arXiv subjects

Shixuan Du

Publications and source records attributed to Shixuan Du.

At least 19 recordsLinked to original sources

arXiv2026

Polymorphic crystallites model for monolayer amorphous materials

Establishing atomistic models of amorphous materials remains a central challenge in materials science. Here, we examine three representative multicomponent monolayer systems using first-principles-trained machine-learning potentials (MLPs) and an energy-guided Monte Carlo structural-search workflow. For monolayer amorphous boron nitride (maBN), independent density-functional-theory (DFT) single-point calculations confirm that the ensemble generated by the MLP-driven search is lower in energy on average than an extended-Tersoff-generated ensemble. Across the sampled maBN structures, local-ring classification combined with strict connected-domain analysis identifies h-BN-like, o-B$_2$N$_2$-like, and o-B$_4$N$_4$-like crystallite domains together with mixed medium-range order. Only individual samples containing at least two distinct phase-pure crystallite-domain types are classified as polymorphic crystallites. The same analysis finds coexisting hexagonal and tetragonal domains in monolayer amorphous LiCl and graphene-like, h-BN-like, borophene-like, and mixed-order regions in monolayer amorphous BCN. Five-nanosecond MLP molecular-dynamics trajectories at 300 K show that the candidate structures are dynamically persistent on the simulated timescale. These results support a polymorphic-crystallite description for the selected model systems, while experimental discrimination from alternative continuous-random-network descriptions will require medium-range-order-sensitive measurements.

cond-mat.mtrl-sci↗

arXiv2026

Realization of Air-Stable Two-Dimensional Superconductor Nb2Pd3Te5 With Quasi-One-Dimensional Pair Density Modulation

Two-dimensional (2D) superconductors provide a fertile platform for exploring reduced-dimensional superconductivity and emergent quantum phenomena. Incorporating quasi-one-dimensional (quasi-1D) structural motifs into 2D superconductors offers a powerful route to engineer strong electronic anisotropy, enabling unconventional superconducting states and anisotropic superconducting transport functionalities. However, such systems remain rarely realized. Here we report the realization of a 2D superconductor Nb2Pd3Te5, exhibiting an intrinsic quasi-1D pair density modulation. Monolayer and bilayer Nb2Pd3Te5 is synthesized via van-der-Waals epitaxy. Using ultralow-temperature scanning tunneling microscopy/spectroscopy, we observe the quasi-1D crystal structure and superconductivity below ~0.6 K with a pronounced quasi-1D pair density modulation. Remarkably, both monolayer and bilayer Nb2Pd3Te5 show strong air stability. Our findings establish atomically 2D Nb2Pd3Te5 as a robust and promising platform for exploring novel low-dimensional quantum phenomena and anisotropy-enabled superconducting devices.

cond-mat.mtrl-sci↗

arXiv2025

Sliding ferroelectric control of unconventional magnetism in stacked bilayers

The control of unconventional magnetism, which displays ferromagnetism-like properties with compensated magnetization, has drawn intense attention for advancing antiferromagnetic spintronics. Here, through symmetry analysis, we propose a general stacking rule, characterized by a connection operator linking two stacked bilayers, for controlling unconventional magnetism via sliding ferroelectricity. Such rule enables the simultaneous switching of both electric polarization and nonrelativistic spin splitting or anomalous Hall effect in altermagnets, a class of collinear unconventional magnets. By comprehensively surveying the 80 layer groups, we identify all the stacking orders that allow for such two types of simultaneous switching. Furthermore, we extend the stacking rule to collinear compensated ferrimagnets, where the opposite-spin sublattices are not connected by any symmetry operator, yet the net magnetization remains zero. Combined with first-principles calculations, we demonstrate the sliding ferroelectric control of spin polarization and anomalous Hall effect in the altermagnetic AgF2 and Fe2MoSe4 bilayers. Our work provides a symmetry strategy for achieving ferroelectric control of unconventional magnetism in bilayer systems and opens avenues for exploring new types of magnetoelectric coupling.

cond-mat.mtrl-sci↗

arXiv2024

Enforced symmetry breaking for anomalous valley Hall effect in two-dimensional hexagonal lattices

