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We report the first numerical prediction of a "spin microemulsion" -- a phase with undulating spin domains resembling classical bicontinuous oil-water-surfactant emulsions -- in two-dimensional systems of spinor Bose-Einstein condensates with isotropic Rashba spin-orbit coupling. Using field-theoretic numerical simulations, we investigated the melting of a low-temperature stripe phase with supersolid character and find that the stripes lose their superfluidity at elevated temperature and undergo a Kosterlitz--Thouless-like transition into a spin microemulsion. Momentum distribution calculations highlight a thermally broadened occupation of the Rashba circle of low-energy states with macroscopic and isotropic occupation around the ring. We provide a finite-temperature phase diagram that positions the emulsion as an intermediate, structured isotropic phase with residual quantum character before transitioning at higher temperature into a structureless normal fluid., Comment: Main text: 7 pages, 5 figures. Supplementary Material: 5 pages, 5 figures

A computational framework that leverages data from self-consistent field theory simulations with deep learning to accelerate the exploration of parameter space for block copolymers is presented. This is a substantial two-dimensional extension of the framework introduced in [1]. Several innovations and improvements are proposed. (1) A Sobolev space-trained, convolutional neural network (CNN) is employed to handle the exponential dimension increase of the discretized, local average monomer density fields and to strongly enforce both spatial translation and rotation invariance of the predicted, field-theoretic intensive Hamiltonian. (2) A generative adversarial network (GAN) is introduced to efficiently and accurately predict saddle point, local average monomer density fields without resorting to gradient descent methods that employ the training set. This GAN approach yields important savings of both memory and computational cost. (3) The proposed machine learning framework is successfully applied to 2D cell size optimization as a clear illustration of its broad potential to accelerate the exploration of parameter space for discovering polymer nanostructures. Extensions to three-dimensional phase discovery appear to be feasible.

We develop a multiscale simulation model for diffusion of solutes through porous triblock copolymer membranes. The approach combines two techniques: self-consistent field theory (SCFT) to predict the structure of the self-assembled, solvated membrane and on-lattice kinetic Monte Carlo (kMC) simulations to model diffusion of solutes. Solvation is simulated in SCFT by constraining the glassy membrane matrix while relaxing the brush-like membrane pore coating against the solvent. The kMC simulations capture the resulting solute spatial distribution and concentration-dependent local diffusivity in the polymer-coated pores; we parameterize the latter using particle-based simulations. We apply our approach to simulate solute diffusion through nonequilibrium morphologies of a model triblock copolymer, and we correlate diffusivity with structural descriptors of the morphologies. We also compare the model's predictions to alternative approaches based on simple lattice random walks and find our multiscale model to be more robust and systematic to parameterize. Our multiscale modeling approach is general and can be readily extended in the future to other chemistries, morphologies, and models for the local solute diffusivity and interactions with the membrane.

QMCPACK is an open source quantum Monte Carlo package for ab-initio electronic structure calculations. It supports calculations of metallic and insulating solids, molecules, atoms, and some model Hamiltonians. Implemented real space quantum Monte Carlo algorithms include variational, diffusion, and reptation Monte Carlo. QMCPACK uses Slater-Jastrow type trial wave functions in conjunction with a sophisticated optimizer capable of optimizing tens of thousands of parameters. The orbital space auxiliary field quantum Monte Carlo method is also implemented, enabling cross validation between different highly accurate methods. The code is specifically optimized for calculations with large numbers of electrons on the latest high performance computing architectures, including multicore central processing unit (CPU) and graphical processing unit (GPU) systems. We detail the program's capabilities, outline its structure, and give examples of its use in current research calculations. The package is available at http://www.qmcpack.org .

Auger recombination is an important non-radiative carrier recombination mechanism in many classes of optoelectronic devices. The microscopic Auger processes can be either direct or indirect, mediated by an additional scattering mechanism such as the electron-phonon interaction. Phonon-assisted Auger recombination is particularly strong in nitride materials and affects the efficiency of nitride optoelectronic devices at high powers. Here we present a first-principles computational formalism for the study of direct and indirect Auger recombination in direct-band-gap semiconductors and apply it to the case of nitride materials. We show that direct Auger recombination is weak in the nitrides and cannot account for experimental measurements. On the other hand, carrier scattering by phonons and alloy disorder enables indirect Auger processes that can explain the observed loss in devices. We analyze the dominant phonon contributions to the Auger recom- bination rate and the influence of temperature and strain on the values of the Auger coefficients. Auger processes assisted by charged-defect scattering are much weaker than the phonon-assisted ones for realistic defect densities and not important for the device performance. The computational formalism is general and can be applied to the calculation of the Auger coefficient in other classes of optoelectronic materials.

