arXiv subjects

Shiyu Du

Publications and source records attributed to Shiyu Du.

At least 19 recordsLinked to original sources

arXiv2026

From Variability to SED Modeling: A Multiwavelength Study of the Neutrino Blazar TXS 0506+056

The blazar TXS 0506+056 is the first source that was reported to be associated with high-energy extragalactic neutrino events and is one of the major targets for multi-messenger studies. We carried out multi-wavelength optical monitoring of this object on 24 nights in the period from 2018 to 2023. The overall light curves exhibit a dimming trend superposed by some small-amplitude fluctuations, and intraday variability was detected on four nights. Bluer-when-brighter behaviors were observed on both intraday and long timescales and were more pronounced on long timescales, while a weak redder-when-brighter trend was detected on one night. No significant time lags were found between variations at different optical wavelengths. We also retrieved the multi-broadband data from some monitoring programs. The data reveal complex, asynchronous flaring in different wavebands. A cross-correlation analysis shows that the high-energy emission (optical to gamma-ray) is co-spatial and leads the radio emission by a substantial time of about 800 to 900 days, suggesting that the radio emission originates from a downstream region of the jet. We performed time-dependent lepto-hadronic modeling of the spectral energy distributions for three representative epochs, the 2017 neutrino-associated flare, a post-flare phase, and a deep quiescent state, revealing an evolution in the radiative properties of the emission regions. The modeling results provide a phenomenological framework for interpreting the long-term multiwavelength behavior of TXS 0506+056 in a multi-messenger context.

astro-ph.HE↗

arXiv2025

Multiple Components and Spectral Evolution of BL Lacertae as Revealed by Multiwavelength Variability and SED Modeling

BL Lac has entered an active state since 2020, with multiwavelength observations revealing intense flares. In this study, we conducted 12-night multicolor optical monitoring using an 85 cm telescope from 2020 September to 2024 June and collected long-term broad-band archived data from radio to $\gamma$-rays. Intraday variabilities were detected on four nights, and most of them exhibited a bluer-when-brighter behavior. Both clockwise and counterclockwise spectral hysteresis loops were found within a single night. However, no reliable intraband time lag was detected for the intranight variabilities. On long timescales, the cross-correlation analysis shows that the variations of the optical, X-ray, and $\gamma$-ray bands do not reveal an obvious time delay, while the variations in the radio bands lagged them by about 370 days. The measured time lags suggest two distinct emission regions respectively responsible for the optical to $\gamma$-ray radiation and for the radio radiation, with a spatial separation of approximately $4.50\times10^{19}\ \rm cm$. We modeled the broad-band spectral energy distributions during four flaring epochs and one quiescent epoch, and found evidence for the possible persistent existence of a very high energy emission region. We also confirmed a spectral evolution of the source from an intermediate synchrotron peaked BL Lac object to a low synchrotron peaked BL Lac object.

astro-ph.HE↗

arXiv2025

Assessment of the Gradient Jump Penalisation in Large-Eddy Simulations of Turbulence

This research investigates the efficacy of the gradient jump penalisation (GJP) in large eddy simulations (LES) when coupled with active subgrid-scale (SGS) models. GJP is a stabilisation method tailored for the continuous Galerkin spectral element method, aiming at mitigating non-physical oscillations induced by discontinuous velocity gradients across element interfaces. We demonstrate that GJP effectively smoothens fields from LES without a salient impact on flow dynamics for the Taylor--Green vortex (TGV) at $Re=1600$, periodic hill flows at bulk Reynolds numbers $Re_b=10595$ and $37000$, as well as turbulent channel flow at $Re_{\tau} \approx 550$. In the TGV case, the application of GJP results in decreased fluctuations at only high wavenumbers compared to simulations without GJP. The periodic hill flow simulations indicate the applicability of GJP in wall-resolved LES (WRLES) involving curved geometries, though it tends to dissipate some of the finer details in the solution. Finally, in the analysis of the canonical turbulent channel flow cases, GJP leads a higher resolved turbulent kinetic energy than simulations without GJP and direct numerical simulations. GJP's mechanism is identified as providing enhanced dissipation at high wavenumbers but accompanied with insufficient dissipation at low wavenumbers, leading to a pronounced spectral cut-off. Non-physical oscillations on element interfaces are reflected as spikes in the power spectral density. By evaluating the sharpness of the strongest spike, GJP is shown to smoothen the spectra, however without completely removing the gradient jumps at low computational resolution.

