CyberSec Research

Integrating solid-state spin defects into classical electronic devices can enable new opportunities for quantum information processing that benefit from existing semiconductor technology. We show, through bias control of an isotopically purified silicon carbide (SiC) p-i-n diode, the depletion of not only electrical noise sources but also magnetic noise sources, resulting in record coherences for SiC electron spin qubits. We also uncover complementary improvements to the relaxation times of nuclear spin registers controllable by the defect, and measure diode-enhanced coherences. These improvements lead to record-long nuclear spin Hahn-echo times on the scale of minutes. These results demonstrate the power of materials control and electronic device integration to create highly coherent solid-state quantum network nodes and processors.

Electron nematicity-the breaking of rotational symmetry while preserving translational symmetry-is the quantum analogue of classical nematic liquid crystals. First predicted in 1998, electronic nematicity has been established in a variety of materials, including two-dimensional electron gases (2DEGs) in magnetic fields, copper-oxide superconductors, and Fe-based superconductors. A long-standing open question is what physical mechanisms drive electronic nematic order. In BaFe$_2$As$_2$ and highly underdoped YBa$_2$Cu$_3$O$_{6+y}$, strong evidence suggests that nematicity arises from vestigial spin-density-wave (SDW) order. However, evidence for nematicity associated with charge-density-wave (CDW) order has been less conclusive, particularly in systems near a superconducting state. Here, we present direct evidence for CDW-driven nematic fluctuations in the pnictide superconductor Ba$_{1-x}$Sr$_x$Ni$_2$As$_2$ (BSNA), a Ni-based homologue of Fe-based superconductors that exhibits CDW rather than SDW order. Previous elastoresistance studies have shown that BSNA displays a large nematic susceptibility-linked to a six-fold enhancement of superconductivity-within a region of the phase diagram occupied by an incommensurate CDW. Using x-ray scattering under uniaxial strain, we demonstrate that even minimal strain levels ($\epsilon \sim 10^{-4}$) significantly break the fourfold symmetry of the CDW. Within a Ginzburg-Landau framework, we define a nematic susceptibility based on the asymmetric response of symmetry-related CDW superlattice reflections, showing strong agreement with elastoresistivity measurements. Our study provides the first clear demonstration of a direct link between charge order and a nematic state, offering key insights into the intertwined superconducting phases of these materials.

The transverse thermoelectric generation and cooling performances in a thermopile module composed of recently developed SmCo$_5$/Bi$_{0.2}$Sb$_{1.8}$Te$_3$ artificially tilted multilayers are evaluated quantitatively. When a large temperature difference of 405 $^\circ$C is applied to the SmCo$_5$/Bi$_{0.2}$Sb$_{1.8}$Te$_3$-based module, the open-circuit voltage and output power reach 0.51 V and 0.80 W, respectively, where the corresponding maximum power density is 0.16 W/cm$^2$. The maximum energy conversion efficiency for our module in this condition is experimentally determined to be 0.92%. Under the cooling operation, the same module exhibits the maximum temperature difference of 9.0 $^\circ$C and heat flow at the cold side of 1.6 W. Although these values are lower than the ideal thermoelectric performance expected from the material parameters due to the imperfections associated with modularization, the systematic investigations reported here clarify a potential of the SmCo$_5$/Bi$_{0.2}$Sb$_{1.8}$Te$_3$ artificially tilted multilayers as thermoelectric generators and cooling devices.

Topological insulators (TIs) and topological crystalline insulators (TCIs) are materials with unconventional electronic properties, making their discovery highly valuable for practical applications. However, such materials, particularly those with a full band gap, remain scarce. Given the limitations of traditional approaches that scan known materials for candidates, we focus on the generation of new topological materials through a generative model. Specifically, we apply reinforcement fine-tuning (ReFT) to a pre-trained generative model, thereby aligning the model's objectives with our material design goals. We demonstrate that ReFT is effective in enhancing the model's ability to generate TIs and TCIs, with minimal compromise on the stability of the generated materials. Using the fine-tuned model, we successfully identify a large number of new topological materials, with Ge$_2$Bi$_2$O$_6$ serving as a representative example--a TI with a full band gap of 0.26 eV, ranking among the largest known in this category.

Properties in crystalline and ordered materials tend to be anisotropic, with their orientation affecting the macroscopic behavior and functionality of materials. The ability to image the orientation of anisotropic material properties in three dimensions (3D) is fundamental for the understanding and functionality-driven development of novel materials. With the development of X ray linear dichroic orientation tomography (XL DOT), it is now possible to non-destructively map three-dimensional (3D) orientation fields in micrometer-sized samples. In this work, we present the iterative, gradient-based reconstruction algorithm behind XL DOT that can be used to map orientations based on linear dichroism in 3D. As linear dichroism can be exhibited by a broad spectrum of materials, XL DOT can be used to map, for example, crystal orientations as well as ferroic alignment, such as ferroelectric and antiferromagnetic order. We demonstrate the robustness of this technique for orientation fields that exhibit smoothly varying and granular configurations, and subsequently identify and discuss optimal geometries for experimental data acquisition and optimal conditions for the reconstruction. We anticipate that this technique will be instrumental in enabling a deeper understanding of the relationship between material structures and their functionality, quantifying, for example, the orientation of charge distributions and magnetic anisotropies at the nanoscale in a wide variety of systems - from functional to energy materials.

