arXiv subjects

Timothy J. Rupert

Publications and source records attributed to Timothy J. Rupert.

At least 73 records · Page 4Linked to original sources

arXiv2018

Amorphous complexions enable a new region of high temperature stability in nanocrystalline Ni-W

Solute segregation is used to limit grain growth in nanocrystalline metals, but this stabilization often breaks down at high temperatures. Amorphous intergranular films can form in certain alloys at sufficiently high temperatures, providing a possible alternative route to lower grain boundary energy and therefore limit grain growth. In this study, nanocrystalline Ni-W that is annealed at temperatures of 1000 °C and above, then rapidly quenched, is found to contain amorphous intergranular films. These complexions lead to a new, unexpected region of nanocrystalline stability at elevated temperatures.

cond-mat.mtrl-sci↗

arXiv2018

Dislocation-assisted linear complexion formation driven by segregation

Atomistic simulations are used to study linear complexion formation at dislocations in a body-centered cubic Fe-Ni alloy. Driven by Ni segregation, precipitation of the metastable B2-FeNi and stable L10-FeNi phases occurs along the compression side of edge dislocations. If the Ni segregation is not intense enough to ensure precipitate growth and coalescence along the dislocation lines, linear complexions in the form of stable nanoscale precipitate arrays are observed. Critical conditions such as global composition and temperature are defined for both linear complexion formation and dislocation-assisted precipitation.

cond-mat.mtrl-sci↗

arXiv2018

Grain boundary complexions and the strength of nanocrystalline metals: Dislocation emission and propagation

Grain boundary complexions have been observed to affect the mechanical behavior of nanocrystalline metals, improving both strength and ductility. While an explanation for the improved ductility exists, the observed effect on strength remains unexplained. In this work, we use atomistic simulations to explore the influence of ordered and disordered complexions on two deformation mechanisms which are essential for nanocrystalline plasticity, namely dislocation emission and propagation. Both ordered and disordered grain boundary complexions in Cu-Zr are characterized by excess free volume and promote dislocation emission by reducing the critical emission stress. Alternatively, these complexions are characterized by strong dislocation pinning regions that increase the flow stress required for dislocation propagation. Such pinning regions are caused by ledges and solute atoms at the grain-complexion interfaces and may be dependent on the complexion state as well as the atomic size mismatch between the matrix and solute elements. The trends observed in our simulations of dislocation propagation align with the available experimental data, suggesting that dislocation propagation is the rate-limiting mechanism behind plasticity in nanocrystalline Cu-Zr alloys.

cond-mat.mtrl-sci↗

arXiv2018

Identifying interatomic potentials for the accurate modeling of interfacial segregation and structural transitions

Chemical segregation and structural transitions at interfaces are important nanoscale phenomena, making them natural targets for atomistic modeling, yet interatomic potentials must be fit to secondary physical properties. To isolate the important factors that interatomic potentials must capture in order to accurately model such behavior, the performance of four interatomic potentials was evaluated for the Cu-Zr system, with experimental observations used to provide validation. While experimental results show strong Zr segregation to grain boundary regions and the formation of nanoscale amorphous complexions at high temperatures and/or dopant compositions, a variety of disparate behaviors can be observed in hybrid Monte Carlo/molecular dynamics simulations of doping, depending on the chosen potential. The potentials that are able to recreate the correct behavior accurately reproduce the enthalpy of mixing as well as the bond energies, providing a roadmap for the exploration of interfacial phenomena with atomistic modeling. Finally, we use our observations to find a reliable potential for the Ni-Zr system and show that this alloy should also be able to sustain amorphous complexions.

cond-mat.mtrl-sci↗

arXiv2017

Materials selection rules for amorphous complexion formation in binary metallic alloys

