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Electron spins in van der Waals materials are playing a crucial role in recent advances in condensed-matter physics and spintronics. However, nuclear spins in van der Waals materials remain an unexplored quantum resource. Here we report optical polarization and coherent control of nuclear spins in a van der Waals material at room temperature. We use negatively charged boron vacancy ([Formula: see text]) spin defects in hexagonal boron nitride to polarize nearby nitrogen nuclear spins. We observe the Rabi frequency of nuclear spins at the excited-state level anti-crossing of [Formula: see text] defects to be 350 times larger than that of an isolated nucleus, and demonstrate fast coherent control of nuclear spins. Further, we detect strong electron-mediated nuclear-nuclear spin coupling that is five orders of magnitude larger than the direct nuclear-spin dipolar coupling, enabling multi-qubit operations. Our work opens new avenues for the manipulation of nuclear spins in van der Waals materials for quantum information science and technology.

Chirality generates spontaneous symmetry breaking and profoundly influences the topology, charge, and spin orders of materials. The chiral charge density wave (CDW) exhibits macroscopic chirality in the achiral crystal during the spontaneous electronic phase transitions. However, the mechanism of chiral CDW formation is shrouded in controversy. In this work, we report that two-dimensional

Despite the recognition of two-dimensional (2D) systems as emerging and scalable host materials of single-photon emitters or spin qubits, the uncontrolled, and undetermined chemical nature of these quantum defects has been a roadblock to further development. Leveraging the design of extrinsic defects can circumvent these persistent issues and provide an ultimate solution. Here, we established a complete theoretical framework to accurately and systematically design quantum defects in wide-bandgap 2D systems. With this approach, essential static and dynamical properties are equally considered for spin qubit discovery. In particular, many-body interactions such as defect–exciton couplings are vital for describing excited state properties of defects in ultrathin 2D systems. Meanwhile, nonradiative processes such as phonon-assisted decay and intersystem crossing rates require careful evaluation, which competes together with radiative processes. From a thorough screening of defects based on first-principles calculations, we identify promising single-photon emitters such as SiVV and spin qubits such as TiVV and MoVV in hexagonal boron nitride. This work provided a complete first-principles theoretical framework for defect design in 2D materials.

Antiferromagnetic insulators are a ubiquitous class of magnetic materials, holding the promise of low-dissipation spin-based computing devices that can display ultra-fast switching and are robust against stray fields. However, their imperviousness to magnetic fields also makes them difficult to control in a reversible and scalable manner. Here we demonstrate a novel proof-of-principle ionic approach to control the spin reorientation (Morin) transition reversibly in the common antiferromagnetic insulator α-Fe2O3 (haematite) – now an emerging spintronic material that hosts topological antiferromagnetic spin-textures and long magnon-diffusion lengths. We use a low-temperature catalytic-spillover process involving the post-growth incorporation or removal of hydrogen from α-Fe2O3 thin films. Hydrogenation drives pronounced changes in its magnetic anisotropy, Néel vector orientation and canted magnetism via electron injection and local distortions. We explain these effects with a detailed magnetic anisotropy model and first-principles calculations. Tailoring our work for future applications, we demonstrate reversible control of the room-temperature spin-state by doping/expelling hydrogen in Rh-substituted α-Fe2O3.

A few two-dimensional (2D) magnets have an intrinsic easy axis, which is essential for long–range magnetic ordering required for applications. Here, we show that in the absence of external magnetic fields, uniaxial strains can stabilize long–range ferromagnetic ordering in a 2D electrene, LaBr2, by effectively changing its magnetic anisotropy from the original easy plane to an easy axis. Importantly, such manipulations do not affect the unique properties of its magnetic anionic electrons. The strain-dependent magnetic anisotropy is further understood by the Bruno's model. Monte Carlo simulations directly show an absence of collective magnetism in the pristine monolayer of LaBr2, but the emergence of long–range magnetic ordering with high Curie temperatures when uniaxial strains were applied. Our results pave way to utilize 2D magnetic materials with interesting properties in the absence of magnetic anisotropy for practical applications.

Lieb lattice, a two-dimensional edge-centered square lattice, has attracted considerable interest due to its exotic electronic and topological properties. Although various optical and photonic Lieb lattices have been experimentally demonstrated, it remains challenging for an electronic Lieb lattice to be realized in real material systems. Here, based on first-principles calculations and tight-binding modeling, a silver sulfide (Ag2S) monolayer is reported as a long-sought-after inorganic electronic Lieb lattice. This Lieb-lattice Ag2S is further found to be ultrasoft, which enables its electronic properties and topological states near the Fermi level to be finely tuned, as evidenced by the strain-induced topologically non-trivial edge states near the valence band edge. These results not only provide an ideal platform to further explore and harvest interesting quantum properties but also pave a way to pursue other inorganic electronic Lieb lattices in a broader material domain.

