arXiv subjects

Jihan Zhou

Publications and source records attributed to Jihan Zhou.

16 recordsLinked to original sources

arXiv2026

Tracking atomic-scale interdiffusion in immiscible bimetallic nanoparticles via four-dimensional electron tomography

The interdiffusion of immiscible elements is generally considered both thermodynamically unfavorable and kinetically hindered. At the nanoscale, however, the mixing behavior of multielements materials often diverges from bulk equilibrium, yet a quantitative, atomically resolved description of this transformation has remained challenging. Using ex situ four dimensional atomic resolution electron tomography combined with in situ scanning transmission electron microscopy, here we reveal the atomic scale miscible transition driven by interdiffusion in immiscible PdIr nanoparticles at temperatures far below the melting point. The pathway involves surface reconstruction atom hopping at 200oC and surface flattening at 300oC, followed by a critical transition at 400oC where Ir interfacial diffusion and discrete Ir intermediates drive miscible intermixing. Upon reaching the nanoscale melting point 900oC, collective inward Ir diffusion yields the thermodynamically stable IrPd configuration. Our findings provide quantitative atomic scale insights into how metastable nanostructures evolve through distinct intermediates, offering a design framework for advanced multielement materials.

cond-mat.mtrl-sci↗

arXiv2026

Physics-aware neural networks enable robust and full atomic structure determination via low-dose atomic electron tomography

Atomic electron tomography (AET) determines the three-dimensional (3D) coordinates and chemical identities of individual atoms from a series of scanning transmission electron microscopy images taken at different tilt angles. However, under the low dose conditions required to mitigate beam damage, the reduced signal-to-noise ratio forces a trade off among accuracy, robustness, and throughput, which ultimately limits the broader application of AET. Here, we introduce a physics aware, two stage neural networks (PANN) that incorporates physical constraints throughout its workflow to achieve accurate AET under low-dose imaging. First, a global local 3D ResUNet refines the initial reconstruction and corrects geometric distortions in the volume. Second, the local density around each identified atom is encoded using 3D Zernike moments. These feature descriptors, along with the atomic coordinates are then processed by a graph attention Transformer to classify the elemental species. We benchmark the PANN workflow using a dataset of 42,588 reconstructed volumes, covering diverse noise models, materials morphologies, and dose settings. Under low dose conditions, PANN significantly improves performance, reducing the atomic coordinates error and leading to an increase in the atomic recovery rate. The framework's performance on experimental lose dose AET data across nanoparticles of varying morphology and composition demonstrate robust generalization. We anticipate this approach will extend the applicability of AET, particularly in investigating materials sensitive to electron dose or chemical state, including halide perovskites, zeolite, and quantum dot.

cond-mat.mtrl-sci↗

arXiv2025

Tracking four-dimensional atomic evolutions of single nanocatalysts throughout the life cycles

Structural changes induced by chemical reactions critically determine the catalytic performance and mechanism. However, precise tracking of the three-dimensional (3D) atomic structural evolution of individual bimetallic nanocatalysts remains challenging. Here we develop four-dimensional electrocatalytic atomic-resolution electron tomography, a method for directly tracking 3D atomic rearrangements in identical nanoparticles by electrocatalytic reactions. Using Pd-Pt bimetallic nanoparticles as a model system, we capture the atomic evolution of single nanocatalysts throughout electrocatalytic cycles. We observe two stages of evolutions: surface reconstruction and atom leaching, which are corroborated with the voltage-dependent behaviors probed by in situ electrochemical transmission electron microscopy. We identify chemical short-range order at atomic level and further reveal anisotropic chemical redistributions across different crystallographic orientations. These findings highlight the necessity of incorporating 3D spatiotemporal and chemical evolutions into the rational design of functional nanocatalysts in the future.

cond-mat.mtrl-sci↗

arXiv2025

Crystal nucleation and growth in high-entropy alloys revealed by atomic electron tomography

