C. Richard A. Catlow, Alexey A. Sokol, Aron Walsh
A novel and direct method is proposed to assess the doping limits of semiconducting materials. Applied to the case of ZnO, our first-principles calculations demonstrate that p-type ZnO is thermodynamically unstable.
机构、总结、中文摘要均由AI分析而来，可能存在错误，请以论文正文为准。
继续探索
We report the structural and magnetic properties of ZnO single crystals implanted at 623 K with up to 10 at. % of Ni. As revealed by X-ray diffraction, crystalline fcc-Ni nanoparticles were formed inside ZnO. The magnetic behavior (magnetization with field reversal and with different temperature protocol) of all samples is well explained by a magnetic Ni-nanoparticle system. Although the formation of Ni:ZnO based diluted magnetic semiconductor cannot be ruled out, the major contribution to the magnetic properties stems from crystalline nanoparticles synthesized under these implantation conditi…
Oxygen vacancy (VO) is a common native point defects that plays crucial roles in determining the physical and chemical properties of metal oxides such as ZnO. However, fundamental understanding of VO is still very sparse. Specifically, whether VO is mainly responsible for the n-type conductivity in ZnO has been still unsettled in the past fifty years. Here we report on a study of oxygen self-diffusion by conceiving and growing oxygen-isotope ZnO heterostructures with delicately-controlled chemical potential and Fermi level. The diffusion process is found to be predominantly mediated by VO. We …
P mono-doped and (P, N) co-doped ZnO are investigated by the first-principles calculations. It is found that substitutive P defect forms a deep acceptor level at O site (PO) and it behaves as a donor at Zn site (PZn), while interstitial P (Pi) is amphoteric. Under equilibrium conditions, these defects contribute little to the p-type conductivity of ZnO samples since the formation energy of PZn is much lower than that of Pi or PO when EF is below mid-gap (a prerequisite p-type condition). Zinc vacancies (VZn) and PZn-2VZn complex are demonstrated to be shallow acceptors with ionization energies…
Due to its wide band gap and high carrier mobility, ZnO is an attractive material for light-harvesting and optoelectronic applications. Its functional efficiency, however, is strongly affected by defect-related in-gap states that open up extrinsic decay channels and modify relaxation timescales. As a consequence, almost every ZnO sample behaves differently, leading to irreproducible or even contradicting observations. Here, a complementary set of time-resolved spectroscopies is applied to two ZnO samples of different defect density to disentangle the competing contributions of charge carriers,…
The origin of room temperature (RT) ferromagnetism (FM) in Ni doped ZnO samples are systematically investigated through physical, optical, and magnetic properties of nanostructure, prepared by simple low-temperature wet chemical method. Reitveld refinement of X-ray diffraction pattern displays an increase in lattice parameters with strain relaxation and contraction in Zn/O occupancy ratio by means of Ni-doping. Similarly scanning electron microscope demonstrates modification in the morphology from nanorods to nanoflakes with Ni doping, suggests incorporation of Ni ions in ZnO. More interesting…
Nitrogen embedded ZnO:N films prepared by pulsed laser deposition exhibit significant ferromagnetism. The nitrogen ions contained in ZnO confirmed by Secondary Ion Microscopic Spectrum and Raman experiments and the embedded nitrogen ions can be regarded as defects. According to the experiment results, a mechanism is proposed based on one of the electrons in the completely filled d-orbits of Zn that compensates the dangling bonds of nitrogen ions and leads to a net spin of one half in the Zn orbits. These one half spins strongly correlate with localized electrons that are captured by defects to…
The origin of room temperature (RT) ferromagneticlike behavior in ZnO-based diluted magnetic semiconductors is still an unclear topic. The present work concentrates on the appearance of RT magnetic moments in just mixed ZnO/Co3O4 mixtures without thermal treatment. In this study, it is shown that the magnetism seems to be related to surface reduction of the Co3O4 nanoparticles, in which, an antiferromagnetic Co3O4 nanoparticle (core) is surrounded by a CoO-like shell. This singular superficial magnetism has also been found in other mixtures with semiconductors such as TiO2 and insulators such …
