arXiv subjects
Publications and source records attributed to Houlong Zhuang.
This study investigates the H2O and CO2 sorption behavior of two ion exchange sorbents: a primary amine and a permanently charged strong base quaternary ammonium (QA) with (bi)carbonate counter-anions.
Ti/TiN coatings are utilized in a wide variety of engineering applications due to their superior properties such as high hardness and toughness. Doping Al into Ti/TiN can also enhance properties and lead to even higher performance. Therefore, studying the atomic-level behavior of the TiAl/TiAlN interface is important. However, due to the large number of possible combinations for the 50 mol% Al-doped Ti/TiN system, it is time-consuming to use the DFT-based Monte Carlo method to find the optimal TiAl/TiAlN system with a high work of adhesion. In this study, we use a graph convolutional neural network as an interatomic potential, combined with reinforcement learning, to improve the efficiency of finding optimal structures with a high work of adhesion. By inspecting the features of structures in neural networks, we found that the optimal structures follow a certain pattern of doping Al near the interface. The electronic structure and bonding analysis indicate that the optimal TiAl/TiAlN structures have higher bonding strength. We expect our approach to significantly accelerate the design of advanced ceramic coatings, which can lead to more durable and efficient materials for engineering applications.
A phenomenological model has been developed for hydrogen absorption in niobium. The model has 9 free parameters that have a physical basis. The model provides an excellent fit to the highly accurate isotherm data by Veleckis et al. and has been cross validated by limiting the fitting procedure to a training set. The model makes it possible to extract more information from the data than could be extracted with the computational methods available when the measurements were made. The partial molal enthalpy and partial molal entropy of hydrogen dissolution were calculated using the parameter values corresponding to the best fit to the isotherms. These quantities are consistent with those reported by Veleckis et al. Interpreting the model parameter values reveals insights into the nature of the interaction between hydrogen atoms in niobium. These insights supports our previous analysis of hydrogen interactions in niobium using density functional theory calculations.
Disorder hyperuniformity (DHU) is a recently discovered exotic state of many-body systems that possess a hidden order in between that of a perfect crystal and a completely disordered system. Recently, this novel DHU state has been observed in a number of quantum materials including amorphous 2D graphene and silica, which are endowed with unexpected electronic transport properties. Here, we numerically investigate 1D atomic chain models, including perfect crystalline, disordered hyperuniform as well as randomly perturbed atom packing configurations to obtain a quantitative understanding of how the unique DHU disorder affects the vibrational properties of these low-dimensional materials. We find that the DHU chains possess lower cohesive energies compared to the randomly perturbed chains, implying their potential reliability in experiments. Our inverse partition ratio (IPR) calculations indicate that the DHU chains can support fully delocalized states just like perfect crystalline chains over a wide range of frequencies, i.e., $ω\in (0, 100)$ cm$^{-1}$, suggesting superior phonon transport behaviors within these frequencies, which was traditionally considered impossible in disordered systems. Interestingly, we observe the emergence of a group of highly localized states associated with $ω\sim 200$ cm$^{-1}$, which is characterized by a significant peak in the IPR and a peak in phonon density of states at the corresponding frequency, and is potentially useful for decoupling electron and phonon degrees of freedom. These unique properties of DHU chains have implications in the design and engineering of novel DHU quantum materials for thermal and phononic applications.
Machine learning (ML) is widely used to explore crystal materials and predict their properties. However, the training is time-consuming for deep-learning models, and the regression process is a black box that is hard to interpret. Also, the preprocess to transfer a crystal structure into the input of ML, called descriptor, needs to be designed carefully. To efficiently predict important properties of materials, we propose an approach based on ensemble learning consisting of regression trees to predict formation energy and elastic constants based on small-size datasets of carbon allotropes as an example. Without using any descriptor, the inputs are the properties calculated by molecular dynamics with 9 different classical interatomic potentials. Overall, the results from ensemble learning are more accurate than those from classical interatomic potentials, and ensemble learning can capture the relatively accurate properties from the 9 classical potentials as criteria for predicting the final properties.
