Electron Spin System Research Articles

In-depth conversion of entangled states for electron-spin systems with error-avoiding parity-check gates

In-depth conversion of entangled states for electron-spin systems with error-avoiding parity-check gates

Dipolar Order Induced Electron Spin Hyperpolarization.

The structure of coupled electron spin systems is of fundamental interest to many applications, including dynamic nuclear polarization (DNP), enhanced nuclear magnetic resonance (NMR), the generation of electron spin qubits for quantum information science (QIS), and quantitative studies of paramagnetic systems by electron paramagnetic resonance (EPR). However, the characterization of electron spin coupling networks is nontrivial, especially at high magnetic fields. This study focuses on a system containing high concentrations of trityl radicals that give rise to a DNP enhancement profile of 1H NMR characteristic of the presence of electron spin clusters. When this system is subject to selective microwave saturation through pump-probe ELectron DOuble Resonance (ELDOR) experiments, electron spin hyperpolarization is observed. We show that the generation of an out-of-equilibrium longitudinal dipolar order is responsible for the transient hyperpolarization of electron spins. Notably, the coupled electron spin system needs to form an AX-like system (where the difference in the Zeeman interactions of two spins is larger than their coupling interaction) such that selective microwave irradiation can generate signatures of electron spin hyperpolarization. We show that the extent of dipolar order, as manifested in the extent of electron spin hyperpolarization generated, can be altered by tuning the pump or probe pulse length, or the interpulse delay in ELDOR experiments that change the efficiency to generate or readout longitudinal dipolar order. Pump-probe ELDOR with selective saturation is an effective means for characterizing coupled electron spins forming AX-type spin systems that are foundational for DNP and quantum sensing.

Photonic Spin Hopfions and Monopole Loops.

Spin textures with various topological orders are of great theoretical and practical interest. Hopfion, a spin texture characterized by a three-dimensional topological order was recently realized in electronic spin systems. Here, we show that monochromatic light can be structured such that its photonic spin exhibits a hopfion texture in the three-dimensional real space. We also provide ways to construct spin textures of arbitrary Hopf charges. When extending the system to four dimensions by introducing a parameter dimension, a new type of topological defect in the form of a monopole loop in photonic spin is encountered. Each point on the loop is a topological spin defect in three dimensions, and the loop itself carries quantized Hopf charges. Such photonic spin texture and defect may find application in control and sensing of nanoparticles, and optical generation of topological texture in motions of particles or fluids.

Multiple electron spin resonance echoes observed for paramagnetic defects in diamond at room temperature

Magnetic resonance offers an invaluable testbed for observing and studying the fundamental concepts of quantum cavity interactions with two-level systems in the microwave regime. Typically, these experiments are conducted at low cryogenic temperatures, utilizing spin systems embedded within a high-quality (Q-factor) superconducting cavity. Recent studies indicate that under these conditions, especially in a high-cooperativity regime with strong collective coupling between an electron spin system and a microwave cavity, multiple spin echoes can be detected. These echoes are interpreted as manifestations of coherent quantum effects. To put it simply, photons within the cavity can excite the spin system, which subsequently can stimulate the cavity, creating a feedback loop. In our research, we demonstrate that a specially designed moderate-Q cavity, paired with diamond crystals rich in nitrogen vacancy (NV) centers, allows us to observe such nonlinear quantum phenomena, even at ambient temperatures. Crucially, our experimental design necessitates amplifying the net number of spins for a specific, limited spin concentration. This is achieved by lowering the spins' thermodynamic temperature (as opposed to their physical temperature) to a few kelvins. Notably, we find that maintaining high cooperativity or strong coupling is not essential for these observations. The potential to observe significant microwave cavity quantum effects at room temperature could be useful for future applications, such as quantum memories and quantum sensing.

