Materials Science (cond-mat.mtrl-sci)

Abstract: Recent theoretical works on two-dimensional molybdenum disulfide, MoS$_2$, with sulfur vacancies predict that the suppression of thermal transport in MoS$_2$ by point defects is more prominent in monolayers and becomes negligible as layer number increases. Here, we investigate experimentally the thermal transport properties of two-dimensional molybdenum disulfide crystals with inherent sulfur vacancies. We study the first-order temperature coefficients of interlayer and intralayer Raman modes of MoS$_2$ crystals with different layer numbers and stacking orders. The in-plane thermal conductivity ($\kappa$) and total interface conductance per unit area ($ g $) across the 2D material-substrate interface of mono-, bi- and tri-layer MoS$_2$ samples are measured using the micro-Raman thermometry. Our results clearly demonstrate that the thermal conductivity is significantly suppressed by sulfur vacancies in monolayer MoS$_2$. However, this reduction in $\kappa$ becomes less evident as the layer number increases, confirming the theoretical predictions. No significant variation is observed in the $\kappa$ and $ g $ values of 2H and 3R stacked bilayer MoS$_2$ samples.

Abstract: The observation of room temperature ferromagnetism along with a low temperature paramagnetic counterpart in undoped Cu-Cu2O-rGO nanocomposite was demonstrated. A phenomenological approach was taken to explain the observations based on 3D Ising model for arbitrary spins generated due to Cu vacancy in the Cu2O system preferably at the interface.

Abstract: Chirality is an indispensable concept that pervades fundamental science and nature, manifesting itself in diverse forms such as chiral quasiparticles and chiral structures. Of particular interest are Weyl phonons carrying specific Chern numbers and chiral phonons doing circular motions in crystals. Up to now, Weyl and chiral phonons have been studied independently and the interpretations of chirality seem to be different in these two concepts, impeding our understanding. Here, we demonstrate that Weyl and chiral phonons are entangled in chiral crystals. Employing a typical chiral crystal of elementary tellurium (Te) as a case study, we expound on the intrinsic relationship between Chern number of Weyl phonons and pseudo-angular momentum (PAM) of chiral phonons. In light of the mutual coupling, we propose Raman scattering as a new technique to demonstrate the existence of Weyl phonons in Te, by detecting the chirality-induced energy splitting between the two constituent chiral phonon branches for Weyl phonons. By using the same experimental approach, we also observe the obstructed phonon surface states for the first time.

Abstract: Weak antilocalization (WAL) effect is commonly observed in 2D systems, or 3D topological insulators, topological semimetal systems. Here we report the clear sign of WAL effect in high quality Ta$_{0.7}$Nb$_{0.3}$Sb$_2$ single crystals, in below 50$^\circ$ K region. The chemical vapor transport method was employed to grow the single crystal samples, the high crystallization quality and uniform element distribution are verified by X-ray diffractions and electron microscopy techniques. Employing the Hall effect and two-band model fitting, the high carrier mobility (> 1000 cm$^2$V$^{-1}$s$^{-1}$ in 2 to 300$^\circ$ K region) and off-compensation electron/hole ratio are obtained. Due to the different angular dependence of WAL effect and the fermiology of Ta$_{0.7}$Nb$_{0.3}$Sb$_2$ single crystal, interesting magnetic-field-induced symmetry change is observed in angular magnetoresistance. These interesting transport properties will lead to more theoretical and applicational exploration in Ta$_{0.7}$Nb$_{0.3}$Sb$_2$ and related semimetal materials.

Abstract: Spin-orbit interaction (SOI) offers a nonferromagnetic scheme to realize spin polarization through utilizing an electric field. Electrically tunable SOI through electrostatic gates have been investigated, however, the relatively weak and volatile tunability limit its practical applications in spintronics. Here, we demonstrate the nonvolatile electric-field control of SOI via constructing ferroelectric Rashba architectures, i.e., 2D Bi2O2Se/PMN-PT ferroelectric field effect transistors. The experimentally observed weak antilocalization (WAL) cusp in Bi2O2Se films implies the Rashba-type SOI that arises from asymmetric confinement potential. Significantly, taking advantage of the switchable ferroelectric polarization, the WAL-to-weak localization (WL) transition trend reveals the competition between spin relaxation and dephasing process, and the variation of carrier density leads to a reversible and nonvolatile modulation of spin relaxation time and spin splitting energy of Bi2O2Se films by this ferroelectric gating. Our work provides a scheme to achieve nonvolatile control of Rashba SOI with the utilization of ferroelectric remanent polarization.

Abstract: As one of the most important n-type thermoelectric (TE) materials, Bi2Te3 has been studied for decades, with efforts to enhance the thermoelectric performance based on element doping, band engineering, etc. In this study, we report a novel bulk-insulating topological material system as a replacement for n-type Bi2Te3 materials: V doped Bi1.08Sn0.02Sb0.9Te2S (V:BSSTS) . The V:BSSTS is a bulk insulator with robust metallic topological surface states. Furthermore, the bulk band gap can be tuned by the doping level of V, which is verified by magnetotransport measurements. Large linear magnetoresistance is observed in all samples. Excellent thermoelectric performance is obtained in the V:BSSTS samples, e.g., the highest figure of merit ZT of ~ 0.8 is achieved in the 2% V doped sample (denoted as V0.02) at 550 K. The high thermoelectric performance of V:BSSTS can be attributed to two synergistic effects: (1) the low conductive secondary phases Sb2S3, and V2S3 are believed to be important scattering centers for phonons, leading to lower lattice thermal conductivity; and (2) the electrical conductivity is increased due to the high-mobility topological surface states at the boundaries. In addition, by replacing one third of costly tellurium with abundant, low-cost, and less-toxic sulfur element, the newly produced BSSTS material is inexpensive but still has comparable TE performance to the traditional Bi2Te3-based materials, which offers a cheaper plan for the electronics and thermoelectric industries. Our results demonstrate that topological materials with unique band structures can provide a new platform in the search for new high performance TE materials.

