Level Anticrossings Research Articles

Magnetic field and angle-dependent photoluminescence of a fiber-coupled nitrogen vacancy rich diamond

Here, we investigate the magnetic field dependent photoluminescence (PL) of a fiber-coupled diamond single crystal with a high density of nitrogen vacancy (NV) centers. Angle-dependent magnetic field sweep measurements between 0 and 111 mT were performed using an oscillating illumination combined with lock-in techniques. Besides the expected superposed PL of differently oriented NV centers, a zoo of features in the PL are found. These features can be associated with level anti-crossings and cross relaxations. In particular, PL measurements allowed us to detect auto-cross relaxation between coupled NV centers. Moreover, the PL measurements at low magnetic fields show dips suggesting an interaction of NV centers with additional spin defects. The results presented here are not only a study for NV-based fiber-coupled sensors made of diamond, but also show a way to investigate with manageable effort and purely an optical multispin interaction with at least one NV center as a constituent.

Low-field microwave-mediated optical hyperpolarization in optically pumped diamond

The emergence of a new class of optically polarizable electronic spins in diamond, nitrogen vacancy (NV) defect centers, has opened interesting new avenues for dynamic nuclear polarization. Here we review methods for the room-temperature hyperpolarization of lattice 13C nuclei using optically pumped NV centers, focusing particular attention to a polarization transfer via rotating-frame level anti-crossings. We describe special features of this optical dynamic nuclear polarization (DNP) mechanism at low-field, in particular, its deployability to randomly oriented diamond nanoparticles. In addition, we detail methods for indirectly obtaining high-resolution NV ESR spectra via hyperpolarization readout. These mechanistic features provide perspectives for interesting new applications exploiting the optically generated 13C hyperpolarization.

Ultra-wide frequency tuning range for optical properties in coaxial quantum well driven by intense laser field

A new approach for controlling intersubband transitions and optical properties of coaxial cylindrical quantum well is proposed. Considering the correct dressing effect for the confinement potential, the new ultra-wide tuning mechanism is based on the variation of quasibound states with the intensity of long-wavelength laser field. By means of the finite difference method, the results provide a new explanation for the anticrossing of energy levels and exhibit great potential for ultra-wide frequency tunability (ranging from terahertz to the mid-infrared region) of the optical absorption coefficient and refractive index changes by modulating the laser parameters and barrier thickness.

Chemically Induced Spin Hyperpolarization: Coherence Formation in Reaction Products

Chemically induced dynamic nuclear polarization (CIDNP) has emerged as a highly informative method to study spin-dependent radical reactions by analyzing enhanced NMR (nuclear magnetic resonance) signals of their diamagnetic reaction products. In this way, one can probe the structure of elusive radical intermediates and determine their magnetic parameters. A careful examination of experimental CIDNP data at variable magnetic fields shows that formation of hyperpolarized molecules in a coherent state is a ubiquitous though rarely discussed phenomenon. The presence of nuclear spin coherences commonly leads to subsequent polarization transfer among coupled spins in the diamagnetic products of radical recombination reaction that must be taken into account when analyzing the results of CIDNP experiments at low magnetic field. Moreover, such coherent polarization transfer can be efficiently exploited to polarize spins, which do not acquire CIDNP directly. Here we explain under what conditions such coherences can be generated, focusing on the key role of level anti-crossings in coherent polarization transfer, and provide experimental approaches to probing nuclear spin coherences and their time evolution. We illustrate the theoretical consideration of the outlined coherent spin phenomena in CIDNP by examples, obtained for the dipeptide tryptophan–tryptophan.