Magnetism in monolayer (ML) VSe2 has attracted broad interest in spintronics, while existing reports have not reached consensus. Using element-specific X-ray magnetic circular dichroism, a magnetic transition in ML VSe2 has been demonstrated at the contamination-free interface between Co and VSe2. Through interfacial hybridization with a Co atomic overlayer, a magnetic moment of about 0.4 NB per V atom in ML VSe2 is revealed, approaching values predicted by previous theoretical calculations. Promotion of the ferromagnetism in ML VSe2 is accompanied by its antiferromagnetic coupling to Co and a reduction in the spin moment of Co. In comparison to the absence of this interface-induced ferromagnetism at the Fe/ML MoSe2 interface, these findings at the Co/ML VSe2 interface provide clear proof that the ML VSe2, initially with magnetic disorder, is on the verge of magnetic transition.

High-intensity short-pulse lasers have made possible the generation of energetic proton beams, unlocking numerous applications in high energy density science. One such application is uniform and isochoric heating of materials to the warm dense matter (WDM) state. We have developed a new experimental platform to simultaneously create and probe WDM at the matter in extreme conditions (MEC) end station at the Linac Coherent Light Source (LCLS). The short pulse optical laser (delivering up to 1 J in 45 fs) and the ultrabright LCLS X-ray laser with tunable frequency, respectively, deliver high power required to heat materials to WDM and precision-timed high-resolution X-rays to probe them. The laser-accelerated proton beam driven from a flat 1.5- $\mu \text{m}$ Cu foil was first measured then directed to a secondary sample of Al or polypropylene (PP), typically 300– $400~\mu \text{m}$ away. The time evolution of the sample electron temperature was measured using streaked optical pyrometry, where we observed a peak temperature of 0.9 ± 0.15 eV on the rear surface of an Al sample heated by the proton beam. Simulations using the hybrid-PIC code LSP and the rad-hydro code HELIOS show that a measured proton beam can heat Al to approximately 4 eV and PP to 1 eV if instead focused by a hemispherical Cu target. Through additional LSP simulations, we anticipate creating hotter WDM states (~20 eV) by increasing the laser energy to 10 J and keeping the other laser parameters fixed.

The development of infrared photodetectors is mainly limited by the choice of available materials and the intricate crystal growth process. Moreover, thermally activated carriers in traditional III-V and II-VI semiconductors enforce low operating temperatures in the infrared photodetectors. Here we demonstrate infrared photodetection enabled by interlayer excitons (ILEs) generated between tungsten and hafnium disulfide, WS2/HfS2. The photodetector operates at room temperature and shows an even higher performance at higher temperatures owing to the large exciton binding energy and phonon-assisted optical transition. The unique band alignment in the WS2/HfS2 heterostructure allows interlayer bandgap tuning from the mid- to long-wave infrared spectrum. We postulate that the sizeable charge delocalization and ILE accumulation at the interface result in a greatly enhanced oscillator strength of the ILEs and a high responsivity of the photodetector. The sensitivity of ILEs to the thickness of two-dimensional materials and the external field provides an excellent platform to realize robust tunable room temperature infrared photodetectors. Agency for Science, Technology and Research (A*STAR) Ministry of Education (MOE) National Research Foundation (NRF) Accepted version The work is supported by the Agency for Science, Technology and Research (A*STAR) under the 2D Materials Pharos Program (grant no. 152 700014 and grant no. 152 700017). Q.J.W. acknowledges funding from the National Research Foundation Competitive Research Program (NRF-CRP18-2017-02 and NRF–CRP19–2017–01). K.S.T. acknowledges support from the Center for Nanostructured Graphene (CNG) under the Danish National Research Foundation (project DNRF103) and from the European Research Council (ERC) under the European Union’s Horizon 2020 research and innovation programme (grant no. 773122, LIMA). G.L. acknowledges the supported under the grant MOE2017-T2-1-114. H.L. acknowledges the support by the Ministry of Science and Technology (MOST) in Taiwan under grant no. MOST 109-2112-M-001-014-MY3. J.T. and S. Lukman thank C. W. Lee, A. Ngo and M. Zhao for their valuable inputs and K Hippalgaonkar for sharing tools in the device fabrication.

Electrical control of magnetism in van der Waals ferromagnetic semiconductors is an important step in creating novel spintronic devices, capable of processing and storing information, with these materials. For practical devices, electrical control at or near room temperature is sought, but most layered ferromagnetic semiconductors exhibit Curie temperatures below 100 K. Here, we show that electrostatic gating of thin chromium germanium telluride (Cr2Ge2Te6) crystals can be used to modulate the magnetic phase transition and magnetic anisotropy of this layered ferromagnetic semiconductor and increase its Curie temperature. Using an electric double-layer transistor device, we observe ferromagnetism in the material at temperatures up to 200 K and find that its magnetic easy axis is in the in-plane direction, in contrast to the out-of-plane easy axis of undoped Cr2Ge2Te6. Our analysis suggests that heavy doping promotes a double-exchange mechanism that is mediated by free carriers, which dominates over the superexchange mechanism of the original insulating state. Electrostatic gating can be used to modulate the magnetic anisotropy of chromium germanium telluride, a layered ferromagnetic semiconductor, and increase its Curie temperature to 200 K.

