The search for a two-dimensional material that simultaneously fulfills some properties for its use in spintronics and optoelectronics, i.e., a suitable bandgap with high in-plane carrier mobility and good environmental stability, is the focus of intense current research. If magnetism is also present, its range of utility is considerably expanded. One of the promising materials fulfilling these features is Bi$_2$O$_2$Se, a non van-der-Waals system whose monolayer has been recently obtained. This study addresses the structure and electronic properties of different monolayers that could be obtained experimentally. It is observed that these monolayers are very sensitive to the introduction of "extra" electrons, changing their electronic character from semiconductor to conductor. Furthermore, we investigate how the properties of each studied monolayer change when the system is doped with magnetic atoms. The result is that the doping introduces bands of low dispersion caused by the d orbitals of the impurities that can hybridize with the oxygen and bismuth atoms in the monolayer. This strongly modifies the electronic properties of the material, producing changes in the valence of certain Bi atoms which can induce a symmetry breaking in the perpendicular plane. Such phenomena lead to metallic or semiconducting characteristics, depending of metal doping.
We theoretically investigate the possibility of establishing ferromagnetism in the topological insulator Bi2Se3 via magnetic doping of 3d transition metal elements. The formation energies, charge states, band structures, and magnetic properties of doped Bi2Se3 are studied using first-principles calculations within density functional theory. Our results show that Bi substitutional sites are energetically more favorable than interstitial sites for single impurities. Detailed electronic structure analysis reveals that Cr and Fe doped materials are still insulating in the bulk but the intrinsic ba…
Ce3+ doped SrS phosphors with a charge-compensating Na+ for light-emitting diode (LED) applications have been successfully synthesized via a solid-state reaction method, which can be indexed to rock-salt-like crystal structures of Fm-3m space group. SrS:(Ce3+)x(x=0.005-0.05) and SrS:(Ce3+)0.01,(Na+)y(y=0.005-0.030) phosphors were excited by 430nm UV-VIS light, associated to the 5d1-4f1 transition of Ce3+. The composition-optimized SrS:(Ce3+)0.01,(Na+)0.015 phosphors showed an intense broad emission band at 430-700nm. The doping of Na+ was probed by solid-state nuclear magnetic resonance. The 4…
The Mott transistor is a paradigm for a new class of electronic devices---often referred to by the term Mottronics---, which are based on charge correlations between the electrons. Since correlation-induced insulating phases of most oxide compounds are usually very robust, new methods have to be developed to push such materials right to the boundary to the metallic phase in order to enable the metal-insulator transition to be switched by electric gating. Here we demonstrate that thin films of the prototypical Mott insulator LaTiO$_3$ grown by pulsed laser deposition under oxygen atmosphere are…
Titanium dioxide is one of the most widely investigated oxides. This is due to its broad range of applications, from catalysis to photocatalysis to photovoltaics. Despite this large interest, many of its bulk properties have been sparsely investigated using either experimental techniques or ab initio theory. Further, some of TiO2's most important properties, such as its electronic band gap, the localized character of excitons, and the localized nature of states induced by oxygen vacancies, are still under debate. We present a unified description of the properties of rutile and anatase phases, …
Transition metal dichalcogenides (TMDs) are a class of widely studied 2D layered materials which exist in various polymorphs. The 1T' phase of MoTe2 is of prime importance as it has been reported to show quantum spin hall (QSH) behavior with a fairly large band-gap of ~ 60 meV, in contrast to most QSH materials known. It is noteworthy that though the monolayer 1T'-MoTe2 was initially predicted to show the QSH behavior, recent theoretical studies claim that the few-layered counterparts also exhibit higher order topological behavior. Besides, 1T'-MoTe2 also undergoes a hysteretic phase transitio…
We have demonstrated that the island nucleation in the initial stage of epitaxial thin film growth can be tuned by substrate surface charge doping. This charge effect was investigated using spin density functional theory calculation in Fe-deposition on graphene substrate as an example. It was found that hole-doping can apparently increase both Fe-adatom diffusion barrier and Fe inter-adatom repulsion energy occurring at intermediate separation, whereas electron-doping can decrease Fe-adatom diffusion barrier but only slightly modify inter-adatom repulsion energy. Further kinetic Monte Carlo si…
