Spin Exchange Processes Research Articles

Magnetically propagating Hund’s exciton in van der Waals antiferromagnet NiPS3

Magnetic van der Waals (vdW) materials have opened new frontiers for realizing novel many-body phenomena. Recently NiPS3 has received intense interest since it hosts an excitonic quasiparticle whose properties appear to be intimately linked to the magnetic state of the lattice. Despite extensive studies, the electronic character, mobility, and magnetic interactions of the exciton remain unresolved. Here we address these issues by measuring NiPS3 with ultra-high energy resolution resonant inelastic x-ray scattering (RIXS). We find that Hund’s exchange interactions are primarily responsible for the energy of formation of the exciton. Measuring the dispersion of the Hund’s exciton reveals that it propagates in a way that is analogous to a double-magnon. We trace this unique behavior to fundamental similarities between the NiPS3 exciton hopping and spin exchange processes, underlining the unique magnetic characteristics of this novel quasiparticle.

Indication of critical scaling in time during the relaxation of an open quantum system

Near continuous phase transitions, universal power-law scaling, characterized by critical exponents, emerges. This behavior reflects the singular responses of physical systems to continuous control parameters like temperature or external fields. Universal scaling extends to non-equilibrium dynamics in isolated quantum systems after a quench, where time takes the role of the control parameter. Our research unveils critical scaling in time also during the relaxation dynamics of an open quantum system. Here we experimentally realize such a system by the spin of individual Cesium atoms dissipatively coupled through spin-exchange processes to a bath of ultracold Rubidium atoms. Through a finite-size scaling analysis of the entropy dynamics via numerical simulations, we identify a critical point in time in the thermodynamic limit. This critical point is accompanied by the divergence of a characteristic length, which is described by critical exponents that turn out to be unaffected by system specifics.

Dichotomy of heavy and light pairs of holes in the t−J model

A key step in unraveling the mysteries of materials exhibiting unconventional superconductivity is to understand the underlying pairing mechanism. While it is widely agreed upon that the pairing glue in many of these systems originates from antiferromagnetic spin correlations, a microscopic description of pairs of charge carriers remains lacking. Here we use state-of-the art numerical methods to probe the internal structure and dynamical properties of pairs of charge carriers in quantum antiferromagnets in four-legged cylinders. Exploiting the full momentum resolution in our simulations, we are able to distinguish two qualitatively different types of bound states: a highly mobile, meta-stable pair, which has a dispersion proportional to the hole hopping t, and a heavy pair, which can only move due to spin exchange processes and turns into a flat band in the Ising limit of the model. Understanding the pairing mechanism can on the one hand pave the way to boosting binding energies in related models, and on the other hand enable insights into the intricate competition of various phases of matter in strongly correlated electron systems.

Benchmark angle-differential cross-section ratios for the electron-impact excitation of the xenon 5p6 1S0→5p56s[3/2]2 , 5p56s[3/2]1 , 5p56s′[1/2]0 , and 5p56s′[1/2]1+5p56p[1/2]1 transitions at low and near-threshold incident electron energies

Experimental benchmark intensity ratios for the angle-differential scattering intensities for electron-impact excitation from the xenon ground state $5{p}^{6}$ ${}^{1}{S}_{0}$ to its lowest five excited states $5{p}^{5}6s{[3/2]}_{2}$, $5{p}^{5}6s{[3/2]}_{1}$, $5{p}^{5}6{s}^{\ensuremath{'}}{[1/2]}_{0}$, and (combined) $5{p}^{5}6{s}^{\ensuremath{'}}{[1/2]}_{1}+5{p}^{5}6p{[1/2]}_{1}$ are reported and compared to predictions from a full-relativistic $B$-spline $R$-matrix close-coupling model as well as earlier experimental work. The above ratios, which provide a stringent test of theoretical electron scattering models, are presented for this heavy rare gas with particular emphasis on the role of spin-exchange and direct excitation processes affecting their angular dependence.

Benchmark Angle-Differential Cross-Section Ratios for Excitation of the 4p5s Configuration in Krypton

Benchmark intensity ratio measurements of the energy loss lines of krypton for excitation of the 4p61S0→4p55s[3/2]2, 4p55s[3/2]1, 4p55s′[1/2]0, and 4p55s′[1/2]1 transitions are reported, these being the lowest electronic excitations for krypton. The importance of these ratios as stringent tests of theoretical electron scattering models for the noble gases is discussed, as well as the role of spin-exchange and direct processes regarding the angular dependence of these ratios. The experimental data are compared with predictions from fully-relativistic B-spline R-matrix (close-coupling) calculations.

