Large-scale Molecular Dynamics Simulations Research Articles

Unified understanding of the impact of semiflexibility, concentration, and molecular weight on macromolecular-scale ring diffusion

Conformationally fluctuating, globally compact macromolecules such as polymeric rings, single-chain nanoparticles, microgels, and many-arm stars display complex dynamic behaviors due to their rich topological structure and intermolecular organization. Synthetic rings are hybrid objects with conformations that display both ideal random walk and compact globular features, which can serve as models of genomic DNA. To date, emphasis has been placed on the effect of ring molecular weight on their unusual behaviors. Here, we combine simulations and a microscopic force-level theory to build a unified understanding for how key aspects of ring dynamics depend on different tunable molecular properties including backbone rigidity, monomer concentration, degree of traditional entanglement, and molecular weight. Our large-scale molecular dynamics simulations of ring melts with very different backbone stiffnesses reveal unanticipated behaviors which agree well with our generalized theory. This includes a universal master curve for center-of-mass diffusion constants as a function of molecular weight scaled by a chemistry and thermodynamic state-dependent critical molecular weight that generalizes the concept of an entanglement cross-over for linear chains. The key physics is how backbone rigidity and monomer concentration induced changes of the entanglement length, interring packing, degree of interpenetration, and liquid compressibility slow down space-time dynamic-force correlations on macromolecular scales. A power law decay of the center-of-mass diffusion constant with inverse molecular weight squared is the first consequence, followed by an ultraslow activated hopping transport regime. Our results set the stage to address slow dynamics and kinetic arrest in different families of compact synthetic and biological polymeric systems.

Role of dislocations on martensitic transformation temperatures and microstructure: A molecular dynamics study

Microstructure and defects strongly affect martensitic transformations in metallic alloys. Significant progress has been made in understanding the atomic-level processes that control the role of grain boundaries and precipitates in these solid-to-solid phase transformations. Yet, the role of dislocations and their structures on martensitic transformation temperature and the resulting microstructure remains unclear. Therefore, we used large-scale molecular dynamics simulations to study the forward and reverse transformation of a martensitic material modeled after Ni63Al37 under cyclic thermal loading. The simulations reveal that dislocations in the austenite phase act as one-dimensional seeds for the martensite phase, which is present at temperatures significantly above the martensite start value. We find a reduction in the dislocation density during cyclic thermal loading, which results in the increase in martensite and austenite transition temperatures, in agreement with experiments. Importantly, we extracted a critical martensitic nuclei size for developing stable domains and found that relatively low dislocation densities are needed to grow independent martensitic variants resulting in a multi-domain structure.

Heterogeneous Structure and Dynamics of Water in a Hydrated Collagen Microfibril.

Collagen type I is well-known for its outstanding mechanical properties which it inherits from its hierarchical structure. Collagen type I fibrils may be viewed as a heterogeneous material made of protein, macromolecules (such as glycosaminoglycans and proteoglycans) and water. Water content modulates the properties of these fibrils. Yet, the properties of water and the fine interactions of water with the protein constituent of these heterofibrils have only received limited attention. Here, we propose to model collagen type I fibrils as a hydrated structure made of tropocollagen molecules assembled in a microfibril crystal. We perform large-scale all-atom molecular dynamics simulations of the hydration of collagen fibrils beyond the onset of disassembly. We found that the structural and dynamic properties of water vary strongly with the level of hydration of the microfibril. More importantly, we found that the properties vary spatially within the 67 nm D-spacing periodic structure. Alteration of the structural and dynamical properties of the collagen microfibril occur first in the gap region. Overall, we identify that the change in the role of water molecules from glue to lubricant between tropocollagen molecules arises around 100% hydration while the microfibril begins to disassemble beyond 130% water content. Our findings are supported by a decrease in hydrogen bonding, recovery of bulk water properties and amorphization of the tropocollagen molecules packing. Our simulations reveal the structure and dynamics of hydrated collagen fibrils with unprecedented spatial resolution from physiological conditions to disassembly. Beyond the process of self-assembly and the emergence of mechanical properties of collagen type I fibrils, our results may also provide new insights into mineralization of collagen fibrils.