The anomalous valley Hall effect (AVHE) is a pivotal phenomenon that allows for the exploitation of the valley degree of freedom in materials. A general strategy for its realization and manipulation is crucial for valleytronics. Here, by considering all possible symmetries, we propose general rules for the realization and manipulation of AVHE in two-dimensional hexagonal lattices. The realization of AVHE requires breaking the enforced symmetry that is associated with different valleys or reverses the sign of Berry curvature. Further manipulation of AVHE requires asymmetry operators connecting two states with opposite signs of Berry curvature. These rules for realizing and manipulating AVHE are extendable to generic points in momentum space. Combined with first-principles calculations, we realize the controllable AVHE in four representative systems, i.e., monolayer AgCrP2Se6, CrOBr, FeCl2 and bilayer TcGeSe3. Our work provides symmetry rules for designing valleytronic materials that could facilitate the experimental detection and realistic applications.

cond-mat.mtrl-sci↗

arXiv2024

Topological Woodward-Hoffmann classification for cycloadditions in polycyclic aromatic azomethine ylides

The study of cycloaddition mechanisms is central to the fabrication of extended sp2 carbon nanostructures. Reaction modeling in this context has focused mostly on putative, energetically preferred, exothermic products with limited consideration for symmetry allowed or forbidden mechanistic effects. Here, we introduce a scheme for classifying symmetry-forbidden reaction coordinates in Woodward-Hoffmann correlation diagrams. Topological classifiers grant access to the study of reaction pathways and correlation diagrams in the same footing, for the purpose of elucidating mechanisms and products of polycyclic aromatic azomethine ylide (PAMY) cycloadditions with pentacene-yielding polycyclic aromatic hydrocarbons with an isoindole core in the solid-state and on surfaces as characterized by mass spectrometry and scanning tunneling microscopy, respectively. By means of a tight-binding reaction model and density functional theory (DFT) we find topologically-allowed pathways if a product is endothermic, and topologically-forbidden if a product is exothermic. Our work unveils topological classification as a crucial element for reaction modeling for nanographene engineering, and highlights its fundamental role in the design of cycloadditions in on-surface and solid-state chemical reactions, while underscoring that exothermic pathways can be topologically-forbidden.

physics.chem-ph↗

arXiv2024

Thermal spin-crossover and temperature-dependent zero-field splitting in magnetic nanographene chains

Nanographene-based magnetism at interfaces offers an avenue to designer quantum materials towards novel phases of matter and atomic-scale applications. Key to spintronics applications at the nanoscale is bistable spin-crossover which however remains to be demonstrated in nanographenes. Here we show that antiaromatic 1,4-disubstituted pyrazine-embedded nanographene derivatives, which promote magnetism through oxidation to a non-aromatic radical are prototypical models for the study of carbon-based thermal spin-crossover. Scanning tunneling spectroscopy studies reveal symmetric spin excitation signals which evolve at Tc to a zero-energy peak, and are assigned to the transition of a S = 3/2 high-spin to a S = 1/2 low-spin state by density functional theory. At temperatures below and close to the spin-crossover Tc, the high-spin S= 3/2 excitations evidence pronouncedly different temperature-dependent excitation energies corresponding to a zero-field splitting in the Hubbard-Kanamori Hamiltonian. The discovery of thermal spin crossover and temperature-dependent zero-field splitting in carbon nanomaterials promises to accelerate quantum information, spintronics and thermometry at the atomic scale.

physics.chem-ph↗

arXiv2024

Building spin-1/2 antiferromagnetic Heisenberg chains with diaza-nanographenes

Understanding and engineering the coupling of spins in nanomaterials is of central importance for designing novel devices. Graphene nanostructures with π-magnetism offer a chemically tunable platform to explore quantum magnetic interactions. However, realizing spin chains bearing controlled odd-even effects with suitable nanographene systems is challenging. Here, we demonstrate the successful on-surface synthesis of spin-1/2 antiferromagnetic Heisenberg chains with parity-dependent magnetization based on antiaromatic diaza-hexa-peri-hexabenzocoronene (diaza-HBC) units. Using distinct synthetic strategies, two types of spin chains with different terminals were synthesized, both exhibiting a robust odd-even effect on the spin coupling along the chain. Combined investigations using scanning tunneling microscopy, non-contact atomic force microscopy, density functional theory calculations, and quantum spin models confirmed the structures of the diaza-HBC chains and revealed their magnetic properties, which has an S = 1/2 spin per unit through electron donation from the diaza-HBC core to the Au(111) substrate. Gapped excitations were observed in even-numbered chains, while enhanced Kondo resonance emerged in odd-numbered units of odd-numbered chains due to the redistribution of the unpaired spin along the chain. Our findings provide an effective strategy to construct nanographene spin chains and unveil the odd-even effect in their magnetic properties, offering potential applications in nanoscale spintronics.

