arXiv subjects

Tomas Polcar

Publications and source records attributed to Tomas Polcar.

At least 19 recordsLinked to original sources

arXiv2026

An integrated viscoelastic modeling framework combining analytical and FEM approaches: Application to WSe2 coatings

This work presents an integrated methodology combining analytical and finite element FEM based viscoelastic modeling for characterizing the nanoindentation response of coatings. The proposed framework combines two complementary modeling approaches: an analytical model based on the Burgers formulation to analyze nanoindentation load displacement data and extract rheological parameters, and a numerical FEM model implemented in ABAQUS using a 2D axisymmetric indenter coating substrate configuration with viscoelasticity represented through Prony series. An automated inverse optimization routine employing the Nelder Mead simplex algorithm minimizes the discrepancy between experimental and simulated responses. The methodology is demonstrated and validated on WSe2 coatings, showing an agreement between the analytical predictions, FEM simulations, and experimental measurements. Despite the geometric simplifications, the FEM approach provides accurate predictions while maintaining high computational efficiency of time dependent mechanical behavior. The proposed framework provides a robust tool for characterizing viscoelastic behavior from nanoindentation data while enabling access to internal stress and strain fields, thereby offering deeper insight into plastic deformation, crack initiation, and failure mechanism.

physics.app-ph↗

arXiv2026

Crystal forming ability of amorphous refractory metals under nanoindentation: a molecular dynamics study

Amorphous refractory metal coatings combine high hardness with chemical inertness, yet their metastability makes them prone to mechanically induced crystallisation (devitrification) under contact loading, and how readily such a glass re-orders to its parent body centred cubic (bcc) crystal is unknown across the refractory series. We prepared amorphous V, Nb, Mo, Ta and W by melt quenching to 300 K, validated each interatomic potential against ab initio liquid radial distribution functions, and probed them by large scale molecular dynamics nanoindentation. Indentation drives a localised amorphous to bcc transformation by bulk nucleation, growth and coalescence. A crystal forming ability (CFA), the maximum slope of the sigmoidal bcc fraction versus depth curve, spans about a factor of four and decreases as V > Mo > Nb > Ta > W; it falls with indenter velocity as CFA $\propto v^{-m}$ with a mean exponent of 1.08, so CFA$\cdot v$ is nearly constant and the transformation rate is almost velocity independent. Transforming atoms carry excess non affine displacement and local shear strain, not hydrostatic pressure, marking a shear associated displacive pathway; the bulk driving force is largest for the most resistant element, W, so resistance tracks cohesive bond strength rather than the thermodynamic driving force. Early bcc like order sets the sharpness and depth of the transition, whereas the mechanical work to half transformation sets the persistent nucleus density. A grain population balance links nucleation, growth and coalescence to a terminal microstructure whose completeness does not follow the CFA order.

cond-mat.mtrl-sci↗

arXiv2026

First principles study of chalcogen vacancy effect on the optoelectronic and photocatalytic properties of transition metal dichalcogenides monolayers

In working conditions, chalcogen vacancies spontaneously occur in two-dimensional transition metal dichalcogenides (TMDCs) monolayers, affecting their optoelectronic and photocatalytic properties. To study how chalcogen vacancies affect such properties, we use quantum mechanical calculations considering prototypical MX$_2$ (M = Mo, W, X = S and Se) TMDCs monolayers. Structural optimisations show that M-X bond lengths about a vacancy are different compared to the bond lengths in the pristine structure. Band structure calculations reveal that the introduction of vacancies produce electronic states about the Fermi level, hence resulting in the reduction of the band gap. Work function and electrostatic potential calculations show that the introduction of vacancies induce an asymmetry in the electrostatic potential facilitating the charge separation; such feature is absent in a pristine monolayer. All the considered defective structures are capable of performing hydrogen evolution reaction, while co-catalyst is required to perform oxygen evolution reaction when used for water splitting. WS$_2$ and WSe$_2$ defective monolayers can serve as an efficient photocatalytic material for reducing CO$_2$ into useful chemical products. The presented results show that vacancy-containing TMDCs monolayers own photocatalytic capabilities compared to the pristine counterparts, thus showing that defective TMD monolayers have prospective applications and should not be regarded as flawed products to be discarded. Finally, the results might constitute guidelines for the experimental synthesis of vacancy-engineered MX$_2$ monolayers for optoelectronic devices and photocatalytic applications.

