Investigation Of Spin Dynamics Research Articles

Quantum Sensing of Spin Dynamics Using Boron-Vacancy Centers in Hexagonal Boron Nitride.

Spin defects embedded in solid-state systems are appealing for quantum sensing of materials and for quantum science and engineering. The spin-sensitive photoluminescence of optically active spin defects in Van der Waals based materials, such as the boron-vacancy (V_{B}^{-}) center in hexagonal boron nitride, enables its application as a quantum sensor to detect weak, spatially localized magnetic static and dynamic fields. However, the utility of V_{B}^{-} centers to probe spin dynamics in magnetic systems has yet to be demonstrated; this is essential to establish the V_{B}^{-} as a modular sensing platform that can be seamlessly integrated with emergent quantum materials to probe a wide range of static and dynamic phenomena. Here, we use V_{B}^{-} centers to experimentally probe uniform mode magnon dynamics and optically perform ferromagnetic resonance spectroscopy on a thin magnetic film.

Tunable Tesla-Scale Magnetic Attosecond Pulses through Ring-Current Gating.

Coherent control over electron dynamics in atoms and molecules using high-intensity circularly polarized laser pulses gives rise to current loops, resulting in the emission of magnetic fields. We propose, and demonstrate with ab initio calculations, "current-gating" schemes to generate direct or alternating-current magnetic pulses in the infrared spectral region, with highly tunable waveform and frequency, and showing femtosecond-to-attosecond pulse duration. In optimal conditions, the magnetic pulse can be highly isolated from the driving laser and exhibits a high flux density (∼1 T at a few hundred nanometers from the source, with a pulse duration of 787 attoseconds) for application in forefront experiments of ultrafast spectroscopy. Our work paves the way toward the generation of attosecond magnetic fields to probe ultrafast magnetization, chiral responses, and spin dynamics.

Methods for Obtaining One Single Larmor Frequency, Either v1 or v2, in the Coherent Spin Dynamics of Colloidal Quantum Dots.

The coexistence of two spin components with different Larmor frequencies in colloidal CdSe and CdS quantum dots (QDs) leads to the entanglement of spin signals, complicating the analysis of dynamic processes and hampering practical applications. Here, we explored several methods, including varying the types of hole acceptors, air or anaerobic atmosphere and laser repetition rates, in order to facilitate the obtention of one single Larmor frequency in the coherent spin dynamics using time-resolved ellipticity spectroscopy at room temperature. In an air or nitrogen atmosphere, manipulating the photocharging processes by applying different types of hole acceptors, e.g., Li[Et3BH] and 1-octanethiol (OT), can lead to pure spin components with one single Larmor frequency. For as-grown QDs, low laser repetition rates favor the generation of the higher Larmor frequency spin component individually, while the lower Larmor frequency spin component can be enhanced by increasing the laser repetition rates. We hope that the explored methods can inspire further investigations of spin dynamics and related photophysical processes in colloidal nanostructures.

Spin dynamics in the axion insulator candidate EuIn2As2

We report the investigation of spin dynamics in the antiferromagnetic metal ${\mathrm{EuIn}}_{2}{\mathrm{As}}_{2}$ with the Zintl phase by using time-resolved magneto-optical Kerr effect (TR-MOKE) and transient reflectivity spectroscopy. In TR-MOKE measurement, we observe a spin precession mode with a frequency of about 18 GHz below 1.4 T and a new emerging coherent acoustic phonon mode near 35 GHz at a higher field where the latter shows a field-independent behavior. With temperature increasing, the spin precession disappears above N\'eel temperature ${T}_{N}$, whereas the acoustic phonon persists up to 25 K due to existence of magnetic-field-induced polarized paramagnetism. In contrast, the quasiparticle dynamics of ${\mathrm{EuIn}}_{2}{\mathrm{As}}_{2}$ does not show dramatic change in the vicinity of ${T}_{N}$. By comparing the spin and quasiparticle dynamics, we attribute the appearance of an acoustic phonon in TR-MOKE to photoinduced transient perturbation of magneto-optical coefficient. Our paper provides an in-depth investigation on the dynamical magnetic properties and broadens the understanding of the ${\mathrm{EuIn}}_{2}{\mathrm{As}}_{2}$ system.

