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Results for “Quantum transport simulation”

Search indexed NASA NTRS and DOE OSTI research on propulsion, heat transfer, battery materials and energy systems. Follow report and document links to the original sources.

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At least 289 records · Page 16
All sourcesNASA NTRSDOE OSTI
DOE OSTI2024

Writing and Detecting Topological Charges in Exfoliated Fe 5– x GeTe 2

Fe 5–x GeTe 2 is a promising two-dimensional (2D) van der Waals (vdW) magnet for practical applications, given its magnetic properties. These include Curie temperatures above room temperature, and topological spin textures–TST (both merons and skyrmions), responsible for a pronounced anomalous Hall effect (AHE) and its topological counterpart (THE), which can be harvested for spintronics. Here, we show that both the AHE and THE can be amplified considerably by just adjusting the thickness of exfoliated Fe 5–x GeTe 2 , with THE becoming observable even in zero magnetic field due to a field-induced unbalance in topological charges. Using a complementary suite of techniques, including electronic transport, Lorentz transmission electron microscopy, and micromagnetic simulations, we reveal the emergence of substantial coercive fields upon exfoliation, which are absent in the bulk, implying thickness-dependent magnetic interactions that affect the TST. We detected a “magic” thickness t ≈ 30 nm where the formation of TST is maximized, inducing large magnitudes for the topological charge density (~6.45 × 10 20 cm –2 ), and the concomitant anomalous (ρ xy A,max ≃22.6 μΩ cm) and topological (ρ xy u,T 1≃5 μΩ cm) Hall resistivities at T ≈ 120 K. These values for ρ xy A,max and ρ xy u,T are higher than those found in magnetic topological insulators and, so far, the largest reported for 2D magnets. Furthermore, the hitherto unobserved THE under zero magnetic field could provide a platform for the writing and electrical detection of TST aiming at energy-efficient devices based on vdW ferromagnets.

77 NANOSCIENCE AND NANOTECHNOLOGY↗
DOE OSTI2021

Geometry and dynamics of passive scalar structures in compressible turbulent mixing

We present a structure-based numerical analysis of passive scalar mixing in decaying homogeneous isotropic turbulence (DHIT) and shock-turbulence interaction canonical configurations. The analysis focuses on the temporal evolution of ensembles of passive scalar structures, initialized as spheres of different sizes relative to the Taylor microscale. An algorithm is introduced to track the evolution of each individual structure and the interactions with other structures in the ensemble, relating changes in the surface geometry and the underlying physical processes (turbulent transport, scalar dissipation, and shock compression). The tracking algorithm is applied to datasets from shock-capturing direct numerical simulations of DHIT, with Taylor microscale Reynolds number Re λ =40 and turbulence Mach number M t =0.2 ⁠, and STI cases in which the turbulence is processed by a shock wave at Mach numbers M = 1.5 and 3.0. Temporal surface convolution increases for initially larger structures, resulting in a higher probability of locally hyperbolic geometries where breakup into smaller structures occurs. Shock-induced deformation of the structures amplifies breakup processes, enhancing mixing, particularly for larger structures. Mixing enhancement by the shock is manifested as an amplification of the surface-averaged scalar gradient, which increases for initially larger structures. The alignment between the scalar gradient and the most extensional strain-rate eigendirection on the scalar isosurfaces also increases across the shock. Larger magnitudes of the scalar gradient and its alignment with the most compressive strain-rate eigendirection correlate with flatter surface regions. Shock-induced structure compression increases the area coverage of flat regions, where the amplification of scalar gradient is localized.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2025

Elucidating ion capture and transport mechanisms of Preyssler anions in aqueous solutions using biased MACE-accelerated MD simulations