15 N SABRE Hyperpolarization of Metronidazole at Natural Isotope Abundance.

Signal Amplification By Reversible Exchange (SABRE) is gaining increased attention as a tool to enhance weak Nuclear Magnetic Resonance (NMR) signals. In SABRE, spin order is transferred from parahydrogen (H2 in its nuclear singlet spin state) to a substrate molecule in a transient Ir-based complex. In recent years, SABRE polarization of biologically active substrates has been demonstrated, notably of metronidazole - an antibiotic and antiprotozoal drug. In this work, we study 15 N SABRE polarization of metronidazole at natural isotope abundance. We are able to demonstrate significant 15 N polarization reaching 15 %, which corresponds to a signal enhancement of 46,000 at 9.4 T for the nitrogen atom with lone electron pair. Additionally, the other two N-atoms can be polarized, although less efficiently. We present a detailed study of the field dependence of polarization and explain the maxima in the field dependence using the concept of coherent polarization transfer at level anti-crossings in the SABRE complex. A study of spin relaxation phenomena presented here enables optimization of the magnetic field for efficient storage of non-thermal polarization.

Initializing 214 Pure 14-Qubit Entangled Nuclear Spin States in a Hyperpolarized Molecular Solid.

Quantum entanglement has been realized on a variety of physical platforms such as quantum dots, trapped atomic ions, and superconductors. Here we introduce specific molecular solids as promising alternative platforms. Our model system is triplet pentacene in a host single crystal at level anticrossing (LAC) conditions. First, a laser pulse generates the triplet state and initiates entanglement between an electron spin and 14 hyperfine coupled proton spins (quantum bits or qubits). This gives rise to large nuclear spin polarization. Subsequently, a resonant high-power microwave (mw) pulse disentangles the electron spin from the nuclear spins. Simultaneously, high-dimensional multiqubit entanglement is formed among the proton spins. We verified the initialization of 214 pure 14-qubit entangled nuclear spin states with an average degree of entanglement of Eav = 0.77 ± 0.03. These results pave the way for large-scale quantum information processing with more than 10 000 multiqubit entangled states corresponding to computational (Hilbert) space dimensions of dim >1053.

Photoluminescence at the ground-state level anticrossing of the nitrogen-vacancy center in diamond: A comprehensive study

The nitrogen-vacancy center (NV center) in diamond at magnetic fields corresponding to the ground state level anticrossing (GSLAC) region gives rise to rich photoluminescence (PL) signals due to the vanishing energy gap between the electron spin states, which enables to have an effect on the NV center's luminescence for a broad variety of environmental couplings. In this article we report on the GSLAC photoluminescence signature of NV ensembles in different spin environments at various external fields. We investigate the effects of transverse electric and magnetic fields, P1 centers, NV centers, and the $^{13}$C nuclear spins, each of which gives rise to a unique PL signature at the GSLAC. The comprehensive analysis of the couplings and related optical signal at the GSLAC provides a solid ground for advancing various microwave-free applications at the GSLAC, including but not limited to magnetometry, spectroscopy, dynamic nuclear polarization (DNP), and nuclear magnetic resonance (NMR) detection. We demonstrate that not only the most abundant $^{14}$NV center but the $^{15}$NV can also be utilized in such applications and that nuclear spins coupled to P1 centers can be polarized directly by the NV center at the GSLAC, through a giant effective nuclear $g$-factor arising from the NV center-P1 center-nuclear spin coupling. We report on new alternative for measuring defect concentration in the vicinity of NV centers and on the optical signatures of interacting, mutually aligned NV centers.

Электронные состояния и персистентные токи в кольцах с неоднородным спин-орбитальным взаимодействием Рашбы

The paper considers one-dimensional isolated quantum rings in a perpendicular magnetic field, in which Rashba spin-orbit coupling parameter changes along the ring. Electronic spectra and persistent currents of such ring structures are calculated for different values of the structure parameters and the magnitude of the magnetic flux. It is shown that the inhomogeneity of the Rashba parameter leads to anticrossing of energy levels and smoothing of the dependence of the persistent charge current on the flux. The influence of inhomogeneity on the spin persistent current turns out to be more significant: the projection of the spin current on the ring axis ceases to be preserved when moving along the ring; additional extrema or zeros appear on the dependence of the absolute value of the spin current on the magnetic flux for a given number of electrons in the ring.

