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It is demonstrated that the inherent structure of Boris pusher may result in the accumulation of errors in numerical integration when estimating the works of electric fields on particles. This, in turn, leads to an incorrect estimations of particle acceleration mechanisms. A method of error correction, reducing error to the acceptable levels of $<10\%$, is implemented. Numerical integration error in question is most pronounced in scenarios where substantial number of electrons are injected into the accelerating structure through wave breaking of plasma waves i.e. in near-critical density plasma.

The field of magnetic resonance imaging with hyperpolarized contrast agents is rapidly expanding, and parahydrogen-induced polarization (PHIP) is emerging as an inexpensive and easy-to-implement method for generating the required hyperpolarized biomolecules. Hydrogenative PHIP delivers hyperpolarized proton spin order to a substrate via chemical addition of H2 in the spin-singlet state, but prior to imaging it is typically necessary to transfer the proton polarization to a heteronucleus (usually 13C) in the molecule. Adiabatic ultralow magnetic field manipulations can be used to induce the polarization transfer, but this is necessarily a slow process, which is undesirable since the spins continually relax back to thermal equilibrium. Here we demonstrate constant-adiabaticity field cycling and field sweeping for optimal polarization transfer on a model AA$'$X spin system, [1-13C]fumarate. We introduce a method for calculating constant-adiabaticity magnetic field ramps and demonstrate that they enable much faster spin-order conversion as compared to linear ramps used before. The present method can thus be utilized to manipulate nonthermal order in heteronuclear spin systems.

Spin chemistry and spintronics developed independently and with different terminology. Until now, the interaction between the two fields has been very limited. In this review, we compile the two "languages" in an effort to enhance communication. We expect that knowledge of spin chemistry will accelerate progress in spintronics., Comment: 28 pages, 12 figures

In this paper we investigate a novel set of polarizing agents -- mixed-valence compounds -- by theoretical and experimental methods and demonstrate their performance in high-field Dynamic Nuclear Polarization (DNP) experiments in the solid state. Mixed-valence compounds constitute a group of molecules, in which molecular mobility persists even in solids. Consequently, such polarizing agents can be used to perform Overhauser-DNP experiments in solid-state, with favorable conditions for dynamic nuclear polarization formation at ultra-high magnetic fields., Comment: 4 pages, 6 figures

Development of the methods to exploit nuclear hyperpolarization and search for molecules whose nuclear spins can be efficiently hyperpolarized is an active area in nuclear magnetic resonance. Of particular interest are those molecules that have long nuclear relaxation times, making them to be suitable candidates as contrast agents in magnetic resonance imaging. In this work, we present a detailed study of SABRE SHEATH (Signal Amplification By Reversible Exchange in Shield Enabled Alignment Transfer to Heteronuclei) experiments of 15N,15N' azobenzene. In SABRE SHEATH experiments nuclear spins of the target are hyperpolarized by transfer of spin polarization from parahydrogen at ultralow fields during a reversible chemical process. The studied system is complicated, and we are concerned only about a subset of the data, presenting details for the molecules that experience fast chemical exchange at the catalytic complex and thus are involved in polarizing the free azobenzene. Azobenzene exists in two isomers trans- and cis-. We show that all nuclear spins in cis-azobenzene can be efficiently hyperpolarized by SABRE at suitable magnetic fields. Enhancement factors (relative to 9.4 T) reach several thousands of times for 15N spins and a few tens of times for the 1H spins. There are two approaches to observe either hyperpolarized magnetization of 15N/1H spins or hyperpolarized singlet order of the 15N spin pair. We compare these approaches and present the field dependencies of SABRE experiments for them. No hyperpolarization of trans 15N,15N' azobenzene was observed. The results presented here will be useful for further experiments where hyperpolarized cis-15N,15N' azobenzene is switched by light to trans 15N,15N' azobenzene for storing the produced hyperpolarization in the long-lived spin state of the 15N pair of trans-15N,15N' azobenzene.

Photochemically induced dynamic nuclear polarization (photo-CIDNP) is a method to hyperpolarize nuclear spins using light. In most cases, CIDNP experiments are performed at a high magnetic field and the sample is irradiated by the light inside a nuclear magnetic resonance (NMR) spectrometer. Here we demonstrate photo-CIDNP hyperpolarization generated in the Earth magnetic field and under zero- to ultralow field (ZULF) conditions. Irradiating a sample for several seconds with inexpensive light-emitting diodes produces a strong hyperpolarization of 1H and 13C nuclear spins enhancing the NMR signals several hundred times. The hyperpolarized spin states at the Earth field and in ZULF are different. In the latter case, the state corresponds to the singlet order between scalar-coupled 1H-13C nuclear spins. This state has a longer lifetime than the state hyperpolarized at Earth field. The method is simple and cost-efficient and should be applicable to many molecular systems known to exhibit photo-CIDNP, including amino acids and nucleotides.