Magnetic 3d-ions doped into wide-gap oxides show signatures of room temperature ferromagnetism, although their concentration is two orders of magnitude smaller than that in conventional magnets. The prototype of these exceptional materials is Co-doped ZnO, for which an explanation of the room temperature ferromagnetism is still elusive. Here we demonstrate that magnetism originates from Co2+ oxygen-vacancy pairs with a partially filled level close to the ZnO conduction band minimum. The magnetic interaction between these pairs is sufficiently long-ranged to cause percolation at moderate concen…
The phases in the ZnO half of the ZnO-In2O3 binary system are natural superlattices consisting of periodic stacking of single InO2 sheets separated by indium doped ZnO blocks with a spacing that depends on the composition according to the relationship In2O3(ZnO)k. Characterization by combined, atomic resolution, aberration-corrected scanning transmission electron microscopy (STEM) and electron energy loss spectroscopy (EELS) analysis, indicates that the atomic structure of each InO2 layer consists of a single continuous sheet of octahedrally-coordinated InO2. The sheets also are crystallograph…
Fe-doped ZnO nanocrystals are successfully synthesized and structurally characterized by using x-ray diffraction and transmission electron microscopy. Magnetization measurements on the same system reveal a ferromagnetic to paramagnetic transition temperature > 450 K with a low-temperature transition from ferromagnetic to spin-glass state due to canting of the disordered surface spins in the nanoparticle system. Local magnetic probes like EPR and Mossbauer indicate the presence of Fe in both valence states Fe2+ and Fe3+. We argue that the presence of Fe3+ is due to the possible hole doping in t…
Cobalt and silver co-doping has been undertaken in ZnO thin films grown by pulsed laser deposition in order to investigate the ferromagnetic properties in ZnO-based diluted magnetic materials and to understand the eventual relation between ferromagnetism and charge carriers. Hall transport measurements reveal that Ag doping up to 5% leads to a progressive compensation of the native n-type carriers. The magnetization curves show ferromagnetic contributions for all samples at both 5 K and room temperature, decreasing with increasing the Ag concentration. First principles modeling of the possible…
On the vibrational properties of transition metal doped ZnO: surface, defect, and bandgap engineering
本研究通过固相反应法制备Mn和Co掺杂ZnO样品，系统分析其结构与光学性质，揭示Raman光谱附加谱带源于结构损伤与表面效应，并阐明非均匀掺杂与带隙减小引起的共振效应是SOP和LO模式增强的机制。
The Origin of Two-dimensional Electron Gas in Zn$_{1-x}$Mg$_x$O/ZnO Heterostructures
本文利用第一性原理计算揭示Zn$_{1-x}$Mg$_x$O/ZnO异质结构中2DEG的起源，指出厚层结构源于界面氧空位缺陷带，薄层结构则由表面氢、氧或OH基团吸收导致。
Making a systematic effort, we have developed a single-crystalline ZnSnN2 on ZnO (0001) by reactive magnetron co-sputtering. Epitaxial growth was achieved at 350 C by co-sputtering from metal targets in nitrogen atmosphere, and confirmed by transmission electron microscopy (TEM) measurements. TEM verified that the layers are single-crystalline of hexagonal phase, exhibiting epitaxial relationship with the substrate. The screw-type threading dislocations originating from the interface were identified as dominant extended defects. More specifically, we report a pioneering measurement of the disl…
During the past years there has been renewed interest in the wide-bandgap II-VI semiconductor ZnO, triggered by promising prospects for spintronic applications. First, ferromagnetism was predicted for dilute magnetic doping. In comprehensive investigation of ZnO:Co thin films based on the combined measurement of macroscopic and microscopic properties, we find no evidence for carrier-mediated itinerant ferromagnetism. Phase-pure, crystallographically excellent ZnO:Co is uniformly paramagnetic. Superparamagnetism arises when phase separation or defect formation occurs, due to nanometer-sized met…
Origin and Reduction of Coercive Fields in ZnO-based Wurtzite Ferroelectrics
本研究通过反应分子动力学揭示ZnO基纤锌矿铁电体矫顽场由反演畴界丝状头部未屏蔽局域极化序控制，电荷掺杂比应变更有效，组合可降E_c约50%，并借层状结构缩短传播路径。