Equilibrium and biased multi-atomic cluster expansion (MACE) accelerated molecular dynamics (MD) simulations in aqueous solutions are performed to investigate the ion capture and transport mechanisms of the {P 5 W 30 } Preyssler anion (PA) as the smallest representative member of the extended polyoxometalate (POM) family with an internal cavity. The unique interatomic interactions present in the internal cavity vs the exterior of PA are carefully investigated using equilibrium MACE MD simulations for two representative Na(H 2 O)@PA and Na@PA complexes in aqueous solutions. Our careful analyses of radial distribution functions and coordination numbers show that the presence of confined water in Na(H 2 O)@PA has profound modulating effects on the nature of the interactions of the encapsulated ion with the oxygens of the PA cavity. Using well-converged MACE-accelerated multiple walker well-tempered metadynamics simulations with nanosecond timescales, two different associative (ion exchange) and dissociative (ion ejection) ion transport mechanisms were carefully investigated for Na + as one of the most abundant and representative ions present in seawater and saline solutions. By comparing systems with and without confined water, it was found that the presence of only one pre-encapsulated confined water in Na(H 2 O)@PA dramatically changes the free energy landscape of ion transport processes. It was also found that the contraction and dilation of the two windows present in PA directly influence the Na + and H 2 O transport. Furthermore, the results from this work are helpful, as they show a viable path toward tuning the ion exchange and transport phenomena in aqueous solutions of POM molecular clusters and frameworks.

25 ENERGY STORAGE↗
DOE OSTI2026

Effect of Magnetic Islands on Neoclassical Heat Diffusivity in a Global Tokamak Simulation

Resonant magnetic perturbations (RMPs) alter magnetic field topology via island formation and can modify core transport in toroidal fusion devices. Using the global gyrokinetic particle‐in‐cell code XGC‐S, originally developed for stellarator geometries, we quantify how island topology affects neoclassical heat transport in a circular tokamak with ($m,n$) = (5,2) RMP‐induced islands. Electron radial heat diffusivity exhibits a two‐peak structure with a dominant enhancement near the O/X‐point region and a secondary peak at the outer island boundary, whereas ion transport remains close to the neoclassical prediction. The observed electron diffusivity is strongly enhanced over the neoclassical baseline but remains well below the Rechester–Rosenbluth estimate, consistent with the non‐ergodic character of the island topology. The density dependence of diffusivity is weaker inside the islands than outside, indicating the presence of topology‐driven transport channels that do not depend strongly on collisionality. Two‐dimensional heat flux maps reveal an up–down antisymmetric structure at the island separatrices consistent with magnetic gradient and curvature drift effects, in contrast to the symmetric temperature flattening inside the islands. These results identify topology‐dependent avenues for electron heat transport in RMP‐perturbed cores and suggest regimes in which island geometry, rather than collisions alone, governs radial transport.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2024

Bipartite mutual information in classical many-body dynamics

Information theoretic measures have helped to sharpen our understanding of many-body quantum states. As perhaps the most well-known example, the entanglement entropy (or more generally, the bipartite mutual information) has become a powerful tool for characterizing the dynamical growth of quantum correlations. By contrast, although computable, the bipartite mutual information (MI) is almost never explored in classical many particle systems; this owes in part to the fact that computing the MI requires keeping track of the evolution of the full probability distribution, a feat which is rarely done (or thought to be needed) in classical many-body simulations. Here, we utilize the MI to analyze the spreading of information in 1D elementary cellular automata (CA). Broadly speaking, we find that the behavior of the MI in these dynamical systems exhibits a few different types of scaling that roughly correspond to known CA universality classes. Of particular note is that we observe a set of automata for which the MI converges parametrically slowly to its thermodynamic value. We develop a microscopic understanding of this behavior by analyzing a two-species model of annihilating particles moving in opposite directions. Furthermore, our work suggests the possibility that information theoretic tools such as the MI might enable a more fine-grained characterization of classical many-body states and dynamics.

Cellular automata↗
DOE OSTI2020

Selectivity of nitrate and chloride ions in microporous carbons: the role of anisotropic hydration and applied potentials

Understanding ion transport in porous carbons is critical for a wide range of technologies, including supercapacitors and capacitive deionization for water desalination, yet many details remain poorly understood. For instance, an atomistic understanding of how ion selectivity is influenced by the molecular shape of ions, morphology of the micropores and applied voltages is largely lacking. In this work, we combined molecular dynamics simulations with enhanced sampling methods to elucidate the mechanism of nitrate and chloride selectivity in subnanometer graphene slit-pores. We demonstrate that nitrate is preferentially adsorbed over chloride in the slit-like micropores. This preferential adsorption was found to stem from the weaker hydration energy and unique anisotropy of the ion solvation of nitrate. Beside the effects of ion dehydration, we found that applied potential plays an important role in determining the ion selectivity, leading to a lower selectivity of nitrate over chloride at a high applied potential. We conclude that the measured ion selectivity results from a complex interplay between voltage, confinement, and specific ion effects-including ion shape and local hydration structure.

