Broadband spectroscopy of thermodynamic magnetization fluctuations through a ferromagnetic spin-reorientation transition.

We use scanning optical magnetometry to study the broadband frequency spectra of spontaneous magnetization fluctuations, or "magnetization noise", in an archetypal ferromagnetic film that can be smoothly tuned through a spin reorientation transition (SRT). The SRT is achieved by laterally varying the magnetic anisotropy across an ultrathin Pt/Co/Pt trilayer, from the perpendicular to in-plane direction, via graded Ar+ irradiation. In regions exhibiting perpendicular anisotropy, the power spectrum of the magnetization noise, S(ν), exhibits a remarkably robust ν -3/2 power law over frequencies ν from 1 kHz to 1 MHz. As the SRT region is traversed, however, S(ν) spectra develop a steadily-increasing critical frequency, ν 0, below which the noise power is spectrally flat, indicating an evolving low-frequency cutoff for magnetization fluctuations. The magnetization noise depends strongly on applied in- and out-of-plane magnetic fields, revealing local anisotropies and also a field-induced emergence of fluctuations in otherwise stable ferromagnetic films. Finally, we demonstrate that higher-order correlators can be computed from the noise. These results highlight broadband spectroscopy of thermodynamic fluctuations as a powerful tool to characterize the interplay between thermal and magnetic energy scales, and as a means of characterizing phase transitions in ferromagnets.

Quantum Effects in Higher-Order Correlators of a Quantum-Dot Spin Qubit.

We measure time correlators of a spin qubit in an optically active quantum dot beyond the second order. Such higher-order correlators are shown to be directly sensitive to pure quantum effects that cannot be explained within the classical framework. They allow direct determination of ensemble and quantum dephasing times, T_{2}^{*} and T_{2}, using only repeated projective measurements and without the need for coherent spin control. Our method enables studies of purely quantum behavior in solid state systems, including tests of the Leggett-Garg type of inequalities that rule out local hidden variable interpretation of the quantum-dot spin dynamics.

Universality in Higher Order Spin Noise Spectroscopy.

Higher order time correlators of spin fluctuations reveal considerable information about spin interactions. We argue that in a broad class of spin systems, one can justify a phenomenological approach to explore such correlators. We predict that the third and fourth order spin cumulants are described by a universal function that can be parametrized by a small set of parameters. We show that the fluctuation theorem constrains this function so that such correlators are fully determined by lowest nonlinear corrections to the free energy and the mean and variance of microscopic spin currents. We also provide an example of microscopic calculations for conduction electrons.

Spin noise spectroscopy beyond thermal equilibrium and linear response.

Per the fluctuation-dissipation theorem, the information obtained from spin fluctuation studies in thermal equilibrium is necessarily constrained by the system's linear response functions. However, by including weak radio frequency magnetic fields, we demonstrate that intrinsic and random spin fluctuations even in strictly unpolarized ensembles can reveal underlying patterns of correlation and coupling beyond linear response, and can be used to study nonequilibrium and even multiphoton coherent spin phenomena. We demonstrate this capability in a classical vapor of (41)K alkali atoms, where spin fluctuations alone directly reveal Rabi splittings, the formation of Mollow triplets and Autler-Townes doublets, ac Zeeman shifts, and even nonlinear multiphoton coherences.

Spin and valley noise in two-dimensional Dirac materials.

We develop a theory for optical Faraday rotation noise in two-dimensional Dirac materials. In contrast to spin noise in conventional semiconductors, we find that the Faraday rotation fluctuations are influenced not only by spins but also the valley degrees of freedom attributed to intervalley scattering processes. We illustrate our theory with two-dimensional transition-metal dichalcogenides and discuss signatures of spin and valley noise in the Faraday noise power spectrum. We propose optical Faraday noise spectroscopy as a technique for probing both spin and valley relaxation dynamics in two-dimensional Dirac materials.

Nonequilibrium spin noise spectroscopy.

Spin noise spectroscopy is an experimental approach to obtain correlators of mesoscopic spin fluctuations in time by purely optical means. We explore the information that this technique can provide when it is applied to a weakly nonequilibrium regime when an electric current is driven through a sample by an electric field. We find that the noise power spectrum of conducting electrons experiences a shift, which is proportional to the strength of the spin-orbit coupling for electrons moving along the electric field direction. We propose applications of this effect to measurements of spin-orbit coupling anisotropy and separation of spin noise of conducting and localized electrons.