Chemical tuning of spin clock transitions in molecular monomers based on nuclear spin-free Ni(ii).

We report the existence of a sizeable quantum tunnelling splitting between the two lowest electronic spin levels of mononuclear Ni complexes. The level anti-crossing, or magnetic “clock transition”, associated with this gap has been directly monitored by heat capacity experiments. The comparison of these results with those obtained for a Co derivative, for which tunnelling is forbidden by symmetry, shows that the clock transition leads to an effective suppression of intermolecular spin–spin interactions. In addition, we show that the quantum tunnelling splitting admits a chemical tuning via the modification of the ligand shell that determines the crystal field and the magnetic anisotropy. These properties are crucial to realize model spin qubits that combine the necessary resilience against decoherence, a proper interfacing with other qubits and with the control circuitry and the ability to initialize them by cooling.

Representation of population exchange at level anti-crossings.

A theoretical framework is proposed to describe the spin dynamics driven by coherent spin mixing at level anti-crossings (LACs). We briefly introduce the LAC concept and propose to describe the spin dynamics using a vector of populations of the diabatic eigenstates. In this description, each LAC gives rise to a pairwise redistribution of eigenstate populations, allowing one to construct the total evolution operator of the spin system. Additionally, we take into account that in the course of spin evolution a "rotation" of the eigenstate basis case take place. The approach is illustrated by a number of examples, dealing with magnetic field inversion, cross-polarization, singlet-state nuclear magnetic resonance and parahydrogen-induced polarization.

High-Temperature Spin Manipulation on Color Centers in Rhombic Silicon Carbide Polytype 21R-SiC

A family of atomic-scale color centers, the spin state of which can be controlled via optical and microwave channels, has been found in the rhombic polytype of silicon carbide 21R-SiC considered as a natural superlattice. Zero-phonon lines are observed in photoluminescence corresponding to spin-3/2 centers, which differ in fine structure splitting in the ground and excited states. Giant changes in the photoluminescence intensity under conditions of magnetic resonance and anticrossing of the spin levels of the ground and excited states are demonstrated, which open up possibilities for applications in magnetometry, thermometry, and quantum computing.

Level anti-crossings of a nitrogen-vacancy center in diamond: decoherence-free subspaces and 3D sensors of microwave magnetic fields

Nitrogen-vacancy (NV) centers in diamond have become an important tool for quantum technologies. All of these applications rely on long coherence times of electron and nuclear spins associated with these centers. Here, we study the energy level anti-crossings of an NV center in diamond coupled to a first-shell 13C nuclear spin in a small static magnetic field. These level anti-crossings (LACs) occur for specific orientations of the static magnetic field due to the strong non-secular components of the Hamiltonian. At these orientations we observe decoherence-free subspaces, where the electron spin coherence times () are 5–7 times longer than those at other orientations. Another interesting property at these LACs is that individual transition amplitudes are dominated by a single component of the magnetic dipole moment. Accordingly, this can be used for vector detection of microwave magnetic fields with a single NV center. This is particularly important to precisely control the center using numerical optimal control techniques.

Dual-frequency spin-resonance spectroscopy of diamond nitrogen-vacancy centers in zero magnetic field

The methods for controlling spin states of negatively charged nitrogen-vacancy (NV) centers using microwave (MW) or radiofrequency (RF) excitation fields for electron spin and nuclear spin transitions are effective in strong magnetic fields where a level anti-crossing (LAC) occurs. A LAC can also occur at zero field in the presence of transverse strain or electric fields in the diamond crystal, leading to mixing of the spin states. In this paper, we investigate zero-field LAC of NV centers using dual-frequency excitation spectroscopy. Under RF modulation of the spin states, we observe sideband transitions and Autler-Townes splitting in the optically detected magnetic resonance (ODMR) spectra. Numerical simulations show that the splitting originates from Landau-Zener transition between electron spin |$\pm$1> states, which potentially provides a new way of manipulating NV center spin states in zero or weak magnetic field.