We theoretically show that the carrier transport in monolayer Fe3GeTe2 experiences a transition between anomalous Hall effect and spin Hall effect when the spin polarization of disorders switches between out-of-plane and in-plane. These Hall effects are allowed when the magnetization is polarized in-plane, breaking the C3 rotation symmetry. The transition originates from the selection rule of spin scattering, the strong spin-orbit coupling, and the van Hove singularities near the Fermi surface. The scattering selection rule tolerates the sign change of the disorder spin, which provides a convenient method to detect the switching of antiferromagnetic insulators regardless of the interfacial roughness in a heterostructure. This provides a convenient platform for the study of 2D spintronics through various van-der-Waals heterostructures.
Disordered hyperuniform (DHU) states are recently discovered exotic states of condensed matter. DHU systems are similar to liquids or glasses in that they are statistically isotropic and lack conventional long-range translational and orientational order. On the other hand, they completely suppress normalized infinite-wavelength density fluctuations like crystals, and in this sense possess a hidden long-range order. Very recently, there are several exciting discoveries of disordered hyperuniformity in solid-state materials, including amorphous carbon nanotubes, amorphous 2D silica, amorphous graphene, defected transition metal dichalcogenides, defected pentagonal 2D materials, and medium/high-entropy alloys. It has been found the DHU states of these materials often possess a significantly lower energy than other disorder models, and can lead to unique electronic and thermal transport properties, which resulted from mechanisms distinct from those identified for their crystalline counterparts. For example, DHU states can enhance electronic transport in 2D amorphous silica; DHU medium/high-entropy alloys realize the Vegard's law, and possess enhanced electronic band gaps and thermal transport at low temperatures. These unique properties open up many promising potential device applications in optoelectronics and thermoelectrics. Here, we provide a focused review on these important new developments of hyperuniformity in solid-state materials, taking an applied and ``materials'' perspective, which complements the existing reviews on hyperuniformity in physical systems and photonic materials. Future directions and outlook are also provided, with a focus on the design and discovery of DHU quantum materials for quantum information science and engineering.
Carbon nanotubes are quasi-one-dimensional systems that possess superior transport, mechanical, optical, and chemical properties. In this work, we generalize the notion of disorder hyperuniformity, a recently discovered exotic state of matter with hidden long-range order, to quasi-one-dimensional materials. As a proof of concept, we then apply the generalized framework to quantify the density fluctuations in amorphous carbon nanotubes containing randomly distributed Stone-Wales defects. We demonstrate that all of these amorphous nanotubes are hyperuniform, i.e., the infinite-wavelength density fluctuations of these systems are completely suppressed, regardless of the diameter, rolling axis, number of rolling sheets, and defect fraction of the nanotubes. We find that these amorphous nanotubes are energetically more stable than nanotubes with periodically distributed Stone-Wales defects. Moreover, certain semiconducting defect-free carbon nanotubes become metallic as sufficiently large amounts of defects are randomly introduced. This structural study of amorphous nanotubes strengthens our fundamental understanding of these systems, and suggests possible exotic physical properties, as endowed by their disordered hyperuniformity. Our findings also shed light on the effect of dimensionality reduction on the hyperuniformity property of materials.
We provide strong numerical evidence for a hidden multihyperuniform long-range order (MHLRO) in SiGeSn medium-entropy alloys (MEAs), in which the normalized infinite-wavelength composition fluctuations for all three atomic species are completely suppressed as in a perfect crystalline state. We show this MHLRO naturally leads to the emergence of short-range order (SRO) recently discovered in MEAs, which results in stable lower-energy states compared to alloy models with random or special quasi-random structures (SQSs) possessing no atomic SROs. The MHLRO MEAs approximately realize the Vegard's law, which offers a rule-of-mixture type predictions of the lattice constants and electronic band gap, and thus can be considered as an ideal mixing state. The MHLRO also directly gives rise to enhanced electronic band gaps and superior thermal transport properties at low temperatures compared to random structures and SQSs, which open up novel potential applications in optoelectronics and thermoelectrics. Our analysis of the SiGeSn system leads to the formulation of general organizing principles applicable in other medium- and high-entropy alloys (HEAs), and a highly efficient computational model for rendering realistic large-scale configurations of MEAs and HEAs.