Designing new quantum materials with long-lived electron spin states urgently requires a general theoretical formalism and computational technique to reliably predict intrinsic spin relaxation times. We present a new, accurate and universal first-principles methodology based on Lindbladian dynamics of density matrices to calculate spin-phonon relaxation time ($\tau_s$) of solids with arbitrary spin mixing and crystal symmetry. This method describes contributions of Elliott-Yafet (EY) and D'yakonov-Perel' (DP) mechanisms to spin relaxation for systems with and without inversion symmetry on an equal footing. We show that intrinsic spin and momentum relaxation times both decrease with increasing temperature; however, for the DP mechanism, spin relaxation time varies inversely with extrinsic scattering time. We predict large anisotropy of spin lifetime in transition metal dichalcogenides. The excellent agreement with experiments for a broad range of materials underscores the predictive capability of our method for properties critical to quantum information science., Comment: 12 pages, 7 figures

Electronic products have been following light, thin, short, small as goals. In recent years, not only do these features have to provide more functionality and reliability. In response to this demand, many new processes such as wafer-level 7 nm euv and electronic packaging solutions have been developed in the market. Stacked wafer technology has been widely used in electronic packaging solutions in a variety of storage devices and electronic products. The accompanying problems and challenges continue to emerge, in which the delamination of the package failure mode leads to the inability of electronic products to operate as the biggest issue. This study is mainly to investigate the thermal stress behavior of the vertical stacking of chip bonds of wafer adhesives to reduce the thickness of the wafer in the stacked wafer structure to Improve package reliability by reducing the amount of deformation Utilize one-half symmetry model and adopt the reflow profile of JESD22-a113 (25 °C ~ 260 °C) As a basis and import into the ansys software for parametric development, Then use the Taguchi experiment method to configure the experimental parameters to explore the optimization parameters. Finally, the experimental results and the delamination results were verified by the Taguchi experiment method, and the stress shrinkage gradient model was introduced to find the next best potential factor for reducing the maximum stress, such as binder material Tg and Young's modulus compensation thermal expansion system. Observe the thermal stress behavior of stacked chips and help provide a reference for providing modified changes during development.

This study used cold forging to produce car components with the desired hardness without using postprocessing methods such as heat treatment, surface blasting, and polishing. Material diameter, mold neck diameter, and hardness of the material after annealing were used as parameters, and nine sets of experimental parameters were obtained using the Taguchi method. Under the premise of high-quality forging, this study determined the optimal hardness and the relationship between formation parameters and forging hardness. By inputting the hardness data obtained from the Taguchi L9 orthogonal array into a Matlab-implemented neural network, this study determined a hardness formula. Finally, using the inbuilt graphical user interface software of Matlab, a simple program was written that can be used to predict hardness and that could extensively reduce the costs and time associated with forging development.

Shrinking the size of a bulk metal into nanoscale leads to the discreteness of electronic energy levels, the so-called Kubo gap δ. Renormalization of the electronic properties with a tunable and size-dependent δ renders fascinating photon emission and electron tunneling. In contrast with usual three-dimensional (3D) metal clusters, here we demonstrate that Kubo gap δ can be achieved with a two-dimensional (2D) metallic transition metal dichalcogenide (i.e., 1T′-phase MoTe 2 ) nanocluster embedded in a semiconducting polymorph (i.e., 1H-phase MoTe 2 ). Such a 1T′/1H MoTe 2 nanodomain resembles a 3D metallic droplet squeezed in a 2D space which shows a strong polarization catastrophe while simultaneously maintaining its bond integrity, which is absent in traditional δ-gapped 3D clusters. The weak screening of the host 2D MoTe 2 leads to photon emission of such pseudometallic systems and a ballistic injection of carriers in the 1T′/1H/1T′ homojunctions which may find applications in sensors and 2D reconfigurable devices.

In this paper, we present the design and fabrication of a novel class of emerging waveguide filters based on chained-functions at the millimeter-wave band. The derivation of chained-functions by chaining of prescribed generalized Chebyshev seed functions based on the partition theory is presented in details, and the implementation to waveguide technology is proposed and evaluated. The waveguide filter is fabricated through two different technologies, namely the Computer Numerical Control (CNC) milling technology and the Direct Metal Laser Sintering (DMLS) based additive manufacturing technology. The chained-function filters, which lie in between the Butterworth and Chebyshev filters, inherit the salient properties of both Butterworth and Chebyshev filters. Therefore, the chained-function waveguide filter exhibits filtering responses that have a superior rejection property and a lower loss with reduced sensitivity to fabrication tolerance than the standard Chebyshev waveguide filter. The efficiency of the proposed waveguide filter is confirmed both theoretically and empirically, using the CNC and DMLS processes. The issues of a higher manufacturing tolerance and apparent surface roughness associated with the DMLS method are found to be electrically insignificant when the chained-function concept is adopted in waveguide filter design. In general, the measured results of all the realized waveguide filters agree well to those of the simulation models. These results positively demonstrate that the chainedfunction concept has robust properties for rapid, high-performance, low-cost, and sustainable filter design and implementation, particularly for higher millimeter-wave frequency bands and for narrowband applications. © 2020.