Complexions are phase-like interfacial features that can influence a wide variety of properties, but the ability to predict which material systems can sustain these features remains limited. Amorphous complexions are of particular interest due to their ability to enhance diffusion and damage tolerance mechanisms, as a result of the excess free volume present in these structures. In this paper, we propose a set of materials selection rules aimed at predicting the formation of amorphous complexions, with an emphasis on (1) encouraging the segregation of dopants to the interfaces and (2) lowering the formation energy for a glassy structure. To validate these predictions, binary Cu-rich metallic alloys encompassing a range of thermodynamic parameter values were created using sputter deposition and subsequently heat treated to allow for segregation and transformation of the boundary structure. All of the alloys studied here experienced dopant segregation to the grain boundary, but exhibited different interfacial structures. Cu-Zr and Cu-Hf formed nanoscale amorphous intergranular complexions while Cu-Nb and Cu-Mo retained crystalline order at their grain boundaries, which can mainly be attributed to differences in the enthalpy of mixing. Finally, using our newly formed materials selection rules, we extend our scope to a Ni-based alloy to further validate our hypothesis, as well as make predictions for a wide variety of transition metal alloys.

cond-mat.mtrl-sci↗

arXiv2017

Mechanisms of near-surface structural evolution in nanocrystalline materials during sliding contact

The wear-driven structural evolution of nanocrystalline Cu was simulated with molecular dynamics under constant normal loads, followed by a quantitative analysis. While the microstructure far away from the sliding contact remains unchanged, grain growth accompanied by partial dislocations and twin formation was observed near the contact surface, with more rapid coarsening promoted by higher applied normal loads. The structural evolution continues with increasing number of sliding cycles and eventually saturates to a stable distinct layer of coarsened grains, separated from the finer matrix by a steep gradient in grain size. The coarsening process is balanced by the rate of material removal when the normal load is high enough. The observed structural evolution leads to an increase in hardness and decrease in friction coefficient, which also saturate after a number of sliding cycles. This work provides important mechanistic understanding of nanocrystalline wear, while also introducing a methodology for atomistic simulations of cyclic wear damage under constant applied normal loads.

cond-mat.mtrl-sci↗

arXiv2017

Nanocrystalline Al-Mg with extreme strength due to grain boundary doping

Nanocrystalline Al-Mg alloys are used to isolate the effect of grain boundary doping on the strength of nanostructured metals. Mg is added during mechanical milling, followed by low homologous temperature annealing treatments to induce segregation without grain growth. Nanocrystalline Al -7 at.% Mg that is annealed for 1 h at 200 °C is the strongest alloy fabricated, with a hardness of 4.56 GPa or approximately three times that of pure nanocrystalline Al. Micropillar compression experiments indicate a yield strength of 865 MPa and a specific strength of 329 kN m/kg, making this one of the strongest lightweight metals reported to date.

cond-mat.mtrl-sci↗

arXiv2017

Spatial variation of short-range order in amorphous intergranular complexions

Amorphous materials lack long-range order but short-range order can still persist through the recurrence of similar local packing motifs. While the short-range order in bulk amorphous phases has been well studied and identified as an intrinsic factor determining the material properties, these features have not been studied in disordered intergranular complexions. In this work, the short-range order in two types of amorphous complexions is studied with a Voronoi tessellation method. Amorphous complexions can have three distinct regions: amorphous-crystalline interfaces, regions deep inside the films that have short-range order identical to a bulk amorphous phase, and transition regions that connect the first two regions. However, thin amorphous films contain only the amorphous-crystalline interface and the transition region, providing further evidence of the constraints imposed by the abutting crystals. The thickness of the transition region depends on film thickness at low temperatures but becomes thickness-independent at high temperatures. Similarly, the complexion short-range order is dependent on the interfacing crystal plane at low temperatures, but this effect is lost at high temperatures. Our findings show that amorphous complexions contain spatial gradients in short-range order, meaning they are both structurally and chemically different from bulk metallic glasses.

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arXiv2016

Formation of ordered and disordered interfacial films in immiscible metal alloys

Atomistic simulations are used to study segregation-induced intergranular film formation in Cu-Zr and Cu-Nb alloys. While Cu-Zr forms structurally disordered or amorphous films, ordered films comprised of a second phase usually precipitate in Cu-Nb, with a critical nucleation size of ~1 nm below which the ordered phase cannot form. While the ordered film is retained at high temperature for a low energy Σ11 (113) boundary, a disordering transition is observed for a high energy Σ5 (310) boundary at low dopant concentrations. Finally, the effect of free surfaces on dopant segregation and intergranular film formation is investigated for both alloys.