Spin-polarization dependence of the Rb-Xe spin-exchange optical pumping process

We experimentally study the Rb-Xe spin-exchange optical pumping process. The dependence of the spin-exchange rate on the intensity of the pumping light is measured at different temperatures under low magnetic fields. We demonstrate that the spin-exchange rate will decrease as the Rb spin polarization increases, which agrees well with the theoretical prediction. In our measurement, three spin exchange and spin relaxation mechanisms, namely, the spin exchange rates between Rb and Xe atoms caused by van der Waals molecule (${\mathrm{\ensuremath{\Gamma}}}_{\mathrm{vdW}}$) and binary collision (${\mathrm{\ensuremath{\Gamma}}}_{\mathrm{bin}}$) processes, and the spin relaxation rate due to the wall collision of Xe atoms (${\mathrm{\ensuremath{\Gamma}}}_{\mathrm{w}}$), have comparable magnitudes. These rates are extracted separately from the measured data with different Rb spin polarization at various temperatures. Our work provides a comprehensive confirmation of the physical picture of the spin-exchange optical pumping process.

Asymmetric conductivity of the Kondo effect in cold atomic systems

Motivated by recent theoretical and experimental advances in quantum simulations using alkaline earth (AE) atoms, we put forward a proposal to detect the Kondo physics in a cold atomic system. It has been demonstrated that the intrinsic spin-exchange interaction in AE atoms can be significantly enhanced near a confinement-induced resonance (CIR), which facilitates the simulation of Kondo physics. Since the Kondo effect appears only for antiferromagnetic coupling, we find that the conductivity of such system exhibits an asymmetry across a resonance of spin-exchange interaction. The asymmetric conductivity can serve as the smoking gun evidence for Kondo physics in the cold atom context. When an extra magnetic field ramps up, the spin-exchange process near Fermi surface is suppressed by Zee-man energy and the conductivity becomes more and more symmetric. Our results can be verified in the current experimental setup.

Kinetic Processes in Fermi–Luttinger Liquids

In this work we discuss extensions of the pioneering analysis by Dzyaloshinskii and Larkin of correlation functions for one-dimensional Fermi systems, focusing on the effects of quasiparticle relaxation enabled by a nonlinear dispersion. Throughout the work we employ both, the weakly interacting Fermi gas picture and nonlinear Luttinger liquid theory to describe attenuation of excitations and explore the fermion-boson duality between both approaches. Special attention is devoted to the role of spin-exchange processes, effects of interaction screening, and integrability. Thermalization rates for electron- and hole-like quasiparticles, as well as the decay rate of collective plasmon excitations and the momentum space mobility of spin excitations are calculated for various temperature regimes. The phenomenon of spin-charge drag is considered and the corresponding momentum transfer rate is determined. We further discuss how momentum relaxation due to several competing mechanisms, viz. triple electron collisions, electron-phonon scattering, and long-range inhomogeneities affect transport properties, and highlight energy transfer facilitated by plasmons from the perspective of the inhomogeneous Luttinger liquid model. Finally, we derive the full matrix of thermoelectric coefficients at the quantum critical point of the first conductance plateau transition, and address magnetoconductance in ballistic semiconductor nanowires with strong Rashba spin-orbit coupling.

Long-time relaxation dynamics of a spin coupled to a Chern insulator

The authors compute the dynamical phase diagram for the relaxation of a classical spin, exchange coupled to the local magnetic moment at an edge site of the one-dimensional spinful Su-Schrieffer-Heeger model. The role of the topological edge state and its internal Zeeman splitting for the spin-relaxation process, as well as incomplete spin relaxation on long time scales, can be explained within the framework of a renormalized linear response approach, when explicitly taking retardation effects and nonequilibrium spin-exchange processes into account.

KINETIC PROCESSES IN FERMI-LUTTINGER LIQUIDS

In this work we discuss extensions of the pioneering analysis by Dzyaloshinskii and Larkin of correlation functions for one-dimensional Fermi systems, focusing on the effects of quasiparticle relaxation enabled by a nonlinear dispersion. Throughout the work we employ both, the weakly interacting Fermi gas picture and nonlinear Luttinger liquid theory to describe attenuation of excitations and explore the fermion-boson duality between both approaches. Special attention is devoted to the role of spin-exchange processes, effects of interaction screening, and integrability. Thermalization rates for electron- and hole-like quasiparticles, as well as the decay rate of collective plasmon excitations and the momentum space mobility of spin excitations are calculated for various temperature regimes. The phenomenon of spin-charge drag is considered and the corresponding momentum transfer rate is determined. We further discuss how momentum relaxation due to several competing mechanisms, viz. triple electron collisions, electron-phonon scattering, and long-range inhomogeneities affect transport properties, and highlight energy transfer facilitated by plasmons from the perspective of the inhomogeneous Luttinger liquid model. Finally, we derive the full matrix of thermoelectric coefficients at the quantum critical point of the first conductance plateau transition, and address magnetoconductance in ballistic semiconductor nanowires with strong Rashba spin-orbit coupling.