High-entropy alloys (HEAs) balance mixing entropy and intermetallic phase formation enthalpy, creating a vast compositional space for structural and functional materials (1-6). They exhibit exceptional strength-ductility trade-offs in metallurgy (4-10) and near-continuum adsorbate binding energies in catalysis (11-16). A deep understanding of crystal nucleation and growth in HEAs is essential for controlling their formation and optimizing their structural and functional properties. However, atomic-scale nucleation in HEAs challenges traditional theories based on one or two principal elements (17-23). The intricate interplay of structural and chemical orders among multiple principal elements further obscures our understanding of nucleation pathways (5,24-27). Due to the lack of direct three-dimensional (3D) atomic-scale observations, previous studies have relied on simulations and indirect measurements (28-32), leaving HEA nucleation and growth fundamentally elusive. Here, we advance atomic electron tomography (33,34) to resolve the 3D atomic structure and chemical composition of 7,662 HEA and 498 medium-entropy alloy nuclei at different nucleation stages. We observe local structural order that decreases from core to boundary, correlating with local chemical order. As nuclei grow, structural order improves. At later stages, most nuclei coalesce without misorientation, while some form coherent twin boundaries. To explain these experimental observations, we propose the gradient nucleation pathways model, in which the nucleation energy barrier progressively increases through multiple evolving intermediate states. We expect these findings to not only provide fundamental insights into crystal nucleation and growth in HEAs, but also offer a general framework for understanding nucleation mechanisms in other materials.

cond-mat.mtrl-sci↗

arXiv2024

Non-Destructive, High-Resolution, Chemically Specific, 3D Nanostructure Characterization using Phase-Sensitive EUV Imaging Reflectometry

Next-generation nano and quantum devices have increasingly complex 3D structure. As the dimensions of these devices shrink to the nanoscale, their performance is often governed by interface quality or precise chemical or dopant composition. Here we present the first phase-sensitive extreme ultraviolet imaging reflectometer. It combines the excellent phase stability of coherent high-harmonic sources, the unique chemical- and phase-sensitivity of extreme ultraviolet reflectometry, and state-of-the-art ptychography imaging algorithms. This tabletop microscope can non-destructively probe surface topography, layer thicknesses, and interface quality, as well as dopant concentrations and profiles. High-fidelity imaging was achieved by implementing variable-angle ptychographic imaging, by using total variation regularization to mitigate noise and artifacts in the reconstructed image, and by using a high-brightness, high-harmonic source with excellent intensity and wavefront stability. We validate our measurements through multiscale, multimodal imaging to show that this technique has unique advantages compared with other techniques based on electron and scanning-probe microscopies.

physics.optics↗

arXiv2024

Three-dimensional atomic interface between metal and oxide in Zr-ZrO2 nanoparticles

Metal-oxide interfaces with poor coherency have unique properties comparing to the bulk materials and offer broad applications in the fields of heterogeneous catalysis, battery, and electronics. However, current understanding of the three-dimensional (3D) atomic metal-oxide interfaces remains limited because of their inherent structural complexity and limitations of conventional two-dimensional imaging techniques. Here, we determine the 3D atomic structure of metal-oxide interfaces in zirconium-zirconia nanoparticles using atomic-resolution electron tomography. We quantitatively analyze the atomic concentration and the degree of oxidation, and find the coherency and translational symmetry of the interfaces are broken. Moreover, we observe porous structures such as Zr vacancies and nano-pores and investigate their distribution. Our findings provide a clear 3D atomic picture of metal-oxide interface with direct experimental evidence. We anticipate this work could encourage future studies on fundamental problems of oxides such as interfacial structures in semiconductor and atomic motion during oxidation process.

cond-mat.mtrl-sci↗

arXiv2023

Janus icosahedral particles: amorphization driven by three-dimensional atomic misfit and edge dislocation compensation

