Materials Science (cond-mat.mtrl-sci)

Abstract: The extraordinary properties of a heterostructure by stacking atom-thick van der Waals (vdW) magnets have been extensively studied. However, the magnetocaloric effect (MCE) of heterostructures that are based on monolayer magnets remains to be explored. Herein, we deliberate MCE of vdW heterostructure composed of a monolayer CrI$_3$ and metal atomic layers (Ag, Hf, Au, and Pb). It is revealed that heterostructure engineering by introducing metal substrate can improve MCE of CrI$_3$, particularly boosting relative cooling power to 471.72 $\mu$Jm$^{-2}$ and adiabatic temperature change to 2.1 K at 5 T for CrI$_3$/Hf. This improved MCE is ascribed to the enhancement of magnetic moment and intralayer exchange coupling in CrI$_3$ due to the CrI$_3$/metal heterointerface induced charge transfer. Electric field is further found to tune MCE of CrI$_3$ in heterostructures and could shift the peak temperature by around 10 K in CrI$_3$/Hf, thus manipulating the working temperature window of MCE. The discovered electric-field and substrate regulated MCE in CrI$_3$/metal heterostructure opens new avenues for low-dimensional magnetic refrigeration.

Abstract: We study ferroelectric domain walls in barium titanate. We search for structurally nontrivial, so-called non-Ising domain walls, where the Polarisation is non-zero along the entire wall. Our approach enables us to find solutions for domain walls in any orientation, and the existence and energy of these walls depend on their particular orientation. We find that, across all phases of the material, there are orientations where the non-Ising walls have lower energy than Ising walls. The most interesting property of these domain walls is their non-monotonic interaction forces, allowing them to form stable domain-wall clusters rather than following standard behavior where domain walls annihilate or repel each other. We found the required external electric field to create the non-Ising configurations. Besides theoretical interest, this unconventional property of domain walls makes them a good candidate for memory application.

Abstract: Electrical switching of magnetization via spin-orbit torque (SOT) is of great potential in fast, dense, energy-efficient nonvolatile magnetic memory and logic technologies. Recently, enormous efforts have been stimulated to investigate switching of perpendicular magnetization in van der Waals systems that have unique, strong tunability and spin-orbit coupling effect compared to conventional metals. In this review, we first give a brief, generalized introduction to the spin-orbit torque and van der Waals materials. We will then discuss the recent advances in magnetization switching by the spin current generated from van der Waals materials and summary the progress in the switching of Van der Waals magnetization by the spin current.

Abstract: Water freezing is ubiquitous on Earth, affecting many areas from biology to climate science and aviation technology. Probing the atomic structure in the homogeneous ice nucleation process from scratch is of great value but still experimentally unachievable. Theoretical simulations have found that ice originates from the low-mobile region with increasing abundance and persistence of tetrahedrally coordinated water molecules. However, a detailed microscopic picture of how the disordered hydrogen-bond network rearranges itself into an ordered network is still unclear. In this work, we use a deep neural network (DNN) model to "learn" the interatomic potential energy from quantum mechanical data, thereby allowing for large-scale and long molecular dynamics (MD) simulations with ab initio accuracy. The nucleation mechanism and dynamics at atomic resolution, represented by a total of 36 $\mu$s-long MD trajectories, are deeply affected by the structural and dynamical heterogeneity in supercooled water. We find that imperfectly coordinated (IC) water molecules with high mobility pave the way for hydrogen-bond network rearrangement, leading to the growth or shrinkage of the ice nucleus. The hydrogen-bond network formed by perfectly coordinated (PC) molecules stabilizes the nucleus, thus preventing it from vanishing and growing. Consequently, ice is born through competition and cooperation between IC and PC molecules. We anticipate that our picture of the microscopic mechanism of ice nucleation will provide new insights into many properties of water and other relevant materials.