cond-mat.mtrl-sci↗

arXiv2026

Microscopic contributions to the deviation from Amontons friction law

We investigate the nanoscale friction behaviour of MX2 monolayers (M = Mo, W; X = S, Se) on Au(111) and Ag(111) substrates with a silicon tip using classical molecular dynamics simulations with machine-learning-based force fields. This approach enables an accurate description of tip-surface interactions and friction mechanisms at the atomic scale. We observe a pronounced non-monotonic dependence of the friction force on the applied normal load, indicating a breakdown of Amontons's law at the nanoscale. Analysis of lateral force' signals and their spatial Fourier transforms reveals the coexistence of multiple sliding modes, including longitudinal sliding, lateral slip, and zig-zag motions. We show that the overall friction response is governed by the relative contributions of these motions. While the qualitative features of friction are largely substrate-independent, both the magnitude of friction and the balance between sliding modes depend sensitively on the substrate-monolayer combination. In particular, Au/MoSe2/Si exhibits significantly reduced friction due to suppression of lateral slip motion. Our results indicate that the method is broadly applicable for probing nanoscale friction in related heterostructures.

cond-mat.mtrl-sci↗

arXiv2026

Cross-sectional helium irradiation reveals interface-controlled bubble evolution in Cr/CrAlSiN multilayer coatings on zirconium alloys

The irradiation stability of Cr based protective coatings on zirconium alloys is critical for the development of accident-tolerant fuel claddings. However, conventional surface irradiation often produces shallow, nonuniform damage, obscuring interfacial behavior. In this study, we perform cross-sectional He irradiation to directly examine the interfacial response and He bubble evolution across Cr monolayer and Cr and CrAlSiN multilayer coatings on Zr substrates. Irradiation was carried out at 500 C and 750 C to doses of 2 and 3 dpa, enabling a direct comparison of temperature-dependent microstructural evolution. In the Cr monolayer, He implantation produced a homogeneous distribution of nanoscale bubbles throughout the damaged region and large cavities at the Cr and Zr interface, indicating severe Kirkendall-type voiding and interfacial decohesion at elevated temperature. In contrast, the Cr/CrAlSiN multilayer exhibited a periodically modulated bubble distribution, with bubble fragmentation and transformation into nanoscale platelets at CrAlSiN interfaces. A N-enriched Zr(N) interlayer formed spontaneously at the CrAlSiN and Zr interface, effectively suppressing bubble accumulation and interdiffusion. The nanochannel interfaces acted as He sinks and diffusion barriers, enhancing interfacial bonding and mitigating swelling. This work demonstrates that cross-sectional ion irradiation is a powerful approach for probing interfacial stability in multilayer systems, offering new insights into He-defect interactions and radiation tolerance engineering at buried interfaces. The findings highlight the potential of Cr and CrAlSiN multilayers as advanced coating architectures for high-temperature nuclear environments.

cond-mat.mtrl-sci↗

arXiv2026

Defect Landscape Engineering Suppresses Helium Damage in Ceramics

Helium accumulation in structural ceramics used in nuclear, fusion, and aerospace systems causes swelling, cracking, and early failure, yet controlling this damage has remained elusive. Here, we introduce defect landscape engineering, the deliberate creation of vacancy clusters prior to helium exposure, as a general strategy to suppress helium-induced degradation. Using {\alpha}-SiC as a model, we combine advanced microscopy, strain mapping, helium depth profiling, positron annihilation spectroscopy, and atomistic simulations to demonstrate that tailored pre-damage transforms helium defect evolution. Instead of forming extended platelets and nanocracks, helium is trapped in stable, uniformly dispersed nanobubbles. Simulations reveal that small vacancy clusters act as dual-function sinks for irradiation-induced interstitials and preferential helium traps, fundamentally altering cascade recombination dynamics. This mechanism is composition-independent and scalable, offering a new design principle for radiation-tolerant ceramics across carbides, nitrides, and oxides. By viewing defect control as a tunable parameter instead of a fixed material property, this work outlines a possible design route toward enhanced radiation tolerance in ceramics used in extreme environments.