Field-theoretic models have been used extensively to study the phase behavior of inhomogeneous polymer melts and solutions, both in self-consistent mean-field calculations and in numerical simulations of the full theory capturing composition fluctuations. The models commonly used can be grouped into two categories, namely {\it species} models and {\it exchange} models. Species models involve integrations of functionals that explicitly depend on fields originating both from species density operators and their conjugate chemical potential fields. In contrast, exchange models retain only linear combinations of the chemical potential fields. In the two-component case, development of exchange models has been instrumental in enabling stable complex Langevin (CL) simulations of the full complex-valued theory. No comparable stable CL approach has yet been established for field theories of the species type. Here we introduce an extension of the exchange model to an arbitrary number of components, namely the multi-species exchange (MSE) model, which greatly expands the classes of soft material systems that can accessed by the complex Langevin simulation technique. We demonstrate the stability and accuracy of the MSE-CL sampling approach using numerical simulations of triblock and tetrablock terpolymer melts, and tetrablock quaterpolymer melts. This method should enable studies of a wide range of fluctuation phenomena in multiblock/multi-species polymer blends and composites., Comment: 22 pages, 9 figures

First-principles calculations reveal a large cooperative coupling of Jahn-Teller (JT) distortion to oxygen-octahedron rotations in perovskite LaMnO$_3$. The combination of the two distortions is responsible for stabilizing the strongly orthorhombic $A$-AFM insulating ($I$) $Pbnm$ ground state relative to a metallic ferromagnetic (FM-$M$) phase. However, epitaxial strain due to coherent matching to a crystalline substrate can change the relative stability of the two states. In particular, coherent matching to a square-lattice substrate favors the less orthorhombic FM-$M$ phase, with the $A$-AFM phase stabilized at higher values of tensile epitaxial strain due to its larger volume per formula unit, resulting in a coupled magnetic and metal-insulator transition at a critical strain close to 1%. At the phase boundary, colossal magneto-resistance is expected. Tensile epitaxial strain enhances the JT distortion and opens the band gap in the $A$-AFM-$I$ $c$-$Pbnm$ phase, offering the opportunity for band-gap engineering. Compressive epitaxial strain induces an orientational transition within the FM-$M$ phase from $c$-$Pbnm$ to $ab$-$Pbnm$ with a change in the direction of the magnetic easy axis relative to the substrate, yielding strain-controlled magnetization at the phase boundary. The strong couplings between the JT distortion, the oxygen-octahedron rotations and the magnetic and electronic properties, and associated functional behavior, motivate interest in other orthorhombic $Pbnm$ perovskites with large JT distortions, which should also exhibit a rich variety of coupled magnetic, structural and electronic phase transitions driven by epitaxial strain., Comment: 5 figures

We introduce a stable and efficient complex Langevin (CL) scheme to enable the first numerical simulations of the coherent-states (CS) formulation of polymer field theory. In contrast with Edwards' well known auxiliary-field (AF) framework, the CS formulation does not contain an embedded non-linear, non-local functional of the auxiliary fields, and the action of the field theory has a fully explicit, finite-order and semi-local polynomial character. In the context of a polymer solution model, we demonstrate that the new CS-CL dynamical scheme for sampling fluctuations in the space of coherent states yields results in good agreement with now-standard AF simulations. The formalism is potentially applicable to a broad range of polymer architectures and may facilitate systematic generation of trial actions for use in coarse-graining and numerical renormalization-group studies., Comment: 14pages 8 figures

We report the first CUDA graphics-processing-unit (GPU) implementation of the polymer field-theoretic simulation framework for determining fully fluctuating expectation values of equilibrium properties for periodic and select aperiodic polymer systems. Our implementation is suitable both for self-consistent field theory (mean-field) solutions of the field equations, and for fully fluctuating simulations using the complex Langevin approach. Running on NVIDIA Tesla T20 series GPUs, we find double-precision speedups of up to 30x compared to single-core serial calculations on a recent reference CPU, while single-precision calculations proceed up to 60x faster than those on the single CPU core. Due to intensive communications overhead, an MPI implementation running on 64 CPU cores remains two times slower than a single GPU., Comment: (12 pages, 7 figures)

