arXiv subjects

Jefferson Zhe Liu

Publications and source records attributed to Jefferson Zhe Liu.

At least 19 recordsLinked to original sources

arXiv2026

Emergent chiral symmetry breaking in moiré domain wall networks redirects topological boundary states in bilayer graphene

Lattice-mismatched bilayer graphene self-organizes into a moiré network of one-dimensional domain walls that conduct electrons with low dissipation, attractive for low-power electronics. We show these channels are not always straight: as the lattice relaxes to minimize strain, the network can spontaneously curve into chiral morphology. Atomistic simulations map a phase diagram in which the strain-flexibility balance selects one of three stable domain wall morphologies-straight, mono-chiral, or dual-chiral. Electronic structure calculations show that this morphology controls where low-energy electrons accumulate: straight channels concentrate states at the domain-wall-connecting nodes, while chiral channels shift that weight onto the domain walls themselves. This network geometric switch lets the same moiré material support either localized electronic hot spots or directional conducting channels-two strategies for guiding electrons in low-power graphene devices.

cond-mat.mes-hall↗

arXiv2025

Beyond Dielectrics: Interfacial Water Polarization Governs Graphene-Based Electrochemical Interfaces

Water molecules are traditionally regarded as passive dielectric media in electrochemical systems. In this work, we challenge this conventional perspective using molecular dynamics simulations and theoretical analysis. We show that interfacial water is polarized differently from bulk water and effectively screens the electrostatic potential between ions and the surface. This goes beyond the classic electric double layer (EDL) model, which treated water as merely a passive dielectric. The observed overscreening occurs because a significant portion of water polarization directly responds to the graphene surface, in addition to screening the electrostatic interactions between ions and charged surfaces. Furthermore, we reveal that this surface-induced polarization of interfacial water governs the electric potential distribution and EDL capacitance, and can even invert the electrode surface potential polarity, overriding the contribution of ions. These molecular-level insights lead to a revised EDL model that more accurately describes the electric and chemical potential distributions in the interfacial EDL regions.

physics.chem-ph↗

arXiv2024

Domain-Pair Intertwined Topological Domain Structure in Elemental Bi Monolayer

Ferroelectric domain structures, separated by domain walls, often display unconventional physics and hold significant potential for applications in nano-devices. Most naturally growth domain walls are charge-neutral to avoid increased electrostatic energy, while the intrinsically stable charged 180° domain walls in Bi monolayer challenged this conventional knowledge and emerged an unexplored field. Here, using machine-learning potential and molecular dynamics (MD) simulations, we investigated the finite-temperature dynamics of domain walls and discovered a domain-pair intertwined topological domain structure in Bi monolayer. In 180° domain walls, a unique polarization switching mechanism is observed, characterized by the out-of-plane shuffle of Bi atoms without bond breaking. This shuffle mechanism reverses the charge properties of Bi atoms, transforming Bi anions into cations and vice versa, ultimately reversing the polarization. Then, we observed a topological multi-domain structure with two groups of domain pairs intertwined. The charged 180° domain walls form local domain pairs, with the 90° domain walls emerge between different domain pairs. This multi-domain maintains a stable topological structure within the strain range (ε_x = 0 to 4.70%) and exhibits rich domain wall reactions under further applied strain. Our findings provide insights into the charged 180° domain walls and the related topological domain structures, enabling new opportunities for applications in electronic and nano-electronic devices.

cond-mat.mtrl-sci↗

arXiv2024

Physics-based Machine Learning Discovered Nano-circuitry for Nonlinear Ion Transport in Nanoporous Electrodes

Confined ion transport is involved in nanoporous ionic systems. However, it is challenging to mechanistically predict its electrical characteristics for rational system design and performance evaluation using electrical circuit model due to the gap between the circuit theory and the underlying physical chemistry. Here we demonstrate that machine learning can bridge this gap and produce physics-based nano-circuitry, based on equation discovery from the modified Poisson-Nernst-Planck simulation results where an anomalous constructive diffusion-migration interplay of confined ions is unveiled. This bridging technique allows us to gain physical insights of ion dynamics in nanoporous electrodes, such as the non-ideal cyclic voltammetry.