cond-mat.mtrl-sci↗

arXiv2016

Plasticity-induced restructuring of a nanocrystalline grain boundary network

The grain boundary-mediated mechanisms that control plastic deformation of nanocrystalline metals should cause evolution of the grain boundary network, since they directly alter misorientation relationships between crystals. Unfortunately, current experimental techniques are unable to track such evolution, due to limits on both spatial and temporal resolution. In this work, molecular dynamics simulations are used to study grain boundary restructuring in nanocrystalline Al during both monotonic tension and cyclic loading. This task is enabled by the creation of new analysis tools for atomistic datasets that allow for a complete characterization and tracking of microstructural descriptors of the grain boundary network. Quantitative measurements of grain boundary character distribution, triple junction type, grain boundary plane normal, and other interfacial network characteristics are extracted and analyzed. The results presented here show that nanocrystalline plasticity leads to an increase in special boundary fraction and disruption of two-dimensional boundary connectivity, with the most dramatic evolution occurring in the smallest grain sizes.

cond-mat.mtrl-sci↗

arXiv2016

Effect of grain boundary character on segregation-induced structural transitions

Segregation-induced structural transitions in metallic grain boundaries are studied with hybrid atomistic Monte Carlo/molecular dynamics simulations using Cu-Zr as a model system, with a specific emphasis on understanding the effect of grain boundary character. With increasing global composition, the six grain boundary types chosen for this study first form ordered complexions, with the local segregation pattern depending on the grain boundary core structure, then transform into disordered complexions when the grain boundary composition reaches a critical value that is temperature dependent. The tendency for this transition to a disordered interfacial structure consistently depends on the relative solute excess, instead of the grain boundary energy or misorientation angle. Grain boundaries with high relative solute excess go through gradual disordering transitions, whereas those with low relative solute excess remain ordered until high global Zr concentrations but then abruptly transform into thick disordered films. The results presented here provide a clear picture of the effect of interface character on both dopant segregation patterns and disordered intergranular film formation, showing that all grain boundaries are not equal when discussing complexion transitions.

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arXiv2015

Grain boundary character distributions in nanocrystalline metals produced by different processing routes

Nanocrystalline materials are defined by their fine grain size, but details of the grain boundary character distribution should also be important. Grain boundary character distributions are reported for ball milled, sputter deposited, and electrodeposited Ni and Ni-based alloys, all with average grain sizes of ~20 nm, to study the influence of processing route. The two deposited materials had nearly identical grain boundary character distributions, both marked by a Σ3 length percentage of 23-25%. In contrast, the ball milled material had only 3% Σ3-type grain boundaries and a large fraction of low angle boundaries (16%), with the remainder being predominantly random high angle (73%). These grain boundary character measurements are connected to the physical events that control their respective processing routes. Consequences for material properties are also discussed with a focus on nanocrystalline corrosion. As a whole, the results presented here show that grain boundary character distribution, which has often been overlooked in nanocrystalline metals, can vary significantly and influence material properties in profound ways.

cond-mat.mtrl-sci↗

arXiv2015

High-temperature stability and grain boundary complexion formation in a nanocrystalline Cu-Zr alloy

Nanocrystalline Cu-3 at.% Zr powders with ~20 nm average grain size were created with mechanical alloying and their thermal stability was studied from 550-950 °C. Annealing drove Zr segregation to the grain boundaries, which led to the formation of amorphous intergranular complexions at higher temperatures. Grain growth was retarded significantly, with 1 week of annealing at 950 °C, or 98% of the solidus temperature, only leading to coarsening of the average grain size to 54 nm. The enhanced thermal stability can be connected to both a reduction in grain boundary energy with doping as well as the precipitation of ZrC particles. High mechanical strength is retained even after these aggressive heat treatments, showing that complexion engineering may be a viable path toward the fabrication of bulk nanostructured materials with excellent properties.

cond-mat.mtrl-sci↗

arXiv2015

Amorphous intergranular films act as ultra-efficient point defect sinks during collision cascades

Atomistic simulations are used to explore the effect of interfacial structure on residual radiation damage. Specifically, an ordered grain boundary is compared to a disordered amorphous intergranular film, to investigate how interface thickness and free volume impacts point defect recombination. The collision cascades induced by neutron bombardment are simulated and residual point defect populations are analyzed as a function of boundary type and primary knock on atom energy. While ordered grain boundaries easily absorb interstitials, these interfaces are inefficient vacancy sinks. Alternatively, amorphous intergranular films act as ultra-efficient, unbiased defect sinks, providing a path for the creation of radiation-tolerant materials.