physics.flu-dyn↗

arXiv2024

Sublayers Editing of Covalent MAX Phase for Nanolaminated Early Transition Metal Compounds

Two-dimensional transition metal carbides and nitrides (MXenes) have gained popularity in fields such as energy storage, catalysis, and electromagnetic interference due to their diverse elemental compositions and variable surface terminations (T). Generally, the synthesis of MXene materials involves etching the weak M-A metallic bonds in the ternary layered transition metal carbides and nitrides (MAX phase) using HF acid or Lewis acid molten salts, while the strong M-X covalent bonds preserve the two-dimensional framework structure of MXenes. On the other hand, the MAX phase material family also includes a significant class of members where the A site is occupied by non-metal main group elements (such as sulfur and phosphorus), in which both M-A and M-X are covalent bond-type sublayers. The aforementioned etching methods cannot be used to synthesize MXene materials from these parent phases. In this work, we discovered that the covalent bond-type M-A and M-X sublayers exhibit different reactivity with some inorganic materials in a high-temperature molten state. By utilizing this difference in reactivity, we can structurally modify these covalent sublayers, allowing for the substitution of elements at the X site (from B to Se, S, P, C) and converting non-metal A site atoms in non-van der Waals (non-vdW) MAX phases into surface atoms in vdW layered materials. This results in a family of early transition metal Xide chalcogenides (TMXCs) that exhibit lattice characteristics of both MXenes and transition metal chalcogenides. Using electron-donor chemical scissors, these TMXC layered materials can be further exfoliated into monolayer nanosheets. The atomic configurations of each atom in these monolayer TMXCs are the same as those of conventional MXenes, but the oxidation states of the M-site atoms can be regulated by both X-site atoms and intercalated cations.

cond-mat.mtrl-sci↗

arXiv2024

A Generation Framework with Strict Constraints for Crystal Materials Design

The design of crystal materials plays a critical role in areas such as new energy development, biomedical engineering, and semiconductors. Recent advances in data-driven methods have enabled the generation of diverse crystal structures. However, most existing approaches still rely on random sampling without strict constraints, requiring multiple post-processing steps to identify stable candidates with the desired physical and chemical properties. In this work, we present a new constrained generation framework that takes multiple constraints as input and enables the generation of crystal structures with specific chemical and properties. In this framework, intermediate constraints, such as symmetry information and composition ratio, are generated by a constraint generator based on large language models (LLMs), which considers the target properties. These constraints are then used by a subsequent crystal structure generator to ensure that the structure generation process is under control. Our method generates crystal structures with a probability of meeting the target properties that is more than twice that of existing approaches. Furthermore, nearly 100% of the generated crystals strictly adhere to predefined chemical composition, eliminating the risks of supply chain during production.

cs.AI↗

arXiv2024

Polymetis:Large Language Modeling for Multiple Material Domains

As the application of large language models in various fields continues to expand, materials science also ushers in opportunities for AI-driven innovation. The traditional way of relying on manual search for materials science-related information is now using artificial intelligence technology as an auxiliary tool to improve the efficiency of materials science research. To accelerate researchers' knowledge acquisition and intelligent decision-making support in materials science research, this paper proposes a large language model Polymetis model for a variety of materials fields, aiming to provide highly professional knowledge answers in the field of materials, covering energy materials, functional materials, alloy materials, physical chemistry, biology, and other material directions. The model uses a dataset of about 2 million material knowledge instructions, and in the process of building the dataset, we developed the Intelligent Extraction Large Model (IELM), which is specially used to extract and form structured knowledge from scientific texts, avoiding a large number of costs that need to be manually annotated, and improving efficiency. We inject this data into the GLM4-9B model for learning to enhance its inference capabilities in a variety of material domains. In addition, we have introduced enhanced prompt strategies to ensure that the answers to the model are more organized and comprehensive, providing efficient and comprehensive intelligent support for the diverse needs of materials science exploration, and promoting the development of material science.