Frequency shifts of the magnetic resonance of Rb and K atoms in the K-Rb tandem magnetometer

Collisions of alkali atoms in the ground state are accompanied by the exchange of electron polarization between the colliding atoms, which lead to the polarization transfer between particles. As a result of this process, the electronic orientation is transferred from the spin oriented atoms to unpolarized atoms, along with the polarization transfer, the magnetic resonance frequency shifts of polarized atoms occur too. In this work the magnetic resonance frequency shifts of arising from spin exchange collisions in a mixture of alkali potassium and rubidium atoms at the optical orientation of atoms are calculated. The situation when optical pumping by resonant polarized radiation is carried out only for atoms of the one kind is considered. The spin exchange process between alkali atoms was described in the formalism of the complex cross section for spin exchange process. The real and imaginary parts of the complex cross section were calculated using the interaction potentials of alkali atom dimers. The calculation of the frequency shifts is carried out on the basis of data on the interaction potentials for the following pairs of alkali atoms K-K, K-Rb and Rb-Rb. Maxwell averaging of the cross sections over the velocities was done and the temperature dependences of the magnetic resonance frequency shifts for K and Rb atoms were plotted.

Highresolution spectroscopic probing of ortho and para nuclear-spin isomers of heavy water in the gas phase

Abstract Doubly deuterated water (D2O) exhibits two distinct nuclear spin-isomers, ortho and para, which have not much been studied and there is hardly any information about the spin-exchange processes of D2O. Here, we investigated the nuclear-spin quantum states of D2O in gas phase by evaluating the ortho-to-para ratio (OPR) using high-resolution cavity ring-down spectroscopy coupled with quantum cascade laser in the mid-IR spectral region at 7.8 μm. We experimentally achieved an OPR of (1.95 ± 0.16):1 for D2O spin-isomers in the isolated gaseous phase. We further analyzed the OPR of the residual D2O in a 1:1 mixture of D2O and H2O, and observed indications of potential alteration of thermodynamic probability of ortho and para nuclear-spin states of D2O associated with the D-H exchange reaction in the system. Our findings pave the way to probe directly the spin behaviour of D2O molecules in the gas phase and thus fostering exploration of spin-dependent chemistry in a wide range of chemical and biological systems.

Intramolecular Mobility in Nitroxide Biradicals with Flexible Linkers

Intramolecular electron spin exchange has been studied by X-band electron paramagnetic resonance (EPR) spectroscopy in two long-chain flexible nitroxide biradicals existing in fluid solutions in three spectroscopy-different spatial conformations as a function of temperature, solvent viscosity and polarity. Certain thermodynamic parameters of the conformational transitions were calculated from the EPR spectra. The process of spin-exchange in these biradicals dissolved in five different alcohols was compared with that in the non-polar solvents (toluene) and aprotic (acetonitrile), as well as with two other biradicals studied earlier, and with thermodynamic characteristics of the solvents. A distinct correlation was found between macroscopic (solvent viscosity) characteristics of solvents and thermodynamic parameters of the intramolecular conformational transitions.

Dynamical Sign Reversal of Magnetic Correlations in Dissipative Hubbard Models.

In quantum magnetism, the virtual exchange of particles mediates an interaction between spins. Here, we show that an inelastic Hubbard interaction fundamentally alters the magnetism of the Hubbard model due to dissipation in spin-exchange processes, leading to sign reversal of magnetic correlations in dissipative quantum dynamics. This mechanism is applicable to both fermionic and bosonic Mott insulators, and can naturally be realized with ultracold atoms undergoing two-body inelastic collisions. The dynamical reversal of magnetic correlations can be detected by using a double-well optical lattice or quantum-gas microscopy, the latter of which facilitates the detection of the magnetic correlations in one-dimensional systems because of spin-charge separation. Our results open a new avenue toward controlling quantum magnetism by dissipation.

Single-Atom Quantum Probes for Ultracold Gases Boosted by Nonequilibrium Spin Dynamics

Quantum probes are atomic-sized devices mapping information of their environment to quantum mechanical states. By improving measurements and at the same time minimizing perturbation of the environment, they form a central asset for quantum technologies. We realize spin-based quantum probes by immersing individual Cs atoms into an ultracold Rb bath. Controlling inelastic spin-exchange processes between probe and bath allows mapping motional and thermal information onto quantum-spin states. We show that the steady-state spin-population is well suited for absolute thermometry, reducing temperature measurements to detection of quantum spin distributions. Moreover, we find that the information gain per inelastic collision can be maximized by accessing the nonequilibrium spin dynamic. The sensitivity of nonequilibrium quantum probing effectively beats the steady-state Cram\'er Rao limit of quantum probing by almost an order of magnitude, while reducing the perturbation of the bath to only three quanta of angular momentum. Our work paves the way for local probing of quantum systems at the Heisenberg limit, and moreover for optimizing measurement strategies via control of nonequilibrium dynamics.