The strong interaction between charge and lattice vibration gives rise to a polaron, which has a profound effect on optical and transport properties of matters. In magnetic materials, polarons are involved in spin dependent transport, which can be potentially tailored for spintronic and opto-spintronic device applications. Here, we identify the signature of ultrafast formation of polaronic states in CrBr3. The polaronic states are long-lived, having a lifetime on the time scale of nanoseconds to microseconds, which coincides with the emission lifetime of ∼4.3 μs. Transition of the polaronic states is strongly screened by the phonon, generating a redshift of the transition energy ∼0.2 eV. Moreover, energy-dependent localization of polaronic states is discovered followed by transport/annihilation properties. These results shed light on the nature of the polarons and their formation and transport dynamics in layered magnetic materials, which paves the way for the rational design of two-dimensional magnetic devices. Ministry of Education (MOE) National Research Foundation (NRF) Published version H.S. and T.Y. acknowledge the support from the Singapore National Research Foundation via Competitive Research Programme (NRF-CRP21-2018-0007 and NRF-CRP23-2019-0007). Y.H. acknowledges financial support from the Knut and Alice Wallenberg Foundation (KAW). Z.S. is supported by project LTAUSA19034 from Ministry of Education Youth and Sports (MEYS). J.Y. and Y.F. are supported by the Ministry of Education, Singapore, under its MOE AcRF Tier 3 Award MOE2018-T3-1-002.

Spin relaxation and decoherence is at the heart of spintronics and spin-based quantum information science. Currently, theoretical approaches that can accurately predict spin relaxation of general solids including necessary scattering pathways and capable for ns to ms simulation time are urgently needed. We present a first-principles real-time density-matrix approach based on Lindblad dynamics to simulate ultrafast spin dynamics for general solid-state systems. Through the complete first-principles descriptions of pump, probe and scattering processes including electron-phonon, electron-impurity and electron-electron scatterings with self-consistent electronic spin-orbit couplings, our method can directly simulate the ultrafast pump-probe measurements for coupled spin and electron dynamics over ns at any temperatures and doping levels. We first apply this method to a prototypical system GaAs and obtain excellent agreement with experiments. We find that the relative contributions of different scattering mechanisms and phonon modes differ considerably between spin and carrier relaxation processes. In sharp contrast to previous work based on model Hamiltonians, we point out that the electron-electron scattering is negligible at room temperature but becomes dominant at low temperatures for spin relaxation in n-type GaAs. We further examine ultrafast dynamics in novel spin-valleytronic materials - monolayer and bilayer WSe2 with realistic defects. We find that spin relaxation is highly sensitive to local symmetry and chemical bonds around defects. Our work provides a predictive computational platform for spin dynamics in solids, which has unprecedented potentials for designing new materials ideal for spintronics and quantum information technology., Comment: 10 pages, 8 figures

Based on the high frequency of concurrent adenomatous polyposis coli (APC) and KRAS mutations and their strong cooperative interaction in human colorectal cancer (CRC) promotion, we herein develop a CRISPR-Cas9-based genome-editing nanomedicine to target both APC and KRAS mutations for the treatment of CRC. To this end, a hyaluronic acid (HA)-decorated phenylboronic dendrimer (HAPD) was designed for the targeted delivery of Cas9 ribonucleoprotein (RNP), by which both APC and KRAS genetic mutations harboring in CRC cells can be synergistically disrupted. Systemic administration of Cas9 RNP targeting APC and KRAS enabled by HAPD significantly inhibits tumor growth on xenografted and orthotopic CRC mouse models and also greatly prevents CRC-induced liver metastasis and lung metastasis. Thus, this duplex genome-editing system provides a promising gene therapy strategy for the treatment of human CRC and can be extended to other types of cancers with activated Wnt/β-catenin and RAS/extracellular signal-regulated kinase (ERK) pathways.