cs.AI↗

arXiv2023

Structure maps for MAX phases formability revisited

The extraordinary chemical diversity of MAX phases raises the question of how many and which novel ones are yet to be discovered. The conventional schemes rely either on executions of well designed experiments or elaborately crafted calculations; both of which have been key tactics within the past several decades that have yielded many of important new materials we are studying and using today. However, these approaches are expensive despite the emergence of high throughput automations or evolution of high speed computers. In this work, we have revisited the in prior proposed light duty strategy, i.e. structure mapping, for describing the genomic conditions under which one MAX phase could form; that allow us to make successful formability and non formability separation of MAX phases with a fidelity of 95.5%. Our results suggest that the proposed coordinates, and further the developed structure maps, are able to offer a useful initial guiding principles for systematic screenings of potential MAX phases and provide untapped opportunities for their structure prediction and materials design.

cond-mat.mtrl-sci↗

arXiv2022

Chemical-scissor-mediated structural editing of layered transition metal carbides

Intercalation of non-van der Waals (vdW) layered materials can produce new 2D and 3D materials with unique properties, but it is difficult to achieve. Here, we describe a structural editing protocol for 3D non-vdW layered ternary carbides and nitrides (MAX phases) and their 2D vdW derivatives (MXenes). Gap-opening and species-intercalating stages were mediated by chemical scissors and guest intercalants, creating a large family of layered materials with unconventional elements and structures in MAX phases, as well as MXenes with versatile termination species. Removal of surface terminations by metal scissors and stitching of carbide layers by metal atoms leads to a reverse transformation from MXenes to MAX phases, and metal-intercalated 2D carbides. This scissor-mediated structural editing may enable structural and chemical tailoring of other layered ceramics.

cond-mat.mtrl-sci↗

arXiv2021

The Rendering from the Periodic System of the Elements on the stability, elastic, and electronic properties of M2AC phases

MAX phases are nanolaminated ternary materials that combine metallic and ceramic properties. Currently, the A-site elements replacement in traditional ones by later transition-metals opens a door to explore new types of MAX phases. In this work, we performed a systematic first-principle study to explore trends in stability, electronic structure and mechanical properties of 288 compositions of M2AX phases (M=Ti, V, Cr, Zr, Nb, Mo, Hf, Ta, W; A=Al, Si, P, S, Ga, Ge, As, Se, In, Sn, Sb, Te, Tl, Pb, Bi, Mn, Fe, Co, Ni, Cu, Zn, Tc, Ru, Rh, Pd, Ag, Cd, Os, Ir, Pt, Au, Hg; X=C). Such a dataset, combined with the rigid-band model been applied to most transition metal carbides, shows us the fundamental trends in bonding mechanisms and mechanical properties of MAX phases endowed with the periodic arrangements of M/A-site elements. It worth noting, in particular, the M-A d-d interactions of MAX phases uniquely contribute to the elastic constant C33.

cond-mat.mtrl-sci↗

arXiv2021

Synthesis and thermal expansion of chalcogenide MAX phase Hf2SeC

Thermal expansion of MAX phases along different directions tended to be different because of the anisotropy of hexagonal crystals. Herein, a new Hf2SeC phase was synthesized and confirmed to be relatively isotropic, whose coefficients of thermal expansion (CTEs) were determined to be 9.73 μK-1 and 10.18 μK-1 along a and c directions. The strong M-S bond endowed Hf2SC and Zr2SC lower CTEs than Hf2SeC and Zr2SeC. A good relationship between the thermal expansion anisotropy and the ratio of elastic stiffness constant c11 and c33 was established. This straightforward approximation could be used to roughly predict the thermal expansion anisotropy of MAX phases.

cond-mat.mtrl-sci↗

arXiv2021

Near-Room-Temperature Ferromagnetic Behavior of Single-Atom-Thick 2D Iron in Nanolaminated Ternary MAX Phases