cond-mat.mes-hall↗

arXiv2023

Unexpected Reversed Piezoelectric Response in Elemental Sb and Bi Monolayers

Sb and Bi monolayers, as single-elemental ferroelectric materials with similar atomic structure, hold intrinsic piezoelectricity theoretically, which makes them highly promising for applications in functional nano-devices such as sensors and actuators. Here, using first-principles calculations, we systematically explore the piezoelectric response of Sb and Bi monolayers. Our findings reveal that Sb exhibits a negative piezoelectric response, whereas Bi displays a positive one. This discrepancy is attributed to the dominant role of different atomic internal distortions (internal-strain terms) in response to applied strain. Further electron-density distribution analysis reveals that the atomic bonding in Sb tends to be covalent, while the atomic bonding in Bi leans more towards ionic. Compared to the Sb monolayer, the Bi monolayer is distinguished by its more pronounced lone-pair orbitals electrons and associated larger Born effective charges. The Coulomb repulsions between lone-pair orbitals electrons and the chemical bonds lead to the Bi monolayer possessing more prominent atomic folds and, consequently, more significant atomic distortion in the z-direction under strain. These differences result in a considerable difference in internal-strain terms, ultimately leading to the reversed piezoelectric response between Sb and Bi monolayers. The present work provides valuable insights into the piezoelectric mechanism of 2D ferroelectric materials and their potential applications in nano-electronic devices.

cond-mat.mtrl-sci↗

arXiv2022

A Simple and Efficient Lattice Summation Method for Metallic Electrodes in Constant Potential Molecular Dynamics Simulation

The constant potential molecular dynamics simulation method proposed by Siepmann and Sprik and reformulated later by Reed (SR-CPM) has been widely employed to investigate the metallic electrolyte/electrode interfaces, especially for conducting nanochannels with complex connectivity, *e.g.*, carbide-derived carbon or graphene-assembled membrane. This work makes substantial extensions of this seminal SR-CPM approach. First, we introduce two numerical techniques to determine electrode atom charges with an order of magnitude improvement in computational efficiency compared with those widely employed methods. The first numerical technique dramatically accelerates the to calculation of the Ewald interaction matrix $\mathbf{E}$, which takes advantage of the existing highly optimised electrostatic codes. The second technique introduces a new preconditioning technique in the conjugate gradient method to considerably increase the computational efficiency of a linear equation system that determines electrode atomic charges. Our improved SR-CPM implemented in the LAMMPS package can handle extra-large systems, *e.g.*, over 8.1 million electrode atoms. Second, after demonstrating the importance of the electroneutrality constraint, we propose a two-step method to enforce electroneutrality in the following post-treatment step, applicable for matrix and iterative techniques. Third, we propose a solid theoretical analysis for the adjustable parameter $α_i$ (namely the atomic Hubbard-U $U_i^0$), which is arbitrarily selected in many SR-CPM simulation practices. We proposed that the optimised $α_i$ or $U_i^0$ should compensate for the electrical potential/energy discrepancy between the discrete atomistic model and the continuum limit. The analytical and optimal $α_i^0$ values are derived for a series of 2D materials.

physics.chem-ph↗

arXiv2022

Tunable ferroelectric topological defects on 2D topological surfaces: strain engineering skyrmion-like polar structures in 2D materials

Polar topological structures in ferroelectric thin films have recently drawn significant interest due to their fascinating physical behaviors and promising applications in high-density nonvolatile memories. However, most polar topological patterns are only observed in the perovskites superlattices. Here, we report the discovery of the tunable ferroelectric polar topological defective structures designed and achieved by strain engineering in two-dimensional PbX (X=S, Se, and Te) materials using multiscale computational simulations. First, the first-principles calculations demonstrate the strain-induced recoverable ferroelectric phase transition in such 2D materials. The unique polar topological vortex pattern is then induced by applied mechanical indentation, evidenced by molecular dynamics simulations based on a developed deep-learning potential. According to the strain phase diagram and applied complex strain loadings, the diverse polar topological structures, including antivortex structure and flux-closure structure, are predicted to be emergent through the finite-element simulations. We conclude that strain engineering is promising to tailor various designed reversible polar topologies in ultra-flexible 2D materials, which provide excellent opportunities for next-generation nanoelectronics and sensor devices.

