arXiv subjects

Linfeng Zhang

Publications and source records attributed to Linfeng Zhang.

At least 307 records · Page 17Linked to original sources

arXiv2021

Modeling liquid water by climbing up Jacob's ladder in density functional theory facilitated by using deep neural network potentials

Within the framework of Kohn-Sham density functional theory (DFT), the ability to provide good predictions of water properties by employing a strongly constrained and appropriately normed (SCAN) functional has been extensively demonstrated in recent years. Here, we further advance the modeling of water by building a more accurate model on the fourth rung of Jacob's ladder with the hybrid functional, SCAN0. In particular, we carry out both classical and Feynman path-integral molecular dynamics calculations of water with the SCAN0 functional and the isobaric-isothermal ensemble. In order to generate the equilibrated structure of water, a deep neural network potential is trained from the atomic potential energy surface based on ab initio data obtained from SCAN0 DFT calculations. For the electronic properties of water, a separate deep neural network potential is trained using the Deep Wannier method based on the maximally localized Wannier functions of the equilibrated trajectory at the SCAN0 level. The structural, dynamic, and electric properties of water were analyzed. The hydrogen-bond structures, density, infrared spectra, diffusion coefficients, and dielectric constants of water, in the electronic ground state, are computed using a large simulation box and long simulation time. For the properties involving electronic excitations, we apply the GW approximation within many-body perturbation theory to calculate the quasiparticle density of states and bandgap of water. Compared to the SCAN functional, mixing exact exchange mitigates the self-interaction error in the meta-generalized-gradient approximation and further softens liquid water towards the experimental direction. For most of the water properties, the SCAN0 functional shows a systematic improvement over the SCAN functional.

physics.chem-ph↗

arXiv2021

Accurate Deep Potential model for the Al-Cu-Mg alloy in the full concentration space

Combining first-principles accuracy and empirical-potential efficiency for the description of the potential energy surface (PES) is the philosopher's stone for unraveling the nature of matter via atomistic simulation. This has been particularly challenging for multi-component alloy systems due to the complex and non-linear nature of the associated PES. In this work, we develop an accurate PES model for the Al-Cu-Mg system by employing Deep Potential (DP), a neural network based representation of the PES, and DP Generator (DP-GEN), a concurrent-learning scheme that generates a compact set of ab initio data for training. The resulting DP model gives predictions consistent with first-principles calculations for various binary and ternary systems on their fundamental energetic and mechanical properties, including formation energy, equilibrium volume, equation of state, interstitial energy, vacancy and surface formation energy, as well as elastic moduli. Extensive benchmark shows that the DP model is ready and will be useful for atomistic modeling of the Al-Cu-Mg system within the full range of concentration.

cond-mat.mtrl-sci↗

arXiv2021

The Phase Diagram of a Deep Potential Water Model

Using the Deep Potential methodology, we construct a model that reproduces accurately the potential energy surface of the SCAN approximation of density functional theory for water, from low temperature and pressure to about 2400 K and 50 GPa, excluding the vapor stability region. The computational efficiency of the model makes it possible to predict its phase diagram using molecular dynamics. Satisfactory overall agreement with experimental results is obtained. The fluid phases, molecular and ionic, and all the stable ice polymorphs, ordered and disordered, are predicted correctly, with the exception of ice III and XV that are stable in experiments, but metastable in the model. The evolution of the atomic dynamics upon heating, as ice VII transforms first into ice VII$''$ and then into an ionic fluid, reveals that molecular dissociation and breaking of the ice rules coexist with strong covalent fluctuations, explaining why only partial ionization was inferred in experiments.

physics.chem-ph↗

arXiv2021

Deep Potential generation scheme and simulation protocol for the Li10GeP2S12-type superionic conductors

It has been a challenge to accurately simulate Li-ion diffusion processes in battery materials at room temperature using {\it ab initio} molecular dynamics (AIMD) due to its high computational cost. This situation has changed drastically in recent years due to the advances in machine learning-based interatomic potentials. Here we implement the Deep Potential Generator scheme to \textit{automatically} generate interatomic potentials for LiGePS-type solid-state electrolyte materials. This increases our ability to simulate such materials by several orders of magnitude without sacrificing {\it ab initio} accuracy. Important technical aspects like the statistical error and size effects are carefully investigated. We further establish a reliable protocol for accurate computation of Li-ion diffusion processes at experimental conditions, by investigating important technical aspects like the statistical error and size effects. Such a protocol and the automated workflow allow us to screen materials for their relevant properties with much-improved efficiency. By using the protocol and automated workflow developed here, we obtain the diffusivity data and activation energies of Li-ion diffusion that agree well with the experiment. Our work paves the way for future investigation of Li-ion diffusion mechanisms and optimization of Li-ion conductivity of solid-state electrolyte materials.