Current definition of high-entropy alloys (HEAs) is commonly based on the configurational entropy. But this definition depends only on the chemical composition of a HEA and therefore cannot distinguish the information content that is encoded in various local atomic arrangements and measurable by the Shannon entropy in information theory. Here, inspired by the finding that two-dimensional (2D) Sudoku matrices exhibit higher average Shannon entropy than 2D random matrix counterparts, we propose high-Shannon-entropy alloys (HSEA), whose structures are based on 3D Sudoku matrices. Despite the constraints on the atomic arrangements to form a 3D Sudoku 4 x 4 x 4 matrix, we find that, a prototypical HSEA, NbMoTaW has a lower energy than the same HEA with a random structure due to the smaller lattice distortion. We compute the electronic structures and mechanical properties and find that the HSEA exhibits enhanced average Fermi velocity and ductility over the random NbMoTaW HEA. Finally, we evaluate the formation energies of single vacancies and a vacancy cluster in the HSEA, whose configurations mimic Sudoku puzzles with one and several missing numbers, respectively. We find that a range of large energies are required to generate such vacancies, which depend on the location and species of missing atoms. Our work shows that introducing the Shannon entropy to HEAs offers a useful metric to reveal more atomic details of HEAs and that HSEAs represent an uncharted domain in the complicated energy landscape of HEAs which may be endowed with improved properties.
The Joint Automated Repository for Various Integrated Simulations (JARVIS) is an integrated infrastructure to accelerate materials discovery and design using density functional theory (DFT), classical force-fields (FF), and machine learning (ML) techniques. JARVIS is motivated by the Materials Genome Initiative (MGI) principles of developing open-access databases and tools to reduce the cost and development time of materials discovery, optimization, and deployment. The major features of JARVIS are: JARVIS-DFT, JARVIS-FF, JARVIS-ML, and JARVIS-Tools. To date, JARVIS consists of 40,000 materials and 1 million calculated properties in JARVIS-DFT, 1,500 materials and 110 force-fields in JARVIS-FF, and 25 ML models for material-property predictions in JARVIS-ML, all of which are continuously expanding. JARVIS-Tools provides scripts and workflows for running and analyzing various simulations. We compare our computational data to experiments or high-fidelity computational methods wherever applicable to evaluate error/uncertainty in predictions. In addition to the existing workflows, the infrastructure can support a wide variety of other technologically important applications as part of the data-driven materials design paradigm. The JARVIS datasets and tools are publicly available at the website: https://jarvis.nist.gov .
Hyperuniform many-body systems in $d$-dimensional Euclidean space are characterized by completely suppressed (normalized) infinite-wavelength density fluctuations, and appear to be endowed with novel exotic physical properties. In this work, we analyze the effects of localized defects on the density fluctuations across length scales and on the hyperuniformity property of experimental samples of two-dimensional transition metal dichalcogenides. In particular, we extract atomic coordinates from time series annular dark field-scanning transmission electron microscopy imaging data of 2D tungsten chalcogenides with the 2H structure showing continuous development and evolution of electron-beam induced defects, and construct the corresponding chemical-bonding informed coordination networks between the atoms. We then compute a variety of pair statistics and bond-orientational statistics to characterize the samples. At low defect concentrations, the corresponding materials are nearly hyperuniform. As more defects are introduced, the (approximate) hyperuniformity of the materials is gradually destroyed, and the system becomes non-hyperuniform even when the material still contains a significant amount of crystalline regions. At high defect concentrations, the structures become antihyperuniform with diverging (normalized) large-scale density fluctuations. Overall, the defected materials possess varying degrees of orientation order, and there is apparently no intermediate hexatic phase emerging. We also construct a minimalist structural model and demonstrate that the experimental samples can be essentially viewed as perturbed honeycomb crystals with small correlated displacements and double chalcogen vacancies.
We discover two distinct topological pathways through which the pentagonal Cairo tiling (P5), a structural model for single-layer $AB_2$ pyrite materials, respectively transforms into a crystalline rhombus-hexagon (C46) tiling and random rhombus-pentagon-hexagon (R456) tilings, by continuously introducing the Stone-Wales (SW) topological defects. We find these topological transformations are controlled by the orientation correlations among neighboring $B$-$B$ bonds, and exhibit a phenomenological analogy of the (anti)ferromagnetic to paramagnetic transition in two-state Ising systems. Unlike the SW defects in hexagonal 2D materials such as graphene, which cause distortions, the defects in pentagonal 2D materials preserve the shape and symmetry of the fundamental cell of P5 tiling and are associated with a minimal energy cost, making the intermediate R456 tilings realizable metastable states at room temperature. Moreover, the intermediate structures along the two pathways are neither crystals nor quasicrystals, and yet these random tilings preserve hyperuniformity of the P5 or C46 crystal (i.e., the infinite-wavelength normalized density fluctuations are completely suppressed), and can be viewed as 2D analogs of disordered Barlow packings in three dimensions. The resulting 2D materials possess metal-like electronic properties, making them promising candidates for forming Schottky barriers with the semiconducting P5 material.