36 MATERIALS SCIENCE↗
DOE OSTI2022

Robust estimation of charge carrier diffusivity using transient photoluminescence microscopy

Transient microscopy has emerged as a powerful tool for imaging the diffusion of excitons and free charge carriers in optoelectronic materials. In many excitonic materials, extraction of diffusion coefficients can be simplified because of the linear relationship between signal intensity and local excited state population. However, in materials where transport is dominated by free charge carriers, extracting diffusivities accurately from multidimensional data is complicated by the nonlinear dependence of the measured signal on the local charge carrier density. To obtain accurate estimates of charge carrier diffusivity from transient microscopy data, statistically robust fitting algorithms coupled to efficient 3D numerical solvers that faithfully relate local carrier dynamics to raw experimental measurables are sometimes needed. Here, we provide a detailed numerical framework for modeling the spatiotemporal dynamics of free charge carriers in bulk semiconductors with significant solving speed reduction and for simulating the corresponding transient photoluminescence microscopy data. To demonstrate the utility of this approach, we apply a fitting algorithm using a Markov chain Monte Carlo sampler to experimental data on bulk CdS and methylammonium lead bromide (MAPbBr 3 ) crystals. Parameter analyses reveal that transient photoluminescence microscopy can be used to obtain robust estimates of charge carrier diffusivities in optoelectronic materials of interest, but that other experimental approaches should be used for obtaining carrier recombination constants. Additionally, simplifications can be made to the fitting model depending on the experimental conditions and material systems studied. Our open-source simulation code and fitting algorithm are made freely available to the scientific community.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2024

Effect of causality constraints on Bayesian analyses of heavy-ion collisions

There have long been questions about the limits to the validity of relativistic fluid dynamics and whether it is being used outside its regime of validity in modern simulations of relativistic heavy-ion collisions. An important new tool for answering this question is a causality analysis in the nonlinear regime—if the solutions of the evolution equations do not respect relativistic causality, then they are not a faithful representation of the underlying relativistic theory (in this case, quantum chromodynamics). Using this nonlinear criterion, it has recently been shown that hydrodynamics is indeed being used outside its regime of validity in simulations, at least sometimes. Here we explore the phenomenological implications, particularly the quantitative effects of demanding limits on acausality in modern Bayesian parameter estimation. We find that, while typically only a small fraction of the system's energy is initially in an acausal regime, placing strict limits on the allowed energy fraction significantly changes the preferred properties of the initial condition, which in turn alters the extracted medium properties such as bulk viscosity, where large values are no longer favored. Furthermore, these findings highlight the importance of developing better theoretical descriptions of the early-time, out-of-equilibrium dynamics of relativistic heavy-ion collisions.

Bayesian methods↗
DOE OSTI2024

Hydrogen Diffusion in Slit Pores: Role of Temperature, Pressure, Confinement, and Roughness

Diffusion of hydrogen (H 2 ) is important to understand the leakage risk and transport behavior for H 2 geologic storage. We applied molecular dynamics simulations to investigate the influencing factors of H2 diffusion in the slit pores of calcite, hematite, and quartz, owing to their abundance. It is revealed that the H2 self-diffusion coefficient increases with the temperature, regardless of the type of pore minerals. The diffusion of H 2 in the 20 nm slit pores falls into the bulk diffusion regime when the pressure is 10 MPa. The self-diffusion of H 2 decreases with pressure in all three types of slit pores, following a power law model with the exponents ranging from -0.825 to -0.964. Furthermore, the impact of confinement on H 2 diffusion is more pronounced for the slit pores with stronger interactions with H 2 -like calcite. The role of surface roughness in H 2 diffusion depends on the slit aperture. The rough surface enhances H 2 diffusion in the larger slit pores due to the enlarged effective pore space, whereas it weakens H 2 diffusion in the small slit pores due to stronger adsorption. These findings will fill the knowledge gap on the coupling effect of different factors influencing H 2 diffusion.