Through First-Principles real-time Density-Matrix (FPDM) dynamics simulations, we investigate spin relaxation due to electron-phonon and electron-impurity scatterings with spin-orbit coupling in two-dimensional Dirac materials - silicene and germanene, at finite temperatures and under external fields. We discussed the applicability of conventional descriptions of spin relaxation mechanisms by Elliott-Yafet (EY) and D'yakonov-Perel' (DP) compared to our FPDM method, which is determined by a complex interplay of intrinsic spin-orbit coupling, external fields, and electron-phonon coupling strength, beyond crystal symmetry. For example, the electric field dependence of spin relaxation time is close to DP mechanism for silicene at room temperature, but rather similar to EY mechanism for germanene. Due to its stronger spin-orbit coupling strength and buckled structure in sharp contrast to graphene, germanene has a giant spin lifetime anisotropy and spin valley locking effect under nonzero Ez and relatively low temperature. More importantly, germanene has extremely long spin lifetime (~100 ns at 50 K) and ultrahigh carrier mobility, which makes it advantageous for spin-valleytronic applications., 9 pages, 4 figures

Designing 2D-materials that exhibit half-metallic properties is crucially important in spintronic devices that are used in low-power high-density logic circuits. The large pores in the C2N morphology can stably accommodate various configurations of transition-metal (TM) atoms that can lead to ferromagnetic (FMC) and anti-ferromagnetic coupling interactions among them, and thus paving the way for achieving half-metallic characteristics. In the present study, we use manganese ‘Mn’ as a promising catalyst and the spin-polarized density-functional theory to search for suitable configurations of metal atoms that yield half-metallicity. Test samples comprised of single-atom catalyst (SAC) and double-atom catalyst (DAC) of Mn embedded in a C2N sample of size 2 × 2 primitive cells as well as their combinations in neighboring large pores (i.e. SAC–SAC, SAC–DAC, and DAC–DAC). Tests were extended to screen many other TM catalysts and the results showed the existence of half metallicity in just five cases: (a) C2N:Mn (DAC, SAC–SAC, and SAC–DAC); (b) C2N:Fe (DAC); and (c) C2N:Ni (SAC–DAC). Our results further showed the origins of half-metallicity to be attributed to FMC interactions between the catalysts with the six mirror images, formed by the periodic-boundary conditions. The FMC interaction is found to have strength of about 20 meV and critical length scale up to about ∼21–29 Å, dependent on both the type of magnetic impurity and the synergetic effects. The potential relevance of half-metallicity to spintronic device application is discussed. Our theoretical results have been benchmarked to the available data in literature and they were found to be in good agreements.

Integrating multiple properties in a single system is crucial for the continuous developments in electronic devices. However, some physical properties are mutually exclusive in nature. Here, we report the coexistence of two seemingly mutually exclusive properties-polarity and two-dimensional conductivity-in ferroelectric Ba$_{0.2}$Sr$_{0.8}$TiO$_3$ thin films at the LaAlO$_3$/Ba$_{0.2}$Sr$_{0.8}$TiO$_3$ interface at room temperature. The polarity of a ~3.2 nm Ba$_{0.2}$Sr$_{0.8}$TiO$_3$ thin film is preserved with a two-dimensional mobile carrier density of ~0.05 electron per unit cell. We show that the electronic reconstruction resulting from the competition between the built-in electric field of LaAlO$_3$ and the polarization of Ba$_{0.2}$Sr$_{0.8}$TiO$_3$ is responsible for this unusual two-dimensional conducting polar phase. The general concept of exploiting mutually exclusive properties at oxide interfaces via electronic reconstruction may be applicable to other strongly-correlated oxide interfaces, thus opening windows to new functional nanoscale materials for applications in novel nanoelectronics., Comment: Main text: 25 pages, 4 figures Supplementary note: 19 pages, 11 figures

We report a large interfacial perpendicular magnetic anisotropy (PMA) in [Fe2CoSi/Pt]n (FCS/Pt) multilayers deposited on thermally oxidized Si substrates. A maximum anisotropy energy density, Ku, of 2.64 Merg/cm3 is achieved with an optimized stack. We are able to tune the PMA by adjusting the Pt and FCS film thicknesses and number of periods of the multilayer structure, as these significantly affect the lattice structure of FCS/Pt stack. Both high-resolution transmission electron microscopy and structural relaxation of the atomistic model using first-principles calculations reveal that while the multilayer structure assumes a monoclinic structure (α = 84°), the FCS films undergo a local orthorhombic distortion from the bulk structure due to the strain imposed by the FCS/Pt interface. By analyzing the orbital-resolved density of states of the system, we propose that both the orthorhombic distortion of the FCS and orbital interactions between interface Pt and Fe atoms are responsible for the high PMA. For ...

The interplay between dimensionality and anisotropicity leads to intriguing optoelectronic properties and exciton dynamics in low dimensional semiconductors. In this study we use nanostructured phosphorene as a prototypical example to unfold such complex physics and develop a general first-principles framework to study exciton dynamics in low dimensional systems. Specifically we derived the radiative lifetime and light emission intensity from 2D to 0D systems based on many-body perturbation theory, and investigated the dimensionality and anisotropicity effects on radiative recombination lifetime both at 0 K and finite temperature, as well as polarization and angle dependence of emitted light. We show that the radiative lifetime at 0 K increases by an order of $10^3$ with the lowering of one dimension (i.e. from 2D to 1D nanoribbons or from 1D to 0D quantum dots). We also show that obtaining the radiative lifetime at finite temperature requires accurate exciton dispersion beyond the effective mass approximation. Finally, we demonstrate that monolayer phosphorene and its nanostructures always emit linearly polarized light consistent with experimental observations, different from in-plane isotropic 2D materials like MoS2 and h-BN that can emit light with arbitrary polarization, which may have important implications for quantum information applications.

