Review of the Synergies Between Computational Modeling and Experimental Characterization of Materials Across Length Scales

With the increasing interplay between experimental and computational approaches at multiple length scales, new research directions are emerging in materials science and computational mechanics. Such cooperative interactions find many applications in the development, characterization and design of complex material systems. This manuscript provides a broad and comprehensive overview of recent trends where predictive modeling capabilities are developed in conjunction with experiments and advanced characterization to gain a greater insight into structure-properties relationships and study various physical phenomena and mechanisms. The focus of this review is on the intersections of multiscale materials experiments and modeling relevant to the materials mechanics community. After a general discussion on the perspective from various communities, the article focuses on the latest experimental and theoretical opportunities. Emphasis is given to the role of experiments in multiscale models, including insights into how computations can be used as discovery tools for materials engineering, rather than to "simply" support experimental work. This is illustrated by examples from several application areas on structural materials. This manuscript ends with a discussion on some problems and open scientific questions that are being explored in order to advance this relatively new field of research.Comment: 25 pages, 11 figures, review article accepted for publication in J. Mater. Sc

Dynamics and control of gold-encapped gallium arsenide nanowires imaged by 4D electron microscopy

Eutectic related reaction is a special chemical/physical reaction involving multiple phases, solid and liquid. Visualization of phase reaction of composite nanomaterials with high spatial and temporal resolution provides a key understanding of alloy growth with important industrial applications. However, it has been a rather challenging task. Here we report the direct imaging and control of the phase reaction dynamics of a single, as-grown free-standing gallium arsenide nanowire encapped with a gold nanoparticle, free from environmental confinement or disturbance, using four-dimensional electron microscopy. The non-destructive preparation of as-grown free-standing nanowires without supporting films allows us to study their anisotropic properties in their native environment with better statistical character. A laser heating pulse initiates the eutectic related reaction at a temperature much lower than the melting points of the composite materials, followed by a precisely time-delayed electron pulse to visualize the irreversible transient states of nucleation, growth and solidification of the complex. Combined with theoretical modeling, useful thermodynamic parameters of the newly formed alloy phases and their crystal structures could be determined. This technique of dynamical control and 4D imaging of phase reaction processes on the nanometer-ultrafast time scale open new venues for engineering various reactions in a wide variety of other systems

The prismatic Sigma 3 (10-10) twin bounday in alpha-Al2O3 investigated by density functional theory and transmission electron microscopy

The microscopic structure of a prismatic $\Sigma 3$ $(10\bar{1}0)$ twin boundary in \aal2o3 is characterized theoretically by ab-initio local-density-functional theory, and experimentally by spatial-resolution electron energy-loss spectroscopy in a scanning transmission electron microscope (STEM), measuring energy-loss near-edge structures (ELNES) of the oxygen $K$-ionization edge. Theoretically, two distinct microscopic variants for this twin interface with low interface energies are derived and analysed. Experimentally, it is demonstrated that the spatial and energetical resolutions of present high-performance STEM instruments are insufficient to discriminate the subtle differences of the two proposed interface variants. It is predicted that for the currently developed next generation of analytical electron microscopes the prismatic twin interface will provide a promising benchmark case to demonstrate the achievement of ELNES with spatial resolution of individual atom columns

Optical tracing of multiple charges in single-electron devices

Single molecules that exhibit narrow optical transitions at cryogenic temperatures can be used as local electric-field sensors. We derive the single charge sensitivity of aromatic organic dye molecules, based on first principles. Through numerical modeling, we demonstrate that by using currently available technologies it is possible to optically detect charging events in a granular network with a sensitivity better than $10^{-5}e/\sqrt{\textrm{Hz}}$ and track positions of multiple electrons, simultaneously, with nanometer spatial resolution. Our results pave the way for minimally-invasive optical inspection of electronic and spintronic nanodevices and building hybrid optoelectronic interfaces that function at both single-photon and single-electron levels.Comment: 7 pages, submitted to Physical Revie