cond-mat.mtrl-sci↗

arXiv2015

Disruption of Thermally-Stable Nanoscale Grain Structures by Strain Localization

Nanocrystalline metals with average grain sizes of only a few nanometers have recently been observed to fail through the formation of shear bands. Here, we investigate this phenomenon in nanocrystalline Ni which has had its grain structure stabilized by doping with W, with a specific focus on understanding how strain localization drives evolution of the nanoscale grain structure. Shear banding was initiated with both microcompression and nanoindentation experiments, followed by site-specific transmission electron microscopy to characterize the microstructure. Grain growth and texture formation were observed inside the shear bands, which had a wide variety of thicknesses. These evolved regions have well-defined edges, which rules out local temperature rise as a possible formation mechanism. No structural evolution was found in areas away from the shear bands, even in locations where significant plastic deformation had occurred, showing that plastic strain alone is not enough to cause evolution. Rather, intense strain localization is needed to induce mechanically-driven grain growth in a thermally-stable nanocrystalline alloy.

cond-mat.mtrl-sci↗

arXiv2015

Amorphous intergranular films as toughening structural features

The ability of amorphous intergranular films to mitigate damage formation at grain boundaries is studied with molecular dynamics simulations. We find that such films can alter both crack nucleation and crack growth rates by efficiently absorbing dislocations, with thicker films being more effective sinks. Local plastic strain brought by incoming dislocations is diffused into a triangular region within the amorphous film and is accommodated by a flow of boundary atoms which resembles a vortex shape; this vortex grows inside of the amorphous intergranular film as more dislocations are absorbed until it reaches the opposite amorphous-crystalline interface, after which cracks can finally be nucleated. Even after nucleation, these cracks grow more sluggishly in an amorphous intergranular film than they do along a clean grain boundary, since the driving force for crack growth is lower in the amorphous film. The results presented here suggest that amorphous intergranular films can act as toughening features within a microstructure, and thus are promising for designing nanostructured materials with better ductility and fracture toughness.

cond-mat.mtrl-sci↗

arXiv2014

Quantitative tracking of grain structure evolution in a nanocrystalline metal during cyclic loading

Molecular dynamics simulations were used to quantify mechanically-induced structural evolution in nanocrystalline Al with an average grain size of 5 nm. A polycrystalline sample was cyclically strained at different temperatures, while a recently developed grain tracking algorithm was used to measure the relative contributions of novel deformation mechanisms such as grain rotation and grain sliding. Sample texture and grain size were also tracked during cycling, to show how nanocrystalline plasticity rearranges overall grain structure and alters the grain boundary network. While no obvious texture is developing during cycling, the processes responsible for plasticity act collectively to alter the interfacial network. Cyclic loading led to the formation of many twin boundaries throughout the sample as well as the occasional coalescence of neighboring grains, with higher temperatures causing more evolution. A temperature-dependent cyclic strengthening effect was observed, demonstrating that both the structure and properties of nanocrystalline metals can be dynamic during loading.

cond-mat.mtrl-sci↗

arXiv2014

Emergence of localized plasticity and failure through shear banding during microcompression of a nanocrystalline alloy

Microcompression testing is used to probe the uniaxial stress-strain response of a nanocrystalline alloy, with an emphasis on exploring how grain size and grain boundary relaxation state impact the complete flow curve and failure behavior. The yield strength, strain hardening, strain-to-failure, and failure mode of nanocrystalline Ni-W films with mean grain sizes of 5, 15, and 90 nm are studied using taper-free micropillars that are large enough to avoid extrinsic size effects. Strengthening is observed with grain refinement, but catastrophic failure through strain localization is found as well. Shear banding is found to cause failure, resembling the deformation of metallic glasses. Finally, we study the influence of grain boundary state by employing heat treatments that relax nonequilibrium boundary structure but leave grain size unchanged. A pronounced strengthening effect and increased strain localization is observed after relaxation in the finer grained samples.

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