physics.app-ph↗

arXiv2025

Ab initio study on photocatalytic properties of PtSSe-WXY Janus heterostructures

Semiconductor photocatalysis offers a sustainable route for converting solar energy into chemical energy, enabling the production of clean fuels and valuable chemical products. To this aim, we explore van der Waals heterostructures made up of Janus PtSSe and WXY (X, Y $=$ S, Se, Te and X $\neq$Y), in the context of photocatalytic applications. The redox capabilities of various heterostructure configurations (atom facing types and stacking orders) are evaluated by aligning the absolute band edge positions with respect to redox potentials of hydrogen and oxygen evolution reaction (HER and OER) and CO$_2$ reduction reactions. The stability of photocatalyst candidates are checked by layer binding energy calculations and ab initio molecular dynamics simulations. The optical absorption spectra suggest good light absorption in the visible range. Further, strain engineering is applied as a way to tune band edges and evaluate the possible use of the heterostructures as photocatalysts. This study shows that van der Waals heterostructure bilayers composed of Janus PtSSe and WSeTe in specific geometric configurations can be potential materials as photocatalysts for HER, OER and CO$_2$ reduction reactions. Finally, we suggest that, although systems made up of PtSSe and WSTe cannot be used for photocatalytic applications, they can be explored for applications in thermoelectric energy conversion or infrared photovoltaics.

cond-mat.mtrl-sci↗

arXiv2025

A comparative nanotribological investigation on amorphous and polycrystalline forms of MoS2

The wear behavior of two amorphous and polycrystalline forms of MoS2 prepared by magnetron sputtering has been characterized in a combined nanoindentation and atomic force microscopy study. From the analysis of the depth and width of wear tracks estimated after scratching the surfaces with a Berkovich indenter and a loading force up to 2 mN, we conclude that both forms follow the Archard wear equation, and the wear resistance is about four times higher on the amorphous MoS2. Moreover, a comparison of lateral force maps on pristine and worn areas shows a considerable reduction of friction on both forms, which is possibly due to the significant smoothing of the surfaces caused by scratching. With normal forces in the micro N range, the analysis is made difficult by the fact that the linear dimensions of the wear tracks are comparable to those of the granular structures forming the surfaces. Even if the Archard equation could not be tested in this case, the wear resistance is considerably larger on amorphous MoS2 also on the nanoscale. In this way, our results disclose information on the nanotribology of MoS2 thin films in forms different from the layered structures commonly discussed in the literature. The amorphous form outperforms the polycrystalline one.

cond-mat.mtrl-sci↗

arXiv2025

Exploring nanoscale metallic multilayer Ta/Cu films: Structure and some insights on deformation and strengthening mechanisms

Nanoscale metallic multilayer (NMM) films are systems offering insight into the role of interfaces in metal plasticity, deformation, and strengthening mechanisms. Magnetron sputtering was used to fabricate the Ta-Cu NMM films with a periodicity (equal Ta and Cu layer thickness) from 6 to 80 nm, with resulting structure exhibiting strongly incoherent tetragonal beta-Ta and face-centered cubic Cu phase. The high-load indentation test, TEM studies, and the rCLS model collectively demonstrate that all NMM films predominantly undergo plastic deformation. This plastic deformation primarily occurs within the soft Cu layer, while the propagation of dislocations across the incoherent interface is largely excluded.

cond-mat.mtrl-sci↗

arXiv2025

Load-Dependent Sliding behavior of WSe2-x solid lubricant coating

Transition-metal dichalcogenides (TMDs) are commonly used as solid lubricants in various environments. Molybdenum disulfide is the most studied and applied TMD solid lubricant, but other members may have similar or even better sliding properties. Tungsten diselenide is one of the materials that has rarely been investigated in terms of tribological properties. This paper provides a comprehensive tribological characterization of substoichiometric tungsten diselenide and molybdenum disulfide coatings deposited by magnetron sputtering. We focused on tribological properties at a macroscopic scale, particularly friction and wear dependence on applied load; however, a nanoscale frictional assessment of worn surfaces was performed as well to identify the major wear mechanisms. Substoichiometric tungsten diselenide outperformed traditional molybdenum disulfide, exhibiting much lower friction in humid air, suggesting lower coating sensitivity to the humid atmosphere. Moreover, a combination of nanotribological experiments in the wear tracks with sliding under different environmental conditions suggests that the key factor causing frictional load-dependence (deviation from Amonton's law) is frictional heating of the surface.