cond-mat.mtrl-sci↗

arXiv2023

Structure and mechanical properties of monolayer amorphous carbon and boron nitride

Amorphous materials exhibit various characteristics that are not featured by crystals and can sometimes be tuned by their degree of disorder (DOD). Here, we report results on the mechanical properties of monolayer amorphous carbon (MAC) and monolayer amorphous boron nitride (maBN) with different DOD. The pertinent structures are obtained by kinetic-Monte-Carlo (kMC) simulations using machine-learning potentials (MLP) with density-functional-theory (DFT)-level accuracy. An intuitive order parameter, namely the areal fraction Fx occupied by crystallites within the continuous random network, is proposed to describe the DOD. We find that Fx captures the essence of the DOD: Samples with the same Fx but different sizes and distributions of crystallites have virtually identical radial distributions functions as well as bond-length and bond-angle distributions. Furthermore, by simulating the fracture process with molecular dynamics, we found that the mechanical responses of MAC and maBN before fracture are solely determined by Fx and are insensitive to the sizes and specific arrangements of the crystallites. The behavior of cracks in the two materials is analyzed and found to mainly propagate in meandering paths in the CRN region and to be influenced by crystallites in distinct ways that toughen the material. The present results reveal the relation between structure and mechanical properties in amorphous monolayers and may provide a universal toughening strategy for 2D materials.

cond-mat.mtrl-sci↗

arXiv2023

Hybrid nodal surface and nodal line phonons in solids

Phonons have provided an ideal platform for a variety of intriguing physical states, such as non-Abelian braiding and the Haldane model. It is promising that phonons will realize the complicated nodal states accompanying unusual quantum phenomena. Here, we propose the hybrid nodal surface and nodal line (NS+NL) phonons beyond the single-genre nodal phonons. We categorize the NS+NL phonons into two- and four-band situations based on symmetry analysis and compatibility relationships. Combining database screening with first-principles calculations, we identify the ideal candidate materials for realizing all categorized NS+NL phonons. Our calculations and tight-binding models further demonstrate that the interplay between NS and NL induces unique phenomena. In space group (SG) 113, the quadratic NL acts as a hub of the Berry curvature between two NSs, generating ribbonlike surface states (SSs). In SG 128, the NS serves as the counterpart of the Weyl NL, in which NS-NL mixed topological SSs are observed. Our findings extend the scope of hybrid nodal states and enrich the phononic states in realistic materials.

cond-mat.mtrl-sci↗

arXiv2023

Twisted bilayer zigzag-graphene nanoribbon junctions with tunable edge states

Stacking two-dimensional layered materials such as graphene and transitional metal dichalcogenides with nonzero interlayer twist angles has recently become attractive because of the emergence of novel physical properties. Stacking of one-dimensional nanomaterials offers the lateral stacking offset as an additional parameter for modulating the resulting material properties. Here, we report that the edge states of twisted bilayer zigzag graphene nanoribbons (TBZGNRs) can be tuned with both the twist angle and the stacking offset. Strong edge state variations in the stacking region are first revealed by density functional theory (DFT) calculations. We construct and characterize twisted bilayer zigzag graphene nanoribbon (TBZGNR) systems on a Au(111) surface using scanning tunneling microscopy. A detailed analysis of three prototypical orthogonal TBZGNR junctions exhibiting different stacking offsets by means of scanning tunneling spectroscopy reveals emergent near-zero-energy states. From a comparison with DFT calculations, we conclude that the emergent edge states originate from the formation of flat bands whose energy and spin degeneracy are highly tunable with the stacking offset. Our work highlights fundamental differences between 2D and 1D twistronics and spurs further investigation of twisted one-dimensional systems.

cond-mat.mes-hall↗

arXiv2023

Superconductivity in an Orbital-reoriented SnAs Square Lattice: a Case Study of Li0.6Sn2As2 and NaSnAs