Atomic simulations of crack propagation in Ni-Al binary single crystal superalloy with a central crack

Nickel (Ni)-based single-crystal superalloys are of great importance in the aircraft industry due to their excellent mechanical properties, and cracks as unavoidable defects may affect the mechanical performances of materials dramatically. In this paper, large scale molecular dynamics (MD) simulations are carried out to understand the deformation mechanisms of Ni-based single crystal with a central crack under tension. Here, the effects of matrixes (γ, γ′ and γ/γ′), strain rates (1 × 109 s−1 ∼ 3 × 109 s−1) and temperatures (300 K∼900 K) on the role of crack propagation are considered. It is observed that dislocations and slip systems in the γ′ model are concentrated near the crack, resulting in the rapid expansion of dislocation, which leads to the fastest crack growth speed and early fracture. While the crack propagation rate of γ and γ/γ′ models are relatively slow, due to the combined action of the Lomer-Cottrell lock and stacking fault tetrahedron structure and Stair-rod dislocation, which hinders crack propagation. In addition, deformation at increased strain rates and/or reduced temperatures, lead to superior yield stress and Young′s modulus for models with a central crack at γ/γ′ interface. On the other hand, high temperature and high strain rate will promote crack propagation in the γ phase, and the higher the strain rate and/or temperature, the faster the crack propagation speed will be. These results will enrich our understanding on the crack propagation and evolution mechanisms in Ni-based single crystal superalloy.

Simultaneous Improvement in the Elastic and Fracture Properties of Graphene-Epoxy Nanocomposites ̶ a Computational Perspective

The incorporation of stiff nano-additives (such as graphene) into a relatively soft polymer material (such as epoxy) usually leads to an improvement in elastic properties (i.e., Young’s modulus) at the expense of fracture properties (i.e., tensile strength and toughness). Despite over a decade of research in polymer nanocomposites, we still lack a clear understanding of their structure-property relationships, which limits us from enhancing both elastic and fracture properties concurrently. Here, we performed large-scale reactive molecular dynamics simulations to study the deformation and fracture of model graphene/epoxy systems under uniaxial tension. A computationally efficient reactive force field was developed for graphene-epoxy system, allowing covalent bond formation, and breaking, which is crucial to model cross-linking in model epoxy as well as fracture. It was found the mechanical properties of the nanocomposite are very sensitive to the strength of the graphene-epoxy interface. As expected, elastic modulus increases with the interfacial strength. However, there appears to be an optimal interfacial strength to enhance the tensile strength and toughness. This is due to stress concentration occurring near the graphene edges at high interfacial strength, which leads to premature fracture. We show that by appropriately selecting an intermediate interface strength, one can simultaneously improve the ultimate tensile strength, toughness and the Young’s modulus of the nanocomposite epoxy at ultra-low (∼0.2% by weight) loading fraction of graphene additives. Our findings highlight the critical importance of properly engineered additive-matrix interfacial strength to develop high-performing polymer nanocomposites that are concurrently stiff, strong as well as tough.

