the pyruvate carbonyl 13C, setting up an ideal initial condition for subsequent coherence transfer by selective INEPT. Furthermore, the selective deuteration of the propargyl side arm increases the efficiency and polarization level. LAC-mediated translation of parahydrogen spin order completes the first step toward a new and highly efficient route for the 13C NMR signal enhancement of pyruvate via side-arm hydrogenation with parahydrogen.

Splitting of Dirac Cones in HgTe Quantum Wells: Effects of Crystallographic Orientation, Interface-, Bulk-, and Structure-Inversion Asymmetry

We develop a microscopic theory of the fine structure of Dirac states in $(0lh)$-grown HgTe/CdHgTe quantum wells (QWs), where $l$ and $h$ are the Miller indices. It is shown that bulk, interface, and structure inversion asymmetry causes the anticrossing of levels even at zero in-plane wave vector and lifts the Dirac state degeneracy. In the QWs of critical thickness, the two-fold degenerate Dirac cone gets split into non-degenerate Weyl cones. The splitting and the Weyl point positions dramatically depend on the QW crystallographic orientation. We calculate the splitting parameters related to bulk, interface, and structure inversion asymmetry and derive the effective Hamiltonian of the Dirac states. Further, we obtain an analytical expression for the energy spectrum and discuss the spectrum for (001)-, (013)- and (011)-grown QWs.

Disorder and wave-function intermixing effects in the luminescence spectra of LiYF4:Ho in external magnetic fields

On the basis of the high-resolution low-temperature photoluminescence spectra of LiYF4:Ho crystals we discuss spectral manifestations of disorder caused by random distribution of either the lithium isotopes or defects in the crystal lattice. A peculiar discrete spectral structure of a different nature was found in the magnetic-field-dependent spectra. We show that it arises due to mixing of the wave functions at the anticrossings of hyperfine levels in a magnetic field.

Electrical-Readout Microwave-Free Sensing with Diamond

While nitrogen-vacancy ($\mathrm{N}$-${V}^{\ensuremath{-}}$) centers have been extensively investigated in the context of spin-based quantum technologies, the spin-state readout is conventionally performed optically, which may limit miniaturization and scalability. Here, we report photoelectric readout of ground-state cross-relaxation features, which serves as a method for measuring electron-spin resonance spectra of nanoscale electronic environments and also for microwave-free sensing. As a proof of concept, by systematically tuning N-$V$ centers into resonance with the target electronic system, we extract the spectra for the P1 electronic spin bath in diamond. Such detection may enable probing optically inactive defects and the dynamics of local spin environment. We also demonstrate a magnetometer based on photoelectric detection of the ground-state level anticrossings (GSLACs), which exhibits a favorable detection efficiency as well as magnetic sensitivity. This approach may offer potential solutions for determining spin densities and characterizing local environment.

Observation of the hyperfine structure and anticrossings of hyperfine levels in the luminescence spectra of LiYF4:Ho3+

Resolved hyperfine structure and narrow inhomogeneously broadened lines in the optical spectra of a rare-earth-doped crystal are favorable for the implementation of various sensors. Here, a well-resolved hyperfine structure in the photoluminescence spectra of LiYF4:Ho single crystals and the anticrossings of hyperfine levels in a magnetic field are demonstrated using a self-made setup based on a Bruker 125HR high-resolution Fourier spectrometer. This is the first observation of the resolved hyperfine structure and anticrossing hyperfine levels in the luminescence spectra of a crystal. The narrowest spectral linewidth is only 0.0022 cm−1. This fact together with a large value of the magnetic g factor of several crystal-field states creates prerequisites for developing magnetic field sensors, which can be in demand in modern quantum information technology devices operating at low temperatures. Very small random lattice strains characterizing the quality of a crystal can be detected using anticrossing points.

Excited-state spin-resonance spectroscopy of V{}_{{{{{{{{rm{B}}}}}}}}}^{-} defect centers in hexagonal boron nitride

The recently discovered spin-active boron vacancy (V{}_{{{{{{{{rm{B}}}}}}}}}^{-}) defect center in hexagonal boron nitride (hBN) has high contrast optically-detected magnetic resonance (ODMR) at room-temperature, with a spin-triplet ground-state that shows promise as a quantum sensor. Here we report temperature-dependent ODMR spectroscopy to probe spin within the orbital excited-state. Our experiments determine the excited-state spin Hamiltonian, including a room-temperature zero-field splitting of 2.1 GHz and a g-factor similar to that of the ground-state. We confirm that the resonance is associated with spin rotation in the excited-state using pulsed ODMR measurements, and we observe Zeeman-mediated level anti-crossings in both the orbital ground- and excited-state. Our observation of a single set of excited-state spin-triplet resonance from 10 to 300 K is suggestive of symmetry-lowering of the defect system from D3h to C2v. Additionally, the excited-state ODMR has strong temperature dependence of both contrast and transverse anisotropy splitting, enabling promising avenues for quantum sensing.

Excited-State Optically Detected Magnetic Resonance of Spin Defects in Hexagonal Boron Nitride.

