CyberSec Research

Recent works indicate that heterogeneous response and non-Markovianity may yield recognizable hallmarks in the microrheology of semisolid viscoelastic materials. Here we perform numerical simulations using a non-Markovian overdamped Langevin approach to explore how the microrheology experienced by probe particles immersed in an effective semisolid material can be influenced by its micro-heterogeneities. Our results show that, besides affecting the mean squared displacement, the time-dependent diffusion coefficient, and the shear moduli, the micro-heterogeneities lead to displacement distributions that deviate from the usual Gaussian behavior. In addition, our study provides an analytical way to characterize the micro-heterogeneities of semisolid viscoelastic materials through their microrheology.

Exciton-exciton annihilation (EEA), in which two excitons interact to generate high-energy excitations, is an important non-radiative channel in light-induced excited-state relaxation. When efficient, this process offers an alternative route to exciton emission, potentially allowing extended energetically excited particles' lifetime and coherence. These properties are significant in designing and understanding materials-based quantum devices, particularly for low-dimensional semiconductors. Here, we present a first-principles framework to compute EEA mechanisms and rates using many-body perturbation theory within the GW and Bethe-Salpeter Equation (GW-BSE) formalism. Our method explicitly accounts for Coulomb-driven and phonon-assisted exciton-exciton scattering by explicitly evaluating the interaction channels between the constituent electrons and holes composing the BSE excitons. We apply this framework to monolayer WSe$_2$ and explore the $A$, $B$ excitation manifolds, finding picosecond-scale annihilation between bright and dark states, cross valleys, and cross peak manifolds. These channels become allowed due to scattering into free electron-hole pairs across the Brillouin zone. Our results supply new insights into non-radiative exciton relaxation mechanisms in two-dimensional materials, providing a predictive and general tool for modeling these interactions in excitonic materials.

Polyradical nanographenes featuring strong spin entanglement and robust many-body spin states against external magnetic perturbations not only enable the exploration of correlated quantum magnetism at the molecular scale, but also constitute promising candidates for developing molecular qubits with chemical tunability and building scalable quantum networks. Here, we employed a predictive design strategy to achieve the on-surface synthesis of two homologues of Clar goblet, C62H22 and C76H26, via lateral and vertical extensions of the parent structure, respectively. Vertical extension increases the number of topologically frustrated zero-energy modes, which scale linearly with the total number of benzene ring rows. In contrast, the lateral extension enhances electron-electron interactions, leading to the emergence of additional radical states beyond those predicted by the topological zero-energy modes. Consequently, both structures exhibit correlated tetraradical character and a many-body singlet ground state as confirmed by multireference theoretical calculations. These magnetic states arise from unique magnetic origins and also display distinct resilience to external perturbations, which can be experimentally validated using nickelocene-functionalized scanning probe techniques. Our work presents a general strategy for rational design of highly entangled polyradical nanographenes with tunable spin numbers and resilience of their many-body spin states to perturbations, opening exciting possibilities for exploring novel correlated spin phases in molecular systems and advancing quantum information technologies.

Recent fabrication of two-dimensional (2D) metallic bismuth (Bi) via van der Waals (vdW) squeezing method opens a new avenue to ultrascaling metallic materials into the {\aa}ngstr\"om-thickness regime [Nature 639, 354 (2025)]. However, freestanding 2D Bi is typically known to exhibit a semiconducting phase [Nature 617, 67 (2023), Phys. Rev. Lett. 131, 236801 (2023)], which contradicts with the experimentally observed metallicity in vdW-squeezed 2D Bi. Here we show that such discrepancy originates from the pressure-induced buckled-to-flat structural transition in 2D Bi, which changes the electronic structure from semiconducting to metallic phases. Based on the experimentally fabricated MoS2-Bi-MoS2 trilayer heterostructure, we demonstrate the concept of layer-selective Ohmic contact in which one MoS2 layer forms Ohmic contact to the sandwiched Bi monolayer while the opposite MoS2 layer exhibits a Schottky barrier. The Ohmic contact can be switched between the two sandwiching MoS2 monolayers by changing the polarity of an external gate field, thus enabling charge to be spatially injected into different MoS2 layers. The layer-selective Ohmic contact proposed here represents a layertronic generalization of metal/semiconductor contact, paving a way towards layertronic device application.