Shock response of gradient nanocrystalline CoCrNi medium entropy alloy

A comprehensive investigation of shock-induced deformation and spallation mechanisms in nanocrystalline CoCrNi medium-entropy alloys (MEAs) is conducted by large-scale molecular dynamics simulations, encompassing both gradient and homogeneous nanocrystalline structures. Under the shock velocity ranging from 0.2 km/s to 1 km/s, the effects of grain heterogeneity on shock wave propagation, spallation and defect evolution are examined. An inverse Hall–Petch relationship, where the Hugoniot elastic limit (HEL) increases with larger grain sizes is observed within the grain size range of 3 to 12 nm for homogeneous nanocrystalline samples. Compared to the localized strain distribution either within grain interior (GI) or at grain boundaries (GB) in homogeneous nanocrystalline structures, gradient-grained counterparts exhibit compatible deformation along shock direction, which coordinates the load partitioning between GB and GI. As a result, lower densities of dislocation and stacking fault are triggered within the GI, while shear localization is mitigated at GB, leading to higher spall strength observed in the gradient nanocrystalline MEA samples at the same shock velocity. The results shed light on the insights of deformation and spallation mechanisms in gradient-grained MEAs under dynamic loading, which may open up a new avenue for the design of advanced structural MEAs with high strength and toughness.

Proton Collective Quantum Tunneling Induces Anomalous Thermal Conductivity of Ice under Pressure.

Proton tunneling is believed to be nonlocal in ice, but its range has been shown to be limited to only a few molecules. Here, we measured the thermal conductivity of ice under pressure up to 50GPa and found it increases with pressure until 20GPa but decreases at higher pressures. We attribute this nonmonotonic thermal conductivity to the collective tunneling of protons at high pressures, supported by large-scale quantum molecular dynamics simulations. The collective tunneling loops span several picoseconds in time and are as large as nanometers in space, which match the phonon periods and wavelengths, leading to strong phonon scattering at high pressures. Our results show direct evidence of global quantum motion existing in high-pressure ice and provide a new perspective to understanding the coupling between phonon propagation and atomic tunneling.

Markov State Models Reveal How Folding Kinetics Influence Absorption Spectra of Foldamers.

Self-assembly of platinum(II) complex foldamers is an essential approach to fabricate advanced luminescent materials. However, a comprehensive understanding of folding kinetics and their absorption spectra remains elusive. By constructing Markov state models (MSMs) from large-scale molecular dynamics simulations, we reveal that two largely similar dinuclear alknylplatinum(II) terpyridine foldamers, Pt-PEG and Pt-PE with slightly different bridges, exhibit distinctive folding kinetics. Particularly, Pt-PEG bears bridge-dominant, plane-dominant, and cooperative pathways, while Pt-PE only prefers the plane-dominant pathway. Such preference originates from their difference in intrabridge electrostatic interactions, leading to contrastive distributions of metastable states. We also found that the bridge-dominant pathway for Pt-PEG becomes more favorable when lowering the temperature. Interestingly, based on the comprehensive conformation ensembles from our MSMs, we reveal the conformation-dependent absorption spectra of Pt-PEG and Pt-PE. Our theoretical spectra not only align with experimental results but also reveal the contributions of diverse conformations to the overall absorption bands explicitly, facilitating the rational design of stimuli-responsive smart luminescent molecules.

Precision Atomistic Structures of Actinium-/Radium-/Barium-Doped Lanthanide Nanoconstructs for Radiotherapeutic Applications.

Lanthanide vanadate (LnVO4) nanoconstructs have generated considerable interest in radiotherapeutic applications as a medium for nanoscale-targeted drug delivery. For cancer treatment, LnVO4 nanoconstructs have shown promise in encapsulating and retaining radionuclides that emit alpha-particles. In this work, we examined the structure formation of LnVO4 nanoconstructs doped with actinium (Ac) and radium (Ra), both experimentally and using large-scale atomistic molecular dynamics simulations. LnVO4 nanoconstructs were synthesized via a precipitation method in aqueous media. The reaction conditions and elemental compositions were varied to control the structure, fluorescence properties, and size distribution of the LnVO4 nanoconstructs. LnVO4 nanoconstructs were characterized by X-ray diffraction, Raman spectroscopy, and fluorescence spectroscopy. Molecular dynamics simulations were performed to obtain a fundamental understanding of the structure-property relationship between radionuclides and LnVO4 nanoconstructs at the atomic length scale. Molecular dynamics simulations with well-established force field (FF) parameters show that Ra atoms tend to distribute across the nanoconstructs' surface in a broader coordination shell, while the Ac atoms are arranged inside a smaller coordination shell within the nanocluster. The Ba atoms prefer to self-assemble around the surface. These theoretical/simulation predictions of the atomistic structures and an understanding of the relationship between radionuclides and LnVO4 nanoconstructs at the atomic scale are important because they provide design principles for the future development of nanoconstructs for targeted radionuclide delivery.