Converse magnetoelectric coupling in artificial multiferroics is generally modelled through three possible mechanisms: charge transfer, strain mediated or ion migration. Here we demonstrate a novel and highly reliable approach, where electrically controlled morphological modifications control the ferromagnetic response of a magnetoelectric heterostructure, specifically FexMn1-x ferromagnetic films on ferroelectric PMN-PT (001) substrates. The ferroelectric PMN-PT substrates present, in correspondence to electrical switching, fully reversible morphological changes at the surface, to which corre…
Two-dimensional (2D) semiconducting transition metal dichalcogenides (TMDCs) and black phosphorus (BP) have beneficial electronic, optical, and physical properties at the few-layer limit. As atomically thin materials, 2D TMDCs and BP are highly sensitive to their environment and chemical modification, resulting in a strong dependence of their properties on substrate effects, intrinsic defects, and extrinsic adsorbates. Furthermore, the integration of 2D semiconductors into electronic and optoelectronic devices introduces unique challenges at metal-semiconductor and dielectric-semiconductor int…
We report a systematic first-principles investigation of the influence of different magnetic insulators on the magnetic proximity effect induced in graphene. Four different magnetic insulators are considered: two ferromagnetic europium chalcogenides namely EuO and EuS and two ferrimagnetic insulators yttrium iron garnet (YIG) and cobalt ferrite (CFO). The obtained exchange-splitting varies from tens to hundreds of meV. We also find an electron doping induced by YIG and europium chalcogenides substrates, that shift the Fermi level up to 0.78 eV and 1.3 eV respectively, whereas hole doping up to…
Surface doping of ZnO allows for tailoring the surface chemistry of the material while preserving the superb electronic structure of the bulk. Apart from obvious changes in adsorption energies and activation energies for catalysis, surface doping can alter the workfunction of the material and allow it to be tuned for specific photocatalytic and optoelectronic applications. We present first-principles electronic structure calculations for surface doping of Mn on the ZnO (0001) surface. Various dopant concentrations have been considered at the out-most (surface) layer of Zn atoms, while the inte…
Advances in manufacturing and characterization of complex molecular systems have created a need for new methods for design at molecular length scales. Emerging approaches are increasingly relying on the use of Artificial Intelligence (AI), and the training of AI models on large data libraries. This paradigm shift has led to successful applications, but shortcomings related to interpretability and generalizability continue to pose challenges. Here, we explore an alternative paradigm in which AI is combined with physics-based considerations for molecular and materials engineering. Specifically, …
Herein we review the remarkable range of modifications to materials properties associated with photoexcitation of the growth surface during physical vapor epitaxy of semiconductors. We concentrate on mechanisms producing measureable, utilizable changes in crystalline perfection, phase, composition, doping, and defect distribution. We outline the relevant physics of different mechanisms, concentrating on those yielding effects orthogonal to the primary growth variables of temperature and atomic or molecular fluxes and document the phenomenological effects reported. Based on experimental observa…
BiVO4, a visible-light response photocatalyst, has shown tremendous potential because of abundant raw material sources, good stability and low cost. There exist some limitations for further applicaitions due to poor capability to separate electron-hole pairs. In fact, a single-component modification strategy is barely adequate to obtain highy efficient photocatalytic performance. In this work, P substituted some of the V atoms from VO4 oxoanions, namely P was doped into the V sites in the host lattice of BiVO4 by a hydrothermal route. Meanwhile, Ag as an attractive and efficient electron-cocat…
Van der Waals single-layer materials are characterized by an inherent extremely low bending rigidity and therefore are prone to nanoscale structural modifications due to substrate interactions. Such interactions can induce excess charge concentration, conformational ripples and residual mechanical strain. In this work, we employed spatially resolved Raman and Photoluminescence images to investigate strain and doping inhomogeneities in a single layer exfoliated Molybdenum disulphide crystal. We have found that correlations between the spectral parameters of the most prominent Raman bands A1' an…