Braid group and topological phase transitions in nonequilibrium stochastic dynamics.

We show that distinct topological phases of the band structure of a non-Hermitian Hamiltonian can be classified with elements of the braid group. As the proof of principle, we consider the non-Hermitian evolution of the statistics of nonequilibrium stochastic currents. We show that topologically nontrivial phases have detectable properties, including the emergence of decaying oscillations of parity and state probabilities, and discontinuities in the steady state statistics of currents.

Nonadiabatic transitions in exactly solvable quantum mechanical multichannel model: role of level curvature and counterintuitive behavior.

We derive an exact solution of an explicitly time-dependent multichannel model of quantum mechanical nonadiabatic transitions. In the limit N≫1, where N is the number of states, we find that the survival probability of the initially populated state remains finite despite an almost arbitrary choice of a large number of parameters. This observation proves that quantum mechanical nonadiabatic transitions among a large number of states can effectively keep memory about the initial state of the system. This property can lead to a strongly nonergodic behavior even in the thermodynamic limit of some systems with a broad distribution of coupling constants and the lack of energy conservation.

Role of nuclear quadrupole coupling on decoherence and relaxation of central spins in quantum dots.

Strain-induced gradients of local electric fields in semiconductor quantum dots can couple to the quadrupole moments of nuclear spins. We develop a theory describing the influence of this quadrupolar coupling on the spin correlators of electron and hole "central" spins localized in such dots. We show that when the quadrupolar coupling strength is comparable to or larger than the hyperfine coupling strength between nuclei and the central spin, the relaxation rate of the central spin is strongly enhanced and can be exponential. We demonstrate a good agreement with recent experiments on spin relaxation in hole-doped (In,Ga)As self-assembled quantum dots.

Sensitivity field for nonautonomous molecular rotors.

We propose a numerical approach to quantify the control of a nonautonomous molecular rotor motion. Unlike straightforward molecular dynamics simulations in an explicitly time-dependent framework, our method is based on the theory of geometric phases. This theory allows us to define a sensitivity field (SF) in control parameter space that characterizes average motion of a molecule induced by a cyclic perturbation. We show that the SF can be obtained using only equilibrium free energy sampling techniques. A density plot of the SF quantifies response of a molecule to an arbitrary cyclic adiabatic evolution of parameters. For demonstration, we numerically find the SFs for two surface mounted molecular rotor molecules that can be driven, in practice, by strong time-dependent electric fields of a STM tip.

Time-dependent corrections to effective rate and event statistics in Michaelis-Menten kinetics.

The authors generalise the concept of the geometric phase in stochastic kinetics to a non-cyclic evolution. Its application is demonstrated on kinetics of the Michaelis-Menten reaction. It is shown that the non-periodic geometric phase is responsible for the correction to the Michaelis-Menten law when parameters, such as a substrate concentration, are changing with time. The authors apply these ideas to a model of chemical reactions in a bacterial culture of a growing size, where the geometric correction qualitatively changes the outcome of the reaction kinetics.

Robust quantization of a molecular motor motion in a stochastic environment.

We explore quantization of the response of a molecular motor to periodic modulation of control parameters. We formulate the pumping-quantization theorem (PQT) that identifies the conditions for robust integer quantized behavior of a periodically driven molecular machine. Implication of PQT on experiments with catenane molecules are discussed.

Adiabatic coarse-graining and simulations of stochastic biochemical networks.

We propose a universal approach for analysis and fast simulations of stiff stochastic biochemical networks, which rests on elimination of fast chemical species without a loss of information about mesoscopic, non-Poissonian fluctuations of the slow ones. Our approach is similar to the Born-Oppenheimer approximation in quantum mechanics and follows from the stochastic path integral representation of the cumulant generating function of reaction events. In applications with a small number of chemical reactions, it produces analytical expressions for cumulants of chemical fluxes between the slow variables. This allows for a low-dimensional, interpretable representation and can be used for high-accuracy, low-complexity coarse-grained numerical simulations. As an example, we derive the coarse-grained description for a chain of biochemical reactions and show that the coarse-grained and the microscopic simulations agree, but the former is 3 orders of magnitude faster.

Mesoscopic statistical properties of multistep enzyme-mediated reactions.