08 HYDROGEN↗
DOE OSTI2022

Oxygen and Proton Transport in Flooded Graphene Pores with N-Dopants and Defects

Reactant transport is an important consideration in the design of ideal electrode structures. For the oxygen reduction reaction catalyzed by Pt/C in proton exchange membrane fuel cell cathodes, O 2 and H + delivery to Pt surfaces and H 2 O transport away are required. Some Pt nanoparticles may only be accessible via micropores that are too small for ionomer molecules to enter, possibly requiring flooding for H + transport. Here, to test if these “buried” Pt particles can play a role in activity through this proposed transport mechanism, we have performed atomic-scale simulations based on reactive force field molecular dynamics with an emphasis on confinement below 20 Å. Diffusion coefficients as a function of the molar concentration and local environment have been evaluated in water domains confined in two-dimensional graphene nanochannels of various channel heights representing a morphological model for micropores in proton exchange fuel cell cathodes. Our study shows that local atomic-scale structures can strongly modify H + , O 2 , and H 2 O transport rates in flooded micropores less than 20 Å in size. We find that there is a critical crossover in diffusion behavior around the 20 Å spacing with larger pores having bulk-like diffusion properties and confinement below 20 Å monotonically decreases diffusion rates. As pore size decreases, we observe locally dispersed water regions that ultimately strand reactants from long-distance transport. These findings suggest that flooded micropores may in fact be viable transport pathways for relevant reactants and products if the pore walls on opposite sides remain separated by ≥10 Å separation. Furthermore, the confinement effect is so strong that N-doping and C-vacancy defects in the C pore wall have only a minimal impact on diffusion rates and their effects are counterintuitively more apparent at larger spacings. These findings provide valuable insight regarding cathode performance and the role “stranded” catalyst particles may play in fuel cell cathodes.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2023

Staggered scheme for the compressible fluctuating hydrodynamics of multispecies fluid mixtures

Here, we present a numerical formulation for the solution of nonisothermal, compressible Navier-Stokes equations with thermal fluctuations to describe mesoscale transport phenomena in multispecies fluid mixtures. The novelty of our numerical method is the use of staggered grid momenta along with a finite volume discretization of the thermodynamic variables to solve the resulting stochastic partial differential equations. The key advantages of the numerical scheme are that it significantly simplifies the discretization of diffusive and stochastic momentum fluxes into a more compact form, and it provides an unambiguous prescription of boundary conditions involving pressure. The staggered grid scheme more accurately reproduces the equilibrium static structure factor of hydrodynamic fluctuations in gas mixtures compared to a collocated scheme described previously by Balakrishnan et al. [Phys. Rev. E 89, 013017 (2014)1539-375510.1103/PhysRevE.89.013017]. The numerical method is tested for ideal noble gases mixtures under various nonequilibrium conditions, such as applied thermal and concentration gradients, to assess the role of cross-diffusion effects, such as Soret and Dufour, on the long-ranged correlations of hydrodynamic fluctuations, which are also more accurately reproduced compared to the collocated scheme. We numerically study giant nonequilibrium fluctuations driven by concentration gradients and fluctuation-driven Rayleigh-Taylor instability in gas mixtures. Wherever applicable, excellent agreement is observed with theory and measurements from the direct simulation Monte Carlo method.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2021

Interpretation of electromagnetic modes in the sub-TAE frequency range in JET plasmas with elevated monotonic q-profiles

Recent JET deuterium experiments with an advanced tokamak scenario using an internal transport barrier (ITB) have been performed to clearly observe destabilized toroidicity-induced Alfvén eigenmodes (TAEs) by fast ions; interestingly, these also exhibit unstable electromagnetic (EM) perturbations in the sub-TAE frequency range. We identify such EM perturbations to be beta-induced ion temperature gradient (BTG) eigenmodes and not beta-induced Alfvén eigenmodes nor beta-induced Alfvén acoustic eigenmodes, which are often unstable in such high-beta plasmas with high-power neutral beam injection (NBI). The BTG modes are the most unstable modes due to the high thermal ion temperature gradient related to the ITB, high thermal ion temperature compared to thermal electron temperature (high T i /T⁠ e ), and a high ion beta regime. BTG mode experimental characteristics match the analytical theory, i.e., location in the vicinity of a rational magnetic surface with a low magnetic shear, mode frequency scaling with the ion diamagnetic frequency (⁠ω$^*_i$⁠), and a coupling among Alfvén and drift waves. We also perform linear gyrokinetic simulations with validated plasma profiles and equilibrium, and find a mode kinetically driven by thermal ions with similar characteristics as the experimental BTG modes.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2025

Exploring transport mechanisms in atomic precision advanced manufacturing enabled pn junctions