Direct observation of hyperfine level anticrossings in the optical spectra of a LiYF47:Ho3+ single crystal

We have investigated the hyperfine structure in high-resolution broadband optical absorption spectra of a strongly diluted paramagnet $^{7}\mathrm{LiYF}_{4}:{\mathrm{Ho}}^{3+}$ (0.1 at. %) in external magnetic fields parallel to the tetragonal symmetry axis of the crystal. Anticrossings in the hyperfine spectral pattern were observed. It is the first direct observation of the hyperfine level anticrossings in optical spectra. Analysis of the spectral envelopes corresponding to transitions between the electron-nuclear sublevels of crystal-field non-Kramers doublets and singlets of the ${\mathrm{Ho}}^{3+}$ ions, based on the microscopic model of the electronic $4{f}^{10}$ configuration, allowed us to retrieve information on the hyperfine structure of electronic singlets, nuclear quadroupole interactions, and random lattice strains.

Magnetic field dependence of triplet-state ONP: theoretical analysis in terms of level anti-crossings

ABSTRACTA theoretical approach to Optical Nuclear Polarisation (ONP) is described, which is based on the analysis of Level Anti-Crossings (LACs) in triplet states. Here we consider ONP formed in molecular crystals doped with suitable guest molecules and ONP generated in diamond crystals containing negatively charged nitrogen-vacancy (NV–) centres. In both cases, electron spin polarisation of triplet states generated by light excitation is transferred to nuclei giving rise to ONP. Polarisation transfer is most efficient at LACs; for this reason, we consider in detail crossings of electron–nuclear energy levels and the role of different perturbation terms (coming from isotropic and anisotropic hyperfine coupling, zero-field splitting and sample orientation), which turn these crossings into LACs and give rise to ONP. Analytical results are supported by numerical calculations of the ONP field dependences. Thus, the outlined LAC analysis is a useful approach for interpreting the ONP magnetic field dependence.

Optimal control of universal quantum gates in a double quantum dot

We theoretically investigate electron spin operations driven by applied electric fields in a semiconductor double quantum dot (DQD). Our model describes a DQD formed in semiconductor nanowire with longitudinal potential modulated by local gating. The eigenstates for two electron occupation, including spin-orbit interaction, are calculated and then used to construct a model for the charge transport cycle in the DQD taking into account the spatial dependence and spin mixing of states. The dynamics of the system is simulated aiming at implementing protocols for qubit operations, that is, controlled transitions between the singlet and triplet states. In order to obtain fast spin manipulation, the dynamics is carried out taking advantage of the anticrossings of energy levels introduced by the spin-orbit and interdot couplings. The theory of optimal quantum control is invoked to find the specific electric-field driving that performs qubit logical operations. We demonstrate that it is possible to perform within high efficiency a universal set of quantum gates $\{$CNOT, H$\otimes$I, I$\otimes$H, T$\otimes$I, and T$\otimes$I$\}$, where H is the Hadamard gate, T is the $\pi/8$ gate, and I is the identity, even in the presence of a fast charge transport cycle and charge noise effects.

Complete magnetic field dependence of SABRE-derived polarization.

Signal amplification by reversible exchange (SABRE) is a promising hyperpolarization technique, which makes use of spin-order transfer from parahydrogen (the H2 molecule in its singlet spin state) to a to-be-polarized substrate in a transient organometallic complex, termed the SABRE complex. In this work, we present an experimental method for measuring the magnetic field dependence of the SABRE effect over an ultrawide field range, namely, from 10nT to 10T. This approach gives a way to determine the complete magnetic field dependence of SABRE-derived polarization. Here, we focus on SABRE polarization of spin-1/2 hetero-nuclei, such as 13 C and 15 N and measure their polarization in the entire accessible field range; experimental studies are supported by calculations of polarization. Features of the field dependence of polarization can be attributed to level anticrossings in the spin system of the SABRE complex. Features at magnetic fields of the order of 100nT-1μT correspond to "strong coupling" of protons and hetero-nuclei, whereas features found in the mT field range stem from "strong coupling" of the proton system. Our approach gives a way to measuring and analyzing the complete SABRE field dependence, to probing NMR parameters of SABRE complexes and to optimizing the polarization value.