cond-mat.mtrl-sci↗

arXiv2025

Optimal boron-doped graphene substrate for glucose Raman signal enhancement

Surface Enhanced Raman Spectroscopy (SERS) is a highly sensitive and selective technique that greatly enhances the signal of an analyte, compared with its signal from classical Raman Spectroscopy, due to its interaction with a substrates surface. It has been shown that low concentration boron-doped graphene (B-graphene) enhances the Raman signal of simple organic molecules like pyridine. Recent studies also suggest that B-graphene can remain thermodynamically stable when doped with significantly higher concentrations of boron than previously observed. In this framework, we use quantum mechanical simulations to investigate the influence of dopant concentration and geometric distribution on the effectiveness of B-doped graphene as a SERS substrate, with glucose as analyte. By combining analysis of interatomic force constants and of phonon eigenvectors composition, we conclude that higher doping concentrations provide a larger enhancement to glucose's Raman signal, while the molecule orientation relative to the surface plays a fundamental role in the Raman response. We suggest that high concentration B-graphene presents itself as a potential substrate for SERS based detection of glucose, while the used phonon-based analysis can be promptly applied for the search of promising candidates as substrate materials for enhanced Raman response.

cond-mat.mtrl-sci↗

arXiv2025

Effect of crystallinity on the frictional and wear performance of molybdenum disulfide: A molecular dynamics study

The frictional and wear performance of molybdenum disulfide (MoS2) is significantly influenced by its intrinsic arrangement of crystals or crystallinity. In this study, we investigate the effect of crystallinty on coefficient of friction (COF) and wear in MoS2 using a suite of reactive molecular dynamics (MD) simulations. A range of configurations, from amorphous to crystalline, is modeled to capture the effect of structural order on the tribological behavior. To study friction and wear, we simulate the sliding of a spherical rigid carbon body over the MoS2 surface under varying crystallinity conditions. Our results reveal a pronounced reduction in COF with decreasing crystallinity, with crystalline MoS2 exhibiting superlubricity. This behavior is attributed to the preservation of a flat sliding surface and frictional anisotropy, which enables lateral movement along low-resistance paths. In contrast, amorphous and polycrystalline MoS2 with lower degrees of crystallinity displays a substantially higher COF, driven by increased surface roughness and atomic-scale energy dissipation. Furthermore, we examine the wear mechanisms under high normal loads, demonstrating that crystallinity enhances wear resistance by mitigating material deformation. These findings provide atomic-scale insights into the tribological performance of MoS2, emphasizing the critical role of structural order in achieving ultralow friction. Our work corroborates with previous studies on superlubricity in MoS2 and extends this understanding to rigid-body sliding conditions, offering valuable implications for designing low-friction and wear resistant solid lubricants.

cond-mat.mtrl-sci↗

arXiv2024

The twisting dynamics of large lattice mismatch van der Waals heterostructures

Van der Waals (vdW) homo-/hetero-structures are ideal systems for studying interfacial tribological properties such as structural superlubricity. Previous studies concentrated on the mechanism of translational motion in vdW interfaces. However, detailed mechanisms and general properties of the rotational motion are barely explored. Here, we combine experiments and simulations to reveal the twisting dynamics of the MoS$_2$/graphite heterostructure. Unlike the translational friction falling into the superlubricity regime with no twist angle dependence, the dynamic rotational resistances highly depend on twist angles. Our results show that the periodic rotational resistance force originates from structural potential energy changes during the twisting. The structural potential energy of MoS$_2$/graphite heterostructure increases monotonically from0 to 30 degrees twist angles, and the estimated relative energy barrier is (1.43 +/- 0.36) x 10 J/m. The formation of Moir\'e superstructures in the graphene layer is the key to controlling the structural potential energy of the MoS$_2$/graphene heterostructure. Our results suggest that in twisting 2D heterostructures, even if the interface sliding friction is negligible, the evolving potential energy change results in a non-vanishing rotational resistance force. The structural change of the heterostructure can be an additional pathway for energy dissipation in the rotational motion, further enhancing the rotational friction force.