We investigate the different transport mechanisms that can occur in pn junction devices made using atomic precision advanced manufacturing at temperatures ranging from cryogenic to room temperature. We first elucidate the potential cause of the anomalous behavior observed in the forward-bias response of these devices in recent cryogenic temperature measurements, which deviates from the theoretical response of a silicon Esaki diode. These anomalous behaviors include current suppression at low voltages in the forward-bias response and a much lower valley voltage at cryogenic temperatures than theoretically expected for a silicon diode. To investigate the potential causes of these anomalies, we studied the effects of a few possible transport mechanisms, including band-to-band tunneling, bandgap narrowing, potential impact of non-Ohmic contacts, band quantization, impact of leakage, and inelastic trap-assisted tunneling, through semi-classical simulations. We find that a combination of two sets of band-to-band tunneling (BTBT) parameters can qualitatively approximate the shape of the tunneling current at low bias. This can arise from band quantization and realignment due to the strong potential confinement in δ-layers. We also find that the lower-than-theoretically-expected valley voltage can be attributed to modifications in the electronic band structure within the δ-layer regions, leading to a significant bandgap narrowing induced by the high density of dopants. Finally, we extend our analyses to room temperature operation and predict that trap-assisted tunneling (TAT) facilitated by phonon interactions may become significant, leading to a complex superposition of BTBT and TAT transport mechanisms in the electrical measurements.

band gap↗
DOE OSTI2024

Wall modes and the transition to bulk convection in rotating Rayleigh-Bénard convection

We investigate states of rapidly rotating Rayleigh-Bénard convection in a cylindrical cell over a range of Rayleigh numbers 3 × 10 5 ≤ Ra ≤ 5 × 10 9 and Ekman numbers 10 − 6 ≤ Ek ≤ 10 − 4 for Prandtl number Pr = 0.8 and aspect ratios 1 / 5 ≤ Γ ≤ 5 using direct numerical simulations. We characterize, for perfectly insulating sidewall boundary conditions, the first transition to convection via wall mode instability and the nonlinear growth and instability of the resulting wall mode states, including a secondary transition to time dependence. We show how the radial structure of the vertical velocity u z and the temperature T is captured well by the linear eigenfunctions of the wall mode instability where the radial width of u z is δ u z ∼ Ek 1 / 3 r / H whereas δ T ∼ e − k r ( k is the wave number of a laterally infinite wall mode state). The disparity in spatial scales for Ek = 10 − 6 means that the heat transport is dominated by the radial structure of u z since T varies slowly over the radial scale δ u z . We further describe how the transition to a state of bulk convection is influenced by the presence of the wall mode states. We use temporal and spatial scales as measures of the local state of convection and the Nusselt number Nu as representative of global transport. Our results elucidate the evolution of the wall state of rotating convection and confirm that wall modes are strongly linked with the boundary zonal flow being the robust remnant of nonlinear wall mode states. We also show how the heat transport ( Nu ) contributions of wall modes and bulk modes are related and discuss approaches to disentangling their relative contributions. Published by the American Physical Society 2024

58 GEOSCIENCES↗
DOE OSTI2021

Relevance of hydrogen bonded associates to the transport properties and nanoscale dynamics of liquid and supercooled 2-propanol

2-Propanol was investigated, in both the liquid and supercooled states, as a model system to study how hydrogen bonds affect the structural relaxation and the dynamics of mesoscale structures, of approximately several Ångstroms, employing static and quasi-elastic neutron scattering and molecular dynamics simulation. Dynamic neutron scattering measurements were performed over an exchanged wave-vector range encompassing the pre-peak, indicative of the presence of H-bonding associates, and the main peak. The dynamics observed at the pre-peak is associated with the formation and disaggregation of the H-bonded associates and is measured to be at least one order of magnitude slower than the dynamics at the main peak, which is identified as the structural relaxation. Additionally, the measurements indicate that the macroscopic shear viscosity has a similar temperature dependence as the dynamics of the H-bonded associates, which highlights the important role played by these structures, together with the structural relaxation, in defining the macroscopic rheological properties of the system. Importantly, the characteristic relaxation time at the pre-peak follows an Arrhenius temperature dependence whereas at the main peak it exhibits a non-Arrhenius behavior on approaching the supercooled state. The origin of this differing behavior is attributed to an increased structuring of the hydrophobic domains of 2-propanol accommodating a more and more encompassing H-bond network, and a consequent set in of dynamic cooperativity.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2021