Searching for functional square lattices in layered superconductor systems offers an explicit clue to modify the electron behavior and find exotic properties. The trigonal SnAs3 structural units in SnAs-based systems are relatively conformable to distortion, which provides the possibility to achieve structurally topological transformation and higher superconducting transition temperatures. In the present work, the functional As square lattice was realized and activated in Li0.6Sn2As2 and NaSnAs through a topotactic structural transformation of trigonal SnAs3 to square SnAs4 under pressure, resulting in a record-high Tc among all synthesized SnAs-based compounds. Meanwhile, the conductive channel transfers from the out-of-plane pz orbital to the in-plane px+py orbitals, facilitating electron hopping within the square 2D lattice and boosting the superconductivity. The reorientation of p-orbital following a directed local structure transformation provides an effective strategy to modify layered superconductors.

cond-mat.supr-con↗

arXiv2022

Strong and tunable magnetoelectric coupling in 2D trilayer heterostructures

The quest for electric-field control of nanoscale magnetic states such as skyrmions, which would impact the field of spintronics, has led to a challenging search for multiferroic materials or structures with strong magnetoelectric coupling and efficient electric-field control. Here we report a theoretical prediction that such phenomena can be realized in two-dimensional (2D) bilayer FE/PMM and trilayer FE/PMM/FE heterostructures (two-terminal and three-terminal devices), where FE is a 2D ferroelectric and PMM is a polar magnetic metal with strong spin-orbit coupling. Such a PMM has strong Dzyaloshinskii-Moriya interactions (DMI) that can generate skyrmions, while the FE can generate strong magnetoelectric coupling through polarization-polarization interactions. In trilayer heterostructures, contact to the metallic PMM layer enables multiple polarization configurations for electric-field control of skyrmions. We report density-functional-theory calculations for particular material choices that demonstrate the effectiveness of these arrangements, with the key driver being the polarization-polarization interactions between the PMM and FE layers. The present findings provide a method to achieve strong magnetoelectric coupling in the 2D limit and a new perspective for the design of related spintronics.

cond-mat.mtrl-sci↗

arXiv2022

Tunable Interband Transitions in Twisted h-BN/Graphene Heterostructures

In twisted h-BN/graphene heterostructures, the complex electronic properties of the fast-traveling electron gas in graphene are usually considered to be fully revealed. However, the randomly twisted heterostructures may also have unexpected transition behaviors, which may influence the device performance. Here, we study the twist angle-dependent coupling effects of h-BN/graphene heterostructures using monochromatic electron energy loss spectroscopy. We find that the moiré potentials alter the band structure of graphene, resulting in a redshift of the intralayer transition at the M-point, which becomes more pronounced up to 0.25 eV with increasing twist angle. Furthermore, the twisting of the Brillouin zone of h-BN relative to the graphene M-point leads to tunable vertical transition energies in the range of 5.1-5.6 eV. Our findings indicate that twist-coupling effects of van der Waals heterostructures should be carefully considered in device fabrications, and the continuously tunable interband transitions through the twist angle can serve as a new degree of freedom to design optoelectrical devices.

cond-mat.mes-hall↗

arXiv2022

The structure of amorphous two-dimensional materials: Elemental monolayer amorphous carbon versus binary monolayer amorphous boron nitride

The structure of amorphous materials has been debated since the 1930's as a binary question: amorphous materials are either Zachariasen continuous random networks (Z-CRNs) or Z-CRNs containing crystallites. It was recently demonstrated, however, that amorphous diamond can be synthesized in either form. Here we address the question of the structure of single-atom-thick amorphous monolayers. We reanalyze the results of prior simulations for amorphous graphene and report kinetic Monte Carlo simulations based on alternative algorithms. We find that crystallite-containing Z-CRN is the favored structure of elemental amorphous graphene, as recently fabricated, whereas the most likely structure of binary monolayer amorphous BN is altogether different than either of the two long-debated options: it is a compositionally disordered "pseudo-CRN" comprising a mix of B-N and noncanonical B-B and N-N bonds and containing "pseudocrystallites", namely honeycomb regions made of noncanonical hexagons. Implications for other non-elemental 2D and bulk amorphous materials are discussed.