cond-mat.mtrl-sci↗

arXiv2021

Interlayer Sliding-Induced Intralayer Ferroelectric Switching in Bilayer Group-IV Monochalcogenides

Two-dimensional materials with ferroelectric properties break the size effect of conventional ferroelectric materials and unlock unprecedented potentials of ferroelectric-related application at small length scales. In this work, using density functional theory (DFT) calculations, we discover a tribo-ferroelectricity behavior in a group of bilayer group-IV monochalcogenides (MX, with M = Ge, Sn and X = S, Se). Upon interlayer sliding over an in-plane unit cell length, the top layer exhibits a reversible intralayer ferroelectric switching, leading to a reversible transition between the ferroelectric (electric polarization of 40$μ$C/cm$^2$) and antiferroelectric states in the bilayer MXs. Our results show that the interlayer van der Waals interaction, which is usually considered to be weak, can actually generate an in-plane lattice distortion and thus cause the breaking/forming of intralayer covalent bonds in the top layer, leading to the observed tribo-ferroelectricity phenomenon. This unique property has several advantages for energy harvesting over existing piezoelectric and triboelectric nanogenerators. The interlayer sliding-induced polarization change is as high as 40$μ$C/cm$^2$, which can generate an open-circuit voltage two orders of magnitude higher than that of MoS$_2$-based nanogenerators. The polarization change occurs over a time period for interlayer sliding over a unit-cell length, leading to an ultrahigh polarization changing rate and thus an ultrahigh short-circuit current. The theoretical prediction of power output for the tribo-ferroelectric bilayer MXs at a moderate sliding speed 1 m/s is four orders of magnitude higher than the MoS$_2$ nanogenerator, indicating great potentials in energy harvesting applications.

cond-mat.mtrl-sci↗

arXiv2020

Diverse electronic and magnetic properties of CrS2 enabling novel strain-controlled 2D lateral heterostructure spintronic devices

Lateral heterostructures of two-dimensional (2D) materials, integrating different phases or materials into a single piece of nanosheet, have attracted intensive research interests in the past few years for high-performance electronic and optoelectronic devices. It also holds promises to significantly improve the performance and enable new functions of spintronic devices. It is imperative to have a 2D material possessing diverse electronic and magnetic properties that are required in spintronics. In this work, using density functional theory calculations, we surveyed all IV, V and VI group transition metal dichalcogenides (TMDs) and discovered that CrS2 has the most diverse electronic and magnetic properties: antiferromagnetic (AFM) metallic 1T phase, nonmagnetic (NM) semiconductor 2H phase, and ferromagnetic (FM) semiconductor 1T_prime phase with a Curie temperature of ~1000 K. More interestingly, we found that a tensile or compressive strain could turn 1T_prime phase into a spin-up or spin-down half metal. Such a unique feature enables designing strain-controlled spintronic devices using a single piece of CrS2 crystal with improved energy efficiency, which remains a challenge in miniaturization of spintronic devices. In-depth analysis attributed the unique strain tunability to the interplay between strain-induced lattice deformation and different spatial orientation of the spin-up/spin-down electronic orbitals. A prototypical design of a simple spin-valve logic device operated by strain is also presented.

cond-mat.mtrl-sci↗

arXiv2019

Modulating Peierls distortion of 1T_prime MoS2 via charge doping: a new charge density wave phase, reversible phase transition, and excellent electromechanical properties

The 1T_prime phase of transition metal dichalcogenides (TMDs) is a low symmetry charge density wave (CDW) phase, which can be regarded as a periodically distorted structure (Peierls distortion) of the high symmetry 1T phase. In this paper, using density functional theory (DFT) calculations, we report that the positive charge (hole) injection is an effective method to modulate the Peierls distortion of MoS2 1T_prime for new CDW phase and superior electromechanical properties. A new stable CDW phase is discovered at hole doping level of ~ 0.10h+/atom, named as 1Tt_prime. The hole charging and discharging can induce a reversible phase transition of MoS2 among the three phases, 1T, 1T_prime and 1Tt_prime. Such reversible phase transition leads to superior electromechanical properties including a strain output as high as -5.8% with a small hysteresis loop, multi-step super-elasticity, and multi-shape memory effect, which are valuable in active electromechanical device designs at nanoscale. In-depth analysis on the change of electronic structure under hole doping was performed to understand the new CDW phase and the observed phase transition. Using charge doping to modulate the Peierls distortion in two-dimensional materials can serve as a general concept for nano-active material designs.