Crystal-structure match (CSM), the atom-to-atom correspondence between two crystalline phases, is used extensively to describe solid-solid phase transition (SSPT) mechanisms. However, existing computational methods cannot account for all possible CSMs. Here, we propose a formalism to classify all CSMs into a tree structure, which is independent of the choices of unit cell and supercell. We rigorously proved that only a finite number of noncongruent CSMs are of practical interest. By representing CSMs as integer matrices, we introduce the crystmatch method to exhaustively enumerate them, which uncontroversially solves the CSM optimization problem under any geometric criterion. For most SSPTs, crystmatch can reproduce all known deformation mechanisms and CSMs within 10 CPU minutes, while also revealing thousands of new candidates. The resulting database can be further used for comparing experimental phenomena, high-throughput energy barrier calculations, or machine learning.

Metastable Co$_2$Ti$_3$O$_8$ was synthesized through a topochemical reaction using Li$_2$CoTi$_3$O$_8$ as the precursor, resulting in a vacancy-ordered spinel structure. Crystal structure analysis confirmed that Co ions selectively occupy the A-site, giving rise to a frustrated diamond lattice. Magnetic susceptibility and heat capacity measurements revealed antiferromagnetic order at 4.4 K, which is markedly suppressed compared to the negative Weiss temperature of ${\sim}-27$ K, indicating a high degree of frustration effects. Pulsed high-field magnetization measurements revealed a four-step successive magnetic phase transition, demonstrating that Co$_2$Ti$_3$O$_8$ is a promising candidate for a frustrated $J_1-J_2$ diamond lattice. Additionally, the $J_2/J_1$ ration estimated from the molecular field approximation suggests the possibility of a spiral ordered ground state. These observations highlight the potential of frustrated magnetism in ordered spinel structures to expand the material search space for quantum magnetism, including magnetic skyrmions.

Using first-principles calculations and an atomistic spin model we predict the stabilization of a bilayer triple-Q state in an atomic Mn bilayer on Ir(111) due to interlayer higher-order exchange interactions. Based on density functional theory (DFT) we study the magnetic interactions and ground state in a Mn monolayer and bilayer on the Ir(111) surface. We calculate the energy dispersion of spin spirals (single-Q states) to scan a large part of the magnetic phase space and to obtain constants of pair-wise exchange interactions. By including spin-orbit coupling we determine the strength of the Dzyaloshinskii-Moriya interaction. To reveal the role of higher-order exchange interactions in these films, we consider multi-Q states obtained by a superposition of spin spirals. For the Mn monolayer in fcc stacking on Ir(111), the triple-Q state exhibits the lowest total energy in DFT, while the N\'eel state is most favorable for hcp stacking. For the Mn bilayer on Ir(111), two types of the triple-Q state are possible. In both magnetic configurations, a triple-Q state occurs within each of the Mn layers. However, only in one of them the spin alignment between the layers is such that nearest-neighbor spins of different layers also exhibit the tetrahedron angles which characterize the triple-Q state. We denote this state -- which has the lowest total energy in our DFT calculations -- as the ideal bilayer triple-Q state. This state exhibits significant topological orbital moments within each of the two Mn layers which are aligned in parallel resulting in a large topological orbital magnetization. We interpret the DFT results within an atomistic spin model which includes pair-wise Heisenberg exchange, the Dzyaloshinskii-Moriya interaction, as well as higher-order exchange interactions....