This work explores the Zn vacancy in ZnO using hybrid density functional theory calculations. The Zn vacancy is predicted to be an exceedingly deep polaronic acceptor that can bind a localized hole on each of the four nearest-neighbor O ions. The hole localization is accompanied by a distinct outward relaxation of the O ions, which leads to lower symmetry and reduced formation energy. Notably, we find that initial symmetry-breaking is required to capture this effect, which might explain the absence of polaronic hole localization in some previous hybrid density functional studies. We present a …
Atomically transparent vertically aligned ZnO-based van der Waals material have been developed by surface passivation and encapsulation with atomic layers of MgO using materials by design; the physical properties investigated. The passivation and encapsulation led to a remarkable improvement in optical and electronic properties. The valence-band offset $ΔE_v$ between MgO and ZnO, ZnO and MgO/ZnO, and ZnO and MgO/ZnO/MgO heterointerfaces are determined to be 0.37 $\pm$0.02, -0.05$\pm$0.02, and -0.11$\pm$0.02 eV, respectively; the conduction-band offset $ΔE_c$ is deduced to be 0.97$\pm$0.02, 0.4…
Since the seminal observation of room-temperature laser emission from ZnO thin films and nanowires, numerous attempts have been carried out for detailed understanding of the lasing mechanism in ZnO. In spite of the extensive efforts performed over the last decades, the origin of optical gain at room temperature is still a matter of considerable discussion,. We show that ZnO microcrystals with a size of a few micrometers exhibit purely excitonic lasing at room temperature without showing any symptoms of electron-hole plasma emission. We then present the distinct experimental evidence that the r…
Effects of spin-orbit coupling and s-d exchange interaction are probed by magnetoresistance measurements carried out down to 50 mK on ZnO and Zn_{1-x}Mn_{x}O with x = 3 and 7%. The films were obtained by laser ablation and doped with Al to electron concentration ~10^{20} cm^{-3}. A quantitative description of the data for ZnO:Al in terms of weak-localization theory makes it possible to determine the coupling constant λ_{so} = (4.4 +- 0.4)*10^{-11} eVcm of the kp hamiltonian for the wurzite structure, H_{so} = λ_{so}*c(s x k). A complex and large magnetoresistance of Zn_{1-x}Mn_{x}O:Al is inter…
Polaronic-Distortion-Driven Enhancement of Excitonic Auger Recombination in ZnO Nanoparticles
本研究利用瞬态吸收光谱和超快电子衍射，揭示了ZnO纳米颗粒中光生空穴经俄歇机制被氧空位捕获并引发局部结构畸变，形成激子-极化子复合物，从而解释了其长寿命可见发光现象。
The formation of "zero" (exponentially small) resistance states (ESRS) in high mobility two-dimensional electron systems (2DES) in a static magnetic field B and subjected to strong microwave (MW) radiation has attracted great theoretical interest. These states appear to be associated with a new kind of energy gap $Δ$. Here I show that the energy gap $Δ$ is explained by a microscopic quantum model that involves the Prime Number Theorem, hitherto reserved for only mathematical contexts.
Microscopic origins of inertial magnetization dynamics
利用非马尔可夫量子主方程，揭示惯性磁化动力学源于与晶格光学声子的相干相互作用，为太赫兹频率下超快自旋动力学调控开辟新途径。
The microscopic origin of the electric Dzyaloshinskii-Moriya interaction (eDMI) is unveiled and discussed by analytical analysis and first-principles based calculations. As similar to the magnetic Dzyaloshinskii-Moriya interaction (mDMI), eDMI also originates from electron-mediated effect and more specifically from certain electron hoppings that are being activated due to certain local inversion symmetry breaking. However, the eDMI energy is found to be at least a third-order interaction in atomic displacements instead of bilinear in magnetic dipole moments for mDMI. Furthermore, the eDMI ener…
A microscopic model of the molecular magnet V15 is used to study mechanisms for the adiabatic change of the magnetization in time-dependent magnetic fields. Effects of the Dzyaloshinskii-Moriya interaction, the most plausible source for the energy-level repulsions that lead to adiabatic changes of the magnetization, are studied in detail. We find that the energy-level repulsions that result from this interaction exhibit a strong dependence on the direction of the applied field. We also discuss the role of magnetic anisotropy in the molecule Mn12 -acetate.