The field of zero- to ultralow-field (ZULF) nuclear magnetic resonance (NMR) is currently experiencing a rapid growth, owing to the progress in optical magnetometry, and also attractive features of ZULF NMR, such as low hardware cost and excellent spectral resolution achieved under ZULF conditions. In this work, an approach is proposed and demonstrated for simultaneous acquisition of ZULF-NMR spectra of individual 13C-containing isotopomers of chemical compounds in a complex mixture. The method makes use of fast field cycling, so that the spin evolution takes place at ZULF conditions, whereas signal detection is performed in a high-field NMR spectrometer. This method has excellent sensitivity, also allowing easy assignment of ZULF-NMR spectra to specific analytes in the mixture. We demonstrate that the spectral information is the same as that given by ZULF-NMR, which makes the method suitable for creating a library of ZULF-NMR spectra of various compounds and their isotopomers. The results of the field-cycling experiments can be presented in a convenient way as 2D-NMR spectra with the direct detection giving the high-field 13C-NMR spectrum (carrying the chemical-shift information) and the indirect dimension giving the ZULF-NMR spectrum (containing information about proton-carbon J-couplings). Hence, the method can be seen as a variant of heteronuclear J-resolved spectroscopy, one of the first 2D-NMR techniques.

SABRE (Signal Amplification By Reversible Exchange) has become a widely used method for hyper-polarizing nuclear spins, thereby enhancing their Nuclear Magnetic Resonance (NMR) signals by orders of magnitude. In SABRE experiments, non-equilibrium spin order is transferred from parahydrogen to a substrate in a transient organometallic complex. Applicability of SABRE is expanded by the methodology of SABRE-relay, in which polarization can be relayed to a second substrate either by direct chemical exchange of hyperpolarized nuclei or by polarization transfer between two substrates in a second organometallic complex. To understand the mechanism of the polarization transfer and study the transfer efficiency, we propose a theoretical approach to SABRE-relay, which can treat both spin dynamics and chemical kinetics as well as the interplay between them. The approach is based on a set of equations for the spin density matrices of the spin systems involved (i.e., SABRE substrates and complexes), which can be solved numerically. Using this method, we perform a detailed study of polarization formation and analyse in detail the dependence of attainable polarization level on various chemical kinetic and spin dynamic parameters. We foresee applications of the present approach for optimizing SABRE-relay experiments with the ultimate goal of achieving maximal NMR signal enhancements for substrates of interest.

A theoretical approach is proposed to treat the spin dynamics in defect color centers. The method explicitly takes into account the spin dynamics in the ground state and excited state of the defect center as well as spin state dependent transitions involving the ground state and excited state, as well as an additional intermediate state. The proposed theory is applied to treat spin-dependent phenomena is silicon carbide, namely, in spin-3/2 silicon-vacancy centers, VSi or V2 centers. Theoretical predictions of magnetic field dependent photoluminescence intensity and optically detected magnetic resonance spectra demonstrate an important role of level crossing phenomena in the spin dynamics of the ground state and excited state. The results are in good agreement with previously published experimental data [Phys. Rev. X, 6 (2016) 031014].

The scheme of generation of ultrasound waves based on optically excited Tamm plasmon structures is proposed. It is shown that Tamm plasmon structures can provide total absorption of a laser pulse with arbitrary wavelength in a metallic layer providing the possibility of the use of an infrared semiconductor laser for the excitation of ultrasound waves. Laser pulse absorption, heat transfer and dynamical properties of the structure are modeled, and the optimal design of the structure is found. It is demonstrated that the Tamm plasmon-based photoacoustic generator can emit ultrasound waves in the frequency band up to 100 MHz with pre-defined frequency spectrum. Optical power to sound power conversion efficiency grows linearly with frequency of the laser modulation and excitation power.

The use of metamaterial as a way to mitigate the negative effects of absorption in metals on the Purcell effect in metal-dielectric structures is investigated. A layered metal-dielectric structure is considered as an anisotropic medium in the long-wavelength limit. The dispersion of the surface plasmon appearing at the boundary between such a structure and a different dielectric material, as well as the position of the peak in the local density of states are studied for various combinations of materials and filling factors of the periodic structure. The calculated frequency dependence of the Purcell factor demonstrates an increase in peak value compared to the conventional plasmonic structure.