Terahertz (THz) lasers provide a new research perspective for spin electronics applications due to their sub-picosecond time resolution and non-thermal ultrafast demagnetization, but the interaction between spin, charge and lattice dynamics remains unclear. This study investigates photoinduced ultrafast demagnetization in monolayer CrSBr, a two-dimensional material with strong spin-orbit and spin-lattice coupling, and resolves its demagnetization process. Two key stages are identified: the first, occurring within 20 fs, is characterized by rapid electron-driven demagnetization, where charge transfer and THz laser are strongly coupled. In the second stage, light-induced lattice vibrations coupled to spin dynamics lead to significant spin changes, with electron-phonon coupling playing a key role. Importantly, the role of various phonon vibration modes in the electron relaxation process was clearly determined, pointing out that the electronic relaxation of the B3g1 phonon vibration mode occurs within 83 fs, which is less than the commonly believed 100 fs. Moreover, the influence of this coherent phonon on the demagnetization change is as high as 215 %. These insights into multiscale magneto-structural coupling advance the understanding of nonequilibrium spin dynamics and provide guidelines for the design of light-controlled quantum devices, particularly in layered heterostructures for spintronics and quantum information technologies.

The pyroelectric effect in ferroelectric thin films is typically composed of different contributions, which are difficult to disentangle. In addition, clamping to the substrate interface plays an important role. We studied epitaxial (Ba,Sr)TiO$_3$ thin films grown on NdScO$_3$ to see if time-resolved measurements can shed more light on the complex interaction. In particular, we compare standard measurements of the pyroelectric coefficient by temperature-dependent hysteresis loops to transient deformation measurements on picosecond timescales in the same material. The advantage of the time-resolved approach lies in its increased sensitivity in thin films compared to that of polarization hysteresis measurements. Whereas a fast thermal expansion of the ferroelectric thin film was observed after femtosecond laser excitation of the intermediate SrRuO$_3$ layer, heat diffusion simulations reveal frustration of the thermal expansion, which might be explained with the charge dynamics at the Schottky barrier formed at the SrRuO$_3$/(Ba,Sr)TiO$_3$. More studies are required to quantitatively assess the individual contributions to the pyroelectric coefficient of the materials used in our layer architecture.

Ferrofluids, composed of magnetic nanoparticles suspended in a non-magnetic carrier liquid, have attracted considerable attention since their discovery in the 1960s. Their combination of liquid and magnetic properties gives rise to complex behaviors and unique functionalities, enabling a wide range of technological applications. Among these is the ability of the magnetic material to be moved by and to absorb heat when exposed to an external magnetic field -- a process that can occur through various dissipation mechanisms depending on the system. A detailed understanding of these mechanisms is crucial for tailoring materials to specific applications. We provide a comprehensive overview of the theoretical principles underlying different energy dissipation processes and propose a coherent framework for their interpretation. Particular attention is devoted to describing the frequency-dependent susceptibility, which is the key parameter to describe dissipation. We demonstrate that dissipation, predicted from magnetometry-based studies, matches well with direct, frequency-dependent calorimetric results, expanding the available frequency range of the characterization. The demonstrating measurements were carried out with a dilute ferrofluid containing magnetite nanoparticles of a mean diameter of 10.6 nm.

Solar water splitting has received a lot of attention due to its high efficiency and clean energy production potential. Herein, based on the band alignment principle, the g-C3N4/TiO2-B(001) heterostructure is strategically designed, then a Li-F co-doping approach is developed and implemented, leading to significant enhancement in the photocatalytic hydrogen evolution efficiency of the heterostructure systems. The decomposition of water molecule on the surface of heterostructures, the migration and diffusion of proton across the interface, and the hydrogen evolution performance are systematically studied and comprehensively analyzed. The results demonstrate that the heterojunction surface exhibits a relatively low energy barrier for water decomposition, facilitating both hydrogen evolution reaction (HER) and oxygen evolution reaction (OER). Proton transfer preferentially occurs from the TiO2-B(001) surface to the g-C3N4 surface through the interface. The presence of polar covalent bonds establishes a substantial energy barrier for proton migration from TiO2-B(001) surface to the interface, representing a rate-determining factor in the hydrogen evolution process. The formation of hydrogen bonds significantly reduces the migration energy barrier for protons crossing the interface to the g-C3N4 surface. Hydrogen adsorption free energy analysis show that that the heterojunction surface exhibits optimal proton adsorption and desorption characteristics. The synergistic combination of low water decomposition energy barrier, reduced proton migration energy barriers and exceptional HER performance endows both g-C3N4/TiO2-B(001) heterostructure and Li-F co-doped g-C3N4/TiO2-B(001) heterojunction with remarkbale potential as efficient HER photocatalyst.