Spin and Optical Properties of Silicon Vacancies in Silicon Carbide − A Review (Phys. Status Solidi B 1/2018)

Atomic-scale defects in silicon carbide, a widely used material in semiconductor industry, reveal high potential for quantum technologies. Spin-3/2 color centers associated with silicon vacancies are of particular interest for fundamental research and applications in sensorics and spintronics. Such centers are characterized by spin-dependent optical cycles: their spin states can be selectively initialized and read-out by optical means and efficiently manipulated by a radiofrequency field. Here, Tarasenko et al. (article no. 1700258) review the fine structure, spin dynamics, and optical properties of the silicon vacancies. The fine structure of the centers turns out to be highly sensitive to mechanical pressure, external magnetic and electric fields, temperature variation, etc., which can be utilized for efficient environment sensing at ambient conditions. Tarasenko et al. discuss the experimental achievements in magnetometry and thermometry based on the spin state mixing at level anticrossings in an external magnetic field and the underlying microscopic mechanisms. The authors also discuss the spin fluctuations in an ensemble of vacancies paving the way for weakly invasive quantum sensing protocols.

Tuning nuclear depolarization under MAS by electron T1e.

The Cross-Effect (CE) Dynamic Nuclear Polarization (DNP) mechanism under Magic Angle Spinning (MAS) induces depletion or "depolarization" of the NMR signal, in the absence of microwave irradiation. In this study, the role of T1e on nuclear depolarization under MAS was tested experimentally by systematically varying the local and global electron spin concentration using mono-, bi- and tri-radicals. These spin systems show different depolarization effects that systematically tracked with their different T1e rates, consistent with theoretical predictions. In order to test whether the effect of T1e is directly or indirectly convoluted with other spin parameters, the tri-radical system was doped with different concentrations of GdCl3, only tuning the T1e rates, while keeping other parameters unchanged. Gratifyingly, the changes in the depolarization factor tracked the changes in the T1e rates. The experimental results are corroborated by quantum mechanics based numerical simulations which recapitulated the critical role of T1e. Simulations showed that the relative orientation of the two g-tensors and e-e dipolar interaction tensors of the CE fulfilling spin pair also plays a major role in determining the extent of depolarization, besides the enhancement. This is expected as orientations influence the efficiency of the various level anti-crossings or the "rotor events" under MAS. However, experimental evaluation of the empirical spectral diffusion parameter at static condition showed that the local vs. global e-e dipolar interaction network is not a significant variable in the commonly used nitroxide radical system studied here, leaving T1e rates as the major modulator of depolarization.

Optically induced cross relaxation via nitrogen-related defects for bulk diamond C13 hyperpolarization

In this Rapid Communication we utilize nuclear magnetic resonance to investigate the hyperpolarization effect of negatively charged nitrogen vacancy (NV) centers on bulk $^{13}\mathrm{C}$ nuclei in a diamond single crystal. We were able to identify several polarization peaks of a different sign at different magnetic fields in a region of some tens of Gauss centered around $50\phantom{\rule{0.28em}{0ex}}\mathrm{mT}$. The bulk $^{13}\mathrm{C}$ hyperpolarization in the investigated field range is usually attributed to the excited state level anticrossing of the NV center. However, we found that this bulk hyperpolarization is caused by optically induced cross relaxation and that it takes place in the NV center ground state. The four-spin coupling between the polarized NV electron spin, the electron spin of a substitutional nitrogen impurity (P1), as well as its $^{14}\mathrm{N}$ nuclei and the $^{13}\mathrm{C}$ nuclear spin have to be considered. We introduce a simple theoretical model which completely fits with the experimental data and which clearly shows that the P1 centers are involved in the polarization process. We expect that the current work has a significant impact on future NV-based polarization applications.