Probing spin dynamics of ultra-thin van der Waals magnets via photon-magnon coupling

Layered van der Waals (vdW) magnets can maintain a magnetic order even down to the single-layer regime and hold promise for integrated spintronic devices. While the magnetic ground state of vdW magnets was extensively studied, key parameters of spin dynamics, like the Gilbert damping, crucial for designing ultra-fast spintronic devices, remains largely unexplored. Despite recent studies by optical excitation and detection, achieving spin wave control with microwaves is highly desirable, as modern integrated information technologies predominantly are operated with these. The intrinsically small numbers of spins, however, poses a major challenge to this. Here, we present a hybrid approach to detect spin dynamics mediated by photon-magnon coupling between high-Q superconducting resonators and ultra-thin flakes of Cr2Ge2Te6 (CGT) as thin as 11 nm. We test and benchmark our technique with 23 individual CGT flakes and extract an upper limit for the Gilbert damping parameter. These results are crucial in designing on-chip integrated circuits using vdW magnets and offer prospects for probing spin dynamics of monolayer vdW magnets.

Probing Spin Dynamics of 2D Excitons with Twisted Light

We propose a mechanism of intravalley spin-flip scattering in spin-valley coupled two dimensional systems by transferring momentum of light into exciton center of mass using optical vortex (OV) beams. By varying the dispersion of light using the topological charge of OV beam, we demonstrate a unique approach to control the intra-valley spin-flip scattering rate of excitons. From our photoluminescence measurements, we demonstrate that the intra-valley scattering rate in W-based TMDs can be tuned externally by OV beams. Variation of photoluminescence intensity with topological charges shows a crossover temperature (> 150 K), indicating competitions among time scales involving radiative recombination, spin-flip scattering, and thermal relaxations. Our proposed technique utilizing a structured light beam can open up a new approach to explore the physics of excitons in 2D systems.

Magnons in AgF2, AgCuF4, and AgNiF4

We report on the analytical derivation of the spin-wave dispersion and magnon density of states in the orthorhombic AgF2 within J1–J2–J3 model and within 2D limit. Numerical calculations allowed us to estimate the effect of the Dzyaloshinskii–Moriya interaction, and explore closely related systems AgCuF4 and AgNiF4 in different pressure-induced phases. Obtained results will pave a direct way to link abinitio calculations with experiments via determination of the exchange and single-ion anisotropy constants based on any method which is able to probe spin dynamics, such as Raman or infrared spectroscopy.

Solid-state MAS NMR at ultra low temperature of hydrated alanine doped with DNP radicals

Magic angle spinning (MAS) nuclear magnetic resonance (NMR) experiments at ultra low temperature (ULT) (≪ 100 K) have demonstrated clear benefits for obtaining large signal sensitivity gain and probing spin dynamics phenomena at ULT. ULT NMR is furthermore a highly promising platform for solid-state dynamic nuclear polarization (DNP). However, ULT NMR is not widely used, given limited availability of such instrumentation from commercial sources. In this paper, we present a comprehensive study of hydrated [U-13C]alanine, a standard bio-solid sample, from the first commercial 14.1 Tesla NMR spectrometer equipped with a closed-cycle helium ULT-MAS system. The closed-cycle helium MAS system provides precise temperature control from 25 K to 100 K and stable MAS from 1.5 kHz to 12 kHz. The 13C CP-MAS NMR of [U-13C]alanine showed 400% signal gain at 28 K compared with at 100 K. The large sensitivity gain results from the Boltzmann factor, radio frequency circuitry quality factor improvement, and the suppression of its methyl group rotation at ULT. We further observed that the addition of organic biradicals widely used for solid-state DNP significantly shortens the 1H T1 spin lattice relaxation time at ULT, without further broadening the 13C spectral linewidth compared to at 90 K. The mechanism of 1H T1 shortening is dominated by the two-electron-one-nucleus triple flip transition underlying the Cross Effect mechanism, widely relied upon to drive solid-state DNP. Our experimental observations suggest that the prospects of MAS NMR and DNP under ULT conditions established with a closed-cycle helium MAS system are bright.