Topological defects in ordered states with spontaneously broken symmetry often have unusual physical properties, such as fractional electric charge or a quantised magnetic field-flux, originating from their non-trivial topology. Coupled topological defects in systems with several coexisting orders give rise to unconventional functionalities, such as the electric-field control of magnetisation in multiferroics resulting from the coupling between the ferroelectric and ferromagnetic domain walls. Hexagonal manganites provide an extra degree of freedom: In these materials, both ferroelectricity and magnetism are coupled to an additional, non-ferroelectric structural order parameter. Here we present a theoretical study of topological defects in hexagonal manganites based on Landau theory with parameters determined from first-principles calculations. We explain the observed flip of electric polarisation at the boundaries of structural domains, the origin of the observed discrete vortices, and the clamping between ferroelectric and antiferromagnetic domain walls. We show that structural vortices induce magnetic ones and that, consistent with a recent experimental report, ferroelectric domain walls can carry a magnetic moment., Comment: 19 pages, 5 figures

The atomic and electronic structures of ErAs nanoparticles embedded within a GaAs matrix are examined via cross-sectional scanning tunneling microscopy and spectroscopy (XSTM/XSTS). The local density of states (LDOS) exhibits a finite minimum at the Fermi level demonstrating that the nanoparticles remain semimetallic despite the predictions of previous models of quantum confinement in ErAs. We also use XSTS to measure changes in the LDOS across the ErAs/GaAs interface and propose that the interface atomic structure results in electronic states that prevent the opening of a band gap., Comment: 9 pages, 3 figure

We evaluate the interplay between epitaxial strain and oxygen vacancy formation in the perovskite-structure oxide lanthanum aluminate, LaAlO$_3$. Using density functional theory within the GGA$+U$ approximation we calculate the dependence of the oxygen vacancy formation energy on the biaxial strain conditions. We find that the change in formation energy with strain is negligible over the range of strain values usually accessible through coherent epitaxial growth. Our findings suggest that experimental reports of different oxygen vacancy concentrations in strained films result from extrinsic factors, or from other impurities such as defect complexes.

We investigated the rare-earth transition metal oxide series, Ln2CuTiO6 (Ln=Y, Dy, Ho, Er and Yb), crystallizing in the hexagonal structure with non-centrosymmetric P63cm space group for possible occurrences of multiferroic properties. Our results show that while these compounds, except Ln=Y, exhibit a low temperature antiferromagnetic transition due to the ordering of the rare-earth moments, the expected ferroelectric transition is frustrated by the large size difference between Cu and Ti at the B-site. Interestingly, this leads these compounds to attain a rare and unique combination of desirable paraelectric properties with high dielectric constants, low losses and weak temperature and frequency dependencies. First-principles calculations establish these exceptional properties result from a combination of two effects. A significant difference in the MO5 polyhedral sizes for M = Cu and M = Ti suppress the expected co-operative tilt pattern of these polyhedra, required for the ferroelectric transition, leading to relatively large values of the dielectric constant for every compound investigated in this series. Additionally, it is shown that the majority contribution to the dielectric constant arises from intermediate-frequency polar vibrational modes, making it relatively stable against any temperature variation. Changes in the temperature stability of the dielectric constant amongst different members of this series are shown to arise from changes in relative contributions from soft polar modes., Comment: Accepted for publication in Phys. Rev. B (21 pages, 2 Table, 8 Figures)

We calculate the temperature-dependent magnetoelectric response of Cr2O3 from first principles. The form of the dominant magnetoelectric coupling is determined using symmetry arguments, its strength is found using ab initio methods, and the temperature dependence of the response is obtained from Monte Carlo simulations. The quantitative agreement of our results with experiment shows that the strong temperature dependence of the magnetoelectric effect in Cr2O3 results from non-relativistic exchange interactions and spin fluctuations., Comment: 5 pages, 2 figures

We demonstrate that the electronic contribution to the linear magnetoelectric response, usually omitted in first-principles studies, can be comparable in magnitude to that mediated by lattice distortions, even for materials in which responses are strong. Using a self-consistent Zeeman response to an applied magnetic field for noncollinear electron spins, we show how electric polarization emerges in linear magnetoelectrics through both electronic- and lattice-mediated components -- in analogy with the high- and low-frequency dielectric response to an electric field. The approach we use is conceptually and computationally simple, and can be applied to study both linear and non-linear responses to magnetic fields., Comment: 5 pages, 3 figures

We compute the electrical conductivity for liquid hydrogen at high pressure using quantum Monte Carlo. The method uses Coupled Electron-Ion Monte Carlo to generate configurations of liquid hydrogen. For each configuration correlated sampling of electrons is performed in order to calculate a set of lowest many-body eigenstates and current-current correlation functions of the system, which are summed over in the many-body Kubo formula to give AC electrical conductivity directly. The extrapolated DC conductivity at 3000 K for several densities shows a liquid semiconductor to liquid-metal transition at high pressure. Our results are in good agreement with shock-wave data., Comment: 4 pages, 5 figures