Abstract: Ren\'e 41 is a cast and wrought Ni-based superalloy with high yield strength and stress-rupture properties contrasted with poor processability. The aim of this thesis is to systematically investigate the influence of C and B microalloying additions on processability of Ren\'e 41. The first approach is an experimental one using hot compression testing and material characterisation. A second approach using machine learning methodology was also used to provide linkage for the experimental observations with industrial Ren\'e 41 materials based on ultrasonic defects and chemical composition. Three Ren\'e 41 variants with nominal, high C, and high B compositions were industrially fabricated and homogenized to be used in this study. The resultant flow stresses from hot compression testing were used to model hyperbolic sine constitutive equations. The activation energy for hot deformation was found to be 757, 728, and 697 kJmol-1 for the nominal, high B, and high C Ren\'e 41 variants respectively. Finite element method simulations based on the obtained flow curves found that effective plastic strain varied considerably through the sample geometry. Quantitative analysis via electron back-scatted diffraction found that while the three Ren\'e 41 variants have nearly identical recrystallised grain size, high C contain 64 vol.% recrystallised fractions compared to that of the nominal variant with 31 vol.% at the same deformation condition.

Abstract: We present an x-ray absorption spectroscopy study from the carbon $K$, sulfur $K$, and sulfur $L_{2,3}$ edges of crystalline oligothiophenes of varying length, i.e. bithiophene (2T), quaterthiophene (4T), and sexithiophene (6T), performed from first principles by means of all-electron density-functional theory and many-body perturbation theory. A comprehensive assignment of all relevant spectral features is performed based on the electronic structure and the character of the target conduction states. The inclusion of electron-hole effects leads to significant redistribution of oscillator strengths and to strongly bound excitons with binding energies ranging from 1.5 to 4.5 eV. When going from 2T to 6T, exciton binding energies decrease by up to 1 eV, which we attribute to the reduction of the average Coulomb attraction with increasing oligomer length. These high values are significantly larger than their counterparts in the optical excitations of these systems and indicative of their localization on the respective molecules. For the same reason, local-field effects which typically dominate the optical absorption of organic crystals, turn out to play only a negligible role at all edges. We identify two sets of carbon atoms, i.e. with or without sulfur bonding, which exhibit distinct features at the C $K$-edge. The sulfur atoms, on the other hand, yield similar contributions in the S, $K$, and $L_{2,3}$ edge spectra. Our results show excellent agreement with available experimental data.

Abstract: Hard and superhard materials are critical components in numerous industrial applications required for sustainable development. However, discovering new materials with high hardness is challenging, because hardness is a complex and multiscale property with a non-trivial connection to atomic properties of the material. Here, we present a low-dimensional physical descriptor for Vickers hardness derived from symbolic-regression artificial intelligence approach to data analysis. The descriptor is a mathematical combination of materials' properties that can be much easier evaluated than hardness itself via the atomistic simulations and it is therefore suitable for a high-throughput screening. The developed artificial intelligence model was trained on the experimental values of hardness and then high-throughput screening were performed among 635 compounds including binary, ternary, and quaternary transition-metal borides, carbides, nitrides, carbonitrides, carboborides, and boronitrides to find the optimal superhard material. The proposed descriptor is an analytic formula, which is physically interpretable, allowing us to get an insight into the multiscale relationship between atomic structure (i.e., micro) and hardness (i.e., macro). In details, we have found that the hardness is proportional to the Voigt-averaged bulk modulus and inversely proportional to the Poisson's ratio and Reuss-averaged shear modulus. Results of high-throughput search showed the possible way of tuning hardness of existing materials by making mixtures with harder, but metastable structures (e.g., metastable VN, TaN, ReN$_2$, Cr$_3$N$_4$, and ZrB$_6$ possess high hardness).