Ultrafast spin-currents and charge conversion at 3d-5d interfaces probed by time-domain terahertz spectroscopy

Spintronic structures are extensively investigated for their spin–orbit torque properties, required for magnetic commutation functionalities. Current progress in these materials is dependent on the interface engineering for the optimization of spin transmission. Here, we advance the analysis of ultrafast spin-charge conversion phenomena at ferromagnetic-transition metal interfaces due to their inverse spin-Hall effect properties. In particular, the intrinsic inverse spin-Hall effect of Pt-based systems and extrinsic inverse spin-Hall effect of Au:W and Au:Ta in NiFe/Au:(W,Ta) bilayers are investigated. The spin-charge conversion is probed by complementary techniques—ultrafast THz time-domain spectroscopy in the dynamic regime for THz pulse emission and ferromagnetic resonance spin-pumping measurements in the GHz regime in the steady state—to determine the role played by the material properties, resistivities, spin transmission at metallic interfaces, and spin-flip rates. These measurements show the correspondence between the THz time-domain spectroscopy and ferromagnetic spin-pumping for the different set of samples in term of the spin mixing conductance. The latter quantity is a critical parameter, determining the strength of the THz emission from spintronic interfaces. This is further supported by ab initio calculations, simulations, and analysis of the spin-diffusion and spin-relaxation of carriers within the multilayers in the time domain, permitting one to determine the main trends and the role of spin transmission at interfaces. This work illustrates that time-domain spectroscopy for spin-based THz emission is a powerful technique to probe spin-dynamics at active spintronic interfaces and to extract key material properties for spin-charge conversion.

NMR Study of Spin Dynamics in V7Zn and V7Ni Molecular Rings

We present a 1H NMR investigation of spin dynamics in two finite integer spin molecular nanomagnetic rings, namely V7Zn and V7Ni. This study could be put in correlation with the problem of Haldane gap in infinite integer spin chains. While V7Zn is an approximation of a homometallic broken chain due to the presence of s = 0 Zn2+ ion uncoupled from nearest neighbor V2+s = 1 ions, the V7Ni compound constitutes an example of a closed periodical s = 1 heterometallic chain. From preliminary susceptibility measurements on single crystals and data analysis, the exchange coupling constant J/kB results in the order of few kelvin. At room temperature, the frequency behavior of the 1H NMR spin–lattice relaxation rate 1/T1 allowed to conclude that the spin–spin correlation function is similar to the one observed in semi-integer spin molecules, but with a smaller cutoff frequency. Thus, the high-T data can be interpreted in terms of, e.g., a Heisenberg model including spin diffusion. On the other hand, the behavior of 1/T1 vs temperature at different constant fields reveals a clear peak at temperature of the order of J/kB, qualitatively in agreement with the well-known Bloembergen–Purcell–Pound model and with previous results on semi-integer molecular spin systems. Consequently, one can suggest that for a small number N of interacting s = 1 ions (N = 8), the Haldane conjecture does not play a key role on spin dynamics, and the investigated rings still keep the quantum nature imposed mainly by the low number of magnetic centers, with no clear topological effect due to integer spins.

Spin-chemical effects on intramolecular photoinduced charge transfer reactions in bisphenanthroline copper(i)-viologen dyad assemblies.

Two covalently linked donor-acceptor copper phenanthroline complexes (C-A dyads) of interest for solar energy conversion/storage schemes, [Cu(i)(Rphen(OMV)2 4+)2]9+ = RC+A4 8+ with RC+ = [Cu(i)Rphen2]+ involving 2,9-methyl (R = Me) or 2,9-phenyl (R = Ph)-phenanthroline ligands that are 5,6-disubstituted by 4-(n-butoxy) linked methylviologen electron acceptor groups (A2+ = OMV2+), have been synthesized and investigated via quantum chemical calculations and nanosecond laser flash spectroscopy in 1,2-difluorobenzene/methanol (dfb/MeOH) mixtures. Upon photoexcitation, charge transfer (CT) states RC2+A+A3 6+ are formed in less than one ns and decay by charge recombination on a time scale of 6-45 ns. The CT lifetime of RC2+A+A3 6+ has a strong dependence on MeOH solvent fraction when R = Me, but is unaffected if R = Ph. This solvent effect is due to coordination of MeOH solvent in MeC+A4 8+ (i.e. exciplex formation) allowed by conformational flattening of the ligand sphere, which cannot occur in PhC+A4 8+ having bulkier Phphen ligand framework. Interestingly, the decay time of the CT state increases for both species at low magnetic fields with a maximum increase of ca. 30% at ca. 150 mT, then decreases as the field is increased up to 1500 mT, the highest field investigated. This magnetic field effect (MFE) is due to magnetic modulation of the spin dynamics interconverting 3CT and 1CT states. A quantitative modeling according to the radical pair mechanism involving ab initio multireference calculations of the complexes revealed that the spin process is dominated by the effect of Cu hyperfine coupling. The external magnetic field suppresses the hyperfine coupling induced spin state mixing thereby lengthening the CT decay time. This effect is counteracted by the field dependent processes of T0-S mixing through the Δg-mechanism and by a local mode spin-orbit mechanism. Further, the maximum MFE is limited by a finite rate of direct recombination of 3CT states and the spin-rotational mechanism of spin relaxation. This study provides a first comprehensive characterization of Cu(ii)-complex spin chemistry and highlights how spin chemistry can be used to manipulate solar energy harvesting and storage materials.