Probing the Interaction of NO with C60: Comparison between Endohedral and Exohedral Complexes

Recent advances in synthetic methodologies have opened new strategies for synthesizing stable metal-free electron spin systems based on fullerenes. Introducing nitric oxide (NO) inside a fullerene cage is one of the methods to attain this goal. In the present study, dispersion corrected density functional theory (B3LYP-D3) has been used to evaluate the structure, stability, and electronic properties of NO encapsulated fullerene NO@C60 and compared those with its exohedral fullerene NO.C60 analog. The calculated stabilization energy for NO@C60 is appreciably higher than NO.C60, and this difference is comprehended via the Quantum theory of atoms in molecules (QTAIM) and noncovalent interaction (NCI) topological analyses. The delocalization of electron density of NO and the C60 cage in NO@C60 is discussed using electrostatic potential analysis. In addition, an attempt has been made to understand the different locations and orientations involving the interaction of two NO radicals and the fullerene C60. It is shown that the encapsulation of the NO dimer inside the C60 cage is an energetically unfavorable process. On the other hand, stable structures are obtained upon the physisorption of other NO on the surface of NO@C60 and NO.C60. The present work provides an in-depth understanding of the interaction of NO and C60 fullerene, its preferable position, and its orientation in both endohedral and exohedral complexes.

Enhanced quantum sensing with room-temperature solid-state masers.

Quantum sensing with solid-state electron spin systems finds broad applications in diverse areas ranging from material and biomedical sciences to fundamental physics. Exploiting collective behavior of noninteracting spins holds the promise of pushing the detection limit to even lower levels, while to date, those levels are scarcely reached because of the broadened linewidth and inefficient readout of solid-state spin ensembles. Here, we experimentally demonstrate that such drawbacks can be overcome by a reborn maser technology at room temperature in the solid state. Owing to maser action, we observe a fourfold reduction in the electron paramagnetic resonance linewidth of an inhomogeneously broadened molecular spin ensemble, which is narrower than the same measured from single spins at cryogenic temperatures. The maser-based readout applied to near zero-field magnetometry showcases the measurement signal-to-noise ratio of 133 for single shots. This technique would be an important addition to the toolbox for boosting the sensitivity of solid-state ensemble spin sensors.

Multicore Quantum Computing

Any architecture for practical quantum computing must be scalable. An attractive approach is to create multiple cores, computing regions of fixed size that are well-spaced but interlinked with communication channels. This exploded architecture can relax the demands associated with a single monolithic device: the complexity of control, cooling and power infrastructure as well as the difficulties of cross-talk suppression and near-perfect component yield. Here we explore interlinked multicore architectures through analytic and numerical modelling. While elements of our analysis are relevant to diverse platforms, our focus is on semiconductor electron spin systems in which numerous cores may exist on a single chip. We model shuttling and microwave-based interlinks and estimate the achievable fidelities, finding values that are encouraging but markedly inferior to intra-core operations. We therefore introduce optimsed entanglement purification to enable high-fidelity communication, finding that $99.5\%$ is a very realistic goal. We then assess the prospects for quantum advantage using such devices in the NISQ-era and beyond: we simulate recently proposed exponentially-powerful error mitigation schemes in the multicore environment and conclude that these techniques impressively suppress imperfections in both the inter- and intra-core operations.

Coherent dynamics of multi-spin V{}_{{{{{{{{rm{B}}}}}}}}}^{-} center in hexagonal boron nitride

Hexagonal boron nitride (hBN) has recently been demonstrated to contain optically polarized and detected electron spins that can be utilized for implementing qubits and quantum sensors in nanolayered-devices. Understanding the coherent dynamics of microwave driven spins in hBN is of crucial importance for advancing these emerging new technologies. Here, we demonstrate and study the Rabi oscillation and related phenomena of a negatively charged boron vacancy (V{}_{{{{{{{{rm{B}}}}}}}}}^{-}) spin ensemble in hBN. We report on different dynamics of the V{}_{{{{{{{{rm{B}}}}}}}}}^{-} spins at weak and strong magnetic fields. In the former case the defect behaves like a single electron spin system, while in the latter case it behaves like a multi-spin system exhibiting multiple-frequency dynamical oscillation as beat in the Ramsey fringes. We also carry out theoretical simulations for the spin dynamics of V{}_{{{{{{{{rm{B}}}}}}}}}^{-} and reveal that the nuclear spins can be driven via the strong electron nuclear coupling existing in V{}_{{{{{{{{rm{B}}}}}}}}}^{-} center, which can be modulated by the magnetic field and microwave field.