physics.comp-ph↗

arXiv2020

DeePKS: a comprehensive data-driven approach towards chemically accurate density functional theory

We propose a general machine learning-based framework for building an accurate and widely-applicable energy functional within the framework of generalized Kohn-Sham density functional theory. To this end, we develop a way of training self-consistent models that are capable of taking large datasets from different systems and different kinds of labels. We demonstrate that the functional that results from this training procedure gives chemically accurate predictions on energy, force, dipole, and electron density for a large class of molecules. It can be continuously improved when more and more data are available.

physics.comp-ph↗

arXiv2020

Isotope effects on molecular structures and electronic properties of liquid water via deep potential molecular dynamics based on SCAN functional

Feynman path-integral deep potential molecular dynamics (PI-DPMD) calculations have been employed to study both light (H$_2$O) and heavy water (D$_2$O) within the isothermal-isobaric ensemble. In particular, the deep neural network is trained based on ab initio data obtained from the strongly constrained and appropriately normed (SCAN) exchange-correlation functional. Because of the lighter mass of hydrogen than deuteron, the properties of light water is more influenced by nuclear quantum effect than those of heavy water. Clear isotope effects are observed and analyzed in terms of hydrogen-bond structure and electronic properties of water that are closely associated with experimental observables. The molecular structures of both liquid H$_2$O and D$_2$O agree well with the data extracted from scattering experiments. The delicate isotope effects on radial distribution functions and angular distribution functions are well reproduced as well. Our approach demonstrates that deep neural network combined with SCAN functional based ab initio molecular dynamics provides an accurate theoretical tool for modeling water and its isotope effects.

physics.chem-ph↗

arXiv2020

Pandemic risk management: resources contingency planning and allocation

Repeated history of pandemics, such as SARS, H1N1, Ebola, Zika, and COVID-19, has shown that pandemic risk is inevitable. Extraordinary shortages of medical resources have been observed in many parts of the world. Some attributing factors include the lack of sufficient stockpiles and the lack of coordinated efforts to deploy existing resources to the location of greatest needs. The paper investigates contingency planning and resources allocation from a risk management perspective, as opposed to the prevailing supply chain perspective. The key idea is that the competition of limited critical resources is not only present in different geographical locations but also at different stages of a pandemic. This paper draws on an analogy between risk aggregation and capital allocation in finance and pandemic resources planning and allocation for healthcare systems. The main contribution is to introduce new strategies for optimal stockpiling and allocation balancing spatio-temporal competitions of medical supply and demand.

q-fin.RM↗

arXiv2020

Deep Learning of Accurate Force Field of Ferroelectric HfO$_2$

The discovery of ferroelectricity in HfO$_2$-based thin films opens up new opportunities for using this silicon-compatible ferroelectric to realize low-power logic circuits and high-density non-volatile memories. The functional performances of ferroelectrics are intimately related to their dynamic responses to external stimuli such as electric fields at finite temperatures. Molecular dynamics is an ideal technique for investigating dynamical processes on large length and time scales, though its applications to new materials is often hindered by the limited availability and accuracy of classical force fields. Here we present a deep neural network-based interatomic force field of HfO$_2$ learned from {\em ab initio} data using a concurrent learning procedure. The model potential is able to predict structural properties such as elastic constants, equation of states, phonon dispersion relationships, and phase transition barriers of various hafnia polymorphs with accuracy comparable with density functional theory calculations. The validity of this model potential is further confirmed by the reproduction of experimental sequences of temperature-driven ferroelectric-paraelectric phase transitions of HfO$_2$ with isobaric-isothermal ensemble molecular dynamics simulations. We suggest a general approach to extend the model potential of HfO$_2$ to related material systems including dopants and defects.

cond-mat.mtrl-sci↗

arXiv2020

Isotope effects in x-ray absorption spectra of liquid water

The isotope effects in x-ray absorption spectra of liquid water are studied by a many-body approach within electron-hole excitation theory. The molecular structures of both light and heavy water are modeled by path-integral molecular dynamics based on the advanced deep-learning technique. The neural network is trained on ab initio data obtained with SCAN density functional theory. The experimentally observed isotope effect in x-ray absorption spectra is reproduced semiquantitatively in theory. Compared to the spectrum in normal water, the blueshifted and less pronounced pre- and main-edge in heavy water reflect that the heavy water is more structured at short- and intermediate-range of the hydrogen-bond network. In contrast, the isotope effect on the spectrum is negligible at post-edge, which is consistent with the identical long-range ordering in both liquids as observed in the diffraction experiment.

