Strain engineering provides the ability to control the ground states and associated phase transition in the epitaxial films. However, the systematic study of intrinsic characters and their strain dependency in transition-metal nitrides remains challenging due to the difficulty in fabricating the stoichiometric and high-quality films. Here we report the observation of electronic state transition in highly crystalline antiferromagnetic CrN films with strain and reduced dimensionality. Shrinking the film thickness to a critical value of ~ 30 unit cells, a profound conductivity reduction accompanied by unexpected volume expansion is observed in CrN films. The electrical conductivity is observed surprisingly when the CrN layer as thin as single unit cell thick, which is far below the critical thickness of most metallic films. We found that the metallicity of an ultrathin CrN film recovers from an insulating behavior upon the removal of as-grown strain by fabrication of first-ever freestanding nitride films. Both first-principles calculations and linear dichroism measurements reveal that the strain-mediated orbital splitting effectively customizes the relatively small bandgap at the Fermi level, leading to exotic phase transition in CrN. The ability to achieve highly conductive nitride ultrathin films by harness strain-controlling over competing phases can be used for utilizing their exceptional characteristics.
Short wavelength ultraviolet (UV-C) light deactivates DNA of any germs, including multiresistive bacteria and viruses like COVID-19. Two-dimensional (2D) material-based UV-C light emitting diodes can potentially be integrated into arbitrary surfaces to allow for shadow-free surface disinfection. In this work, we perform a series of first-principles calculations to identify the core components of ultrathin LEDs based on hexagonal boron nitride (hBN). The electrons and holes are predicted to be confined in multiple quantum wells (MQWs) by combining hBN layers with different stacking orders. Vari…
When combined with graphene, hexagonal boron nitride (h-BN) is an ideal substrate and gate dielectric with which to build metalh-BN|graphene field-effect devices. We use first-principles density functional theory (DFT) calculations for Cu|h-BN|graphene stacks to study how the graphene doping depends on the thickness of the h-BN layer and on a potential difference applied between Cu and graphene. We develop an analytical model that describes the doping very well, allowing us to identify the key parameters that govern the device behaviour. A predicted intrinsic doping of graphene is particularly…
The impact of oxygen vacancies on local tunneling properties across rf-sputtered MgO thin films was investigated by optical absorption spectroscopy and conducting atomic force microscopy. Adding O$_2$ to the Ar plasma during MgO growth alters the oxygen defect populations, leading to improved local tunneling characteristics such as a lower density of current hotspots and a lower tunnel current amplitude. We discuss a defect-based potential landscape across ultrathin MgO barriers.
Direct Realization of Near-Ideal Carbyne in Ultrathin Boron Nitride Nanotubes
Karlsruhe Institute of Technology（卡尔斯鲁厄理工学院）；Humboldt-Universität zu Berlin（柏林洪堡大学）；Center for the Science of Materials Berlin, Humboldt-Universität zu Berlin（柏林材料科学中心）；Politecnico di Milano（米兰理工大学）；Huzhou Normal University（湖州师范学院）
The defect-mediated hexagonal boron nitride (hBN) supercell display the visible optical spectra and electronic characteristics. The defects in the hBN supercell include the atomic vacancy, antisite, antisite vacancy, and substitution of a foreign atom for boron or nitrogen. The hBN supercell with VB, CB, and NB-VN has the high electron density of states across the Fermi level which indicates the high conductive electronic characteristics. The hBN with defects including atomic vacancy, antisite vacancy, and substitution of a foreign atom for boron or nitride exhibit the distinct spin-resolved o…
We investigate tunneling in metal-insulator-metal junctions employing few atomic layers of hexagonal boron nitride (hBN) as the insulating barrier. While the low-bias tunnel resistance increases nearly exponentially with barrier thickness, subtle features are seen in the current-voltage curves, indicating marked influence of the intrinsic defects present in the hBN insulator on the tunneling transport. In particular, single electron charging events are observed, which are more evident in thicker-barrier devices where direct tunneling is substantially low. Furthermore, we find that annealing th…
Employing the density-functional theory with local density approximation, we show that the fully hydrogenated monolayer-hexagonal boron nitride (H$_2$BN) has a direct-band gap of 2.96 eV in the blue-light region while the pristine $\textit{h}$-BN has a wider indirect-band gap of 4.78 eV. The hole-doped H$_2$BN is stable at low carrier density ($n$) but becomes dynamically unstable at higher $n$. We predict that it is a phonon-mediated superconductor with a transition temperature ($T_c$) which can reach $\sim$31 K at $n$ of $1.5\times$ $10^{14}$ holes cm$^{-2}$ near the lattice instability. The…
Being one of the strongest materials, ternary TiSiN exhibits a very interesting family of binary transition metal nitride and silicide systems. A novel technique to fabricate morphologically fascinating nano and micro structures of TiSiN is reported here. The referred TiSiN films, majorly constituted with cubic TiN phase, are enriched with crystalline nanoparticles, micro-flowers and faceted micro-crystals which possess attractive functionalities towards plasmon mediated optoelectronic applications. Reactivity of titanium to silicon nitride based dielectric topping on the substrate at high tem…