Icosahedral nanoparticles composed of fivefold twinned tetrahedra have broad applications. The strain relief mechanism and angular deficiency in icosahedral multiply twinned particles are poorly understood in three dimensions. Here, we resolved the three-dimensional atomic structures of Janus icosahedral nanoparticles using atomic resolution electron tomography. A geometrically fivefold face consistently corresponds to a less ordered face like two hemispheres. We quantify rich structural variety of icosahedra including bond orientation order, bond length, strain tensor; and packing efficiency, atom number, solid angle of each tetrahedron. These structural characteristics exhibit two-sided distribution. Edge dislocations near the axial atoms and small disordered domains fill the angular deficiency. Our findings provide new insights how the fivefold symmetry can be compensated and the geometrically-necessary internal strains relived in multiply twinned particles.

cond-mat.mtrl-sci↗

arXiv2023

Three-dimensional atomic positions and local chemical order of medium- and high-entropy alloys

Medium- and high-entropy alloys (M/HEAs) mix multiple principal elements with near-equiatomic composition and represent a paradigm-shift strategy for designing new materials for metallurgy, catalysis, and other fields. One of the core hypotheses of M/HEAs is lattice distortion. However, experimentally determining the 3D local lattice distortion in M/HEAs remains a challenge. Additionally, the presumed random elemental mixing in M/HEAs has been questioned by atomistic simulations, energy dispersive x-ray spectroscopy (EDS), and electron diffraction, which suggest the existence of local chemical order in M/HEAs. However, the 3D local chemical order has eluded direct experimental observation since the EDS elemental maps integrate the composition of atomic columns along the zone axes, and the diffuse reflections/streaks in electron diffraction of M/HEAs may originate from planar defects. Here, we determine the 3D atomic positions of M/HEA nanocrystals using atomic electron tomography, and quantitatively characterize the local lattice distortion, strain tensor, twin boundaries, dislocation cores, and chemical short-range order (CSRO) with unprecedented 3D detail. We find that the local lattice distortion and strain tensor in the HEAs are larger and more heterogeneous than in the MEAs. We observe CSRO-mediated twinning in the MEAs. that is, twinning occurs in energetically unfavoured CSRO regions but not in energetically favoured CSRO ones. This observation confirms the atomistic simulation results of the bulk CrCoNi MEA and represents the first experimental evidence of correlating local chemical order with structural defects in any material system. We expect that this work will not only expand our fundamental understanding of this important class of materials, but also could provide the foundation for tailoring M/HEA properties through lattice distortion and local chemical order.

cond-mat.mtrl-sci↗

arXiv2022

Probing the atomically diffuse interfaces in core-shell nanoparticles in three dimensions

Deciphering the three-dimensional atomic structure of solid-solid interfaces in core-shell nanomaterials is the key to understand their remarkable catalytical, optical and electronic properties. Here, we probe the three-dimensional atomic structures of palladium-platinum core-shell nanoparticles at the single-atom level using atomic resolution electron tomography. We successfully quantify the rich structural variety of core-shell nanoparticles including bond length, coordination number, local bond orientation order, grain boundary, and five-fold symmetry, all in 3D at atomic resolution. Instead of forming an atomically-sharp boundary, the core-shell interface is atomically diffuse with an average thickness of 4.2 A, irrespective of the particle's size, morphology, or crystallographic texture. The high concentration of Pd in the interface is highly related to the electric double layers of the Pd seeds. These results advance our understanding of core-shell structures at the fundamental level, providing potential strategies into nanomaterial manipulation and chemical property regulation.