cond-mat.dis-nn↗

arXiv2020

Pushing the limit of molecular dynamics with ab initio accuracy to 100 million atoms with machine learning

For 35 years, {\it ab initio} molecular dynamics (AIMD) has been the method of choice for modeling complex atomistic phenomena from first principles. However, most AIMD applications are limited by computational cost to systems with thousands of atoms at most. We report that a machine learning-based simulation protocol (Deep Potential Molecular Dynamics), while retaining {\it ab initio} accuracy, can simulate more than 1 nanosecond-long trajectory of over 100 million atoms per day, using a highly optimized code (GPU DeePMD-kit) on the Summit supercomputer. Our code can efficiently scale up to the entire Summit supercomputer, attaining $91$ PFLOPS in double precision ($45.5\%$ of the peak) and {$162$/$275$ PFLOPS in mixed-single/half precision}. The great accomplishment of this work is that it opens the door to simulating unprecedented size and time scales with {\it ab initio} accuracy. It also poses new challenges to the next-generation supercomputer for a better integration of machine learning and physical modeling.

physics.comp-ph↗

arXiv2020

86 PFLOPS Deep Potential Molecular Dynamics simulation of 100 million atoms with ab initio accuracy

We present the GPU version of DeePMD-kit, which, upon training a deep neural network model using ab initio data, can drive extremely large-scale molecular dynamics (MD) simulation with ab initio accuracy. Our tests show that the GPU version is 7 times faster than the CPU version with the same power consumption. The code can scale up to the entire Summit supercomputer. For a copper system of 113, 246, 208 atoms, the code can perform one nanosecond MD simulation per day, reaching a peak performance of 86 PFLOPS (43% of the peak). Such unprecedented ability to perform MD simulation with ab initio accuracy opens up the possibility of studying many important issues in materials and molecules, such as heterogeneous catalysis, electrochemical cells, irradiation damage, crack propagation, and biochemical reactions.

physics.comp-ph↗

arXiv2020

Ground state energy functional with Hartree-Fock efficiency and chemical accuracy

We introduce the Deep Post-Hartree-Fock (DeePHF) method, a machine learning based scheme for constructing accurate and transferable models for the ground-state energy of electronic structure problems. DeePHF predicts the energy difference between results of highly accurate models such as the coupled cluster method and low accuracy models such as the the Hartree-Fock (HF) method, using the ground-state electronic orbitals as the input. It preserves all the symmetries of the original high accuracy model. The added computational cost is less than that of the reference HF or DFT and scales linearly with respect to system size. We examine the performance of DeePHF on organic molecular systems using publicly available datasets and obtain the state-of-art performance, particularly on large datasets.

physics.chem-ph↗

arXiv2020

Deep neural network for the dielectric response of insulators

We introduce a deep neural network to model in a symmetry preserving way the environmental dependence of the centers of the electronic charge. The model learns from ab-initio density functional theory, wherein the electronic centers are uniquely assigned by the maximally localized Wannier functions. When combined with the Deep Potential model of the atomic potential energy surface, the scheme predicts the dielectric response of insulators for trajectories inaccessible to direct ab-initio simulation. The scheme is non-perturbative and can capture the response of a mutating chemical environment. We demonstrate the approach by calculating the infrared spectra of liquid water at standard conditions, and of ice under extreme pressure, when it transforms from a molecular to an ionic crystal.

physics.comp-ph↗

arXiv2020

Integrating Machine Learning with Physics-Based Modeling

Machine learning is poised as a very powerful tool that can drastically improve our ability to carry out scientific research. However, many issues need to be addressed before this becomes a reality. This article focuses on one particular issue of broad interest: How can we integrate machine learning with physics-based modeling to develop new interpretable and truly reliable physical models? After introducing the general guidelines, we discuss the two most important issues for developing machine learning-based physical models: Imposing physical constraints and obtaining optimal datasets. We also provide a simple and intuitive explanation for the fundamental reasons behind the success of modern machine learning, as well as an introduction to the concurrent machine learning framework needed for integrating machine learning with physics-based modeling. Molecular dynamics and moment closure of kinetic equations are used as examples to illustrate the main issues discussed. We end with a general discussion on where this integration will lead us to, and where the new frontier will be after machine learning is successfully integrated into scientific modeling.

