Nanocrystalline metals: transient testing during in situ X-ray diffraction and molecular dynamics

Nanocrystalline (NC) metals have attracted widespread interest in materials science due to their high strength compared to coarse-grained counterparts. It is well know that during uniaxial deformation, the stress-strain behaviour exhibits an extraordinary work-hardening followed by an early observation of constant flow stress. Information on possible deformation mechanisms have been gathered by extensive research combining in situ deformation experiments, electron microscopy observations and computational modelling. Generally, these mechanisms are categorized into two types: dislocation slip and grain boundary (GB) accommodation processes, as for instance, GB sliding based mechanisms and GB migration eventually coupled to the shear stress. However, the interplay between these mechanisms resulting in the constant deformation resistance is not fully understood. Transient testing has proven to be a suitable tool to gather information on the rate limiting deformation mechanisms that are activated during the deformation path. In particular in stress reduction experiments, after an intermediate/large stress drop thermally activated dislocation slip is suppressed so that other underlying mechanisms are brought into foreground during subsequent transient creep. Those mechanisms may play a minor role in the determination of the flow stress but might still be essential to the development of a constant deformation resistance. Within this thesis, transient testing is combined with in situ X-ray diffraction at the Swiss Light Source. Therefore, the transient responses are captured in terms of evolution of macrostrain as well as diffraction peak broadening. Since dislocation slip and GB accommodation have an opposite footprint on the peak broadening, the presence of these two types of mechanisms can be distinguished. Three electrodeposited NC materials with different grain sizes are investigated: two NC Ni batches and one NC Ni50Fe50 batch. The results reveal that the constant flow stress reached during uniaxial deformation of electrodeposited NC metals reflects a quasi-stationary balance between dislocation-based mechanisms and GB-mediated accommodation. The latter plays an important role in producing plastic strain and recovering the defects and internal stress. Depending on the magnitude of the stress drop, a non-monotonic behaviour of the diffraction peak width is observed, suggesting an alternation of mechanisms. Also, by comparing transient responses among different NC materials, the relative contributions of dislocation slip and GB accommodation mechanisms are discussed in terms of grain size and alloying. Finally, different magnitudes of stress reduction are carried out by molecular dynamics (MD) simulations with the aim to verify in situ experimental results and explore the mechanisms responsible for GB accommodation. MD simulations confirm that dislocation slip is reduced after a moderate stress drop, however can continue to operate after adaption of the GB structures by a variety of GB accommodation mechanisms explaining the non-monotonic behaviour of the peak broadening during transient creep.

Deformation mechanism in nanocrystalline FCC metals studied by atomistic simulations

Christian Brandl

Polycrystalline materials with crystallite diameters below hundred nanometer exhibit extraordinary strength which goes along with a decrease in ductility. In order to tailor tough materials, which combine strength and ductility, the underlying deformation mechanisms have to be understood. Molecular dynamics suggested partial dislocation mediated plasticity in nanocrystalline face-centred cubic (FCC) metals in terms of 1) dislocation nucleation at the grain boundaries, 2) dislocation propagation through the nano-grain, and 3) eventual dislocation absorption in the neighbouring grain boundary network. The partial dislocation nucleation sites were seen to exhibit stress concentrations such as in triple junctions. Moreover, it has been shown that the partial dislocation nucleation is energetically related to the so-called general stacking fault energies (GSFEs). Transmission electron microscopy, in-situ X-ray diffraction, and deformation experiments can be interpreted in terms of the aforementioned dislocation processes. On basis of this knowledge this thesis utilizes atomistic simulation methods to extend the understanding of the fundamental deformation mechanisms which mediate the plasticity in bulk nanocrystalline FCC metals. In the first part of this thesis, ab-initio simulations are exploited to investigate the effect of the superimposed strains in Ni, Al, and Cu on the GSFEs, which describe the energy penalty for rigidly shearing of the crystal. The energy curves are discussed in terms of a) the second and third order elastic constants b) the energy difference between hexagonal closed packed and face centred cubic structures, c) the GSFE / unstable-twinning-fault-energy interdependence and c) the implication on dislocation nucleation. The second part explores the strain rate, temperature, applied stress, and grain size dependence of nanocrystalline Al utilizing classical molecular dynamics simulations. The deformation behaviour is examined on the basis of the underlying deformation mechanism. The higher the strain rate the more the onset of dislocation mediated plasticity is delayed. This can manifest itself into a stress overshoot that diminishes as the strain rate is lowered. The associated critical resolved shear stresses are seen to cause the strain rate sensitivity in the flow stress. In conjunction with the rate dependence of the critical resolved shear stresses, the temperature dependence of the flow stresses supports the picture of thermally activated dislocation processes which control the deformation of nanocrystalline Al in molecular dynamics. Moreover, the strain rate simulations evidence that a subset of dislocation processes operate at the athermal limit which indicates, once more, the difficulty to extrapolate from the high strain rate regime of molecular dynamics towards common experimental conditions. Furthermore, using an iterative strain/relaxation method, athermal critical stresses are calculated for an isolated nano-grain with a nucleated dislocation therein. Dislocation cross-slip is seen to enable a dislocation to by-pass stress concentration, which can hinder the dislocation propagation through the grain, and allows the dislocation to be deposited in preferred grain regions as e.g. triple junctions. This rationalized the observed lack of strain hardening in the molecular dynamics study. Additionally dislocation cross-slip is more pronounced at lower strain rates which indicate the growing importance of the grain boundary structure for dislocation motion as the stresses are lowered. Slip transfer through a high angle grain boundary is observed and is understood in terms of the grain boundary structure, which exhibits regions of preferred dislocation transmission sites. Such structural features are discussed by means of the implication on mesoscopic models of dislocation transmission. Moreover, the grain size study shows discrete stress-drops, which are associated with dislocation mediated processes, in the so-called "inverse" Hall-Petch regime. The deformation behaviour of nanocrystalline Al in molecular dynamics is rationalized in terms of thermally activated processes, and therein the implications of the grain size dependencies are qualitatively discussed.