Force-induced acoustic phonon transport across single-digit nanometre vacuum gaps

Heat transfer between bodies separated by nanoscale vacuum gap distances has been extensively studied for potential applications in thermal management, energy conversion and data storage. For vacuum gap distances down to 20 nm, state-of-the-art experiments demonstrated that heat transport is mediated by near-field thermal radiation, which can exceed Planck's blackbody limit due to the tunneling of evanescent electromagnetic waves. However, at sub-10-nm vacuum gap distances, current measurements are in disagreement on the mechanisms driving thermal transport. While it has been hypothesized that acoustic phonon transport across single-digit nanometre vacuum gaps (or acoustic phonon tunneling) can dominate heat transfer, the underlying physics of this phenomenon and its experimental demonstration are still unexplored. Here, we use a custom-built high-vacuum shear force microscope (HV-SFM) to measure heat transfer between a silicon (Si) tip and a feedback-controlled platinum (Pt) nanoheater in the near-contact, asperity-contact, and bulk-contact regimes. We demonstrate that in the near-contact regime (i.e., single-digit nanometre or smaller vacuum gaps before making asperity contact), heat transfer between Si and Pt surfaces is dominated by force-induced acoustic phonon transport that exceeds near-field thermal radiation predictions by up to three orders of magnitude. The measured thermal conductance shows a gap dependence of $d^{-5.7\pm1.1}$ in the near-contact regime, which is consistent with acoustic phonon transport modelling based on the atomistic Green's function (AGF) framework. Our work suggests the possibility of engineering heat transfer across single-digit nanometre vacuum gaps with external force stimuli, which can make transformative impacts to the development of emerging thermal management technologies.Comment: 9 pages with 4 figures (Main text), 13 pages with 7 figures (Methods), and 13 pages with 6 figures and 1 table (Supplementary Information

Polymorphic Aβ42 fibrils adopt similar secondary structure but differ in cross-strand side chain stacking interactions within the same β-sheet.

Formation of polymorphic amyloid fibrils is a common feature in neurodegenerative diseases involving protein aggregation. In Alzheimer's disease, different fibril structures may be associated with different clinical sub-types. Structural basis of fibril polymorphism is thus important for understanding the role of amyloid fibrils in the pathogenesis and progression of these diseases. Here we studied two types of Aβ42 fibrils prepared under quiescent and agitated conditions. Quiescent Aβ42 fibrils adopt a long and twisted morphology, while agitated fibrils are short and straight, forming large bundles via lateral association. EPR studies of these two types of Aβ42 fibrils show that the secondary structure is similar in both fibril polymorphs. At the same time, agitated Aβ42 fibrils show stronger interactions between spin labels across the full range of the Aβ42 sequence, suggesting a more tightly packed structure. Our data suggest that cross-strand side chain packing interactions within the same β-sheet may play a critical role in the formation of polymorphic fibrils

Role of disordered bipolar complexions on the sulfur embrittlement of nickel general grain boundaries

Minor impurities can cause catastrophic fracture of normally ductile metals. Here, a classic example is represented by the sulfur embrittlement of nickel, whose atomic-level mechanism has puzzled researchers for nearly a century. In this study, coupled aberration-corrected electron microscopy and semi-grand-canonical-ensemble atomistic simulation reveal, unexpectedly, the universal formation of amorphous-like and bilayer-like facets at the same general grain boundaries. Challenging the traditional view, the orientation of the lower-Miller-index grain surface, instead of the misorientation, dictates the interfacial structure. We also find partial bipolar structural orders in both amorphous-like and bilayer-like complexions (a.k.a. thermodynamically two-dimensional interfacial phases), which cause brittle intergranular fracture. Such bipolar, yet largely disordered, complexions can exist in and affect the properties of various other materials. Beyond the embrittlement mechanism, this study provides deeper insight to better understand abnormal grain growth in sulfur-doped Ni, and generally enriches our fundamental understanding of performance-limiting and more disordered interfaces