Light and spins in rare-earth doped garnets

Spin-dependent optical properties of garnet crystals and garnet based ceramics, doped with cerium and also, along with cerium, co-doped with gadolinium and/or terbium, were studied by the method of optically detected of magnetic resonance by monitoring luminescence. The intensity of photoluminescence excited by circularly polarized light in the absorption bands of Ce3+ proved to be useful for selective monitoring of the population of the spin sublevels of the Ce3+ ground state. It was shown that due to cross-relaxation between the cerium and gadolinium electron spin systems the intensity of Ce3+ emission can be used to detect magnetic resonance of Gd3+. High-frequency EPR allowed finding a family of non-Kramers Tb3+ centers in yttrium aluminum garnet crystals. The influence of the magnetic resonance of Tb3+ on the luminescence of Ce3+ was observed. This suggests a coupling between the Tb3+ and Ce3+ systems, which are promising for coherent information processing. In irradiated crystals and ceramics of cerium-doped gadolinium-gallium garnet, magnetic field stimulation of the recombination of radiation defects was found, that is, it was shown that the energy accumulated during irradiation can be released in an external magnetic field. A huge increase in the afterglow intensity in a magnetic field and magnetic memory effects of magnetic memory were explained by the influence of strong internal magnetic fields on spin-dependent recombination.

Implementation of Quantum Level Addressability and Geometric Phase Manipulation in Aligned Endohedral Fullerene Qudits.

Endohedral nitrogen fullerenes have been proposed as building blocks for quantum information processing due to their long spin coherence time. However, addressability of the individual electron spin levels in such a multiplet system of 4 S3/2 has never been achieved because of the molecular isotropy and transition degeneracy among the Zeeman levels. Herein, by molecular engineering, we lifted the degeneracy by zero-field splitting effects and made the multiple transitions addressable by a liquid-crystal-assisted method. The endohedral nitrogen fullerene derivatives with rigid addends of spiro structure and large aspect ratios of regioselective bis-addition improve the ordering of the spin ensemble. These samples empower endohedral-fullerene-based qudits, in which the transitions between the 4 electron spin levels were respectively addressed and coherently manipulated. The quantum geometric phase manipulation, which has long been proposed for the advantages in error tolerance and gating speed, was implemented in a pure electron spin system using molecules for the first time.

Implementation of Quantum Level Addressability and Geometric Phase Manipulation in Aligned Endohedral Fullerene Qudits

AbstractEndohedral nitrogen fullerenes have been proposed as building blocks for quantum information processing due to their long spin coherence time. However, addressability of the individual electron spin levels in such a multiplet system of 4S3/2 has never been achieved because of the molecular isotropy and transition degeneracy among the Zeeman levels. Herein, by molecular engineering, we lifted the degeneracy by zero‐field splitting effects and made the multiple transitions addressable by a liquid‐crystal‐assisted method. The endohedral nitrogen fullerene derivatives with rigid addends of spiro structure and large aspect ratios of regioselective bis‐addition improve the ordering of the spin ensemble. These samples empower endohedral‐fullerene‐based qudits, in which the transitions between the 4 electron spin levels were respectively addressed and coherently manipulated. The quantum geometric phase manipulation, which has long been proposed for the advantages in error tolerance and gating speed, was implemented in a pure electron spin system using molecules for the first time.

Analysis of the Coupled Electron and Nuclear Spin Systems from Optically Induced Dynamic Nuclear Polarization in GaAs

Analysis of the Coupled Electron and Nuclear Spin Systems from Optically Induced Dynamic Nuclear Polarization in GaAs

S = 1 antiferromagnetic electron-spin systems on hydrogenated phenalenyl-tessellation molecules for material-based quantum-computation resources

A resource state for measurement-based quantum computation is proposed using a material design of S = 1 antiferromagnetic spin chains. Specifying hydrogen adsorption positions on polymerized phenalenyl-tessellation molecules gives rise to formation of graphene zero modes that produce local S = 1 spins or S = 1/2 spins in the required order through exchange interactions. When the S = 1 antiferromagnetic Heisenberg models serve as quantum-computation resources, hydrogen adatoms inducing zero modes can also work as local electron-spin probes in nuclear spin spectroscopy, which could be used for controlling and measuring local spins.