cond-mat.mtrl-sci↗

arXiv2019

Electromechanical actuation of pristine graphene and graphene oxide: origin, optimization, and comparison

It is well recognized that the miniaturization of electromechanical devices will bring a revolution to humanity in the coming decades synonymous with the effects of miniaturizing electronic devices in those previous. An electromechanical actuator - a device that converts electrical energy to mechanical deformation or motion - is the core component of many such devices. Consequently, research interrogating mili-, micro-, and nano-actuation has, and will continue to become increasingly essential. The challenge is that behaviour of actuators at small size scales vastly differs to those at the macroscale. We cannot simply shrink the size of conventional actuators at the macroscale down to the micro/nanoscale. In addition, conventional actuation materials (such as piezoelectric ceramics and shape memory alloys) have poor properties and performances when fabricated at a small length scale. There is an urgent need to discover novel actuation materials at small length scale. This paper will review recent advances in graphene-based actuation materials. We will focus on different actuation physical mechanisms of this most well-known two-dimension material. The in-depth physical understanding and insights will lay the ground for further optimization/development of graphene-based actuators. They may also provide valuable knowledge for the design and development of other two-dimensional actuation materials and actuators.

cond-mat.mtrl-sci↗

arXiv2014

Mechanical buckling induced periodic kinking/stripe microstructures in mechanically peeled graphite flakes from HOPG

Mechanical exfoliation is a widely used method to isolate high quality graphene layers from bulk graphite. In our recent experiments, some ordered microstructures, consisting of a periodic alternation of kinks and stripes, were observed in thin graphite flakes that were mechanically peeled from highly oriented pyrolytic graphite (HOPG). A theoretical model is presented in this paper to understand the formation of such ordered microstructures, based on elastic buckling of a graphite flake being subjected to a bending moment. The width of the stripes predicted from this model agrees reasonably well with our experimental measurements.

cond-mat.mtrl-sci↗

arXiv2014

Cation ordering induced polarization enhancement for $PbTiO_3$-$SrTiO_3$ ferroelectric-dielectric superlattices

In this paper, an efficient computational material design approach (cluster expansion) is employed for the ferroelectric $PbTiO_3$/$SrTiO_3$ system. Via exploring a conguration space including over $3 \times 10^6$ candidates, two special cation ordered configurations: either perfect or mixed 1/1 (101) superlattice, are identified with the mostly enhanced ferroelectric polarization by up to about 100% in comparison with the (001) superlattice. Analyzing these two special configurations reveals the exotic couplings between the antiferrodistortive distortion (AFD) and ferroelectric polarization (FE) modes, e.g., tilting along x or y axis and polarization in z direction, as the origin for the best polarization property in this system. The identified cation ordering motifs and the exotic AFD-FE couplings could provide fresh ideas to design multifunctional perovskite heterostructures.

cond-mat.mtrl-sci↗

arXiv2014

Piezoelectric properties of graphene oxide from the first-principles calculations

Some highly ordered compounds of graphene oxide (GO), e.g., the so-called clamped and unzipped GO, are shown to have piezoelectric responses via first-principles density functional calculations. By applying an electric field perpendicular to the GO basal plane, the largest value of in-plane strain and strain piezoelectric coefficient, d31 are found to be 0.12% and 0.24 pm/V, respectively, which are comparable with those of some advanced piezoelectric materials. An in-depth molecular structural analysis reveals that deformation of the oxygen doping regions in the clamped GO dominates its overall strain output, whereas deformation of the regions without oxygen dopant in the unzipped GO determines its overall piezoelectric strain. This understanding explains the observed dependence of d31 on oxygen doping rate, i.e., higher oxygen concentration giving rise to a larger d31 in the clamped GO whereas leading to a reduced d31 in the unzipped GO. As the thinnest two-dimensional piezoelectric materials, GO has a great potential for a wide range of MEMS/NEMS actuators and sensors.