Two dimensional (2D) ferromagnetic materials have attracted much attention in the fields of condensed matter physics and materials science, but their synthesis is still a challenge given their limitations on structural stability and susceptibility to oxidization. MAX phases nanolaminated ternary carbides or nitrides possess a unique crystal structure in which single-atom-thick A sublayers are interleaved by two dimensional MX slabs, providing nanostructured templates for designing 2D ferromagnetic materials if the non-magnetic A sublayers can be substituted replaced by magnetic elements. Here, we report three new ternary magnetic MAX phases (Ta2FeC, Ti2FeN and Nb2FeC) with A sublayers of single-atom-thick 2D iron through an isomorphous replacement reaction of MAX precursors (Ta2AlC, Ti2AlN and Nb2AlC) with a Lewis acid salts (FeCl2). All these MAX phases exhibit ferromagnetic (FM) behavior. The Curie temperature (Tc) of Ta2FeC and Nb2FeC MAX phase are 281 K and 291 K, respectively, i.e. close to room temperature. The saturation magnetization of these ternary magnetic MAX phases is almost two orders of magnitude higher than that of V2(Sn,Fe)C MAX phase whose A-site is partial substituted by Fe. Theoretical calculations on magnetic orderings of spin moments of Fe atoms in these nanolaminated magnetic MAX phases reveal that the magnetism can be mainly ascribed to intralayer exchange interaction of the 2D Fe atomic layers. Owning to the richness in composition of MAX phases, there is a large compositional space for constructing functional single-atom-thick 2D layers in materials using these nanolaminated templates.

cond-mat.mtrl-sci↗

arXiv2021

MAX Phase Zr2SeC and Its Thermal Conduction Behavior

The elemental diversity is crucial to screen out ternary MAX phases with outstanding properties via tuning of bonding types and strength between constitutive atoms. As a matter of fact, the interactions between M and A atoms largely determine the physical and chemical properties of MAX phases. Herein, Se element was experimentally realized to occupy the A site of a MAX phase, Zr2SeC, becoming a new member within this nanolaminated ternary carbide family. Comprehensive characterizations including Rietveld refinement of X-ray Diffraction and atom-resolved transmission electron microscopy techniques were employed to validate this novel MAX phase. The distinct thermal conduction behaviors emerged are attributed to the characteristic interactions between Zr and Se atoms.

cond-mat.mtrl-sci↗

arXiv2021

The impacts of optimization algorithm and basis size on the accuracy and efficiency of variational quantum eigensolver

Variational quantum eigensolver (VQE) is demonstrated to be the promising methodology for quantum chemistry based on near-term quantum devices. However, many problems are yet to be investigated for this methodology, such as the influences of optimization algorithm and basis size on the accuracy and efficiency for quantum computing. To address these issues, five molecules (H2, LiH, HF, N2 and F2) are studied in this work based on the VQE method using unitary coupled cluster (UCC) ansatz. The performance of the gradient optimization L-BFGS-B is compared with that of the direct search method COBYLA. The former converges more quickly, but the accuracy of energy surface is a little lower. The basis set shows a vital influence on the accuracy and efficiency. A large basis set generally provides an accurate energy surface, but induces a significant increase in computing time. The 631g basis is generally required from the energy surface of the simplest H2 molecule. For practical applications of VQE, complete active space (CAS) is suggested based on limited quantum resources. With the same number of qubits, more occupied orbitals included in CAS gives a better accuracy for the energy surface and a smaller evaluation number in the VQE optimization. Additionally, the electronic structure, such as filling fraction of orbitals, the bond strength of a molecule and the maximum nuclear charge also influences the performance of optimization, where half occupation of orbitals generally requires a large computation cost.

physics.chem-ph↗

arXiv2020

Molten salt synthesis of a nanolaminated Sc2SnC MAX Phase

The MAX phases are a family of of ternary layered material with both metal and ceramic properties, and it is also precursor ma-terials for synthesis of two-dimensional MXenes. The theory predicted that there are more than 600 stable ternary layered MAX phases. At present, there are more than 80 kinds of ternary MAX phases synthesized through experiments, and few reports on MAX phases where M is a rare earth element. In this study, a new MAX phase Sc2SnC with rare earth element Sc at the M sites was synthesized through the reaction sintering of Sc, Sn, and C mixtures. Phase composition and microstructure of Sc2SnC were confirmed by X-ray diffraction, scanning electron microscopy and X-ray energy spectrum analysis. And structural stability, mechanical and electronic properties of Sc2SnC was investigated via density functional theory. This study open a door for ex-plore more unknown ternary layered rare earth compounds Ren+1SnCn (Re=Sc, Y, La-Nd, n=1) and corresponding rare earth MXenes.