Abstract: Ultrathin, solution-processed emerging solar cells with high power-per-weight (PPW) outputs demonstrate unique potential for applications where low weight, high power output, and flexibility are indispensable. The following perspective explores the literature of emerging PVs and highlights the maximum reported PPW values of Perovskite Solar Cells (PSCs) 29.4 W/g, Organic Solar Cells (OSCs) 32.07 W/g and Quantum Dot Solar Cells (QDSC) 15.02 W/g, respectively. The record PPW values of OSCs and PSCs are approximately one order of magnitude higher compared to their inorganic ultrathin solar cells counterparts (approx. 3.2 W/g for CIGS and a-Si). This consists emerging PVs, very attractive for a variety of applications where the PPW is the key parameter. In particular, both OSCs and PSCs can be implemented in different scenarios of applications (indoor and biocompatible applications for OSCs and outdoor and high-energy radiation conversion conditions for the PSCs) due to their unique optoelectronic and physiochemical properties. Finally, our theoretical optical and electrical simulation and optimization study for the most promising and well-suited PV technologies, showed an impressive maximum realistic theoretical PPW limit of 74.3 and 93.7 W/g for PSCs and OSCs, respectively. Our finding shows that the literature PSCs and OSCs towards high PPW outputs, is not quite close to the theoretical maximum and thus more work needs to be done to further increase the PPW output of these promising PV technologies.

Abstract: The current challenge to realizing continuously tunable magnetism lies in our inability to systematically change properties such as valence, spin, and orbital degrees of freedom as well as crystallographic geometry. Here, we demonstrate that ferromagnetism can be externally turned on with the application of low-energy helium implantation and subsequently erased and returned to the pristine state via annealing. This high level of continuous control is made possible by targeting magnetic metastability in the ultra-high conductivity, non-magnetic layered oxide PdCoO2 where local lattice distortions generated by helium implantation induce emergence of a net moment on the surrounding transition metal octahedral sites. These highly-localized moments communicate through the itinerant metal states which triggers the onset of percolated long-range ferromagnetism. The ability to continuously tune competing interactions enables tailoring precise magnetic and magnetotransport responses in an ultra-high conductivity film and will be critical to applications across spintronics.

Abstract: The experimental discovery of single-pulse ultrafast magnetization switching in ferrimagnetic alloys, such as GdFeCo and MnRuGa, opened the door to a promising route toward faster and more energy efficient data storage. A recent semi-phenomenological theory has proposed that a fast, laser-induced demagnetization below a threshold value puts the system into a dynamical regime where angular momentum transfer between sublattices dominates. Notably, this threshold scales inversely proportional to the number of exchange-coupled nearest neighbours considered in the model, which in the simplest case is directly linked to the underlying lattice structure. In this work, we study the role of the lattice structure on the laser-induced ultrafast magnetization switching in ferrimagnets by complementing the phenomenological theory with atomistic spin dynamics computer simulations. We consider a spin model of the ferrimagnetic GdFeCo alloy with increasing number of exchange-coupled neighbours. Within this model, we demonstrate that the laser-induced magnetization dynamics and switching depends on the lattice structure. Further, we determine that the critical laser energy for switching reduces for decreasing number of exchange-coupled neighbours.

Abstract: A nonperturbative dynamical coupling approach based on tight-binding molecular dynamics is used to evaluate the electron-ion (electron-phonon) coupling parameter in irradiated semiconductors as a function of the electronic temperature up to ~25,000 K. The method accounts for arbitrary electronic distribution function via the Boltzmann equation, enabling a comparative analysis of various models: fully equilibrium electronic distribution, band-resolved local equilibria (distinct temperatures and chemical potential of electrons in the valence and the conduction band), and a full nonequilibrium distribution. It is demonstrated that the nonequilibrium produces the electron-phonon coupling parameter different by at most ~35% from its equilibrium counterpart for identical deposited energy density, allowing to use the coupling parameter as a function of the single electronic equivalent (or kinetic) temperature. The following 14 semiconductors are studied here - group IV: Si, Ge, SiC; group III-V: AlAs, AlP, GaP, GaAs, GaSb; oxides: ZnO, TiO2, Cu2O; layered PbI2; ZnS and B4C.

Abstract: The rapid design of advanced materials is a topic of great scientific interest. The conventional, ``forward'' paradigm of materials design involves evaluating multiple candidates to determine the best candidate that matches the target properties. However, recent advances in the field of deep learning have given rise to the possibility of an ``inverse'' design paradigm for advanced materials, wherein a model provided with the target properties is able to find the best candidate. Being a relatively new concept, there remains a need to systematically evaluate how these two paradigms perform in practical applications. Therefore, the objective of this study is to directly, quantitatively compare the forward and inverse design modeling paradigms. We do so by considering two case studies of refractory high-entropy alloy design with different objectives and constraints and comparing the inverse design method to other forward schemes like localized forward search, high throughput screening, and multi objective optimization.