Electrical and thermal transport properties of disordered materials have long been of both theoretical interest and engineering importance. As a new class of materials with an intrinsic compositional disorder, high/medium-entropy alloys (HEAs/MEAs) are being immensely studied mainly for their excellent mechanical properties. By contrast, electrical and thermal transport properties of HEAs/MEAs are less well studied. Here we investigate these two properties of silicon (Si)-germanium (Ge)-tin (Sn) MEAs, where we keep the same content of Si and Ge while increasing the content of Sn from 0 to 1/3 to tune the configurational entropy and thus the degree of compositional disorder. We predict all SiyGeySnx MEAs to be semiconductors with a wide range of bandgaps from near-infrared (0.28 eV) to visible (1.11 eV) in the light spectrum. We find that the bandgaps and effective carrier masses decrease with increasing Sn content. As a result, increasing the compositional disorder in SiyGeySnx MEAs enhances their electrical conductivity. For the thermal transport properties of SiyGeySnx MEAs, our molecular dynamics simulations show an opposite trend in the thermal conductivity of these MEAs at room temperature, which decreases with increasing compositional disorder, owing to enhanced Anderson localization and strong phonon-phonon anharmonic interactions. The enhanced electrical conductivity and weakened thermal conductivity make SiyGeySnx MEAs with high Sn content promising functional materials for thermoelectric applications. Our work demonstrates that HEAs/MEAs not only represent a new class of structural alloys but also a novel category of functional alloys with unique electrical and thermal transport properties.
Crystalline two-dimensional (2D) materials such as graphene possess unique physical properties absent in their bulk form, enabling many novel device applications. Yet, little is known about their amorphous counterparts, which can be obtained by introducing the Stone-Wales (SW) topological defects via proton radiation. Here we provide strong numerical evidence that SW defects preserve hyperuniformity in hexagonal 2D materials, a recently discovered new state of matter characterized by vanishing normalized infinite-wavelength density fluctuations, which implies that all amorphous states of these materials are hyperuniform. Specifically, the static structure factor S(k) of these materials possesses the scaling S(k) ~ k^α for small wave number k, where 1<=α(p)<=2 is monotonically decreasing as the SW defect concentration p increases, indicating a transition from type-I to type-II hyperuniformity at p ~= 0.12 induced by the saturation of the SW defects. This hyperuniformity transition marks a structural transition from perturbed lattice structures to truly amorphous structures, and underlies the onset of strong correlation among the SW defects as well as a transition between distinct electronic transport mechanisms associated with different hyperuniformity classes.
Past experiments about hydrogen absorption in niobium have revealed specific properties about interactions between interstitial hydrogen atoms. It has been reported that there are long-range attractive and short-range repulsive interactions between interstitial hydrogen atoms in niobium. It has also been reported that these interactions are of many-body nature. While previous understanding of these interactions is based on experimental inferences from past experiments, through these calculations, for the first time, we can understand the nature of the interactions at a fundamental level. In this work, we use Density Functional Theory calculations to study the interactions of interstitial hydrogen atoms in niobium. We report here that these interactions are a combination of an attractive, indirect image interaction and a repulsive, direct interaction. Through our calculations, we also infer here that these interactions indeed have many-body characteristics.
Disordered hyperuniformity (DHU) is a recently proposed new state of matter, which has been observed in a variety of classical and quantum many-body systems. DHU systems are characterized by vanishing infinite-wavelength density fluctuations and are endowed with unique novel physical properties. Here we report the first discovery of disordered hyperuniformity in atomic-scale 2D materials, i.e., amorphous silica composed of a single layer of atoms, based on spectral-density analysis of high-resolution transmission electron microscope images. Subsequent simulations suggest that the observed DHU is closely related to the strong topological and geometrical constraints induced by the local chemical order in the system. Moreover, we show via large-scale density functional theory calculations that DHU leads to almost complete closure of the electronic band gap compared to the crystalline counterpart, making the material effectively a metal. This is in contrast to the conventional wisdom that disorder generally diminishes electronic transport and is due to the unique electron wave localization induced by the topological defects in the DHU state.