Hydrogen-based direct reduction offers a sustainable pathway to decarbonize the metal production industry. However, stable metal oxides, like Cr$_2$O$_3$, are notoriously difficult to reduce, requiring extremely high temperatures (above 1300 $^\circ$C). Herein, we show how reducing mixed oxides can be leveraged to lower hydrogen-based reduction temperatures of stable oxides and produce alloys in a single process. Using a newly developed thermodynamic framework, we predict the precise conditions (oxygen partial pressure, temperature, and oxide composition) needed for co-reduction. We showcase this approach by reducing Cr$_2$O$_3$ mixed with Fe$_2$O$_3$ at 1100 $^\circ$C, significantly lowering reduction temperatures (by $\geq$200 $^\circ$C). Our model and post-reduction atom probe tomography analysis elucidate that the temperature-lowering effect is driven by the lower chemical activity of Cr in the metallic phase. This strategy achieves low-temperature co-reduction of mixed oxides, dramatically reducing energy consumption and CO$_2$ emissions, while unlocking transformative pathways toward sustainable alloy design.

During laser-induced phase transitions, fast transformations of electronic, atomic, and spin configurations often involve emergence of hidden and metastable phases. Being inaccessible under any other stimuli, such phases are indispensable for unveiling mechanisms and controlling the transitions. We experimentally explore spin kinetics during ultrafast first-order 90$^{\circ}$ spin-reorientation (SR) transition in a canted antiferromagnet Fe$_3$BO$_6$, and reveal that the transition is controlled by the canting between the magnetic sublattices. Laser-induced perturbation of the Dzyaloshinskii-Moriya interaction results in a change of the intersublattice canting within first picoseconds, bringing Fe$_3$BO$_6$ to a hidden phase. Once this phase emerges, laser-induced heating activates precessional 90$^\circ$ spin switching. Combination of the spin canting and heating controls the final spin configuration comprising coexisting initial and switched phases. Extended phase coexistence range is in a striking contrast to the narrow SR transition in Fe$_3$BO$_6$ induced by conventional heating.

Grain microstructures are crucial to the mechanical properties, performance, and often lifetime of metallic components. Hence, the prediction of grain microstructures emerging from solidification processes at relevant macroscopic scale is essential to the design or optimization of new alloys and processing conditions. Yet, despite the broad range of multi-scale models proposed so far, all of them suffer from computational limitations, such that advances from computational and algorithm perspectives remain needed. Here, we present a novel approach for tracking crystallographic solidification grain envelopes capable of predicting competitive growth scenarios and columnar-to-equiaxed transitions for stationary grains. The model relies on classical assumptions and equations in use in several broadly used and thoroughly validated approaches (e.g. cellular automata). Yet, our approach defines the grain envelope using Lagrangian particles and tracks their evolution using an algorithm and an implementation relying on scalable libraries and using modern CPU/GPU architectures. The model is used to simulate several benchmarks of increasing complexity, and the results are compared to analytical, experimental, and numerical results from literature for the purpose of model validation. To highlight the applicability to real-world processes and the possibility of coupling the model with existing physics-based simulation tools, the model is also (one-way) coupled with a multiphysics laser-material-interaction model to simulate competitive grain growth during laser beam welding of steel.

Bands away from the Fermi energy do not influence the electrical conduction. In typical rare-earth lanthanide compounds, the localized 4$\textit{f}$-electrons have a weak effect on the electrical conduction, limiting their influence on the Berry curvature and, hence, the intrinsic anomalous Hall effect. However, a comprehensive study of the magnetic, thermodynamic, and transport properties of single-crystalline NdGaSi, guided by first-principles calculations, reveals a ferromagnetic ground state that induces a splitting of quasi-flat 4$\textit{f}$-electronic bands and positions them near the Fermi energy. The observation of an extraordinarily large intrinsic anomalous Hall conductivity of 1165 $\Omega^{-1}$cm$^{-1}$ implies the direct involvement of localized states in the generation of non-trivial band crossings around the Fermi energy. These results are remarkable when compared to ferrimagnetic NdAlSi, which differs only in a non-magnetic atom (a change in the principal quantum number $\textit{n}$ of the outer $\textit{p}$ orbital) with the same number of valence electrons and does not exhibit any measurable anomalous Hall conductivity.