Hot-electron dynamics in quantum dots manipulated by spin-exchange Auger interactions.

The ability to effectively manipulate non-equilibrium 'hot' carriers could enable novel schemes for highly efficient energy harvesting and interconversion. In the case of semiconductor materials, realization of such hot-carrier schemes is complicated by extremely fast intraband cooling (picosecond to subpicosecond time scales) due to processes such as phonon emission. Here we show that using magnetically doped colloidal semiconductor quantum dots we can achieve extremely fast rates of spin-exchange processes that allow for 'uphill' energy transfer with an energy-gain rate that greatly exceeds the intraband cooling rate. This represents a dramatic departure from the usual situation where energy-dissipation via phonon emission outpaces energy gains due to standard Auger-type energy transfer at least by a factor of three. A highly favourable energy gain/loss rate ratio realized in magnetically doped quantum dots can enable effective schemes for capturing kinetic energy of hot, unrelaxed carriers via processes such as spin-exchange-mediated carrier multiplication and upconversion, hot-carrier extraction and electron photoemission.

Fast spin exchange across a multielectron mediator

Scalable quantum processors require tunable two-qubit gates that are fast, coherent and long-range. The Heisenberg exchange interaction offers fast and coherent couplings for spin qubits, but is intrinsically short-ranged. Here, we demonstrate that its range can be increased by employing a multielectron quantum dot as a mediator, while preserving speed and coherence of the resulting spin-spin coupling. We do this by placing a large quantum dot with 50–100 electrons between a pair of two-electron double quantum dots that can be operated and measured simultaneously. Two-spin correlations identify coherent spin-exchange processes across the multielectron quantum dot. We further show that different physical regimes of the mediated exchange interaction allow a reduced susceptibility to charge noise at sweet spots, as well as positive and negative coupling strengths up to several gigahertz. These properties make multielectron dots attractive as scalable, voltage-controlled coherent coupling elements.

Nonuniversal critical aging scaling in three-dimensional Heisenberg antiferromagnets

We numerically investigate the stationary and non-equilibrium critical dynamics in three-dimensional isotropic Heisenberg antiferromagnets. Since the non-conserved staggered magnetization couples dynamically to the conserved magnetization density, we employ a hybrid simulation algorithm that combines reversible spin precession with relaxational Kawasaki spin exchange processes. We measure the dynamic critical exponent and identify a suitable intermediate time window to obtain the aging scaling exponents. Our results support an earlier renormalization group prediction: While the critical aging collapse exponent assumes a universal value, the associated temporal decay exponent in the two-time spin autocorrelation function depends on the initial distribution of the conserved fields; here, specifically on the width of the initial spin orientation distribution.

The xenon hyperpolarization by alexandrite laser spin exchange optical pumping

This paper shows the possibility of the use of a solid-state alexandrite laser as a radiation source for the method of spin-exchange optical pumping of noble gases (xenon, krypton). The use of dispersive optical elements in the laser cavity will allows the adjusting of the radiation wavelength exactly in the rubidium spectral absorption lines 794.7 nm and 780 nm. To obtain a hyperpolarized state of noble gases, it is necessary to excite rubidium atoms for further spin-exchange process with the noble gas nuclei. This fact will allow the increasing of the magnetic resonance imaging contrast in the field of diagnosis of respiratory organs diseases.

Interaction between spin polarized alkali atoms

Collisions of alkali-metal atoms in the ground state with the electron spin S = 1/2 are accompanied by exchange of electron coordinates between colliding particles, which leads to polarization transfer between them (i.e., to the well-known phenomenon of spin exchange). In addition, along with the polarization transfer from one partner to another, the magnetic resonance lines of colliding atoms are broadened and shifted in spin-exchange collisions. In particular the last two processes depend on the complex spin-exchange cross section. The real part of the cross section determines the so-called “spin-exchange cross section,” which is responsible for the broadening of magnetic resonance lines, while the imaginary part determines the shift cross section, which governs the frequency shift of magnetic resonance.In order to describe the spin-exchange process one have to know complex spin-exchange cross sections. Complex spin-exchange cross sections are calculated on the basis of the data on the singlet (X1Σ+) and triplet (a3Σ+) potentials describing the interaction alkali-metal atoms in the ground state.Collisions of alkali-metal atoms Cs, Rb, K, Na in the ground state are considered in the energy interval of 10−4−10−2 au.