Understanding the Linewidth of the ESR Spectrum Detected by a Single NV Center in Diamond

Spectral analysis of electron spin resonance (ESR) is a powerful technique for various investigations including characterization of spin systems, measurements of spin concentration, and probing spin dynamics. The nitrogen-vacancy (NV) center in diamond is a promising magnetic sensor enabling improvement of ESR sensitivity to the level of a single spin. Therefore, understanding the nature of the NV-detected ESR (NV-ESR) spectrum is critical for applications to nanoscale ESR. Within this work, we investigate the linewidth of NV-ESR from single substitutional nitrogen centers (called P1 centers). NV-ESR is detected by a double electron-electron resonance (DEER) technique. By studying the dependence of the DEER excitation bandwidth on the NV-ESR linewidth, we find that the spectral resolution is improved significantly and eventually limited by inhomogeneous broadening of the detected P1 ESR. Moreover, we show that the NV-ESR linewidth can be as narrow as 0.3 MHz.

Sub-eikonal corrections to scattering amplitudes at high energy

Most of the progress in high-energy Quantum Chromodynamics has been obtained within the eikonal approximation and infinite Wilson-line operators. Evolution equations of Wilson lines with respect to the rapidity parameter encode the dynamics of the hadronic processes at high energy. However, even at high energy many interesting aspects of hadron dynamics are not accessible within the eikonal approximation, the spin physics being an obvious example. The higher precision reached by the experiments and the possibility to probe spin dynamics at future Electron Ion Colliders make the study of deviations from eikonal approximation especially timely. In this paper, I derive the sub-eikonal quark and gluon propagators which can serve as a starting point of studies of these effects.

Theory of time-resolved Raman scattering in correlated systems: Ultrafast engineering of spin dynamics and detection of thermalization

Ultrafast characterization and control of many-body interactions and elementary excitations are critical to understanding and manipulating emergent phenomena in strongly correlated systems. In particular, spin interaction plays an important role in unconventional superconductivity, but efficient tools for probing spin dynamics especially out of equilibrium, are still lacking. To address this question, we develop a theory for nonresonant time-resolved Raman scattering, which can be a generic and powerful tool for nonequilibrium studies. We also use exact diagonalization to simulate the pump-probe dynamics of correlated electrons in the square-lattice single-band Hubbard model. Different ultrafast processes are shown to exist in the time-resolved Raman spectra and dominate under different pump conditions. For high-frequency and off-resonance pumps, we show that the Floquet theory works well in capturing the softening of bimagnon excitation. By comparing the Stokes/anti-Stokes spectra, we also show that effective heating dominates at small pump fluences, while a coherent many-body effect starts to take over at larger pump amplitudes and frequencies on resonance to the Mott gap. Time-resolved Raman scattering thereby provides the platform to explore different ultrafast processes and design material properties out of equilibrium.

One-Dimensional Spin Channel in Two-Dimensional Transition Metal Dichalcogenide Heterostructures

We show that it is possible to obtain one-dimensional (1D) spin channels at the lateral heterojunction of 2D transition metal dichalcogenides by a current flow without the necessity of any external magnetic field. This originates from the native spin orbit coupling of 2D materials in conjunction with the electric field that develops due to conduction band-offset at the junction. Nonetheless, we show that the underlying physics is very different from the well-known spin Hall effect. We find that the degree of spin polarization could be as high as 0.1 $\%$ for conduction band transport and 0.75 $\%$ for valence band transport at room temperature in a lateral heterostructure of typical 2D semiconductors such as ${\rm MoS}_2$ / ${\rm WSe}_2$ . We also find that the spin polarization increases with longitudinal (transport) effective mass due to increased momentum of the flowing electrons. Such 1D spin channels might allow probing of spin dynamics in confined phase spaces in addition to potentially contributing to spintronics applications.