cond-mat.mtrl-sci↗

arXiv2013

Binding and interlayer force in the near-contact region of two graphite slabs: experiment and theory

Via a novel experiment, Liu \emph{et al.} [Phys. Rev. B, {\bf 85}, 205418 (2012)] estimated the graphite binding energy, specifically the cleavage energy, an important physical property of bulk graphite. We re-examine the data analysis and note that within the standard Lennard-Jones model employed, there are difficulties in achieving internal consistency in the reproduction of the graphite elastic properties. By employing similar models which guarantee consistency with the elastic constant, we find a wide range of model dependent binding energy values from the same experimental data. We attribute some of the difficulty in the determination of the binding energy to: i) limited theoretical understanding of the van der Waals dispersion of graphite cleavage, ii) the mis-match between the strong bending stiffness of the graphite-SiO$_2$ cantilever and the weak asymptotic inter-layer forces that are integrated over to produce the binding energy. We find, however, that the data does support determination of a maximum inter-layer force that is relatively model independent. We conclude that the peak force per unit area is $1.1 \pm 0.15$GPa for cleavage, and occurs at an inter-layer spacing of $0.377\pm 0.013$nm.

cond-mat.mtrl-sci↗

arXiv2013

Control of Surface Wettability via Strain Engineering

Reversible control of surface wettability has wide applications in lab-on-chip systems, tunable optical lenses, and microfluidic tools. Using a graphene sheet as a sample material and molecular dynamic (MD) simulations, we demonstrate that strain engineering can serve as an effective way to control the surface wettability. The contact angles $θ$ of water droplets on a graphene vary from 72.5$^\circ$ to 106$^\circ$ under biaxial strains ranging from -10% to 10% that are applied on the graphene layer. For an intrinsic hydrophilic surface (at zero strain), the variation of $θ$ upon the applied strains is more sensitive, i.e., from 0$^\circ$ to 74.8$^\circ$. Overall the cosines of the contact angles exhibit a linear relation with respect to the strains. In light of the inherent dependence of the contact angle on liquid-solid interfacial energy, we develop an analytic model to show the $\cos θ$ as a linear function of the adsorption energy $E_{ads}$ of a single water molecule over the substrate surface. This model agrees with our MD results very well. Together with the linear dependence of $E_{ads}$ on biaxial strains, we can thus understand the effect of strains on the surface wettability. Thanks to the ease of reversibly applying mechanical strains in micro/nano-electromechanical systems (MEMS/NEMS), we believe that strain engineering can be a promising means to achieve the reversibly control of surface wettability.

cond-mat.mes-hall↗

arXiv2012

Interlayer shear strength of single crystalline graphite

Reported values (0.2 MPa ~ 7.0 GPa) of the interlayer shear strength (ISS) of graphite are very dispersed. The main challenge to obtain a reliable value of ISS is the lack of precise experimental methods. Here we present a novel experimental approach to measure the ISS, and obtain the value as 0.14 GPa. Our result can serve as an important basis for understanding mechanical behavior of graphite or graphene-based materials.

cond-mat.mtrl-sci↗

arXiv2011

Strain Engineering Water Transport in Graphene Nano-channels

Using equilibrium and non-equilibrium molecular dynamic (MD) simulations, we found that engineering the strain on the graphene planes forming a channel can drastically change the interfacial friction of water transport through it. There is a sixfold change of interfacial friction stress when the strain changes from -10% to 10%. Stretching the graphene walls increases the interfacial shear stress, while compressing the graphene walls reduces it. Detailed analysis of the molecular structure reveals the essential roles of the interfacial potential energy barrier and the structural commensurateness between the solid walls and the first water layer. Our results suggest that the strain engineering is an effective way of controlling the water transport inside nano-channels. The resulting quantitative relations between shear stress and slip velocity and the understanding of the molecular mechanisms will be invaluable in designing graphene nano-channel devices.

physics.flu-dyn↗