The magnetic and electronic properties of strontium titanate with different carbon dopant configurations are explored using first-principles calculations with a generalized gradient approximation (GGA) and the GGA+U approach. Our results show that the structural stability, electronic properties and magnetic properties of C-doped SrTiO3 strongly depend on the distance between carbon dopants. In both GGA and GGA+U calculations, the doping structure is mostly stable with a nonmagnetic feature when the carbon dopants are nearest neighbors, which can be ascribed to the formation of a C-C dimer pair…
The anomalous Nernst effect in nanostructured magnetic materials is a key phenomenon to optimally control and employ the internal energy dissipated in electronic devices, being dependent on for instance the magnetic anisotropy of the active element. Thereby, here we report a theoretical and experimental investigation of the magnetic properties and anomalous Nernst effect in a flexible magnetostrictive film with induced uniaxial magnetic anisotropy and under external stress. Specifically, we calculate the magnetization behavior and the thermoelectric voltage response from a theoretical approach…
We demonstrated doping in 2D monolayer graphene via local electrical stressing. The doping, confirmed by the resistance-voltage transfer characteristics of the graphene system, is observed to continuously tunable from N-type to P-type as the electrical stressing level (voltage) increases. Two major physical mechanisms are proposed to interpret the observed phenomena: modifications of surface chemistry for N-type doping (at low-level stressing) and thermally-activated charge transfer from graphene to SiO2 substrate for P-type doping (at high-level stressing). The formation of P-N junction on 2D…
We report on the on-surface synthesis of 7 armchair graphene nanoribbons (7-AGNRs) substituted with nitrile (CN) functional groups. The CN groups are attached to the GNR backbone by modifying the 7-AGNR precursor. While many of these groups survive the on-surface synthesis, the reaction process causes the cleavage of some CN from the ribbon backbone and the on-surface cycloisomerization of few nitriles onto pyridine rings. Scanning Tunneling Spectroscopy and Density Functional Theory reveal that CN groups behave as very efficient n-dopants, significantly downshifting the bands of the ribbon, a…
Two-dimensional (2D) van der Waals (vdW) magnetic materials have attracted a lot of attention owing to the stabilization of long-range magnetic order down to atomic dimensions, and the prospect of novel spintronic devices with unique functionalities. The clarification of the magnetoresistive properties and its correlation to the underlying magnetic configurations is essential for 2D vdW-based spintronic devices. Here, the effect of Co-doping on the magnetic and magnetotransport properties of Fe3GeTe2 have been investigated. Magnetotransport measurements reveal an unusual Hall effect behavior w…
Engineering the anomalous Hall effect (AHE) in the emerging magnetic topological insulators (MTIs) has great potentials for quantum information processing and spintronics applications. In this letter, we synthesize the epitaxial Bi2Te3/MnTe magnetic heterostructures and observe pronounced AHE signals from both layers combined together. The evolution of the resulting hybrid AHE intensity with the top Bi2Te3 layer thickness manifests the presence of an intrinsic ferromagnetic phase induced by the topological surface states at the heterolayer-interface. More importantly, by doping the Bi2Te3 laye…
Photoluminescence Quenching in WSe$_2$ via p-Doping Induced by Functionalized Rylene Dyes
Carl-von-Ossietzky Universität Oldenburg（奥尔登堡卡尔·冯·奥西茨基大学）；Friedrich-Schiller-Universität Jena（耶拿弗里德里希·席勒大学）；Leibniz Institute of Photonic Technology（莱布尼茨光子技术研究所）；Center for Energy and Environmental Chemistry Jena (CEEC Jena)（耶拿能源与环境化学中心）；sciclus GmbH & Co. KG（sciclus有限公司）
We report a family of two-dimensional hybrid perovskites (2DHPs) based on phenethylammonium lead iodide ((PEA)$_2$PbI$_4$) that show complex structure in their low-temperature excitonic absorption and photoluminescence (PL) spectra as well as hot exciton PL. We replace the 2-position (ortho) H on the phenyl group of the PEA cation with F, Cl, or Br to systematically increase the cation's cross-sectional area and mass and study changes in the excitonic structure. These single atom substitutions substantially change the observable number of and spacing between discrete resonances in the excitoni…