Shear-promoted graphite-to-diamond phase transition at the grain boundary of nanocrystalline graphite

High pressure has traditionally been considered essential for the transformation of graphite into diamond. However, reducing the transition pressure required for this graphite-to-diamond (G2D) conversion holds significant appeal in both scientific research and engineering applications. In this study, we conducted large-scale molecular dynamics (MD) simulations using an environment-dependent interaction potential (EDIP) to examine the shear deformation of nanocrystalline graphite (n-graphite) with a grain size of approximately 6.5 nm. We discovered that the G2D transition pressure in n-graphite can be reduced to 2–3 GPa, significantly lower than the ∼90 GPa uniaxial stress required in crystalline graphite. This reduction is primarily due to concentrated local shear stresses at grain boundaries (GBs), which induce substantial rotations of graphite layers. These rotations facilitate the initial formation of diamond bonds at sites of pre-existing imperfections at the GBs, assisted by shear. Once initiated at the GBs, the G2D transition rapidly propagates within grains aligned parallel to the shear components, resulting in the formation of nanocrystalline diamond. Our findings underscore the critical roles of GBs and shear stress in enabling the G2D transition in n-graphite.

Rational Design of Dual-Functionalized Gd@C82 Nanoparticles to Relieve Neuronal Cytotoxicity in Alzheimer's Disease via Inhibition of Aβ Aggregation.

The accumulation of amyloid-β (Aβ) peptides is a major hallmark of Alzheimer's disease (AD) and plays a crucial role in its pathogenesis. Particularly, the structured oligomeric species rich in β-sheet formations were implicated in neuronal organelle damage. Addressing this formidable challenge requires identifying candidates capable of inhibiting peptide aggregation or disaggregating preformed oligomers for effective antiaggregation-based AD therapy. Here, we present a dual-functional nanoinhibitor meticulously designed to target the aggregation driving force and amyloid fibril spatial structure. Leveraging the exceptional structural stability and facile tailoring capability of endohedral metallofullerene Gd@C82, we introduce desired hydrogen-binding sites and charged groups, which are abundant on its surface for specific designs. Impressively, these designs endow the resultant functionalized-Gd@C82 nanoparticles (f-Gd@C82 NPs) with high capability of redirecting peptide self-assembly toward disordered, off-pathway species, obstructing the early growth of protofibrils, and disaggregating the preformed well-ordered protofibrils or even mature Aβ fibrils. This results in considerable alleviation of Aβ peptide-induced neuronal cytotoxicity, rescuing neuronal death and synaptic loss in primary neuron models. Notably, these modifications significantly improved the dispersibility of f-Gd@C82 NPs, thus substantially enhancing its bioavailability. Moreover, f-Gd@C82 NPs demonstrate excellent cytocompatibility with various cell lines and possess the ability to penetrate the blood-brain barrier in mice. Large-scale molecular dynamics simulations illuminate the inhibition and disaggregation mechanisms. Our design successfully overcomes the limitations of other nanocandidates, which often overly rely on hydrophobic interactions or photothermal conversion properties, and offers a viable direction for developing anti-AD agents through the inhibition and even reversal of Aβ aggregation.