cond-mat.mes-hall↗

arXiv2022

Design guidelines for two-dimensional transition metal dichalcogenide alloys

Two-dimensional (2D) materials and Transition Metal Dichalcogenides (TMD) in particular are at the forefront of nanotechnology. To tailor properties for engineering applications, alloying strategies used for bulk metals in the last century need to be extended to this novel class of materials. Here we present a systematic analysis of the phase behaviour of substitutional 2D alloys in the TMD family on both the metal and chalcogenide site. The phase behaviour is quantified in terms of a metastability metric and benchmarked against systematic computational screening of configurational energy landscapes. The resulting Pettifor maps can be used to identify broad trends across chemical spaces and as starting point for setting up rational search strategies in phase space, thus allowing for targeted computational analysis of properties on likely thermodynamically stable compounds. The results presented here also constitute a useful guideline for synthesis of binary metal 2D TMDs alloys via a range of synthesis techniques.

cond-mat.mtrl-sci↗

arXiv2022

Pettifor Maps of Complex Ternary Two-dimensional Transition Metal Sulphides

Alloying is an established strategy to tune the properties of bulk compounds for desired applications. With the advent of nanotechnology, the same strategy can be applied to 2D materials for technological applications, like single-layer transistors and solid lubricants. Here we present a systematic analysis of the phase behaviour of substitutional 2D alloys in the Transition Metal Disulphides (TMD) family. The phase behaviour is quantified in terms of a metastability metric and benchmarked against many-body expansion of the energy landscape. We show how the metastability metric can be directly used as starting point for setting up rational search strategies in phase space, thus allowing for targeted further computational prediction and analysis of properties. The results presented here also constitute a useful guideline for synthesis of TMDs binary alloys via a range of synthesis techniques.

cond-mat.mtrl-sci↗

arXiv2022

Multi-scale model predicting friction of crystalline materials

We present a multi-scale computational framework suitable for designing solid lubricant interfaces fully in silico. The approach is based on stochastic thermodynamics founded on the classical thermally activated two-dimensional Prandtl-Tomlinson model, linked with First Principles methods to accurately capture the properties of real materials. It allows investigating the energy dissipation due to friction in materials as it arises directly from their electronic structure, and naturally accessing the time-scale range of a typical friction force microscopy. This opens new possibilities for designing a broad class of material surfaces with atomically tailored properties. We apply the multi-scale framework to a class of two-dimensional layered materials and reveal a delicate interplay between the topology of the energy landscape and dissipation that known static approaches based solely on the energy barriers fail to capture.

cond-mat.mtrl-sci↗

arXiv2020

Phase behaviour of (Ti:Mo)S$_2$ binary alloys arising from electron-lattice coupling

While 2D materials attract considerable interests for their exotic electronic and mechanical properties, their phase behaviour is still largely not understood. This work focuses on (Mo:Ti)S$_2$ binary alloys which have captured the interest of the tribology community for their good performance in solid lubrication applications and whose chemistry and crystallography is still debated. Using electronic structures calculations and statistical mechanics we predict a phase-separating behaviour for the system and trace its origin to the energetics of the $d$-band manifold due to crystal field splitting. Our predicted solubility limits as a function of temperature are in accordance with experimental data and demonstrate the utility of this protocol in understanding and designing TMD alloys.

cond-mat.mtrl-sci↗

arXiv2020

Exploring the stability of twisted van der Waals heterostructures

Recent research showed that the rotational degree of freedom in stacking 2D materials yields great changes in the electronic properties. Here we focus on an often overlooked question: are twisted geometries stable and what defines their rotational energy landscape? Our simulations show how epitaxy theory breaks down in these systems and we explain the observed behaviour in terms of an interplay between flexural phonons and the interlayer coupling, governed by Moiré superlattice. Our argument applied to the well-studied MoS$_2$/Graphene system rationalize experimental results and could serve as guidance to design twistronics devices.

cond-mat.mtrl-sci↗