This study reports the decomposition of beta-SnWO4 into Sn, SnO2, and WO3 induced by static compression. We performed high-pressure synchrotron powder angle-dispersive X-ray diffraction measurements and found that decomposition occurs at a pressure of 13.97(5) GPa and is irreversible. This result contradicts a previous study that, based on density-functional theory calculations and crystal-chemistry arguments, predicted a pressure-driven transition from beta-SnWO4 to alpha-SnWO4. Our analysis indicates that the observed decomposition is unrelated to mechanical or dynamic instabilities. Instead, it likely stems from frustration of the beta-alpha transition, as this transformation requires a change in Sn coordination from octahedral to tetrahedral. The assessment of how pressure influences the volume of the unit cell provided an accurate determination of the room-temperature pressure-volume equation of state for beta-SnWO4. Furthermore, the elastic constants and moduli, as well as the pressure dependence of Raman and infrared modes of beta-SnWO4, were derived from density-functional theory calculations. Several phonon modes exhibited softening, and three cases of phonon anti-crossing were observed.

NiBr2, similar to NiI2, exhibits the onset of collinear antiferromagnetism at a subroom temperature and, with further cooling, undergoes a transition to a helimagnetic ordering associated with multiferroic behavior. This work investigates the hydrostatic pressure effects on magnetic phase transitions in NiBr2. We measured isobaric temperature dependencies of AC magnetic susceptibility at various pressures up to 3 GPa. The experimental data are interpreted in conjunction with the results of theoretical calculations focused on pressure influence on the hierarchy of exchange interactions. Contrary to the NiI2 case, the phase transition to helimagnetism rapidly shifts to lower temperatures with increasing pressure. Similar to the NiI2, the Neel temperature increases with pressure. The rate of increase accelerates when the helimagnetic phase is suppressed by pressure. The ab initio calculations link these contrasting trends to pressure-enhanced magnetic exchange interactions. Similarly to the NiI2 case, the stabilization of the collinear AFM phase is driven primarily by the second-nearest interlayer coupling (j2'). Furthermore, the ratio of in-plane interactions makes helimagnetic order in NiBr2 much more volatile, which permits its suppression with already small pressures. These findings highlight the principal role of interlayer interactions in the distinct response of NiBr2 and NiI2 magnetic phases to external pressure.

Optical generation of transverse coherent phonons by femtosecond light pulses is appealing for high-speed sub-THz active control of material properties. Lead-free double perovskite semiconductors, such as Cs2AgBiBr6, attract particular interest due to their cubic to tetragonal phase transition below room temperature and strong polaron effects from carrier-lattice coupling. Here, we reveal that the anisotropic photostriction in halide perovskites with tetragonal crystal structure represents an efficient non-thermal tool for generating transverse coherent phonons. In particular, we demonstrate that along with compressive strain, optical generation of photoexcited carriers leads to strong shear strain in Cs2AgBiBr6 below the phase transition temperature of 122 K. Using time-domain Brillouin spectroscopy, we observe coherent transverse and longitudinal acoustic phonons with comparable amplitudes in the tetragonal phase, while in the cubic phase only longitudinal phonons are generated. The polarization of the photoinduced transverse phonons is dictated by the projection of the c-axis on the surface plane, which leads to a prominent anisotropic polarization response in the detection. The generated strain pulses correspond to transverse acoustic soft eigenmodes with a strong temperature dependence of dispersion, which provides an additional degree of freedom for active hypersonic control.