We report the results of Monte Carlo simulations with the aim to clarify the microscopic origin of exchange bias in the magnetization hysteresis loops of a model of individual core/shell nanoparticles. Increase of the exchange coupling across the core/shell interface leads to an enhancement of exchange bias and to an increasing asymmetry between the two branches of the loops which is due to different reversal mechanisms. A detailed study of the magnetic order of the interfacial spins shows compelling evidence that the existence of a net magnetization due to uncompensated spins at the shell int…
Classification of materials with phonon angular momentum and microscopic origin of angular momentum
本文按对称性将材料分为五类，确定声子携带角动量的类别，揭示其源于原子位移或速度诱导的力，并由自旋-轨道相互作用驱动。
In this study, the magnetic reversal process of exchange-coupled bilayer systems, consisting of a ferrimagnetic TbFeCo alloy layer and a ferromagnetic [Co/Ni/Pt]N multilayer, was investigated. In particular, minor loop studies, probing solely the reversal characteristics of the softer ferromagnetic layer, reveal two distinct reversal mechanisms, which depend strongly on the thickness of the ferromagnetic layer. For thick layers, irreversible switching of the macroscopic minor loop is observed. The underlying microscopic origin of this reversal process was studied in detail by high-resolution m…
The origins of an ultrahigh dielectric constant in polycrystalline CaCu3Ti4O12 (CCTO) was studied using the combination of impedance spectroscopy, electron microscopy, and scanning probe microscopy (SPM). Impedance spectra indicate that the transport properties in the 0.1 Hz .. 1 MHz frequency range are dominated by a single parallel resistive-capacitive (RC) element with a characteristic relaxation frequency of 16 Hz. Dc potential distributions measurements by SPM illustrate that significant potential drops occur at the grain boundaries, which thus can be unambiguously identified as the domin…
Skyrmions are widely regarded as promising candidates for emergent spintronic devices. Dzyaloshinskii-Moriya interaction (DMI) is often critical to the generation and manipulation of skyrmions. However, there is a fundamental lack of understanding of the origin of DMI or the mechanism by which DMI generates skyrmions in magnetic bilayers. Very little is known of the material parameters that determine the value of DMI. This knowledge is vital for rational design of skyrmion materials and further development of skyrmion technology. To address this important problem, we investigate DMI in magneti…
Modern magnetic thin film devices owe their success in large part to effects emerging from interlayer coupling and exchange interaction at interfaces. A prominent example is exchange bias (EB), a magnetic coupling phenomenon found in ferromagnet (F)/antiferromagnet (AF) systems. Uncompensated pinned moments in the AF couple to the F via the interface causing an additional unidirectional anisotropy. As a result, the hysteresis of the F is shifted. The existence of such pinned moments is nowadays accepted although their physical nature and origin is still unknown. Here we present a thorough spec…
We report a direct observation of the microscopic origin of the bipolar resistive switching behavior in nanoscale titanium oxide films. Through a high-resolution transmission electron microscopy, an analytical TEM technique using energy-filtering transmission electron microscopy and an in situ x-ray photoelectron spectroscopy, we demonstrated that the oxygen ions piled up at top interface by an oxidation-reduction reaction between the titanium oxide layer and the top Al metal electrode. We also found that the drift of oxygen ions during the on/off switching induced the bipolar resistive switch…
A simple but general microscopic mechanism to understand the interplay between the electric and magnetic degrees of freedom is developed. Within this mechanism, the magnetic structure generates an electric current which induce an counterbalance electric current from the spin orbital coupling. When the magnetic structure is described by a single order parameter, the electric polarization is determined by the single spin orbital coupling parameter, and the material is predicted to be a half insulator. This mechanism provides a simple estimation of the value of ferroelectricity and sets a physica…
Spin-orbit splitting of surface states is analyzed within and beyond the Rashba model using as examples the (111) surfaces of noble metals, Ag2Bi surface alloy, and topological insulator Bi2Se3. The ab initio analysis of relativistic velocity proves the Rashba model to be fundamentally inapplicable to real crystals. The splitting is found to be primarily due to a spin-orbit induced in-plane modification of the wave function, namely to its effect on the nonrelativistic Hamiltonian. The usual Rashba splitting -- given by charge distribution asymmetry -- is an order of magnitude smaller.