Algorithmic cooling methods manipulate an open quantum system in order to lower its temperature below that of the environment. We show that significant cooling is achieved on an ensemble of spin-pair systems by exploiting the long-lived nuclear singlet state, which is an antisymmetric quantum superposition of the "up" and "down" qubit states. The effect is demonstrated by nuclear magnetic resonance (NMR) experiments on a molecular system containing a coupled pair of near-equivalent 13C nuclei. The populations of the system are subjected to a repeating sequence of cyclic permutations separated by relaxation intervals. The long-lived nuclear singlet order is pumped well beyond the unitary limit, and the nuclear magnetization is enhanced by 21% relative to its thermal equilibrium value. To our knowledge this is the first demonstration of algorithmic cooling using a quantum superposition state and without making a distinction between rapidly and slowly relaxing qubits., Comment: 22 pages, 6 figures

GaN-based resonators supporting whispering gallery modes are suggested as a promising approach for fabrication of efficient nanophotonic applications. A modification of excitonic emission due to coupling with cavity modes is observed experimentally in the GaN planar hexagonal microcavities grown by a selective area metal-organic vapor phase epitaxy. Low temperature cathodoluminescence spectra measured in-situ scanning electron microscope show two or three emission peaks split by 100 meV or 160 meV for the resonators formed by double- and single-wall micro-nuts, respectively. The results are compared with numerical calculations of the cavity mode energies, their Q-factors and the spatial distribution of the modes intensities. Although most modes are characterized by a small Purcell coefficient, there are a limited number of isolated cavity modes with a large Purcell factor. Such modes can efficiently interact with the bulk exciton in GaN. The results are also analyzed by diagonalization of Hamiltanion describing the system of interacting exciton and cavity modes. Theoretically, it is shown that a strong coupling between the exciton and the cavity modes is possible in such micro-resonators.

Control over spontaneous emission rate is important for improving efficiency in different semiconductor applications including lasers, LEDs and photovoltaics. Usually, an emitter should be placed inside the cavity to increase spontaneous emission rate, although it is technologically challenging. Here we experimentally demonstrate a phenomenon of super-radiance observed in a cavity-less periodic Bragg structure based on InAs monolayer-thick multiple quantum wells (MQW). The collective super-radiant mode shows enhanced emission rate for specific angles and frequencies. This behaviour correlates with the calculations demonstrating individual spots of enhanced Purcell coefficient near the Bragg condition curve. This study provides a perspective for realization of surface emitting cavity-less lasers with distributed feedback.

A theoretical approach is proposed for quantitative modeling of SABRE (Signal Amplification By Reversible Exchange) experiments performed at a high magnetic field of an NMR spectrometer. SABRE is a method, which exploits the spin order of parahydrogen (the H$_2$ molecule in its nuclear singlet state) for hyper-polarizing the spins of various substrates to enhance their NMR signals. An important feature of SABRE is that the substrate is not modified chemically: instead spin order transfer takes place in a transient complex with parahydrogen. In high-field SABRE experiments, such a transfer is achieved by using suitable NMR excitation schemes. The approach presented here can explicitly treat the spin dynamics in the SABRE complex as well as the kinetics of substrate exchange (between the free and bound form) and complex interplay of spin evolution and chemical processes. One more important effect included in the model is the alteration of the spin state of parahydrogen giving rise to the formation of anti-phase spin order from the initial singlet order. Such a treatment enables a detailed analysis of known high-field SABRE schemes, quantitative comparison with experiments and elucidation of the key factors that limit the resulting NMR signal enhancement., Comment: 19 pages, 1 scheme, 8 figures, 2 tables

We propose an efficient method for calculating level anti-crossing spectra (LAC spectra) of interacting paramagnetic defect centers in crystals. By LAC spectra we mean the magnetic field dependence of the photoluminescence intensity of paramagnetic color centers: such field dependences often exhibit sharp features, such as peaks or dips, originating from LACs in the spin system. Our approach takes into account the electronic Zeeman interaction with the external magnetic field, dipole-dipole interaction of paramagnetic centers, hyperfine coupling of paramagnetic defects to magnetic nuclei and zero-field splitting. By using this method, we can not only obtain the positions of lines in LAC spectra, but also reproduce their shapes as well as the relative amplitudes of different lines. As a striking example, we present a calculation of LAC spectra in diamond crystals containing negatively charged NV centers., Comment: 12 pages, 10 figures

A method is implemented to perform "fast" adiabatic variation of the spin Hamiltonian by imposing the constant adiabaticity condition. The method is applied to improve the performance of singlet-state Nuclear Magnetic Resonance (NMR) experiments, specifically, for efficient generation and readout of the singlet spin order in coupled spin pairs by applying adiabatically ramped RF-fields. Test experiments have been performed on a specially designed molecule having two strongly coupled C-13 spins and on selectively isotopically labelled glycerol having two pairs of coupled protons. Optimized RF-ramps show improved performance in comparison, for example, to linear ramps. We expect that the methods described here are useful, not only for singlet-state NMR experiments, but also for other experiments in magnetic resonance, which utilize adiabatic variation of the spin Hamiltonian., Comment: 14 pages, 13 figures, 2 tables