cond-mat.mtrl-sci↗

arXiv2022

Atomic-scale identification of the active sites of nanocatalysts

Alloy nanocatalysts have found broad applications ranging from fuel cells to catalytic converters and hydrogenation reactions. Despite extensive studies, identifying the active sites of nanocatalysts remains a major challenge due to the heterogeneity of the local atomic environment. Here, we advance atomic electron tomography to determine the 3D local atomic structure, surface morphology and chemical composition of PtNi and Mo-doped PtNi nanocatalysts. Using machine learning trained by density functional theory calculations, we identify the catalytic active sites for the oxygen reduction reaction from experimental 3D atomic coordinates, which are corroborated by electrochemical measurements. By quantifying the structure-activity relationship, we discover a local environment descriptor to explain and predict the catalytic active sites at the atomic level. The ability to determine the 3D atomic structure and chemical species coupled with machine learning is expected to expand our fundamental understanding of a wide range of nanocatalysts.

physics.chem-ph↗

arXiv2020

Direct observation of 3D atomic packing in monatomic amorphous materials

Liquids and solids are two fundamental states of matter. However, due to the lack of direct experimental determination, our understanding of the 3D atomic structure of liquids and amorphous solids remained speculative. Here we advance atomic electron tomography to determine for the first time the 3D atomic positions in monatomic amorphous materials, including a Ta thin film and two Pd nanoparticles. We observe that pentagonal bipyramids are the most abundant atomic motifs in these amorphous materials. Instead of forming icosahedra, the majority of pentagonal bipyramids arrange into networks that extend to medium-range scale. Molecular dynamic simulations further reveal that pentagonal bipyramid networks are prevalent in monatomic amorphous liquids, which rapidly grow in size and form icosahedra during the quench from the liquid state to glass state. The experimental method and results are expected to advance the study of the amorphous-crystalline phase transition and glass transition at the single-atom level.

cond-mat.mtrl-sci↗

arXiv2020

Determining the three-dimensional atomic structure of a metallic glass

Amorphous solids such as glass are ubiquitous in our daily life and have found broad applications ranging from window glass and solar cells to telecommunications and transformer cores. However, due to the lack of long-range order, the three-dimensional (3D) atomic structure of amorphous solids have thus far defied any direct experimental determination without model fitting. Here, using a multi-component metallic glass as a proof-of-principle, we advance atomic electron tomography to determine the 3D atomic positions in an amorphous solid for the first time. We quantitatively characterize the short-range order (SRO) and medium-range order (MRO) of the 3D atomic arrangement. We find that although the 3D atomic packing of the SRO is geometrically disordered, some SRO connect with each other to form crystal-like networks and give rise to MRO. We identify four crystal-like MRO networks - face-centred cubic, hexagonal close-packed, body-centered cubic and simple cubic - coexisting in the sample, which show translational but no orientational order. These observations confirm that the 3D atomic structure in some parts of the sample is consistent with the efficient cluster packing model. Looking forward, we anticipate this experiment will open the door to determining the 3D atomic coordinates of various amorphous solids, whose impact on non-crystalline solids may be comparable to the first 3D crystal structure solved by x-ray crystallography over a century ago.

cond-mat.dis-nn↗

arXiv2020

X-ray linear dichroic ptychography

Biominerals such as seashells, corals skeletons, bone, and enamel are optically anisotropic crystalline materials with unique nano- and micro-scale organization that translates into exceptional macroscopic mechanical properties, providing inspiration for engineering new and superior biomimetic structures. Here we use particles of Seriatopora aculeata coral skeleton as a model and demonstrate, for the first time, x-ray linear dichroic ptychography. We map the aragonite (CaCO3) crystal c-axis orientations in coral skeleton with 35 nm spatial resolution. Linear dichroic phase imaging at the O K-edge energy shows strong polarization-dependent contrast and reveals the presence of both narrow (< 35°) and wide (> 35°) c-axis angular spread in sub-micrometer coral particles. These x-ray ptychography results were corroborated using 4D scanning transmission electron nano-diffraction on the same particles. Evidence of co-oriented but disconnected corallite sub-domains indicates jagged crystal boundaries consistent with formation by amorphous nanoparticle attachment. Looking forward, we anticipate that x-ray linear dichroic ptychography can be applied to study nano-crystallites, interfaces, nucleation and mineral growth of optically anisotropic materials with sub-ten nanometers spatial resolution in three dimensions.