physics.comp-ph↗

arXiv2020

Neural Canonical Transformation with Symplectic Flows

Canonical transformation plays a fundamental role in simplifying and solving classical Hamiltonian systems. We construct flexible and powerful canonical transformations as generative models using symplectic neural networks. The model transforms physical variables towards a latent representation with an independent harmonic oscillator Hamiltonian. Correspondingly, the phase space density of the physical system flows towards a factorized Gaussian distribution in the latent space. Since the canonical transformation preserves the Hamiltonian evolution, the model captures nonlinear collective modes in the learned latent representation. We present an efficient implementation of symplectic neural coordinate transformations and two ways to train the model. The variational free energy calculation is based on the analytical form of physical Hamiltonian. While the phase space density estimation only requires samples in the coordinate space for separable Hamiltonians. We demonstrate appealing features of neural canonical transformation using toy problems including two-dimensional ring potential and harmonic chain. Finally, we apply the approach to real-world problems such as identifying slow collective modes in alanine dipeptide and conceptual compression of the MNIST dataset.

cond-mat.stat-mech↗

arXiv2020

Raman Spectrum and Polarizability of Liquid Water from Deep Neural Networks

We introduce a scheme based on machine learning and deep neural networks to model the environmental dependence of the electronic polarizability in insulating materials. Application to liquid water shows that training the network with a relatively small number of molecular configurations is sufficient to predict the polarizability of arbitrary liquid configurations in close agreement with ab initio density functional theory calculations. In combination with a neural network representation of the interatomic potential energy surface,the scheme allows us to calculate the Raman spectra along 2-nanosecond classical trajectories at different temperatures for H2O and D2O. The vast gains in efficiency provided by the machine learning approach enable longer trajectories and larger system sizes relative to ab initio methods, reducing the statistical error and improving the resolution of the low-frequency Raman spectra. Decomposing the spectra into intramolecular and intermolecular contributions elucidates the mechanisms behind the temperature dependence of the low-frequency and stretch modes.

physics.chem-ph↗

arXiv2020

Non-Structured DNN Weight Pruning -- Is It Beneficial in Any Platform?

Large deep neural network (DNN) models pose the key challenge to energy efficiency due to the significantly higher energy consumption of off-chip DRAM accesses than arithmetic or SRAM operations. It motivates the intensive research on model compression with two main approaches. Weight pruning leverages the redundancy in the number of weights and can be performed in a non-structured, which has higher flexibility and pruning rate but incurs index accesses due to irregular weights, or structured manner, which preserves the full matrix structure with lower pruning rate. Weight quantization leverages the redundancy in the number of bits in weights. Compared to pruning, quantization is much more hardware-friendly, and has become a "must-do" step for FPGA and ASIC implementations. This paper provides a definitive answer to the question for the first time. First, we build ADMM-NN-S by extending and enhancing ADMM-NN, a recently proposed joint weight pruning and quantization framework. Second, we develop a methodology for fair and fundamental comparison of non-structured and structured pruning in terms of both storage and computation efficiency. Our results show that ADMM-NN-S consistently outperforms the prior art: (i) it achieves 348x, 36x, and 8x overall weight pruning on LeNet-5, AlexNet, and ResNet-50, respectively, with (almost) zero accuracy loss; (ii) we demonstrate the first fully binarized (for all layers) DNNs can be lossless in accuracy in many cases. These results provide a strong baseline and credibility of our study. Based on the proposed comparison framework, with the same accuracy and quantization, the results show that non-structrued pruning is not competitive in terms of both storage and computation efficiency. Thus, we conclude that non-structured pruning is considered harmful. We urge the community not to continue the DNN inference acceleration for non-structured sparsity.

cs.LG↗

arXiv2019

Fine-Grained Emotion Classification of Chinese Microblogs Based on Graph Convolution Networks

Microblogs are widely used to express people's opinions and feelings in daily life. Sentiment analysis (SA) can timely detect personal sentiment polarities through analyzing text. Deep learning approaches have been broadly used in SA but still have not fully exploited syntax information. In this paper, we propose a syntax-based graph convolution network (GCN) model to enhance the understanding of diverse grammatical structures of Chinese microblogs. In addition, a pooling method based on percentile is proposed to improve the accuracy of the model. In experiments, for Chinese microblogs emotion classification categories including happiness, sadness, like, anger, disgust, fear, and surprise, the F-measure of our model reaches 82.32% and exceeds the state-of-the-art algorithm by 5.90%. The experimental results show that our model can effectively utilize the information of dependency parsing to improve the performance of emotion detection. What is more, we annotate a new dataset for Chinese emotion classification, which is open to other researchers.

cs.CL↗