Negatively charged boron vacancy (V_{B}^{-}) centers in hexagonal boron nitride (h-BN) are promising spin defects in a van der Waals crystal. Understanding the spin properties of the excited state (ES) is critical for realizing dynamic nuclear polarization. Here, we report zero-field splitting in the ES of D_{ES}=2160 MHz and its associated optically detected magnetic resonance (ODMR) contrast of 12% at cryogenic temperature. In contrast to nitrogen vacancy (NV^{-}) centers in diamond, the ODMR contrast of V_{B}^{-} centers is more prominent at cryotemperature than at room temperature. The ES has a g factor similar to the ground state. The ES photodynamics is further elucidated by measuring the level anticrossing of the V_{B}^{-} defects under varying external magnetic fields. Our results provide important information for utilizing the spin defects of h-BN in quantum technology.

Low-Temperature Photophysics of Single Nitrogen-Vacancy Centers in Diamond.

We investigate the magnetic field dependent photophysics of individual nitrogen-vacancy (NV) color centers in diamond under cryogenic conditions. At distinct magnetic fields, we observe significant reductions in the NV photoluminescence rate, which indicate a marked decrease in the optical readout efficiency of the NV's ground state spin. We assign these dips to excited state level anticrossings, which occur at magnetic fields that strongly depend on the effective, local strain environment of the NV center. Our results offer new insights into the structure of the NVs' excited states and a new tool for their effective characterization. Using this tool, we observe strong indications for strain-dependent variations of the NV's orbital g factor, obtain new insights into NV charge state dynamics, and draw important conclusions regarding the applicability of NV centers for low-temperature quantum sensing.

Atomic collapse in graphene quantum dots in a magnetic field

We investigate finite size and external magnetic field effects on the atomic collapse due to a Coulomb impurity placed at the center of a hexagonal graphene quantum dot within tight binding and mean-field Hubbard approaches. For large quantum dots, the atomic collapse effect persists when the magnetic field is present, characterized by a series of Landau level crossings and anticrossings, in agreement with previous bulk graphene results. However, we show that a new regime arises if the size of the quantum dot is comparable to or smaller than the magnetic length: While the lowest bound states cross the Fermi level at a lower value of coupling constant β<0.5 , a size independent critical coupling constant βc∗>0.5 emerges in the local density of states spectrum, which increases with the applied magnetic field. These effects are found to be persistent in the presence of electron–electron interactions within mean-field Hubbard approximation.

Improving SABRE hyperpolarization with highly nonintuitive pulse sequences: Moving beyond avoided crossings to describe dynamics.

Signal amplification by reversible exchange (SABRE) creates “hyperpolarization” (large spin magnetization) using a transition metal catalyst and parahydrogen, addressing the sensitivity limitations of magnetic resonance. SABRE and its heteronuclear variant X-SABRE are simple, fast, and general, but to date have not produced polarization levels as large as more established methods. We show here that the commonly used theoretical framework for these applications, which focuses on avoided crossings (also called level anticrossings or LACs), steer current SABRE and X-SABRE experiments away from optimal solutions. Accurate simulations show astonishingly rich and unexpected dynamics in SABRE/X-SABRE, which we explain with a combination of perturbation theory and average Hamiltonian approaches. This theoretical picture predicts simple pulse sequences with field values far from LACs (both instantaneously and on average) using different terms in the effective Hamiltonian to strategically control evolution and improve polarization transfer. Substantial signal enhancements under such highly nonintuitive conditions are verified experimentally.

Scanning Nuclear Spin Level Anticrossings by Constant-Adiabaticity Magnetic Field Sweeping of Parahydrogen-Induced 13C Polarization.

The polarization transfer between 1H protons and 13C heteronuclei is of central importance in the development of parahydrogen-based hyperpolarization techniques dedicated to the production of 13C-hyperpolarized molecular probes. Here we unveil the spin conversion efficiency in the polarization transfer between parahydrogen-derived protons and 13C nuclei of an ethyl acetate biomolecule, formed by the homogeneous hydrogenation of vinyl acetate with parahydrogen, obtained by applying constant-adiabaticity sweep profiles at ultralow magnetic fields. The experiments employed natural C-13 abundance. Spin level anticrossings can be detected experimentally using a scanning approach and are selected to improve the polarization transfer efficiency. 13C polarization of up to 12% is readily achieved on the carbonyl center. The results demonstrate the simplicity, reproducibility, and high conversion efficiency of the technique, opening the door for a refined manipulation of hyperpolarized spins in both basic science experiments (e.g., state-selected spectroscopy in the strong-coupling regime) and biomedical nuclear magnetic resonance applications.

Microwave-Free Dynamic Nuclear Polarization via Sudden Thermal Jumps.

Dynamic nuclear polarization (DNP) presently stands as the preferred strategy to enhance the sensitivity of nuclear magnetic resonance measurements, but its application relies on the use of high-frequency microwave to manipulate electron spins, an increasingly demanding task as the applied magnetic field grows. Here we investigate the dynamics of a system hosting a polarizing agent formed by two distinct paramagnetic centers near a level anticrossing. We theoretically show that nuclear spins polarize efficiently under a cyclic protocol that combines alternating thermal jumps and radio-frequency pulses connecting hybrid states with opposite nuclear and electronic spin alignment. Central to this process is the difference between the spin-lattice relaxation times of either electron spin species, transiently driving the electronic spin bath out of equilibrium after each thermal jump. Without the need for microwave excitation, this route to enhanced nuclear polarization may prove convenient, particularly if the polarizing agent is designed to feature electronic level anticrossings at high magnetic fields.