Phonon-induced decoherence of a spin based qubit made with asymmetric coupled quantum dots

A semiconductor heterostructure made with two asymmetric coupled self-assembled quantum dots (ACSAQDs) has been studied. Such a structure can serve as a spin based quantum dot qubit which is an important manufacture for quantum communication and quantum information processing . The shape of the confinement potential, the used semiconductor materials and the size of the investigated quantum dots have been chosen to be comparable to the fabricated and the experimentally studied quantum dots. The spin-flip decoherence and more specifically the effects associated with acoustic phonons have been researched. A rather sophisticated theoretical model (8-band strain dependent k ⋅ p theory) has been employed to evaluate the carrier eigenfunctions and eigenvalues within the quantum dots. Using the Fermis golden rule, the spin-flip relaxation time ( T 1 ) due to phonon coupling to electrons has been evaluated. The volume of the quantum dots is a parameter of crucial importance for controlling the spin-flip relaxation mechanism. Moreover, other parameters like the space between the coupled quantum dots, the lattice temperature and the presence of an external applied magnetic field (along the quantum dots growth direction) have considerable effects on the spin-flip relaxation time. • In this paper, a heterostructure made of two asymmetric coupledquantum dots and which can be implemented as quantum logic gate has been studied. • The qubit is manipulated by controlling the two-level electron spin systems. • The electron-spin eigenfunctions and eigenvalues have been calculated by using the 8-band strain dependent k . p theory. • The dependence of the electron energy on the quantum structure geometry and the existence of an applied magnetic field was highlighted. • The evaluation of spin-flip time T 1 via the emission of acoustic phonons showed that T 1 strongly depends on the size and on the relative volume of the dots under certain circumstances (geometry and small magnetic field).

Simulating the Palmer-Chalker state in an orbital superfluid

We consider a bosonic $s$ and $p$ orbital system in a face-centered cubic (FCC) optical lattice, and predict a fluctuation-induced instability towards the orbital analogue of Palmer-Chalker state, which is originally proposed in an electronic spin system. For bosons loaded in the FCC optical lattice, the single-particle spectrum has four degenerate band minima with their crystal momenta forming a tetrahedron in Brillouin zone. In the weakly interacting regime, the ensuing many-particle ground state, at the classical level, underlies a four-sublattice tetrahedral supercell of spontaneously generated $p$-orbital angular momenta through the Bravias-Bloch duality between real and momentum space, and is macroscopically degenerate originating from the geometric frustration. The fluctuations on top of the classical ground state lift its degeneracy and select the Palmer-Chalker ordering of $p$-orbital angular momenta as the quantum ground state through order-by-disorder mechanism. These findings raise the exciting possibility of simulating the Palmer-Chalker state with its orbital counterpart in ultracold atomic gases.

Observation of a Quantum Phase from Classical Rotation of a Single Spin.

The theory of angular momentum connects physical rotations and quantum spins together at a fundamental level. Physical rotation of a quantum system will therefore affect fundamental quantum operations, such as spin rotations in projective Hilbert space, but these effects are subtle and experimentally challenging to observe due to the fragility of quantum coherence. We report on a measurement of a single-electron-spin phase shift arising directly from physical rotation, without transduction through magnetic fields or ancillary spins. This phase shift is observed by measuring the phase difference between a microwave driving field and a rotating two-level electron spin system, and it can accumulate nonlinearly in time. We detect the nonlinear phase using spin-echo interferometry of a single nitrogen-vacancy qubit in a diamond rotating at 200 000rpm. Our measurements demonstrate the fundamental connections between spin, physical rotation, and quantum phase, and they will be applicable in schemes where the rotational degree of freedom of a quantum system is not fixed, such as spin-based rotation sensors and trapped nanoparticles containing spins.

Spin coherence and optical properties of alkali-metal atoms in solid parahydrogen

We present a joint experimental and theoretical study of spin coherence properties of 39K, 85Rb, 87Rb, and 133Cs atoms trapped in a solid parahydrogen matrix. We use optical pumping to prepare the spin states of the implanted atoms and circular dichroism to measure their spin states. Optical pumping signals show order-of-magnitude differences depending on both matrix growth conditions and atomic species. We measure the ensemble transverse relaxation times (T2*) of the spin states of the alkali-metal atoms. Different alkali species exhibit dramatically different T2* times, ranging from sub-microsecond coherence times for high mF states of 87Rb, to ~100 microseconds for 39K. These are the longest ensemble T2* times reported for an electron spin system at high densities (n > 10^16 cm^-3). To interpret these observations, we develop a theory of inhomogenous broadening of hyperfine transitions of ^2S atoms in weakly-interacting solid matrices. Our calculated ensemble transverse relaxation times agree well with experiment, and suggest ways to longer coherence times in future work.