SABRE (Signal Amplification By Reversible Exchange) is a technique for enhancement of NMR (Nuclear Magnetic Resonance) signals, which utilizes parahydrogen (pH2, the H2 molecule in its nuclear spin state) as a source of non-thermal spin order. In SABRE experiments, pH2 binds to an organometallic complex with a to-be-polarized substrate; subsequently, spin order transfer takes place and the substrate acquires non-thermal spin polarization resulting in strong NMR signal enhancement. In this work we argue that the spin order of H2 in SABRE experiments performed at high magnetic fields is not necessarily the singlet order but rather anti-phase polarization, $S_{1z}S_{2z}$. Although SABRE exploits pH2, i.e., the starting spin order of H2 is supposed to be the singlet order, in solution S-T0 conversion becomes efficient once pH2 binds to a complex. Such a variation of the spin order, which becomes $S_{1z}S_{2z}$, has an important consequence: NMR methods used for transferring SABRE polarization need to be modified. Here we demonstrate that methods proposed for the initial singlet order may not work for the S_1z S_2z order; however, a simple modification makes them efficient again. A theoretical treatment of the problem under consideration is proposed; these considerations are supported by high-field SABRE experiments. Hence, for efficient use of SABRE one should note that polarization formation is a complex multi-stage process: careful optimization of this process may not only deal with chemical aspects but also with the spin dynamics, including the spin dynamics of H2., Comment: 17 pages, 5 figures, 2 schemes, 1 table

We report a study of the magnetic field dependence of photoluminescence of NV$^-$ centers (negatively charged nitrogen-vacancy centers) in diamond single crystals. In such a magnetic field dependence characteristic sharp features are observed, which are coming from Level Anti-Crossings (LACs) in a coupled electron-nuclear spin system. For sensitive detection of such LAC-lines we use lock-in detection to measure the photoluminescence intensity. This experimental technique allows us to obtain new LAC lines. Additionally, a remarkably strong dependence of the LAC-lines on the modulation frequency is found. Specifically, upon decrease of the modulation frequency from 12 kHz to 17 Hz the amplitude of the LAC-lines increases by approximately two orders of magnitude. To take a quantitative account for such effects, we present a theoretical model, which describes the spin dynamics in a coupled electron-nuclear spin system under the action of an oscillating external magnetic field. Good agreement between experiments and theory allows us to conclude that the observed effects are originating from coherent spin polarization exchange in a coupled spin system comprising the spin-polarized NV$^-$ center. Our results are of great practical importance allowing one to optimize the experimental conditions for probing LAC-derived lines in diamond crystals comprising NV$^-$ centers and for indirect detection and identification of other paramagnetic defect centers., Comment: 9 pages, 8 figures. arXiv admin note: substantial text overlap with arXiv:1609.06661

We report a study of the magnetic field dependence of the photo-luminescence of NV$^-$ centers (negatively charged nitrogen-vacancy centers) in diamond single crystals. In such a magnetic field dependence characteristic lines are observed, which are coming from Level Anti-Crossings (LACs) in the coupled electron-nuclear spin system. For enhancing the sensitivity, we used lock-in detection to measure the photo-luminescence intensity and observed a remarkably strong dependence of the LAC-derived lines on the modulation frequency. Upon decreasing of the modulation frequency from 12 kHz to 17 Hz the amplitude of the lines increases by approximately two orders of magnitude. To take a quantitative account for such effects, we developed a theoretical model, which describes the spin dynamics in the coupled electron-nuclear spin system under the action of an oscillating external magnetic field. Good agreement between experiments and theory allows us to conclude that the observed effects are originating from coherent spin polarization exchange in the NV$^-$ center. Our results are of great practical importance allowing one to optimize the experimental conditions for probing LAC-derived lines in diamond defect centers., Comment: 6 pages, 3 figures

We propose a robust and highly efficient NMR technique to create singlet spin order from longitudinal spin magnetization in coupled spin-1/2 pairs and to perform backward conversion (singlet order)$\to$magnetization. In this method we exploit adiabatic switching of an RF-field in order to drive transitions between the singlet state and the $T_\pm$ triplet states of a spin pair under study. We demonstrate that the method works perfectly for both strongly and weakly coupled spin pairs, providing a conversion efficiency between the singlet spin order and magnetization, which is equal to the theoretical maximum. We anticipate that the proposed technique is useful for generating long-lived singlet order, for preserving spin hyperpolarization and for assessing singlet spin order in nearly equivalent spin pairs in specially designed molecules and in low-field NMR studies., Comment: 21 pages, 11 figures