Acceptor and donor doping is a standard for tailoring semiconductors. More recently, doping was adapted to optimize the behavior at ferroelectric domain walls. In contrast to more than a century of research on semiconductors, the impact of chemical substitutions on the local electronic response at domain walls is largely unexplored. Here, the hexagonal manganite ErMnO$_3$ is donor doped with Ti$^{4+}$. Density functional theory calculations show that Ti$^{4+}$ goes to the B-site, replacing Mn$^{3+}$. Scanning probe microscopy measurements confirm the robustness of the ferroelectric domain temp…
Antiferromagnetic (AFM) van der Waals (vdW) materials provide a novel platform for synthetic AFM spintronics, in which the spin-related functionalities are derived from manipulating spin configurations between the layers. Metallic vdW antiferromagnets are expected to have several advantages over the widely-studied insulating counterparts in switching and detecting the spin states through electrical currents but have been much less explored due to the lack of suitable materials. Here, utilizing the extreme sensitivity of the vdW interlayer magnetism to material composition, we report the itiner…
Two-dimensional (2D) van der Waals (vdW) magnetic materials have garnered considerable attention owing to the existence of magnetic order down to atomic dimensions and flexibility towards interface engineering, offering an attractive platform to explore novel spintronic phenomena and functionalities. Understanding of the magnetoresistive properties and their correlation to the underlying magnetic configurations is essential for 2D vdW-based spintronic or quantum information devices. Among the promising candidates, vdW ferromagnet (FM) Fe3GeTe2 shows an unusual magnetotransport behavior, tunabl…
We show a method to control magnetic interfacial effects in multilayers with Dzyaloshinskii-Moriya interaction (DMI) using helium (He$^{+}$) ion irradiation. We report results from SQUID magnetometry, ferromagnetic resonance as well as Brillouin light scattering results on multilayers with DMI as a function of irradiation fluence to study the effect of irradiation on the magnetic properties of the multilayers. Our results show clear evidence of the He$^{+}$ irradiation effects on the magnetic properties which is consistent with interface modification due to the effects of the He$^{+}$ irradiat…
The charge redistribution at grain boundaries determines the applicability of high-Tc superconductors in electronic devices, because the transport across the grains can be hindered considerably. We investigate the local charge transfer and the modification of the electronic states in the vicinity of the grain-grain interface by first principles calculations for a (normal-state) 45^o tilted [001] grain boundary in YBa2Cu3O7. Our results explain the suppressed interface transport and the influence of grain boundary doping in a quantitative manner, in accordance with the experimental situation. T…
Electrical control of magnetism of a ferromagnetic semiconductor offers exciting prospects for future spintronic devices for processing and storing information. Here, we report observation of electrically modulated magnetic phase transition and magnetic anisotropy in thin crystal of Cr$_2$Ge$_2$Te$_6$ (CGT), a layered ferromagnetic semiconductor. We show that heavily electron-doped ($\sim$ $10^{14}$ cm$^{-2}$) CGT in an electric double-layer transistor device is found to exhibit hysteresis in magnetoresistance (MR), a clear signature of ferromagnetism, at temperatures up to above 200 K, which …
Silicene is a two-dimensional material, which is composed of a single layer of silicon atoms with sp2-sp3 mixed hybridization. The sp2-sp3 mixed hybridization renders silicene excellent reactive ability, facilitating the chemical modification of silicene. It has been demonstrated that chemical modification effectively enables the tuning of the properties of silicene. We now review all kind of chemical modification methods for silicene including hydrogenation, halogenation, organic surface modification, oxidation, doping and alloying. The effects of these chemical modification methods on the ge…
Our First-principles Full-Potential Density Functional Theory (DFT) calculations show that a monolayer of ZnS (ML-ZnS), which is predicted to adopt a graphene-like planar honeycomb structure with a direct band gap, undergoes strain-induced modifications in its structure and band gap when subjected to in-plane homogeneous biaxial strain ($δ$). ML-ZnS gets buckled for compressive strain greater than 0.92%; the buckling parameter $Δ$ (= 0.00 Å\, for planar ML-ZnS) linearly increases with increasing compressive strain ($Δ= 0.435$ Å\,at $δ= - 5.25$%). A tensile strain of 2.91% turns the direct band…