The realization of long-range magnetic ordering in 2D systems can potentially revolutionize next-generation information technology. Here, the successful fabrication of crystalline Cr3 Te4 monolayers with room temperature (RT) ferromagnetism is reported. Using molecular beam epitaxy, the growth of 2D Cr3 Te4 films with monolayer thickness is demonstrated at low substrate temperatures (≈100 °C), compatible with Si complementary metal oxide semiconductor technology. X-ray magnetic circular dichroism measurements reveal a Curie temperature (Tc ) of v344 K for the Cr3 Te4 monolayer with an out-of-plane magnetic easy axis, which decreases to v240 K for the thicker film (≈7 nm) with an in-plane easy axis. The enhancement of ferromagnetic coupling and the magnetic anisotropy transition is ascribed to interfacial effects, in particular the orbital overlap at the monolayer Cr3 Te4 /graphite interface, supported by density-functional theory calculations. This work sheds light on the low-temperature scalable growth of 2D nonlayered materials with RT ferromagnetism for new magnetic and spintronic devices.

Manipulation of the valley degree of freedom provides a novel paradigm in quantum information technology. In this work, through first principles calculations, we demonstrate that monolayer $\mathrm{Gd}{\mathrm{I}}_{2}$ is a promising candidate material for valleytronic applications. Monolayer $\mathrm{Gd}{\mathrm{I}}_{2}$ can be easily exfoliated from bulk, and it is spontaneously valley polarized with a giant splitting of 149 meV due to its intrinsic ferromagnetism and large spin orbital coupling. The anomalous valley Hall effect could be realized in monolayer $\mathrm{Gd}{\mathrm{I}}_{2}$ by an appropriate external electric field. Furthermore, the valley polarization feature is stable against the biaxial in-plane strain. Our findings provide an extraordinary and potential material platform for experimental studies and practical applications in the emergent field of valleytronics.

The complex oxide heterostructures such as LaAlO3/SrTiO3 (LAO/STO) interface are paradigmatic platforms to explore emerging multi-degrees of freedom coupling and the associated exotic phenomena. In this study, we reveal the effects of multiorbital and magnetic ordering on Rashba spin-orbit coupling (SOC) at the LAO/STO (001) interface. Based on first-principles calculations, we show that the Rashba spin splitting near the conduction band edge can be tuned substantially by the interfacial insulator-metal transition due to the multiorbital effect of the lowest t_2g bands. We further unravel a competition between Rashba SOC and intrinsic magnetism, in which the Rashba SOC induced spin polarization is suppressed by the interfacial magnetic ordering. These results deepen our understanding of intricate electronic and magnetic reconstruction at the perovskite oxide interfaces and shed light on the engineering of oxide heterostructures for all-oxides-based spintronic devices., 24 pages, 4 figures

The high recombination rate of photogenerated carriers is the bottleneck of photocatalysis, severely limiting the photocatalytic efficiency. Here, we develop a dipole-scheme (D-scheme for short) photocatalytic model and materials realization. The D-scheme heterojunction not only can effectively separate electrons and holes by a large polarization field, but also boosts photocatalytic redox reactions with large driving photovoltages and without any carrier loss. By means of first-principles and GW calculations, we propose a D-scheme heterojunction prototype with two real polar materials, PtSeTe/LiGaS2. This D-scheme photocatalyst exhibits a high capability of the photogenerated carrier separation and near-infrared light absorption. Moreover, our calculations of the Gibbs free energy imply a high ability of the hydrogen and oxygen evolution reaction by a large driving force. The proposed D-scheme photocatalytic model is generalized and paves a valuable route of significantly improving the photocatalytic efficiency., Comment: 10 pages, 5 figures

The phase stability and electronic properties of two-dimensional Si1-xGex alloys are investigated via the first-principles method in combination with the cluster expansion and Monte Carlo simulations. The calculated composition-temperature phase diagram indicates that at low temperatures (below 200 K) monolayer Si1-xGex alloys energetically favor phase separation, whereas when the temperature is increased above 550 K, Si1-xGex alloys can be stabilized and thereby form solid solutions across the whole composition range. Special quasi-random structures were constructed to model the monolayer Si1-xGex. The Si1-xGex alloys are found to possess a robust Dirac cone against composition variation. These results provide a guideline for the experimental realization of Si1-xGex alloys and monolayer Si1-xGex alloys are believed to hold great potential for realization of applications in nanoelectronics and nano-optoelectronics.