The nanometer-scale size-dependent electronic transport properties of crystalline (c-) and amorphous (a-) germanium telluride (GeTe) ultrathin films sandwiched by titanium nitride (TiN) electrodes are investigated using ab initio molecular dynamics (AIMD), density functional theory (DFT), and Green's function calculations. We find that a-GeTe ultrathin films scaled down to about 38 Angstrom (12 atomic layers) still shows a band gap and the electrical conductance is mainly due to electron transport via intra-gap states. If the ultrathin films are further scaled, the a-GeTe band gap disappears d…
Ultrathin cerium oxide films have been deposited on chlorine, gallium, and silver passivated Si(111) by reactive molecular beam epitaxy in a comparative study. The crystallinity of these films has been characterized by x-ray standing waves while the oxidation state of the rare-earth oxide (REOx) films and the chemical interface composition have been revealed by hard x-ray photoelectron spectroscopy. The use of Cl as passivating agent results in the epitaxial growth of highly crystalline REOx films with the RE metal in the 3+ oxidation state while effectively suppressing silicate and silicon ox…
Thermal detectors are a cornerstone of infrared (IR) and terahertz (THz) technology due to their broad spectral range. These detectors call for suitable broad spectral absorbers with minimalthermal mass. Often this is realized by plasmonic absorbers, which ensure a high absorptivity butonly for a narrow spectral band. Alternativly, a common approach is based on impedance-matching the sheet resistance of a thin metallic film to half the free-space impedance. Thereby, it is possible to achieve a wavelength-independent absorptivity of up to 50 %, depending on the dielectric properties of the unde…
The dewetting dynamics of an ultrathin film is studied in the presence of evaporation - or reaction - of adatoms on the substrate. KMC simulations are in good agreement with an analytical model with diffusion, rim facetting, and substrate sublimation. As sublimation is increased, we find a transition from the usual dewetting regime where the front slows down with time, to a sublimation-controlled regime where the front velocity is approximately constant. The rim width exhibits an unexpected non-monotonous behavior, with a maximum in time.
We report results of large-scale molecular-dynamics (MD) simulations of dynamic deformation under biaxial tensile strain of pre-strained single-crystalline nanometer-scale-thick face-centered cubic (fcc) copper films. Our results show that stacking faults, which are abundantly present in fcc metals, may play a significant role in the dissociation, cross-slip, and eventual annihilation of dislocations in small-volume structures of fcc metals. The underlying mechanisms are mediated by interactions within and between extended dislocations that lead to annihilation of Shockley partial dislocations…
Ionic gating is a powerful technique for tuning the physical properties of a material via electric field-induced charge doping, but is prone to introduce extrinsic disorder and undesired electrochemical modifications in the gated material beyond pure electrostatics. Conversely, reversible, volatile and electrostatic modulation is pivotal in the reliable design and operation of novel device concepts enabled by the ultrahigh induced charge densities attainable via ionic gating. Here we demonstrate a simple and effective method to achieve reversible and volatile gating of surface-sensitive ultrat…
The conversion of multilayer graphenes into sp^3-bonded carbon films on metal surfaces (through hydrogenation or fluorination of the outer surface of the top graphene layer) is indicated through first-principles computations. The main driving force for this conversion is the hybridization between carbon sp^3 orbitals and metal surface dz^2 orbitals. The induced electronic gap states in the carbon layers are confined in a region within 0.5 nm of the metal surface. Whether the conversion occurs depend on the fraction of hydrogenated (fluorinated) C atoms and on the number of stacked graphene lay…
Hexagonal boron nitride (h-BN) is unique among two-dimensional materials, with a large band gap (~6 eV) and high thermal conductivity (>400 W/m/K), second only to diamond among electrical insulators. Most electronic studies to date have relied on h-BN exfoliated from bulk crystals; however, for scalable applications the material must be synthesized by methods such as chemical vapor deposition (CVD). Here, we demonstrate single- and few-layer h-BN synthesized by CVD on single crystal platinum and on carbon nanotube (CNT) substrates, also comparing these films with h-BN deposited on the more com…
Magnetoelectric coupling between magnetic and electric dipoles is one of the cornerstones of modern physics towards developing the most energy-efficient magnetic data storage. Conventionally, magnetoelectric coupling is achieved in single-phase multiferroics or in magnetoelectric composite nanostructures consisting of ferromagnetic and ferroelectric/piezoelectric materials. Here, we demonstrate an electric-field-induced strain-mediated magnetoelectric effect in ultrathin CoFeB/MgO magnetic tunnel junction employing non-piezoelectric material, which is a vitally important structure for spintron…