physics.app-ph↗

arXiv2019

Capturing Nucleation at 4D Atomic Resolution

Nucleation plays a critical role in many physical and biological phenomena ranging from crystallization, melting and evaporation to the formation of clouds and the initiation of neurodegenerative diseases. However, nucleation is a challenging process to study in experiments especially in the early stage when several atoms/molecules start to form a new phase from its parent phase. Here, we advance atomic electron tomography to study early stage nucleation at 4D atomic resolution. Using FePt nanoparticles as a model system, we reveal that early stage nuclei are irregularly shaped, each has a core of one to few atoms with the maximum order parameter, and the order parameter gradient points from the core to the boundary of the nucleus. We capture the structure and dynamics of the same nuclei undergoing growth, fluctuation, dissolution, merging and/or division, which are regulated by the order parameter distribution and its gradient. These experimental observations differ from classical nucleation theory (CNT) and to explain them we propose the order parameter gradient (OPG) model. We show the OPG model generalizes CNT and energetically favours diffuse interfaces for small nuclei and sharp interfaces for large nuclei. We further corroborate this model using molecular dynamics simulations of heterogeneous and homogeneous nucleation in liquid-solid phase transitions of Pt. We anticipate that the OPG model is applicable to different nucleation processes and our experimental method opens the door to study the structure and dynamics of materials with 4D atomic resolution.

cond-mat.mtrl-sci↗

arXiv2017

GENFIRE: A generalized Fourier iterative reconstruction algorithm for high-resolution 3D imaging

Tomography has made a radical impact on diverse fields ranging from the study of 3D atomic arrangements in matter to the study of human health in medicine. Despite its very diverse applications, the core of tomography remains the same, that is, a mathematical method must be implemented to reconstruct the 3D structure of an object from a number of 2D projections. In many scientific applications, however, the number of projections that can be measured is limited due to geometric constraints, tolerable radiation dose and/or acquisition speed. Thus it becomes an important problem to obtain the best-possible reconstruction from a limited number of projections. Here, we present the mathematical implementation of a tomographic algorithm, termed GENeralized Fourier Iterative REconstruction (GENFIRE). By iterating between real and reciprocal space, GENFIRE searches for a global solution that is concurrently consistent with the measured data and general physical constraints. The algorithm requires minimal human intervention and also incorporates angular refinement to reduce the tilt angle error. We demonstrate that GENFIRE can produce superior results relative to several other popular tomographic reconstruction techniques by numerical simulations, and by experimentally by reconstructing the 3D structure of a porous material and a frozen-hydrated marine cyanobacterium. Equipped with a graphical user interface, GENFIRE is freely available from our website and is expected to find broad applications across different disciplines.

physics.comp-ph↗

arXiv2016

Deciphering chemical order/disorder and material properties at the single-atom level

Correlating 3D arrangements of atoms and defects with material properties and functionality forms the core of several scientific disciplines. Here, we determined the 3D coordinates of 6,569 iron and 16,627 platinum atoms in a model iron-platinum nanoparticle system to correlate 3D atomic arrangements and chemical order/disorder with material properties at the single-atom level. We identified rich structural variety and chemical order/disorder including 3D atomic composition, grain boundaries, anti-phase boundaries, anti-site point defects and swap defects. We show for the first time that experimentally measured 3D atomic coordinates and chemical species with 22 pm precision can be used as direct input for first-principles calculations of material properties such as atomic magnetic moments and local magnetocrystalline anisotropy. This work not only opens the door to determining 3D atomic arrangements and chemical order/disorder of a wide range of nanostructured materials with high precision, but also will transform our understanding of structure-property relationships at the most fundamental level.

cond-mat.mtrl-sci↗