Enzyme-mediated reactions may proceed through multiple intermediate conformational states before creating a final product molecule, and one often wishes to identify such intermediate structures from observations of the product creation. In this study, the authors address this problem by solving the chemical master equations for various enzymatic reactions. A perturbation theory analogous to that used in quantum mechanics allows the determination of the first (n) and the second (σ2) cumulants of the distribution of created product molecules as a function of the substrate concentration and the kinetic rates of the intermediate processes. The mean product flux V=d(n)/dt (or 'dose-response' curve) and the Fano factor F= σ2/(n) are both realistically measurable quantities, and whereas the mean flux can often appear the same for different reaction types, the Fano factor can be quite different. This suggests both qualitative and quantitative ways to discriminate between different reaction schemes, and the authors explore this possibility in the context of four sample multistep enzymatic reactions. Measuring both the mean flux and the Fano factor can not only discriminate between reaction types, but can also provide some detailed information about the internal, unobserved kinetic rates, and this can be done without measuring single-molecule transition events.

Pumping restriction theorem for stochastic networks.

We formulate an exact result, which we refer to as the pumping restriction theorem (PRT). It imposes strong restrictions on the currents generated by periodic driving in a generic dissipative system with detailed balance, and provides a universal nonperturbative approach to explore the stochastic pump effect in nonadiabatically driven systems.

Absence of skew scattering in two-dimensional systems: testing the origins of the anomalous Hall effect.

We study the anomalous Hall conductivity in spin-polarized, asymmetrically confined two-dimensional electron and hole systems, taking into account the intrinsic, side-jump, and skew-scattering contributions to the transport. We find that the skew scattering, principally responsible for the extrinsic contribution to the anomalous Hall effect, vanishes for the two-dimensional electron system if both chiral Rashba subbands are partially occupied, and vanishes always for the two-dimensional hole gas studied here, regardless of the band filling. Our prediction can be tested with the proposed coplanar two-dimensional electron-hole gas device and can be used as a benchmark to understand the crossover from the intrinsic to the extrinsic anomalous Hall effect.

Universal geometric theory of mesoscopic stochastic pumps and reversible ratchets.

We construct a unifying theory of geometric effects in mesoscopic stochastic kinetics. We demonstrate that the adiabatic pump and the reversible ratchet effects, as well as similar new phenomena in other domains, such as in epidemiology, all follow from very similar geometric phase contributions to the effective action in the stochastic path integral representation of the moment generating function. The theory provides the universal technique for identification, prediction, and calculation of pumplike phenomena in an arbitrary mesoscopic stochastic framework.

Charge and spin Hall conductivity in metallic graphene.

Graphene has an unusual low-energy band structure with four chiral bands and half-quantized and quantized Hall effects that have recently attracted theoretical and experimental attention. We study the Fermi energy and disorder dependence of its spin Hall conductivity sigma(xy)(SH). In the metallic regime we find that vertex corrections enhance the intrinsic spin Hall conductivity and that skew scattering can lead to sigma(xy)(SH) values that exceed the quantized ones expected when the chemical potential is inside the spin-orbit induced energy gap. We predict that large spin Hall conductivities will be observable in graphene even when the spin-orbit gap does not survive disorder.

Semiclassical spin transport in spin-orbit-coupled bands.

Motivated by recent interest in novel spintronics effects, we develop a semiclassical theory of spin transport that is valid for spin-orbit coupled bands. Aside from the obvious convective term in which the average spin is transported at the wave packet group velocity, the spin current has additional contributions from the wave packet's spin and torque dipole moments. Electric field corrections to the group velocity and carrier spin contribute to the convective term. Summing all terms we obtain an expression for the intrinsic spin-Hall conductivity of a hole-doped semiconductor, which agrees with the Kubo formula prediction for the same quantity. We discuss the calculation of spin accumulation, which illustrates the importance of the torque dipole near the boundary of the system.

Universal intrinsic spin Hall effect.

We describe a new effect in semiconductor spintronics that leads to dissipationless spin currents in paramagnetic spin-orbit coupled systems. We argue that in a high-mobility two-dimensional electron system with substantial Rashba spin-orbit coupling, a spin current that flows perpendicular to the charge current is intrinsic. In the usual case where both spin-orbit split bands are occupied, the intrinsic spin-Hall conductivity has a universal value for zero quasiparticle spectral broadening.