Two-dimensional (2D) chromium tellurides have attracted considerable research interest for their high Curie temperatures. Their magnetic properties have been found diverse in various experiments, the understanding of which however remains limited. In this work, we report that the magnetic ordering of ultrathin chromium tellurides is structure dependent and can be tuned by external strain. Based on first-principles calculations and Monte Carlo simulations, we show long-range stable magnetism with high and low Curie temperature, and short-range magnetism in 2D Cr5Te8, CrTe2, and Cr2Te3 layers, respectively. We further find that ferromagnetic-to-antiferromagnetic transition can be realized by 2% compressive strain for CrTe2 and 2% tensile strain for Cr2Te3, and their magnetic easy axis is tuned from out-of-plane to in-plane by the medium tensile and compressive strain. This strain dependent magnetic coupling is found to be related to Cr-Cr direct exchange and the change of magnetic anisotropy is understood by the atom and orbital resolved magnetic anisotropy energy and second order perturbation theory. Our results reveal the important roles of the structure and strain in determining the magnetic ordering in 2D chromium telluride, shedding light on understanding of the diverse magnetic properties observed in experiments.

Substrates have strong effects on optoelectronic properties of two-dimensional (2D) materials, which have emerged as promising platforms for exotic physical phenomena and outstanding applications. To reliably interpret experimental results and predict such effects at 2D interfaces, theoretical methods accurately describing electron correlation and electron-hole interaction such as first-principles many-body perturbation theory are necessary. In our previous work [Phys. Rev. B 102, 205113(2020)], we developed the reciprocal-space linear interpolation method that can take into account the effects of substrate screening for arbitrarily lattice-mismatched interfaces at the GW level of approximation. In this work, we apply this method to examine the substrate effect on excitonic excitation and recombination of 2D materials by solving the Bethe-Salpeter equation. We predict the nonrigid shift of 1s and 2s excitonic peaks due to substrate screening, in excellent agreements with experiments. We then reveal its underlying physical mechanism through 2D hydrogen model and the linear relation between quasiparticle gaps and exciton binding energies when varying the substrate screening. At the end, we calculate the exciton radiative lifetime of monolayer hexagonal boron nitride with various substrates at zero and room temperature, as well as the one of WS2 where we obtain good agreement with experimental lifetime. Our work answers important questions of substrate effects on excitonic properties of 2D interfaces., Comment: 8 pages, 5 figures

Atomic orbitals play fundamental roles in the modern theory of magnetism, not only providing local moments via their partial occupation, but also offering exchange interactions through their direct or indirect hybridization. Here, we report atomic-orbital-free intrinsic ferromagnetism in monolayer electrides or electrenes, in which excess electrons act as anions. Taking the honeycomb ${\mathrm{LaBr}}_{2}$ (${\mathrm{La}}^{3+}{\mathrm{Br}}_{2}{}^{\ensuremath{-}}\ifmmode\cdot\else\textperiodcentered\fi{}{e}^{\ensuremath{-}}$) as an example, our first-principles calculations, in combination with a low-energy effective model in the basis of the Wannier function and Anderson's superexchange theory, reveal that the excess electron is localized at the center of the hexagon, which leads to the spontaneous formation of a local moment due to the strong Stoner instability of the associated state near the Fermi level (${E}_{f}$). The large off-site Coulomb interaction and extended tails of both wave and Wannier functions indicate a significant spatial extension of the anionic electron state in ${\mathrm{LaBr}}_{2}$. The overlap of the long tails mediates an extended ferromagnetic direct exchange to second-nearest neighbors (up to 7--8 \AA{}), in sharp contrast to the conventional direct exchange which is short ranged due to the overlap of atomic orbitals with limited spatial extension. The dual nature, localization and extension, of the anionic electron state results in a unique magnetic mechanism in such atomic-orbital-free intrinsic two-dimensional ferromagnets.

The ferroelectric switching effect on perpendicular magnetic anisotropy is examined for the case of the BaTiO3/L10-CoFe interface through first-principles calculations of film magnetocrystalline anisotropy energy (MAE), both with the frozen-potential method and the second-order perturbation theory. The ferroelectric switching-MAE relationship is shown to have opposite trends for BaO- and TiO2-terminated interfaces because of the distinct orbital interaction mechanisms predominant in each termination configuration. The ferroelectric switching effect, changes in Fe-O bond lengths, and termination constitute three different contributors to MAE change, each with a different penetration depth into the CoFe film. The top surface CoFe atoms are shown to feature a high density of minority-spin 3dxz states, which could play a role in influencing the ferroelectric switching-MAE relationship in cases where the top surface undergoes modifications.