The electrical and optoelectronic properties of transition-metal dichalcogenides (TMDs), such as MoS2, are highly dependent on carrier doping and layer thickness. The ability to selectively control these two critical characteristics is of great importance to develop TMD-based multifunctional device applications, which remains challenging. Here, we report a strategy for controllable surface modification and layer thinning of MoS2 via ultraviolet (UV) light irradiation in a silver ionic solution environment. The results show that by adjusting UV irradiation time, nanostructured silver ultrathin …
Due to their graphene-like properties after oxygen reduction, incorporation of graphene oxide (GO) sheets into correlated-electron materials offers a new pathway for tailoring their properties. Fabricating GO nanocomposites with polycrystalline MgB2 superconductors leads to an order of magnitude enhancement of the supercurrent at 5 K/8 T and 20 K/4 T. Herein, we introduce a novel experimental approach to overcome the formidable challenge of performing quantitative microscopy and microanalysis of such composites, so as to unveil how GO doping influences the structure and hence the material prop…
The optical properties of graphene are strongly affected by electron-electron (e-e) and electron-hole (e-h) interactions. Here we tune these many-body interactions through varying the density of free charge carriers. Measurements from the infrared to the ultraviolet reveal significant changes in the optical conductivity of graphene for both electron and hole doping. The shift, broadening, and modification in shape of the saddle-point exciton resonance reflect strong screening of the many-body interactions by the carriers, as well as changes in quasi-particle lifetimes. Ab initio calculations b…
It has been reported that conversion yield and coherence time of ion-implanted NV centers improve if the Fermi level is raised or lowered during the annealing step following implantation. Here we investigate whether surface transfer doping and surface charging, by UV light, can be harnessed to induce this effect. We analyze the coherence times and the yield of NV centers created by ion implantation and annealing, applying various conditions during annealing. Specifically, we study coating the diamond with nickel, palladium or aluminum oxide, to induce positive surface transfer doping, as well …
Dopant-induced modifications of the optical properties of GaSe
Faculty of Physics, University of Warsaw（华沙大学物理学院）；Advanced Materials Research Group, Faculty of Engineering, University of Nottingham（诺丁汉大学工程学院先进材料研究组）；Institute for Problems of Material Science, National Academy of Sciences of Ukraine（乌克兰国家科学院材料科学问题研究所）
We have studied the graphene/gold interface by means of density functional theory (DFT) and scanning tunneling spectroscopy (STS). Weak interaction between graphene and the underlying gold surface leaves unperturbed Dirac cones in the band-structure, but they can be shifted with respect to the Fermi level of the whole system, which results in effective doping of graphene. DFT calculations revealed that the interface is extremely sensitive to the adsorption distance and to the structure of metal's surface, in particular strong variation in doping can be attributed to the specific rearrangements…
The modification and tailoring the characteristics of nanostructured materials are of great interest due to controllable and unusual inherent properties in such materials. A simple spray pyrolysis technique is used to prepare pure and La-doped ZnO films. The influence of La concentration (0, 0.33, 0.45, 0.66, 0.92 and 1.04 at. %) on the structural, optical, and magnetic properties of ZnO was investigated. The exact nominal compositions of the prepared films were determined from the field emission scanning electron microscope occupied with EDX. X-ray diffraction confirmed that the samples posse…
The effect of chemical doping of graphene films on the photovoltaic properties of the graphene/silicon Schottky junction solar cells was investigated. Thionyl chloride modification greatly enhanced the conductivity of graphene film, resulting in a significant improvement in cell performance with a 3-fold increase in conversion efficiency (up to 3.9%) and good short-term stability.
We present a first-principles theoretical study of electric field-and strain-controlled intrinsic half-metallic properties of zigzagged aluminium nitride (AlN) nanoribbons. We show that the half-metallic property of AlN ribbons can undergo a transition into fully-metallic or semiconducting behavior with application of an electric field or uniaxial strain. An external transverse electric field induces a full charge screening that renders the material semiconducting. In contrast, as uniaxial strain varies from compressive to tensile, a spin-resolved selective self-doping increases the half-metal…