Theory of the effect of external stress on the activated dynamics and transport of dilute penetrants in supercooled liquids and glasses

We generalize the self-consistent cooperative hopping theory for a dilute spherical penetrant or tracer activated dynamics in dense metastable hard sphere fluids and glasses to address the effect of external stress, the consequences of which are systematically established as a function of matrix packing fraction and penetrant-to-matrix size ratio. All relaxation processes speed up under stress, but the difference between the penetrant and matrix hopping (alpha relaxation) times decreases significantly with stress corresponding to less time scale decoupling. A dynamic crossover occurs at a critical “slaving onset” stress beyond which the matrix activated hopping relaxation time controls the penetrant hopping time. This characteristic stress increases (decreases) exponentially with packing fraction (size ratio) and can be well below the absolute yield stress of the matrix. Below the slaving onset, the penetrant hopping time is predicted to vary exponentially with stress, differing from the power law dependence of the pure matrix alpha time due to system-specificity of the stress-induced changes in the penetrant local cage and elastic barriers. An exponential growth of the penetrant alpha relaxation time with size ratio under stress is predicted, and at a fixed matrix packing fraction, the exponential relation between penetrant hopping time and stress for different size ratios can be collapsed onto a master curve. Direct connections between the short- and long-time activated penetrant dynamics and between the penetrant (or matrix) alpha relaxation time and matrix thermodynamic dimensionless compressibility are also predicted. The presented results should be testable in future experiments and simulations.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2021

Resonant amplification of enzymatic chemical oscillations by oscillating flow

Using theory and simulation, we analyzed the resonant amplification of chemical oscillations that occur due to externally imposed oscillatory fluid flows. The chemical reactions are promoted by two enzyme-coated patches located sequentially on the inner surface of a pipe that transports the enclosed chemical solution. In the case of diffusion-limited systems, the period of oscillations in chemical reaction networks is determined by the rate of the chemical transport, which is diffusive in nature and, therefore, can be effectively accelerated by the imposed fluid flows. In this work, we first identify the natural frequencies of the chemical oscillations in the unperturbed reaction–diffusion system and, then, use the frequencies as a forcing input to drive the system to resonance. We demonstrate that flow-induced resonance can be used to amplify the amplitude of the chemical oscillations and to synchronize their frequency to the external forcing. In particular, we show that even 10% perturbations in the flow velocities can double the amplitude of the resulting chemical oscillations. Particularly, effective control can be achieved for the two-step chemical reactions where during the first half-period, the fluid flow accelerates the chemical flux toward the second catalytic patch, while during the second half-period, the flow amplifies the flux to the first patch. The results can provide design rules for regulating the dynamics of coupled reaction–diffusion processes and can facilitate the development of chemical reaction networks that act as chemical clocks.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2021

Ab initio ultrafast spin dynamics in solids

Spin relaxation and decoherence is at the heart of spintronics and spin-based quantum information science. Currently, theoretical approaches that can accurately predict spin relaxation of general solids including necessary scattering pathways and are capable of nanosecond to millisecond simulation time are urgently needed. We present a first-principles real-time density-matrix approach based on Lindblad dynamics to simulate ultrafast spin dynamics for general solid-state systems. Through the complete first-principles descriptions of pump, probe, and scattering processes including electron-phonon, electron-impurity, and electron-electron scatterings with self-consistent electronic spin-orbit couplings, our method can directly simulate the ultrafast pump-probe measurements for coupled spin and electron dynamics over nanoseconds at any temperatures and doping levels. We first apply this method to a prototypical system GaAs and obtain excellent agreement with experiments. We found that the relative contributions of different scattering mechanisms and phonon modes differ considerably between spin and carrier relaxation processes. In sharp contrast to previous work based on model Hamiltonians, we point out that the electron-electron scattering is negligible at room temperature but becomes dominant at low temperatures for spin relaxation in n-type GaAs. We further examine ultrafast dynamics in novel spin-valleytronic materials: monolayer and bilayer WSe 2 with realistic defects. We find that spin relaxation is highly sensitive to local symmetry and chemical bonds around defects. For the bilayer WSe 2 , we identify the scattering pathways in ultrafast dynamics and determine relevant dynamical properties, essential to its utilization of unique spin-valley-layer locking effects. In conclusion, our work provides a predictive computational platform for spin dynamics in solids, which has potential for designing new materials ideal for spintronics and quantum information technology.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