Two-dimensional (2D) alloys represent a versatile platform that extends the properties of atomically thin transition-metal dichalcogenides. Here, using molecular beam epitaxy, we investigate the growth of 2D vanadium-molybdenum diselenide alloys, VxMo1-xSe2, on highly oriented pyrolytic graphite and unveil their structural, chemical, and electronic integrities via measurements by scanning tunneling microscopy/spectroscopy, synchrotron X-ray photoemission, and X-ray absorption spectroscopy (XAS). Essentially, we found a critical value of x = similar to 0.44, below which phase separation occurs and above which a homogeneous metallic phase is favored. Another observation is an effective increase in the density of mirror twin boundaries of constituting MoSe2 in the low V concentration regime (x

Electric-field control of magnetocrystalline anisotropy energy (MAE) is important for the optimal performance of the tunnel junction components of the STT-MRAM. In such a device, a high MAE of the free magnetic layer improves storage robustness, whereas a low MAE is also useful to keep energy expenditure in the switching process at a minimum. Using the frozen potential method to calculate the MAE of the CoFe layer, the electric-field control of MAE in the BaTiO3/CoFe/(Hf, Ta, W, Re, Os, Ir, Pt, or Au) heterostructure is studied. Electric field tuning of MAE is determined to be possible through switching the direction of BaTiO3 ferroelectric polarization, although both the tuning effect and the MAE depend strongly on the choice of the 5d transition metal element in the capping layer. The results predict a complicated behavior of both MAE and the underlayer polarization effect as we progress down the 5d series of elements as the choice of the capping layer element. Using the second-order perturbation theoretical framework, this behavior can nevertheless be explained by mechanisms including CoFe/capping layer interface hybridization and 5d band-filling trends in the capping layer.

The quasimetallic 1T′ phase 2D transition‐metal dichalcogenides (TMDs) consist of 1D zigzag metal chains stacked periodically along a single axis. This gives rise to its prominent physical properties which promises the onset of novel physical phenomena and applications. Here, the in‐plane electronic correlations are explored, and new mid‐infrared plasmon excitations in 1T′ phase monolayer WSe2 and MoS2 are observed using optical spectroscopies. Based on an extensive first‐principles study which analyzes the charge dynamics across multiple axes of the atomic‐layered systems, the collective charge excitations are found to disperse only along the direction perpendicular to the chains. Further analysis reveals that the interchain long‐range coupling is responsible for the coherent 1D charge dynamics and the spin–orbit coupling affects the plasmon frequency. Detailed investigation of these charge collective modes in 2D‐chained systems offers opportunities for novel device applications and has implications for the underlying mechanism that governs superconductivity in 2D TMD systems., New 1D mid‐infrared anisotropic plasmons are observed in the quasimetallic phase of WSe2 and MoS2 monolayers. In‐depth analysis reveals that the long‐range inter‐chain coupling is responsible for this 1D charge dynamics, and the plasmon energy is dictated by the effects of spin–orbit coupling. This study establishes an inextricable link between the 1D‐chain structure and charge dynamics in quasimetallic phase 2D transition‐metal dichalcogenides.

Two-dimensional (2D) materials1,2 and the associated van der Waals (vdW) heterostructures3-7 have provided great flexibility for integrating distinct atomic layers beyond the traditional limits of lattice-matching requirements, through layer-by-layer mechanical restacking or sequential synthesis. However, the 2D vdW heterostructures explored so far have been usually limited to relatively simple heterostructures with a small number of blocks8-18. The preparation of high-order vdW superlattices with larger number of alternating units is exponentially more difficult, owing to the limited yield and material damage associated with each sequential restacking or synthesis step8-29. Here we report a straightforward approach to realizing high-order vdW superlattices by rolling up vdW heterostructures. We show that a capillary-force-driven rolling-up process can be used to delaminate synthetic SnS2/WSe2 vdW heterostructures from the growth substrate and produce SnS2/WSe2 roll-ups with alternating monolayers of WSe2 and SnS2, thus forming high-order SnS2/WSe2 vdW superlattices. The formation of these superlattices modulates the electronic band structure and the dimensionality, resulting in a transition of the transport characteristics from semiconducting to metallic, from 2D to one-dimensional (1D), with an angle-dependent linear magnetoresistance. This strategy can be extended to create diverse 2D/2D vdW superlattices, more complex 2D/2D/2D vdW superlattices, and beyond-2D materials, including three-dimensional (3D) thin-film materials and 1D nanowires, to generate mixed-dimensional vdW superlattices, such as 3D/2D, 3D/2D/2D, 1D/2D and 1D/3D/2D vdW superlattices. This study demonstrates a general approach to producing high-order vdW superlattices with widely variable material compositions, dimensions, chirality and topology, and defines a rich material platform for both fundamental studies and technological applications.

Herein, a low-temperature thermal decomposition method is utilized to grow new stable tetragonal Fe3O4-based thick ferrite films. The tetragonal Fe3O4-based film possesses high saturation magnetization of ∼800 emu/cm3. Doping with approximately 10% Co results in a high-energy product of ∼10.9 MGOe with perpendicular magnetocrystalline anisotropy, whereas doping with Ni increases electrical resistivity by a factor of 6 and retains excellent soft magnetic properties (high saturation magnetization and low coercivity). A combined experimental and first-principles study reveals that carbon interstitials (CiB) and oxygen vacancies (VO) form CiB–VO pairs which stabilize the tetragonal phase and enhance saturation magnetization. The magnetization enhancement is further attributed to local ferromagnetic coupling between FeA and FeB induced by CiB–VO pairs in a tetragonal spinel ferrite lattice.