Spin-rotation mode in a quantum Hall ferromagnet

A spin-rotation mode emerging in a quantum Hall ferromagnet due to laser pulse excitation is studied. This state, macroscopically representing a rotation of the entire electron spin-system to a certain angle, is not microscopically equivalent to a coherent turn of all spins as a single-whole and is presented in the form of a combination of eigen quantum states corresponding to all possible Sz spin numbers. The motion of the macroscopic quantum state is studied microscopically by solving a non-stationary Schrödinger equation and by means of a kinetic approach where damping of the spin-rotation mode is related to an elementary process, namely, transformation of a ‘Goldstone spin exciton’ to a ‘spin-wave exciton’. The system exhibits a spin stochastization mechanism (determined by spatial fluctuations of the Landé factor) ensuring damping, transverse spin relaxation, but irrelevant to decay of spin-wave excitons and thus not involving longitudinal relaxation, i.e. recovery of the Sz number to its equilibrium value.

UWB DEER and RIDME distance measurements in Cu(II)-Cu(II) spin pairs.

Distance determination by Electron Paramagnetic Resonance (EPR) based on measurements of the dipolar coupling are technically challenging for electron spin systems with broad spectra due to comparatively narrow microwave pulse excitation bandwidths. With Na4[{CuII(PyMTA)}-(stiff spacer)-{CuII(PyMTA)}] as a model compound, we compared DEER and RIDME measurements and investigated the use of frequency-swept pulses. We found very large improvements in sensitivity when substituting the monochromatic pump pulse by a frequency-swept one in DEER experiments with monochromatic observer pulses. This effect was especially strong in X band, where nearly the whole spectrum can be included in the experiment. The RIDME experiment is characterised by a trade-off in signal intensity and modulation depth. Optimal parameters are further influenced by varying steepness of the background decay. A simple 2-point optimization experiment was found to serve as good estimate to identify the mixing time of highest sensitivity. Using frequency-swept pulses in the observer sequences resulted in lower SNR in both the RIDME and the DEER experiment. Orientation selectivity was found to vary in both experiments with the detection position as well as with the settings of the pump pulse in DEER. In RIDME, orientation selection by relaxation anisotropy of the inverted spin appeared to be negligible as form factors remain relatively constant with varying mixing time. This reduces the overall observed orientation selection to the one given by the detection position. Field-averaged data from RIDME and DEER with a shaped pump pulse resulted in the same dipolar spectrum. We found that both methods have their advantages and disadvantages for given instrumental limitations and sample properties. Thus the choice of method depends on the situation at hand and we discuss which parameters should be considered for optimization.

Toward Achieving the Theoretical Limit of Electron Spin Polarization in Covalently Linked Radical-Chromophore Dyads.

Electron spin systems with non-Boltzmann spin distributions are commonly observed in photophysical and photochemical processes involving free radicals. Understanding the origin of electron spin polarization (ESP) reveals detailed insight into the spin-dependent interactions occurring in these processes. The ability to transfer ESP to the nuclear spins of the solvent to produce large nuclear polarization is itself an active area of research in the field called dynamic nuclear polarization (DNP). Harnessing ESP in such fields demands a large magnitude of ESP and importantly on free radicals that are stable. In this work, we explored various factors that could play a prominent role in generation of ESP on the stable nitroxyl radical. By exploiting the dependence of ESP on the zero-field splitting parameter DT of the chromophore triplets and a careful choice of the chromophores for efficient quenching of their excited states by a free radical, we present here our strategies for designing covalently linked chromophore-free radical dyads, which could generate high magnitudes of ESP. Syntheses and EPR studies on a series of such dyads to demonstrate successful realization of our strategy are reported here. Our work reveals that, along with the DT value and the triplet quenching efficiency, the relative orientational dynamics of the radical and chromophore moiety and an efficient intersystem crossing of the chromophore primarily govern the ESP of the chromophore-radical dyads. One such molecule, an anthraquinone moiety linked to a TEMPO free radical that optimally satisfies the above criteria, produces a very large value of ESP-about 300 times its Boltzmann value-reaching almost half of the theoretical maximum of the radical-triplet pair mechanism of ESP. Coupled with its excellent photostability in benzene and the use of ambient conditions, this molecule should prove to be highly desirable in photoinduced DNP studies and other applications such as highly sensitive magnetometers, which require generation of large nuclear spin polarization in the solvent by transferring the electron spin polarization.