The origin of phase separation in binary aluminosilicate glasses

The quest for hard and tough transparent oxide glasses is at the core of glass science and technology. Aluminosilicate glasses exhibiting nanoscale phase separation emerge as promising candidates for such materials. Nevertheless, proper control of the phase separation represents a daunting challenge due to its elusive origins. Here we employ large-scale molecular dynamics simulations and structural analysis to unravel the underlying mechanisms of the phase separation in aluminosilicate. The observed phase separation originates from an arrangement of SiO4 and AlOn polyhedra, which manifests from the second coordination shell and extends to higher shells. This specific arrangement is driven by repulsion between the polyhedra, reaching its maximum at around 50 mol% of Al2O3. This behavior becomes pronounced around and below the glass transition temperature. This work sheds light on the origin of phase separation and provides a route for further exploration across other compositions to develop glasses with adapted mechanical performance.

Understanding anti-corrosion mechanisms of the 2,6-dithiopurine (DTP) inhibitor molecule on iron surfaces

Purine derivatives present a high efficiency for anti-corrosion purposes while the nanoscale mechanisms are not yet fully understood. In this work, the inhibition mechanism of the 2,6-dithiopurine (DTP) molecule was investigated using advanced characterizations and atomic simulations. We revealed that the DTP molecule undergoes a multi-layer adsorption mode and is governed by both chemisorption and physisorption processes. An organometallic layer at a thickness of ∼3.8 nm was captured using TEM, comprised of Fe-N and Fe-S bonds strongly anchored to the iron interfaces, as confirmed by the XPS analysis. Our quantum chemical calculations showed that heteroatoms such as N or S in the DTP molecule offer reactive sites that facilitate its chemisorption onto iron surfaces, to form metal-organic bonds (specifically, Fe-N and Fe-S) at the DTP-iron interfaces. We further employed molecular dynamics simulations to investigate the interaction between DTP molecule and various substrates. Our findings suggest that the hydroxyl groups on the lepidocrocite surface can significantly promote bonding between DTP and iron surfaces. Based on large-scale molecular dynamics simulations, we discovered that DTP can exhibit a strong binding affinity for aggressive ions, leading to a considerable decrease in the self-diffusion coefficient of hydronium ions of up to 70 %. This work provides a new understanding of anti-corrosion mechanisms and offers opportunities to design new corrosion inhibitors possessing multiple reactive sites and strong bonding with the substrate.

Micro-jetting: Areal density calculation from a triangular groove

We present a method for calculating the mass ejected during the reflection of a shock wave on a triangular groove. This calculation is based on the combination of two models taken from the literature, BMPT-2, on the one hand, for the calculation of the velocity and density of the jet, and fragmentation zone propagation (FZP ) on the other hand, for the calculation of the ejected mass, certain parameters required for FZP being determined by BMPT-2. Compared with previous work, FZP has been extended to deal with the various stages of jet formation. The approach was first evaluated on tin using a large-scale molecular dynamics simulation. This first step validated the overall phenomenology and the associated theoretical tools, and enabled us to propose a procedure for adjusting FZP. Next, we used the BMPT-2/FZP combination to analyze ejected mass measurement experiments using Asay foil. The areal mass curves are well reproduced with few parameters, showing that there is no inconsistency between BMPT-2/FZP and the experiments. Finally, a more detailed analysis of the results obtained enables us to set the limits of the jet thickness at the moment of rupture, and to propose a simple analytical form of its profile compatible with the model used.

Molecular Dynamics Simulation of the Interaction within the Carboxymethyl Cellulose-Modified Montmorillonite Lamellae at Aggressive CuCl2 Concentrations.