We have characterized the high-pressure behavior of alpha-SnWO4. The compound has been studied up to 30 GPa using a diamond-anvil cell and synchrotron powder X-ray diffraction. We report evidence of two structural phase transitions in the pressure range covered in our study, and we propose a crystal structure for the two high-pressure phases. The first one, observed around 12.9 GPa, has been obtained combining indexation using DICVOL and density-functional theory calculations. The second high-pressure phase, observed around 17.5 GPa, has been determined by using the CALYPSO code, the prediction of which was supported by a Le Bail fit to the experimental X-ray diffraction patterns. The proposed structural sequence involves two successive collapses of the unit-cell volume and an increase in the coordination number of Sn and W atoms. The room-temperature equations of state, the principal axes of compression and their compressibility, the elastic constants, and the elastic moduli are reported for {\alpha}-SnWO4 and for the two high-pressure phases.

The topological quantum phases in antiferromagnetic topological insulator MnBi$_2$Te$_4$ hold promise for next-generation spintronics, but their experimental realization has been constrained by challenges in preparing high-quality devices. In this work, we report a new wax-assisted exfoliation and transfer method that enables the fabrication of MnBi$_2$Te$_4$ heterostructures with both surfaces encapsulated by AlO$_x$. This strategy strongly enhances the topological quantum phases in MnBi$_2$Te$_4$ flakes. We observe the robust axion insulator state in even-layer device with wide zero Hall plateau and high longitudinal resistivity, and the quantum anomalous Hall effect in odd-layer device with large hysteresis and sharp plateau transition. These results demonstrate that the combination of wax exfoliation and AlO$_x$ encapsulation provides great potentials for exploring novel topological quantum phenomena and potential applications in MnBi$_2$Te$_4$ and other two-dimensional materials.

Organic crystal waveguides, known for excellent light-guiding and photonic versatility, present a promising alternative to conventional optical media in visible light communication (VLC) systems. In a novel approach, the high photoluminescence quantum yield organic crystal 2,2dash-((1E,1Edash)-hydrazine-1,2-diylidenebis(methaneylylidene))diphenol (SAA) is used as an optical waveguide medium for real-time data communication in the visible range, employing a microcontroller unit with on off keying modulation. Leveraging its spectral properties, the SAA crystal demonstrates dual active and passive waveguiding capabilities for signal modulation. Error-free signal detection is achieved thanks to the smooth, defect-free surface morphology of the crystal. The relationship between incident angle and light intensity reveals stable fluorescence under narrow angle excitation, positioning the crystal as an all-angle signal receiver that surpasses conventional optical fibers. A real time data transfer setup is demonstrated, enabling direct transmission from a serial interface and accurate reconstruction of grayscale images. This represents the first implementation of a fully organic crystal-based VLC platform, integrating wavelength conversion, omnidirectional waveguiding, and real time signal processing. The results establish a foundation for compact, efficient, and integrable photonic communication technologies.

Core-shell nanoparticles, particularly those having a gold core, have emerged as a highly promising class of materials due to their unique optical and thermal properties, which underpin a wide range of applications in photothermal therapy, imaging, and biosensing. In this study, we present a comprehensive study of the thermal dynamics of gold-core silica-shell nanoparticles immersed in water under pulse illumination. The plasmonic response of the core-shell nanoparticle is described by incorporating Mie theory with electronic temperature corrections to the refractive indices of gold, based on a Drude Lorentz formulation. The thermal response of the core-shell nanoparticles is modeled by coupling the two temperature model with molecular dynamics simulations, providing an atomistic description of nanoscale heat transfer. We investigate nanoparticles with both dense and porous silica shells (with 50% porosity) under laser pulse durations of 100 fs, 10 ps, and 1 ns, and over a range of fluences between 0.05 and 5mJ/cm2. We show that nanoparticles with a thin dense silica shell (5 nm) exhibit significantly faster water heating compared to bare gold nanoparticles. This behavior is attributed to enhanced electron-phonon coupling at the gold silica interface and to the relatively high thermal conductance between silica and water. These findings provide new insights into optimizing nanoparticle design for efficient photothermal applications and establish a robust framework for understanding energy transfer mechanisms in heterogeneous metal dielectric nanostructures.