Two-dimensional massless Dirac fermions exhibit Dirac cones, which are classified into three types: type-I, type-II, and type-III. In both type-I and type-II cones, the energy dispersion is linear in all momentum directions. Type-I cones are characterized by a non-overtilted structure, where the Dirac point serves as a local minimum (maximum) for the upper (lower) band. In contrast, type-II cones exhibit overtilted dispersions, leading to the coexistence of electron and hole pockets. At the critical tilt, the linear energy dispersion vanishes in one momentum direction, corresponding to a type-III Dirac cone. We further define a special case, termed the "narrow-sense" type-III cone, where not only the linear term but also quadratic and higher-order terms vanish, resulting in a completely flat dispersion along one direction. In this work, we numerically investigate the temperature ($T$) -dependence of the electronic specific heat ($C$), as the Dirac cone is continuously tilted from type-I to narrow-sense type-III. A model with particle-hole symmetry is employed to ensure that the chemical potential ($\mu$) remains temperature independent. Our results reveal a notable crossover in $C$ near narrow-sense type-III, where $C$ changes from $C \propto T^{2}$ below the crossover temperature ($T_{\rm co}$) to $C \propto T^{\frac{1}{2}}$ above $T_{\rm co}$. This crossover is attributed to the energy-dependent structure of the density of states. The present findings suggest a feasible approach for experimentally probing the degree of Dirac cone tilting near the narrow-sense type-III limit.

The random phase approximation (RPA) and the $GW$ approximation share the same total energy functional but RPA is defined on a restricted domain of Green's functions determined by a local Kohn-Sham (KS) potential. In this work, we perform self-consistent RPA calculations by optimizing the local KS potential through the optimized effective potential equation. We study a number of solids (C, Si, BN, LiF, MgO, TiO$_2$), and find in all cases a lowering of the total energy with respect to non-self-consistent RPA. We then propose a variational approach to optimize PBE0-type hybrid functionals based on the minimization of the RPA total energy with respect to the fraction of exact exchange used to generate the input KS orbitals. We show that this scheme leads to hybrid functionals with a KS band structure in close agreement with RPA, and with lattice constants of similar accuracy as within RPA. Finally, we evaluate $G_0W_0$ gaps using RPA and hybrid KS potentials as starting points. Special attention is given to TiO$_2$, which exhibits a strong starting-point dependence.

Magnon-phonon coupling has garnered increasing interest in condensed matter physics due to its fertile physics and potential applications in devices with novel functionalities. Surface acoustic waves (SAWs) are commonly employed as a source of coherent acoustic phonons. The strain associated with SAWs couples to magnetization of magnetic materials via magnetoelastic coupling and/or spin-rotation coupling. A typical SAW device is formed on a piezoelectric substrate with anisotropic crystal structure. Since the form of strain depends on the material parameters and structure of the SAW device, it is of vital importance to understand its character. In this paper, we present a comprehensive methodology to numerically calculate the SAW velocity, SAW excitation efficiency, lattice displacement and all strain components associated with SAW. LiNbO$_3$ is used as a prototypical material system. All quantities depend on the SAW propagation direction with respect to the crystalline axis and on the electrical boundary conditions. In contrast to non-piezoelectric isotropic media, we find that all shear strain components can be induced in LiNbO$_3$, with their amplitude and relative phase (with respect to the longitudinal strain) dependent on the propagation direction and the boundary conditions at the LiNbO$_3$ surface. These results offer a robust foundation for analyzing strain-driven magnon-phonon coupling mechanisms and contribute to designing strain-engineered functional magnonic and phononic devices.

We present a protocol for computing core-ionisation energies for molecules, which is essential for reproducing X-Ray photoelectron spectroscopy experiments. The electronic structure of both the ground state and the core-ionised states are computed using Multiwavelets and Density-Functional Theory, where the core ionisation energies are computed by virtue of the $\Delta$SCF method. To avoid the collapse of the core-hole state or its delocalisation, we make use of the Maximum Overlap Method, which provides a constraint on the orbital occupation. Combining Multiwavelets with the Maximum Overlap Method allows for the first time an all-electron calculation of core-ionisation energies with Multiwavelets, avoiding known issues connected to the use of Atomic Orbitals (slow convergence with respect to the basis set limit, numerical instabilities of core-hole states for large systems). We show that our results are consistent with previous Multiwavelet calculations which made use of pseudopotentials, and are generally more precise than corresponding Atomic Orbital calculations. We analyse the results in terms of precision compared to both Atomic Orbital calculations and Multiwavelets+pseudopotentials calculations. Moreover, we demonstrate how the protocol can be applied to target molecules of relatively large size. Both closed-shell and open-shell methods have been implemented.