cond-mat.mtrl-sci↗

arXiv2021

Thermal transport of amorphous carbon and boron-nitride monolayers

Two-dimensional (2D) materials like graphene and h-BN usually show high thermal conductivity, which enables rich applications in thermal dissipation and nanodevices. Disorder, on the other hand, is often present in 2D materials. Structural disorder induces localization of electrons and phonons and alters the electronic, mechanical, thermal, and magnetic properties. Here we calculate the in-plane thermal conductivity of both monolayer carbon and monolayer boron nitride in the amorphous form, by reverse nonequilibrium molecular dynamics simulations. We find that the thermal conductivity of both monolayer amorphous carbon (MAC) and monolayer amorphous boron nitride (ma-BN) are about two orders of magnitude smaller than their crystalline counterparts. Moreover, the ultralow thermal conductivity is independent of the temperature due to the extremely short phonon mean free path in these amorphous materials. The relation between the structure disorder and the reduction of the thermal conductivity is analyzed in terms of the vibrational density of states and the participation ratio. ma-BN shows strong vibrational localization across the frequency range, while MAC exhibits a unique extended G' mode at high frequency due to its sp2 hybridization and the broken E2g symmetry. The present results pave the way for potential applications of MAC and ma-BN in thermal management.

cond-mat.mtrl-sci↗

arXiv2021

Intrinsically Honeycomb-patterned Hydrogenated Graphene with Spin Polarized Edge-states

Since the advent of graphene ushered the era of two-dimensional materials, many forms of hydrogenated graphene have been reported, exhibiting diverse properties ranging from a tunable band gap to ferromagnetic ordering. Patterned hydrogenated graphene with micron-scale patterns has been fabricated by lithographic means. Here we report successful millimeter-scale synthesis of an intrinsically honeycomb patterned form of hydrogenated graphene on Ru(0001) by epitaxial growth followed by hydrogenation. Combining scanning tunneling microscopy observations with density-functional-theory (DFT) calculations, we reveal that an atomic-hydrogen layer intercalates between graphene and Ru(0001). The result is a hydrogen honeycomb structure that serves as a template for the final hydrogenation, which converts the graphene into graphane only over the template, yielding honeycomb-patterned hydrogenated graphene (HPHG). In effect, HPHG is a form of patterned graphane. DFT calculations find that the unhydrogenated graphene regions embedded in the patterned graphane exhibit spin-polarized edge states. This type of growth mechanism provides new pathways for the fabrication of intrinsically patterned graphene-based materials.

cond-mat.mtrl-sci↗

arXiv2021

Database Construction for Two-Dimensional Material-Substrate Interfaces

The interfacial structures and interactions of two-dimensional (2D) materials on solid substrates are of fundamental importance for the fabrication and application of 2D materials. However, selection of a suitable solid substrate to grow 2D material, determination and control of the 2D material-substrate interface remain a big challenge due to the large diversity of possible configurations. Here, we propose a computational framework to select an appropriate substrate for epitaxial growth of 2D material and to predict possible 2D material-substrate interface structures and orientations using density functional theory calculations performed for all non-equivalent atomic structures satisfying the symmetry constraints. The approach was validated by the correct prediction of three experimentally reported 2D material-substrate interface systems with only the given information of two parent materials. Several possible interface configurations are also proposed based on this approach. We therefore construct a database that contains these interface systems and has been continuously expanding. This database serves as preliminary guidance for epitaxial growth and stabilization of new materials in experiments.

cond-mat.mtrl-sci↗

arXiv2021

Observation of magnetic adatom-induced Majorana vortex and its hybridization with field-induced Majorana vortex in an iron-based superconductor

Braiding Majorana zero modes is essential for fault-tolerant topological quantum computing. Iron-based superconductors with nontrivial band topology have recently emerged as a surprisingly promising platform for creating distinct Majorana zero modes in magnetic vortices in a single material and at relatively high temperatures. The magnetic field-induced Abrikosov vortex lattice makes it difficult to braid a set of Majorana zero modes or to study the coupling of a Majorana doublet due to overlapping wave functions. Here we report the observation of the proposed quantum anomalous vortex with integer quantized vortex core states and the Majorana zero mode induced by magnetic Fe adatoms deposited on the surface. We observe its hybridization with a nearby field-induced Majorana vortex in iron-based superconductor FeTe0.55Se0.45. We also observe vortex-free Yu-Shiba-Rusinov bound states at the Fe adatoms with a weaker coupling to the substrate, and discover a reversible transition between Yu-Shiba-Rusinov states and Majorana zero mode by manipulating the exchange coupling strength. The dual origin of the Majorana zero modes, from magnetic adatoms and external magnetic field, provides a new single-material platform for studying their interactions and braiding in superconductors bearing topological band structures.

cond-mat.supr-con↗