To elucidate the degradation mechanism of the CMC-modified MMT composite at aggressive Cu2+ concentrations, large scale molecular dynamics simulation was conducted for CuCl2 concentrations ranging from 0 to 800 mM. Both CMC and MMT followed the Langmuir isotherm for Cu2+ adsorption, and the adsorption capacity of CMC (8.75 mmol/g) was much higher than that of MMT (0.83 mmol/g). Despite the CMC mass ratio being only 4.1%, it adsorbed up to 34.3% of the total adsorbed Cu2+. The Cu2+ attraction ability hierarchy of oxygen-containing functional groups in the CMC is as follows: carboxylic oxygens > alcoholic oxygens > carbinolic oxygens > bridging oxygens > glucose oxygens. Carboxyls were the most effective in chelating and complexing with Cu2+, and they could be intentionally added in artificially synthesized polymer-MMT composites for Cu2+ containment. Formation of the Cu2+ cation bridge between CMC and MMT at aggressive CuCl2 concentrations contributed to the transition of CMC density distribution from unimodality to bimodality and enhanced resistance of polymer elution. As the CuCl2 concentration increased, the stoichiometric ratio between the chelated Cu2+ and carboxylic oxygens increased from 1:2 to 1:1, suggesting the evolution of the Cu2+ chelation mechanism.

Unraveling the Hall-Petch to inverse Hall-Petch transition in nanocrystalline high entropy alloys under shock loading

The transition from Hall-Petch (HP) to inverse Hall-Petch (IHP) behaviors associated with grain size reduction has been recognized for over two decades. However, the underlying mechanisms for such transition in high entropy alloys (HEAs) under dynamic loading, in which abundant deformation mechanisms could be activated either sequentially or simultaneously, remain unclear. Here, we investigate the HP to IHP transition in nanocrystalline CoCrFeMnNi HEAs under shock loading by examining their deformation mechanisms and flow stresses using large-scale molecular dynamics (MD) simulations. It is found that this transition is strongly dependent on the shock pressure as a result of the complex interplay among multiple competing deformation mechanisms, including the hardening mechanisms such as dislocations interactions and grain boundary (GB) blocking, as well as the softening mechanisms like phase formation, amorphization, GB thickening, and grain rotation. Moreover, there exists a critical shock pressure, which corresponds to the largest critical grain size for the HP-IHP transition. Below the critical shock pressure, the critical grain size increases with pressure due to a stronger hardening effect in grain interior (GIs), while above the critical pressure, the critical grain size first decreases and then undergoes a pressure-insensitive plateau before further decrease due to softening effects in GIs. A theoretical model that includes different deformation mechanisms is proposed for the first time to capture the shock pressure-dependent HP-IHP transition. Our work provides valuable guidance for optimizing the grain size of nanocrystalline HEAs for applications involving dynamic loadings.

Enhancing surface strength of tungsten by gradient nano-grained structure

A gradient nano-grained (GNG) structure demonstrates satisfactory surface strength. However, the underlying mechanism responsible for its strengthening lacks sufficient research. To explain how gradient nano-grained structures improve surface strength in detail, large-scale parallel molecular dynamics simulations are utilized in this study to investigate the mechanical deformation behavior of BCC tungsten with varying grain sizes during spherical nanoindentation. The findings suggest that a well-designed gradient structure can promote rational plasticity and an appropriate distribution of internal atomic stress. The critical point of maximum stress and hardness is observed when the initial grain size is 4.5 nm, with an average grain size of 7.1 nm. The interaction between grain boundary slip and migration in small grains, along with the enhanced activity of grain boundary dislocations in large grains, collectively contributes to the enhancement of the strength and hardness of the GNG structure. Compared with a homogeneous nano-grained structure, the gradient nano-grained structure exhibits a more rational distribution of dislocations and stress relaxation effects to enhance strength. The present work utilizes the molecular dynamics nanoindentation method to study GNG materials, providing a methodology for investigating the surface strengthening effects of GNG structures at the atomic scale and effectively revealing potential mechanisms for resisting surface deformation in GNG structures.

Strain Engineering of Ion-Coordinated Nanochannels in Nanocellulose.