EPFL2010

An Atomistic Simulation Method for Oxygen Impurities in Aluminium Based on Variable Charge Molecular Dynamics

Andreas Elsener

Impurities are known to have a significant impact on materials properties. In particular, the presence of impurities can change mechanical properties and stabilize the microstructure by reducing grain growth and recrystallization processes. In the past atomistic simulations, in particular molecular dynamics, have contributed a lot to the understanding of deformation mechanisms in nanocrystalline metals. Especially, insights into details of dislocation/GB interactions have been gained. Additionally, simulations on coupled grain boundary migration in bicrystalline samples have played an important role in understanding stress assisted grain growth in nanocrystalline metals. However, all these simulations have been performed on monatomic systems. This means that the role of impurities has not yet been considered in these simulations. Some of the important difference between experiments and simulations could be removed by introducing dilute O distributions to computational Al samples. For this purpose, a simulation method is required which can deal with the oxidation of Al atoms around the O impurities and which can simulate the ionic and metallic nature of bonding simultaneously. Here, a method is suggested which fulfills the requirements by modifying the variable charge method of Streitz and Mintmire [Phys. Rev. B 50, 11996 (1994)]. A local chemical potential approach which optimizes the charge on only those atoms expected to be ionic is developed. Additionally the EAM potential for the non-electrostatic interaction given in the publication of Streitz and Mintmire is substituted by empirical potentials which treat the Al-Al interactions with a well-known Al potential. The Al-O and O-O interactions in these EAM potentials are fitted for the simulation of dilute O impurities in Al and additionally for the simulation of corundum in case of a second potential. The aforementioned developments are applied to study the effect of O impurities on the deformation of nc Al. A fully three-dimensional nc sample containing 15 grains of 12 nm grain-size is deformed with a dilute O content in the triple junction lines. The impact of O impurities on dislocation propagation is also considered in a sample which consists of a single grain extracted from a large molecular dynamics simulation. This simulation geometry contains a perfect dislocation, which is pinned at the surrounding grain boundary network. Therefore it allows the study of pinning strength and after unpinning the propagation behavior of the dislocation under various O impurity distributions. Additionally, the role of O impurities on coupled GB migration is investigated by studying two bicrystalline samples with different O distributions in both of them. In the discussion, the emphasis is on the simulation method. Especially, the significance of the samples, simulation conditions and the performance of the method in the different applications are discussed. Additionally, the different developments (local chemical potential approach and EAM potentials) are critically analyzed and improvements for future simulations of impurities are suggested.

EPFL2010

Deformation behavior of nanoporous polycrystalline silver layers sintered by low temperature bonding: experiment and simulation

Saba Zabihzadeh

Integrated circuit packaging technology has become a prime design consideration for the develop-ment of electronic system concepts. One key issue is the bonding layer between chip and substrate. Currently, high-lead solder materials are being used, which apart from their environmental problem, limit the reliable operation temperature of devices to temperatures lower than 175ºC. Low-temperature bonding by sintering nanograin sized silver is emerging as a promising replacement in power electronics modules working at high temperatures. Although silver has been studied as bonding material since three decades, it has not been widely used in the packaging industry which might be ascribed to the limited knowledge on its mechanical behavior. In this work, the microstructure of thin layers of nanoporous silver sintered under different conditions are studied and linked to the mechanical behavior (at room temperature) using X-ray diffraction in-situ deformation tests and finite element simulations. First the microstructure of several samples such as grain size distribution, defect structures, porosity, pore morphology and ligament size distribution are investigated and are related to the corresponding sintering conditions. Electron microscopy, high resolution X-ray imaging, and X-ray diffraction techniques are the employed characterization methods. We found a strong dependency of the microstructure on the sintering conditions. Afterward, series of X-ray diffraction in-situ continuous, load-unload and stress relaxation tensile tests are performed to study the deformation mechanisms at room temperature. All samples exhibit small elongation and a large hysteresis in the stress-strain curve. From the change in the peak position upon unloading the residual elastic strain inside the sample is calculated while the evolution of the peak broadening provides information on the recovery mechanisms and induced dislocations. A significant recovery in the peak position and peak broadening after unloading and during relaxation is observed for all specimens. This is attributed to the presence of the pores. We found that the density of generated dislocations during tensile deformation depends on the porous structure. The results suggest that there exist two contributions to deformation: one related to the pores and other to intra-granular dislocations. The competition between both mechanisms is discussed in terms of porosity and grain size. Finally, 3D FE microstructure-based simulations are performed to allow a better correlation between the porous morphology and mechanical behavior. The 3D reconstructed images of nanoporous silver obtained from X-ray ptychography are used as an input to create finite element meshes of the actual porous morphology. For homogenization purpose, a representative volume element approach is chosen. The apparent elastoplastic response of the bulk silver is extracted from the porous samples using inverse homogenization method. The simulations allow distinguishing between the interplay and role of the ligament size, pore morphology and porosity, and provide a better comprehension on the experimental observations. We show that the proposed model has a predictive character for general nanoporous silver microstructures.

EPFL2016

An Atomistic Simulation Method for Oxygen Impurities in Aluminium Based on Variable Charge Molecular Dynamics

Andreas Elsener

EPFL2010

Deformation behavior of nanoporous polycrystalline silver layers sintered by low temperature bonding: experiment and simulation

Saba Zabihzadeh

EPFL2016

Deformation mechanism in nanocrystalline FCC metals studied by atomistic simulations

Christian Brandl

EPFL2010