We report Auger recombination rates for wurtzite InGaN calculated from first principles density-functional and many-body-perturbation theory. Two different mechanisms are examined -- inter- and intra-band recombination -- that affect different parts of the emission spectrum. In the blue to green spectral region and at room temperature the Auger coefficient can be as large as 2x10^-30cm^6s^-1; in the infrared even larger. Since Auger recombination scales with the cubic power of the free-carrier concentration it becomes an important non-radiative loss mechanism at high current densities. Our results indicate that Auger recombination may be responsible for the loss of quantum efficiency that affects InGaN-based light emitters., Comment: 4 pages including 2 figures

We demonstrate that magnetic vortices in which spins are coupled to polar lattice distortions via superexchange exhibit an unusually large linear magnetoelectric response. We show that the periodic arrays of vortices formed by frustrated spins on Kagom\'e lattices provide a realization of this concept; our {\it ab initio} calculations for such a model structure yield a magnetoelectric coefficient that is 30 times larger than that of prototypical single phase magnetoelectrics. Finally, we identify the design rules required to obtain such a response in a practical material., Comment: 5 pages, 6 figures

We demonstrate that a theoretical framework fully incorporating intra-atomic correlations and multiplet structure of the localized 4f states is required in order to capture the essential physics of rare-earth semiconductors and semimetals. We focus in particular on the rare-earth semimetal erbium arsenide (ErAs), for which effective one-electron approaches fail to provide a consistent picture of both high and low-energy electronic states. We treat the many-body states of the Er 4f shell within an atomic approximation in the framework of dynamical mean-field theory. Our results for the magnetic-field dependence of the 4f local moment, the influence of multiplets on the photoemission spectrum, and the exchange splitting of the Fermi surface pockets as measured from Shubnikov-de Haas oscillations, are found to be in good agreement with experimental results., Comment: 5 pages, 3 figures, 2 tables

Many body trial wave functions are the key ingredient for accurate Quantum Monte Carlo estimates of total electronic energies in many electron systems. In the Coupled Electron-Ion Monte Carlo method, the accuracy of the trial function must be conjugated with the efficiency of its evaluation. We report recent progress in trial wave functions for metallic hydrogen implemented in the Coupled Electron-Ion Monte Carlo method. We describe and characterize several types of trial functions of increasing complexity in the range of the coupling parameter $1.0 \leq r_s \leq1.55$. We report wave function comparisons for disordered protonic configurations and preliminary results for thermal averages., Comment: 11 pages, 6 figures, submitted to Computer Physics Communications

Within many-body perturbation theory we apply vertex corrections to various closed-shell atoms and to jellium, using a local approximation for the vertex consistent with starting the many-body perturbation theory from a DFT-LDA Green's function. The vertex appears in two places -- in the screened Coulomb interaction, W, and in the self-energy, \Sigma -- and we obtain a systematic discrimination of these two effects by turning the vertex in \Sigma on and off. We also make comparisons to standard GW results within the usual random-phase approximation (RPA), which omits the vertex from both. When a vertex is included for closed-shell atoms, both ground-state and excited-state properties demonstrate only limited improvements over standard GW. For jellium we observe marked improvement in the quasiparticle band width when the vertex is included only in W, whereas turning on the vertex in \Sigma leads to an unphysical quasiparticle dispersion and work function. A simple analysis suggests why implementation of the vertex only in W is a valid way to improve quasiparticle energy calculations, while the vertex in \Sigma is unphysical, and points the way to development of improved vertices for ab initio electronic structure calculations., Comment: 8 Pages, 6 Figures. Updated with quasiparticle neon results, extended conclusions and references section. Minor changes: Updated references, minor improvements

A first-order liquid-liquid phase transition in high-pressure hydrogen between molecular and atomic fluid phases has been predicted in computer simulations using ab initio molecular dynamics approaches. However, experiments indicate that molecular dissociation may occur through a continuous crossover rather than a first-order transition. Here we study the nature of molecular dissociation in fluid hydrogen using an alternative simulation technique in which electronic correlation is computed within quantum Monte Carlo, the so-called Coupled Electron Ion Monte Carlo (CEIMC) method. We find no evidence for a first-order liquid-liquid phase transition., Comment: 4 pages, 5 figures; content changed; accepted for publication in Phys. Rev. Lett