Probe of spin dynamics in superconducting NbN thin films via spin pumping

The emerging field of superconductor (SC) spintronics has attracted intensive attentions recently. Many fantastic spin dependent properties in SC have been discovered, including the observation of large magnetoresistance, long spin lifetimes and the giant spin Hall effect in SC, as well as spin supercurrent in Josephson junctions, etc. Regarding the spin dynamic in SC films, few studies has been reported yet. Here, we report the investigation of the spin dynamics in an s-wave superconducting NbN film via spin pumping from an adjacent insulating ferromagnet GdN layer. A profound coherence peak of the Gilbert damping is observed slightly below the superconducting critical temperature of the NbN layer, which is consistent with recent theoretical studies. Our results further indicate that spin pumping could be a powerful tool for investigating the spin dynamics in 2D crystalline superconductors.

Control of quasi-phase-matching of high-harmonics in a spatially structured plasma.

High-harmonic generation is widely used for providing extreme ultraviolet radiation in attosecond science. Such experiments include photoelectron spectroscopy, diffractive imaging, or the investigation of spin dynamics. Many applications are restricted by a low photon flux which originates from the low efficiency of the generation process. In this article an effective method based on the quasi-phase-matched generation of high harmonics in spatially structured, laser ablated plasma is demonstrated. Through a proper dimensioning of the plasma structure, the harmonic yield is optimized for a controllable range of harmonic orders. By using four coherent zones, the intensity of a single harmonic is increased to a maximal possible value of 16 compared to using a single zone. The Gouy phase shift of the fundamental field is identified as the primary effect responsible for constructive interference of the harmonic fields generated in the individual plasma jets of the plasma structure.

Novel Pulsed Electron Paramagnetic Resonance Techniques for the Studies of Structure and Dynamics of Photo‐excited Triplet State of Organic Molecules: A Professional Journey

We present a few novel pulsed electron paramagnetic resonance techniques developed in our laboratory for the studies of structure and dynamics of the photo‐excited triplet state of organic molecules. We discuss many aspects of these new techniques and the significances of these measurements: (1) enhancing NMR signal intensity by dynamic nuclear polarization ‐ integrated solid effect, (2) performing magnetic resonance in zero‐field and low‐field by pulsed microwave, (3) mapping molecular motion of organic crystals by pulsed zero‐field and low‐field experiments, (4) probing spin dynamics at level anti‐crossing by fast field switching, (5) measuring hyperfine interaction by electron spin echo envelop modulation and spin‐echo electron nuclear double resonance and (6) detecting spin dynamics, nuclear quantum oscillation, entanglements and new avenues for quantum computer. We have employed the highly electron spin polarized pentacene triplet state as the model system in all of our pulsed EPR experiments. We performed most of our experiments at room temperature. The goals of our studies are aiming to improve spin detectability, to probe molecular dynamics, to determine electronic structures, to measure molecular interaction and motion, and to examine quantum coherence and oscillation which may yield new avenues in the applications of pulsed EPR techniques to quantum computer.

Spin pumping into superconductors: A new probe of spin dynamics in a superconducting thin film

Spin pumping refers to the microwave-driven spin current injection from a ferromagnet into the adjacent target material. We theoretically investigate the spin pumping into superconductors by fully taking account of impurity spin-orbit scattering that is indispensable to describe diffusive spin transport with finite spin diffusion length. We calculate temperature dependence of the spin pumping signal and show that a pronounced coherence peak appears immediately below the superconducting transition temperature Tc, which survives even in the presence of the spin-orbit scattering. The phenomenon provides us with a new way of studying the dynamic spin susceptibility in a superconducting thin film. This is contrasted with the nuclear magnetic resonance technique used to study a bulk superconductor.

Probing spin dynamics from the Mott insulating to the superfluid regime in a dipolar lattice gas

We analyze the spin dynamics of an out-of-equilibrium large spin dipolar atomic Bose gas in an optical lattice. We observe a smooth crossover from a complex oscillatory behavior to an exponential behavior throughout the Mott to superfluid transition. While both of these regimes are well described by our theoretical models, we provide data in the intermediate regime where dipolar interactions, contact interactions, and super-exchange mechanisms compete. In this strongly correlated regime, spin dynamics and transport are coupled, which challenges theoretical models for quantum magnetism.