Abstract: Metal halide perovskites (MHPs) have shown an incredible rise in efficiency, reaching as high as 25.7%, which now competes with traditional photovoltaic technologies. Herein, we excluded CsX and RbX, the most commonly used cations to stabilize FAPbI3, from the bulk of perovskite thin films and applied them on the surface, as passivation agents. Extensive device optimization led to a power conversion efficiency (PCE) of 24.1% with a high fill factor (FF) of 82.2% upon passivation with CsI. We investigated in-depth the effect of CsI passivation on structural and optoelectronic properties using X-ray diffraction (XRD), angle resolved X-ray photoelectron spectroscopy (ARXPS), Kelvin Probe Force (KPFM) microscopy, time-resolved photoluminescence (TRPL), photoluminescence quantum yield (PLQY) and electroabsorption spectroscopy (TREAS). Furthermore, passivated devices exhibit enhanced operational stability, with optimized passivation with CsI leading to a retention of ~90% of initial PCE under 1 Sun illumination with maximum power point tracking for 600 h.

Abstract: Defects, i.e. inhomogeneities of the underlying lattice, are ubiquitous in magnetic materials and can have a crucial impact on their applicability in spintronic devices. For magnetic skyrmions, localized and topologically non-trivial spin textures, they give rise to a spatially inhomogeneous energy landscape and can lead to pinning, resulting in an exponentially increased dwell time at certain positions and typically a strongly reduced mobility. Using atomistic spin dynamics simulations, we reveal that under certain conditions defects can instead enhance thermal diffusion of ferromagnetic skyrmions. By comparing with results for the diffusion of antiferromagnetic skyrmions and using a quasi-particle description based on the Thiele equation, we demonstrate that this surprising finding can be traced back to the partial lifting of the impact of the topologigal gyrocoupling, which governs the dynamics of ferromagnetic skyrmions in the absence of defects.

Abstract: Ferroelectricity in sputtered undoped-HfO$_2$ is attractive for composition control for low power and non-volatile memory and logic applications. Unlike doped HfO$_2$, evolution of ferroelectricity with annealing and film thickness effect in sputter deposited undoped HfO$_2$ on Si is not yet reported. In present study, we have demonstrated the impact of post metallization annealing temperature and film thickness on ferroelectric properties in dopant-free sputtered HfO$_2$ on Si-substrate. A rich correlation of polarization with phase, lattice constant, and crystallite size and interface reaction is observed. First, anneal temperature shows o-phase saturation beyond 600 oC followed by interface reaction beyond 700 oC to show an optimal temperature window on 600-700 oC. Second, thickness study at the optimal temperature window shows an alluring o-phase crystallite scaling with thickness till a critical thickness of 20 nm indicating that the films are completely o-phase. However, the lattice constants (volume) are high in the 15-20 nm thickness range which correlates with the enhanced value of 2Pr. Beyond 20 nm, crystallite scaling with thickness saturates with the correlated appearance of m-phase and reduction in 2Pr. The optimal thickness-temperature window range of 15-20 nm films annealed at 600-700 oC show 2Pr of ~35.5 micro-C/cm$^2$ is comparable to state-of-the-art. The robust wakeup-free endurance of ~$10^$8 cycles showcased in the promising temperature-thickness window has been identified systematically for non-volatile memory applications.

Abstract: It is widely known that antiferromagnets (AFMs) display a high frequency response in the terahertz (THz) range, which opens up the possibility for ultrafast control of their magnetization for next generation data storage and processing applications. However, because the magnetization of the different sublattices cancel, their state is notoriously difficult to read. One way to overcome this is to couple AFMs to ferromagnets - whose state is trivially read via magneto-resistance sensors. Here we present conditions, using theoretical modelling, that it is possible to switch the magnetization of an AFM/FM bilayer using THz frequency pulses with moderate field amplitude and short durations, achievable in experiments. Consistent switching is observed in the phase diagrams for an order of magnitude increase in the interface coupling and a tripling in the thickness of the FM layer. We demonstrate a range of reversal paths that arise due to the combination of precession in the materials and the THz-induced fields. Our analysis demonstrates that the AFM drives the switching and results in a much higher frequency dynamics in the FM due to the exchange coupling at the interface. The switching is shown to be robust over a broad range of temperatures relevant for device applications.