Microscopic origin of the spin-splitting in altermagnets
本研究提出了一种直观框架，揭示了交替磁体中自旋分裂的微观机制，通过原子交换驱动和各向异性跃迁模型，解释了其能带结构特征。
The microscopic origin of the spin-induced linear and quadratic magnetoelectric effects
本研究提出一种基于局域自旋与晶格对称性分析的通用方法，可揭示磁有序材料中磁电效应的微观起源，定位各机制的贡献，为探索强自旋诱导磁电材料提供指导。
We summarize the existing experimental data on electromagnons in multiferroic RMn2O5 compounds, where R denotes a rare earth ion, Y or Bi, and discuss a realistic microscopic model of these materials based on assumption that the microscopic mechanism of magnetically-induced ferroelectricity and electromagnon absorption relies entirely on the isotropic Heisenberg exchange and magnetostrictive coupling of spins to a polar lattice mode and does not involve relativistic effects. This model explains many magnetic and optical properties of RMn2O5 manganites, such as the spin re-orientation transitio…
Combining experiments on luminescent centres in hexagonal boron nitride with the polaron model and ab initio methods towards the identification of their microscopic origin
本研究结合ab initio计算与非微扰开放量子系统理论，分析了26种缺陷跃迁，将hBN中发光中心的微观起源缩小至三种碳基缺陷，并验证了基于极化子的理论方法与PLE实验高度一致。
We present first-principles calculations of AlGaN/GaN superlattice, clarifying the microscopic origin of the light emission and revealing the effect of local polarization within the quantum well. Profile of energy band and distributions of electrons and holes demonstrate the existence of a main active site in the well responsible for the main band-edge light emission. This site appears at the position where the local polarization becomes zero. With charge injection, the calculated optical spectra show that the broadening of the band gap at the active site leads to the blueshift of emission wav…
With a combined ab initio density functional and model Hamiltonian approach we establish that in the recently discovered multiferroic phase of the manganite Sr$_{1/2}$Ba$_{1/2}$MnO$_{3}$ the polar distortion of Mn and O ions is stabilized via enhanced in-plane Mn-O hybridizations. The magnetic superexchange interaction is very sensitive to the polar bond-bending distortion, and we find that this dependence directly causes a strong magnetoelectric coupling. This novel mechanism for multiferroicity is consistent with the experimentally observed reduced ferroelectric polarization upon the onset o…
Chiral spin textures at the interface between ferromagnetic and heavy nonmagnetic metals, such as Neel-type domain walls and skyrmions, have been studied intensively because of their great potential for future nanomagnetic devices. The Dyzaloshinskii-Moriya interaction (DMI) is an essential phenomenon for the formation of such chiral spin textures. In spite of recent theoretical progress aiming at understanding the microscopic origin of the DMI, an experimental investigation unravelling the physics at stake is still required. Here, we experimentally demonstrate the close correlation of the DMI…
Microscopic origin of Rashba coupling from first principles: Layer-resolved orbital asymmetry in transition metal dichalcogenides
本研究通过微观模型揭示了过渡金属二硫化物中Rashba耦合的微观起源，发现轨道极化不平衡是决定自旋分裂的关键因素。
The purpose of this paper is to provide a mathematical analysis of the Adler-Wiser formula relating the macroscopic relative permittivity tensor to the microscopic structure of the crystal at the atomic level. The technical level of the presentation is kept at its minimum to emphasize the mathematical structure of the results. We also briefly review some models describing the electronic structure of finite systems, focusing on density operator based formulations, as well as the Hartree model for perfect crystals or crystals with a defect.