Graphene and other two-dimensional (2D) materials have emerged as promising materials for broadband and ultrafast photodetection and optical modulation. These optoelectronic capabilities can augment complementary metal-oxide-semiconductor (CMOS) devices for high-speed and low-power optical interconnects. Here, we demonstrate an on-chip ultrafast photodetector based on a two-dimensional heterostructure consisting of high-quality graphene encapsulated in hexagonal boron nitride. Coupled to the optical mode of a silicon waveguide, this 2D heterostructure-based photodetector exhibits a maximum res…
The paper discusses the magnetic state of zeta phase of iron nitride viz. $ζ$-Fe$_2$N on the basis of spin polarized first principles electronic structure calculations together with a review of already published data. Results of our first principles study suggest that the ground state of $ζ$-Fe$_2$N is ferromagnetic (FM) with a magnetic moment of 1.528 $μ_\text{B}$ on the Fe site. The FM ground state is lower than the anti-ferromagnetic (AFM) state by 8.44 meV and non-magnetic(NM) state by 191 meV per formula unit. These results are important in view of reports which claim that $ζ$-Fe$_2$N und…
The scalable synthesis of two-dimensional (2D) hexagonal boron nitride (h-BN) is of great interest for its numerous applications in novel electronic devices. Highly-crystalline h-BN films, with single-crystal sizes up to hundreds of microns, are demonstrated via a novel Ni foam assisted technique reported here for the first time. The nucleation density of h-BN domains can be significantly reduced due to the high boron solubility, as well as the large specific surface area of the Ni foam. The crystalline structure of the h-BN domains is found to be well aligned with, and therefore strongly depe…
Time-resolved study of carbonization and growth of ultrathin 3C-SiC on Si(111) under ultra-high vacuum
Central European Institute of Technology, Brno University of Technology（中欧技术研究所，布尔诺理工大学）；Institute of Physical Engineering, Brno University of Technology（物理工程学院，布尔诺理工大学）
Single-atom-thick two-dimensional materials such as graphene usually have a hexagonal lattice while the square-planar lattice is uncommon in the family of two-dimensional materials. Here, we demonstrate that single-atom-thick transition metal nitride CrN$_4$ monolayer is a stable free-standing layer with a square-planar network. The stability of square-planar geometry is ascribed to the combination of N=N double bond, Cr-N coordination bond, and $π$-d conjugation, in which the double $π$-d conjugation is rarely reported in previous studies. This mechanism is entirely different from that of the…
Nitrogen-Vacancy-Mediated Magnetism in Sputtered GdN Thin Films
Indian Institute of Science（印度科学研究所）；Jawaharlal Nehru Center for Advanced Scientific Research（贾瓦哈拉尔·尼赫鲁高级科学研究中心）；Indian Institute of Technology Madras（马德拉斯印度理工学院）；IISER Thiruvananthapuram（特凡纳普拉姆印度科学教育研究院）；BITS Pilani K. K. Birla Goa Campus（比拉工业与科学研究所皮拉尼校区K.K.比尔拉果阿分校）
The transport and magnetic properties of correlated La{0.53}Sr{0.47}MnO{3} ultrathin films, grown epitaxially on SrTiO{3}, show a sharp cusp at the structural transition temperature of the substrate. Using a combination of experiment and theory we show that the cusp is a result of resonant coupling between the charge carriers in the film and a soft phonon mode in the SrTiO{3}, mediated through oxygen octahedra in the film. The amplitude of the mode diverges towards the transition temperature, and phonons are launched into the first few atomic layers of the film affecting its electronic state.
Anisotropic hot carrier relaxation mediated by electron phonon scattering in TiN thin films
National Taiwan University（国立台湾大学）；Research Center for Applied Sciences, Academia Sinica（中央研究院应用科学研究中心）；Nano Science and Technology Program, TIGP, Academia Sinica（中央研究院纳米科技计划，全球研究生学位学程）；Institute of Atomic and Molecular Sciences, Academia Sinica（中央研究院原子与分子科学研究所）
Our ability to understand and tailor metal-organic interfaces is mandatory to functionalize organic complexes for next generation electronic and spintronic devices. For magnetic data storage applications, metal-carrying organic molecules, so called single molecular magnets (SMM) are of particular interest as they yield the possibility to store information on the molecular scale. In this work, we focus on the adsorption properties of the prototypical SMM Sc3N@C80 grown in a monolayer film on the Ag(111) substrate. We provide clear evidence of a pyramidal distortion of the otherwise planar Sc3N …
Without a periodic reference framework, local structures in noncrystalline solids are difficult to specify, but they still exert an enormous influence on materials properties. For example, thermomechanical responses of organic and inorganic glasses sensitively depend on the distribution of free volume or soft spots$^{1,2}$. Meanwhile, strong electron localization$^{3}$ that endows unparalleled electrical breakdown strengths to amorphous insulators is easily compromised by local defects that promote inelastic tunneling over a variable range$^{4,5}$. Here we report how metallic conduction can ov…
Diffusion mediated interaction in metal-substrate assembly during high temperature annealing leads to possible formation of new composite materials. Here, sputtered grown Ti films on Si3N4/Si substrate has been reported to produce titanium nitride and silicide based binary composites while undergoing high vacuum annealing process at temperatures 650°C and above. Diffusion of thermally decomposed Si and N atoms from Si3N4 and their subsequent chemical reaction with Ti have been probed by X-ray photo electron spectroscopy. For annealing at 800°C and above, most of the Si atoms show preferences t…