cond-mat.mtrl-sci↗

arXiv2020

The role of Hume-Rothery's rules play in the MAX phases formability

MAX phases are a family of layered, hexagonal-structure ternary carbides or nitrides of a transitional metal and an A-group element. What makes this type of material fascinating and potentially useful is their remarkable combinations of metallic and ceramic characteristics; as well as the indispensable role in 'top-down' synthesis of their 2D counterparts, MXenes. To enhance the efficiency in the successful search for potential novel MAX phases, the main efforts could go toward creating an informationprediction system incorporating all MAX phases' databases, as well as generally valid principles and the high-quality regularities. In this work, we employ structure mapping methodology, which has shown its merit of being useful guides in materials design, with Hume-Rothery parameters to provide guiding principles in the search of novel MAX phases. The formable/non-formable data on MAX phases can be ordered within a twodimensional plot by using proposed expression of geometrical and electron concentration factors.

cond-mat.mtrl-sci↗

arXiv2020

Halogenated MXenes with Electrochemically Active Terminals for High Performance Zinc Ion Batteries

The class of two-dimensional metal carbides and nitrides known as MXenes offer a distinct manner of property tailoring for a wide range of applications. The ability to tune the surface chemistry for expanding the property space of MXenes is thus an important topic, although experimental exploration of new surface terminals remains a challenge. Here, we synthesized Ti3C2 MXene with unitary, binary and ternary halogen terminals, e.g. -Cl, -Br, -I, -BrI and -ClBrI, to investigate the effect of surface chemistry on the properties of MXenes. The electrochemical activity of Br and I element result in the extraordinary electrochemical performance of the MXenes as cathodes for aqueous zinc ion batteries. The -Br and -I containing MXenes, e.g. Ti3C2Br2 and Ti3C2I2, exhibit distinct discharge platforms with considerable capacities of 97.6 mAh g-1 and 135 mAh g-1. Ti3C2(BrI) and Ti3C2(ClBrI) exhibit dual discharge platforms with capacities of 117.2 mAh g-1 and 106.7 mAh g-1. In contrast, the previously discovered MXenes Ti3C2Cl2 and Ti3C2(OF) exhibit no discharge platforms, and only ~50% of capacities and energy densities of Ti3C2Br2. These results emphasize the effectiveness of the Lewis-acidic-melt etching route for tuning the surface chemistry of MXenes, and also show promise for expanding the MXene family towards various applications.

cond-mat.mtrl-sci↗

arXiv2019

A general Lewis acidic etching route for preparing MXenes with enhanced electrochemical performance in non-aqueous electrolyte

Two-dimensional carbides and nitrides of transition metals, known as MXenes, are a fast-growing family of 2D materials that draw attention as energy storage materials. So far, MXenes are mainly prepared from Al-containing MAX phases (where A = Al) by Al dissolution in F-containing solution, but most other MAX phases have not been explored. Here, a redox-controlled A-site-etching of MAX phases in Lewis acidic melts is proposed and validated by the synthesis of various MXenes from unconventional MAX phase precursors with A elements Si, Zn, and Ga. A negative electrode of Ti3C2 MXene material obtained through this molten salt synthesis method delivers a Li+ storage capacity up to 738 C g-1 (205 mAh g-1) with high-rate performance and pseudocapacitive-like electrochemical signature in 1M LiPF6 carbonate-based electrolyte. MXene prepared from this molten salt synthesis route offer opportunities as high-rate negative electrode material for electrochemical energy storage applications.

physics.app-ph↗

arXiv2019

Multielemental single-atom-thick A layers in nanolaminated V2(Sn, A)C (A=Fe, Co, Ni, Mn) for tailoring magnetic properties

Tailoring of individual single-atom-thick layers in nanolaminated materials offers atomic-level control over material properties. Nonetheless, multielement alloying in individual atomic layers in nanolaminates is largely unexplored. Here, we report a series of inherently nanolaminated V2(A'xSn1-x)C (A'=Fe, Co, Ni and Mn, and combinations thereof, with x=1/3) synthesized by an alloy-guided reaction. The simultaneous occupancy of the four magnetic elements and Sn, the individual single-atom-thick A layers in the compound constitute high-entropy-alloy analogues, two-dimensional in the sense that the alloying exclusively occurs in the A layers. V2(A'xSn1-x)C exhibit distinct ferromagnetic behavior that can be compositionally tailored from the multielement A-layer alloying. This two-dimensional alloying provides a structural-design route with expanded chemical space for discovering materials and exploit properties.

cond-mat.mtrl-sci↗