Microscopic Origin of Spin Splitting in Altermagnetic CrSb Thin Films
本研究通过第一性原理计算揭示，CrSb薄膜的自旋分裂微观起源与块体不同，需长程晶胞间Cr-Sb等跳跃，且自旋分裂具强表面依赖性，为低维交替磁体自旋分裂调控提供了通用原理。
Microscopic description in the study of immiscibility and segregating properties of liquid metallic binary alloys has gained a renewed scientific and technological interests during the last eight years for the physicists, metallurgists and chemists. Especially, in understanding the basic mechanisms, from the point of interionic interaction, and how and why segregation in some metallic alloys takes place at and under certain thermodynamic state specified by temperature and pressure. An overview of the theoretical and experimental works done by different authors or groups in the area of segregat…
The surface of a Cr2O3 (0001) film epitaxially grown on Cr undergoes an unusual reentrant sequence of structural phase transitions. In order to understand the underlying microscopic mechanisms, the structural and magnetic properties of the Cr2O3 (0001) surface are here studied using first-principles electronic structure calculations. Two competing surface Cr sites are identified. The energetics of the surface is described by a configurational Hamiltonian with parameters determined using total energy calculations for several surface supercells. Effects of epitaxial strain and magnetic ordering …
The origins of hydrodynamic transport in strongly interacting Dirac and Weyl semimetals have remained elusive in theoretical descriptions and experimental measurements. We investigate the structure and microscopic properties of transport in WP$_2$, a type-II Weyl semimetal, to probe the emergence of hydrodynamic phenomena. We characterize the quantum behavior underlying the hydrodynamic transport regime as a function of temperature through ab initio calculations of the relevant microscopic scattering processes, including electron-phonon, electron-electron, and phonon-mediated electron-electron…
The discovery of multiferroic behavior in monolayer NiI$_2$ provides a new symmetry-broken state in van der Waals monolayers, featuring the simultaneous emergence of helimagnetic order and ferroelectric order at a critical temperature of $T=21$ K. However, the microscopic origin of multiferroic order in NiI$_2$ monolayer has not been established, and in particular, the role of non-colinear magnetism and spin-orbit coupling in this compound remains an open problem. Here we reveal the origin of the two-dimensional multiferroicity in NiI$_2$ using first-principles electronic structure methods. We…
Diamine-appended metal{organic frameworks (MOFs) of the form Mg2(dobpdc)(diamine)2 adsorb CO2 in a cooperative fashion, exhibiting an abrupt change in CO2 occupancy with pressure or temperature. This change is accompanied by hysteresis. While hysteresis is suggestive of a firstorder phase transition, we show that hysteretic temperature-occupancy curves associated with this material are qualitatively unlike the curves seen in the presence of a phase transition; they are instead consistent with CO2 chain polymerization, within one-dimensional channels in the MOF, in the absence of a phase transi…
Glass formation is encountered in diverse materials. Experiments have revealed that dynamic relaxation spectra of supercooled liquids generically become asymmetric near the glass transition temperature, $T_g$, where an extended power law emerges at high frequencies. The microscopic origin of this "wing" remains unknown, and was so far inaccessible to simulations. Here, we develop a novel computational approach and study the equilibrium dynamics of model supercooled liquids near $T_g$. We demonstrate the emergence of a power law wing in numerical spectra, which originates from relaxation at rar…
The atomic theory of elasticity of amorphous solids, based on the nonaffine response formalism, is extended into the nonlinear stress-strain regime by coupling with the underlying irreversible many-body dynamics. The latter is implemented in compact analytical form using a qualitative method for the many-body Smoluchowski equation. The resulting nonlinear stress-strain (constitutive) relation is very simple, with few fitting parameters, yet contains all the microscopic physics. The theory is successfully tested against experimental data on metallic glasses, and it is able to reproduce the ubiq…
扫码添加微信好友，提出您的宝贵建议 👇
💡 备注请填写：网站反馈
发表机构由 AI 从论文文本抽取，如发现错误，欢迎反馈修正建议。