Expanding the interlayer spacing plays a significant role in improving the conductivity of a cellulose-based conductor. However, it remains a challenge to regulate the cellulose nanochannel expanded by ion coordination. Herein, starting from multiscale mechanics, we proposed a strain engineering method to regulate the interlayer spacing of the cellulose nanochannels. First-principles calculations were conducted to select the most suitable ions for coordination. Large-scale molecular dynamics simulations were performed to reveal the mechanism of interlayer spacing expansion by the ion cross-linking. Combining the shear-lag model, we established the relationship between interfacial cross-link density and interlayer spacing of an ion-coordinated cellulose nanochannel. Consequently, fast ion transport and current regulation were realized via the strain engineering of nanochannels, which provides a promising strategy for the current regulation of a cellulose-based conductor.

Low-index mesoscopic surface reconstructions of Au surfaces using Bayesian force fields

Metal surfaces have long been known to reconstruct, significantly influencing their structural and catalytic properties. Many key mechanistic aspects of these subtle transformations remain poorly understood due to limitations of previous simulation approaches. Using active learning of Bayesian machine-learned force fields trained from ab initio calculations, we enable large-scale molecular dynamics simulations to describe the thermodynamics and time evolution of the low-index mesoscopic surface reconstructions of Au (e.g., the Au(111)-‘Herringbone,’ Au(110)-(1 × 2)-‘Missing-Row,’ and Au(100)-‘Quasi-Hexagonal’ reconstructions). This capability yields direct atomistic understanding of the dynamic emergence of these surface states from their initial facets, providing previously inaccessible information such as nucleation kinetics and a complete mechanistic interpretation of reconstruction under the effects of strain and local deviations from the original stoichiometry. We successfully reproduce previous experimental observations of reconstructions on pristine surfaces and provide quantitative predictions of the emergence of spinodal decomposition and localized reconstruction in response to strain at non-ideal stoichiometries. A unified mechanistic explanation is presented of the kinetic and thermodynamic factors driving surface reconstruction. Furthermore, we study surface reconstructions on Au nanoparticles, where characteristic (111) and (100) reconstructions spontaneously appear on a variety of high-symmetry particle morphologies.

Orientation-dependent deformation mechanisms of alpha-uranium single crystals under shock compression

Large-scale non-equilibrium molecular dynamics (NEMD) simulations were employed to investigate the dynamic deformations of alpha-uranium (α-U) single crystals subjected to varying shock strengths along low-index crystallographic orientations. The pronounced anisotropy of α-U gives rise to a complex microstructural evolution under shock loading. In-depth microstructural analysis of post-shock specimens reveals the identification of multiple dynamic deformation mechanisms. Notably, when the shock loading direction aligns with the a-axis, dynamic deformation of the α-U single crystals is primarily dominated by lattice instability, which attributes to a crystalline-to-amorphous transition serving as the dominant shear stress relaxation pathway. On the other hand, shock loading along the b-axis results in an abundance of deformation twins, with twinning planes identified as (130) and (13¯0). During the twinning event, the α-U matrix undergoes a transition to a metastable intermediate phase, subsequently decomposing into a composite structure comprising α-U twins and matrix. This unconventional twinning mechanism significantly deviates from classical theories. Furthermore, upon loading along the c-axis, twinning and a phase transition from α-U to body-centered tetragonal phase (bct-U) occur in α-U single crystal samples. Given that the pressure threshold of this phase transition predicted by ab initio calculations is as high as ∼270 GPa, the phase transition from α-U to bct-U might be implausible. An alternative interatomic potential of uranium with the higher pressure threshold was employed to reinvestigate the shock response of α-U single crystals along the c-axis. The phase transition of α-U to bct-U disappears, and twinning dominates the plastic deformation, with the twinning orientation conforming to the {112} twinning. The strong anisotropy of the α-U lattice triggers a wealth of orientation-dependent dynamic deformation mechanisms. The activation of the twinning system is evidently associated with the loading direction, constituting the potential cause for the discovery of multiple twinning variants during the deformation in polycrystalline uranium.