This study demonstrates one of the first implementations of time-resolved resonant inelastic X-ray scattering (tr-RIXS), marking a seminal extension of RIXS spectroscopy into the ultrafast time domain. By investigating the ultrafast dynamics of vibronically dressed core excitons in graphite using femtosecond X-ray pulses from a Free Electron Laser, we reveal previously inaccessible insights into the transient coupling between core excitons and specific optical phonon modes. Our approach establishes tr-RIXS as a powerful, transformative tool capable of elucidating the intricate interplay between electronic and lattice dynamics, opening new avenues in ultrafast materials research.

In the present work, we develop the Green's function apparatus and extend its applicability to the study of microscopic anisotropic effects in real conducting materials. The problem of the previously proposed approaches written in terms of inter-atomic Green's functions is the presence of a spatial sum over all atoms of the crystal, which greatly complicates their application to systems with itinerant electrons. To provide a solution we derived expressions for magnetic torque vector and Dzyaloshinskii-Moriya interactions based on $\bf{k}$-dependent Green's functions, which allow numerical evaluations with guaranteed stability of spatial sums over the crystal lattice and moreover with much lower computational cost. Approbation of the approaches on the case of Fe$_3$GeTe$_2$ monolayer, which is based on first-principles DFT calculations, confirmed the numerical stability and allowed us to reproduce the characteristic length of experimentally observed collective spin excitations in the domain structure of this promising conducting material.

We report on the design and demonstration of ultra-wide bandgap (UWBG) AlGaN-channel metal-insulator heterostructure field effect transistors (HEFTs) for high-power, high-frequency applications. We find that the integration of gate dielectrics and field plates greatly improves the breakdown field in these devices, with state-of-art average breakdown field of 5.3 MV/cm (breakdown voltage > 260 V) with an associated maximum current density of 342 mA/mm, and cut-off frequency of 9.1 GHz. Furthermore, low trap-related impact was observed from minimal gate and drain lag estimated from pulsed I-V characteristics. The reported results provide the potential of UWBG AlGaN HEFTs for the next generation high-power radio frequency applications.

Lithium fluoride (LiF) is a critical component for stabilizing lithium metal anode and high-voltage cathodes towards the next-generation high-energy-density lithium batteries.Recent modeling study reported the formation of wurtzite LiF below about 550 K (J. Am. Chem. Soc. 2023, 145, 1327-1333), in contrast to experimental observation of rocksalt LiF under ambient conditions. To address this discrepancy, we employ molecular dynamics (MD) simulations with a refined machine-learned force field (MLFF), and demonstrate the nucleation and crystallization of rocksalt LiF from the molten phase at temperatures below about 800 K. The rocksalt phase remains stable in LiF nanoparticles. Complementary density functional theory (DFT) calculations show that dispersion interactions are essential for correctly predicting the thermodynamic stability of rocksalt LiF over the wurtzite phase on top of the commonly used PBE functional. Furthermore, we show that inclusion of virial stresses--alongside energies and forces--in the training of MLFFs is crucial for capturing phase nucleation and crystallization of rocksalt LiF under the isothermal-isobaric ensemble. These findings underscore the critical role of dispersion interactions in atomistic simulations of battery materials, where such effects are often non-negligible, and highlight the necessity of incorporating virial stresses during the training of MLFF to enable accurate modeling of solid-state systems.

A new ternary compound Fe$_{4-x}$VTe$_{4-y}$ ($x=1.01$, $y=0.74$) with Ti5Te4-type structure is identified. Fe and V atoms tend to occupy different crystallographic positions and form quasi-one-dimensional (quasi-1D) Fe-V chains along the c-axis. Millimeter-sized single crystal of Fe$_{2.99}$VTe$_{3.26}$ (FVT) with slender-stick shape could be grown by chemical vapor transport method which reflects its quasi-1D crystal structure. Magnetization measurements reveal that FVT orders antiferromagnetically below T$_N$=93 K with strong easy ab-plane magnetic anisotropy. Although a weak glassy-like behavior appears below 10 K, FVT is dominant by long-range antiferromagnetic order in contrast to the spin-glass state in previously reported isostructural Fe$_{5}$Te$_{4}$. We also synthesize V$_{4.64}$Te$_4$ with similar quasi-1D V-chains and find it has weak anomalies at 144 K on both resistivity and susceptibility curves. However, no clear evidence is found for the development of magnetic or charge order. X-ray photoelectron spectroscopy and Curie-Weiss fit reveal that the effective moments for Fe$^{2+}$ and V$^{4+}$ in both compounds have large deviations from the conventional local moment model, which may possibly result from the formation of Fe/V metal-metal bondings. Furthermore the resistivity of both FVT and V$_{4.64}$Te$_4$ exhibits semiconducting-like temperature-dependent behavior but with average values close to typical bad metals, which resembles the transport behavior in the normal state of Fe-based superconductors. These quasi-1D compounds have shown interesting physical properties for future condensed matter physics research.