arXiv subjects

Hua Wu

Publications and source records attributed to Hua Wu.

At least 235 records · Page 13Linked to original sources

arXiv2014

Rare case of magnetic Ag$^{3+}$ ion: double perovskite Cs$_{2}$KAgF$_{6}$

Normally $4d$ or $5d$ transition metals are in a low-spin state. Here using first-principles calculations, we report on a rare case of a high-spin $S$=1 magnetic state for the Ag$^{3+}$ ion in the double perovskite Cs$_{2}$KAgF$_{6}$. We also explored a possibility of a conventional low-spin $S$=0 ground state and find an associated tetragonal distortion to be 0.29 Å. However, the lattice elastic energy cost and the Hund exchange loss exceed the e$_{g}$ crystal-field energy gain, thus making the low-spin tetragonal structure less favorable than the high-spin cubic structure. We conclude that the compact perovskite structure of Cs$_{2}$KAgF$_{6}$ is an important factor in stabilizing the unusual high-spin ground state of Ag$^{3+}$.

cond-mat.str-el↗

arXiv2014

Black phosphorus field-effect transistors

Two-dimensional crystals have emerged as a new class of materials with novel properties that may impact future technologies. Experimentally identifying and characterizing new functional two-dimensional materials in the vast material pool is a tremendous challenge, and at the same time potentially rewarding. In this work, we succeed in fabricating field-effect transistors based on few-layer black phosphorus crystals with thickness down to a few nanometers. Drain current modulation on the order of 10E5 is achieved in samples thinner than 7.5 nm at room temperature, with well-developed current saturation in the IV characteristics, both are important for reliable transistor performance of the device. Sample mobility is also found to be thickness dependent, with the highest value up to ~ 1000 cm2/Vs obtained at thickness ~ 10 nm. Our results demonstrate the potential of black phosphorus thin crystal as a new two-dimensional material for future applications in nano-electronic devices.

cond-mat.mtrl-sci↗

arXiv2013

Impact of spin-orbit coupling on the magnetism of Sr3MIrO6 (M = Ni, Co)

Using density functional calculations, we demonstrate that the spin-orbit coupling (SOC) of the Ir4+ ion plays an essential role in determining the antiferromagnetism of the hexagonal spin-chain system Sr3MIrO6 (M = Ni, Co) by tuning the crystal-field level sequence and altering the Ir-M inter-orbital interactions. The SOC splits the e'_{g} doublet of the octahedral Ir4+ ion (t_{2g}^5) in a trigonal crystal field, and the single t_{2g} hole resides on the e'_{g} upper branch and gives rise to the antiferromagnetic superexchange. In absence of the SOC, however, the single t_{2g} hole would occupy the a_{1g} singlet instead, which would mediate an unreal ferromagnetic exchange due to a direct a_{1g} hopping along the Ir-M chain. We also find that the Ni2+ and Co2+ ions are both in a high-spin state and moreover the Co2+ ion carries a huge orbital moment. This work well accounts for the recent experiments and magnifies again the significance of the SOC in iridates.

cond-mat.str-el↗

arXiv2013

Geometric Phase Gates with Adiabatic Control in Electron Spin Resonance

High-fidelity quantum operations are a key requirement for fault-tolerant quantum information processing. In electron spin resonance, manipulation of the quantum spin is usually achieved with time-dependent microwave fields. In contrast to the conventional dynamic approach, adiabatic geometric phase operations are expected to be less sensitive to certain kinds of noise and field inhomogeneities. Here, we investigate such phase gates applied to electron spins both through simulations and experiments, showing that the adiabatic geometric phase gate is indeed inherently robust against inhomogeneity in the applied microwave field strength. While only little advantage is offered over error-correcting composite pulses for modest inhomogeneities <=10%, the adiabatic approach reveals its potential for situations where field inhomogeneities are unavoidably large.

quant-ph↗

arXiv2012

Local correlations, non-local screening, multiplets, and band formation in NiO

We report on a comparative study of the valence band electronic structure of NiO as bulk material and of NiO as impurity in MgO. From the impurity we have been able to determine reliably the parameters which describe the local correlations, thereby establishing the compensated-spin character of the first ionization state or the state created by hole doping. Using bulk-sensitive x-ray photoemission we identify pronounced satellite features in the valence band of bulk NiO which cannot be explained by single-site many body approaches nor by mean field calculations. We infer the presence of screening processes involving local quasi-core states in the valence band and non-local coherent many body states. These processes are strong and the propagation of an extra hole in the valence band of NiO will therefore be accompanied by a range of high energy excitations. This in turn will make the observation of the dispersion relations in the Ni 3d bands difficult, also because the effective band width is no more than 0.25 eV as estimated from multi-site calculations.

cond-mat.str-el↗

arXiv2012

Metal-insulator transition in Sr2-xLaxCoO4 driven by spin-state transition

We sought the origin of the metal-insulator transition in Sr2-xLaxCoO4, using electron-correlation corrected density functional calculations. Our results show that Sr2CoO4 is in an intermediate-spin (IS) state and a strong Co4+ 3d-O 2p hybridization is responsible for its ferromagnetic metallicity. Upon La doping, however, a spin-state transition occurs in Sr1.5La0.5CoO4: IS-Co4+ x 2 + 1e --> LS-Co4+ + HS-Co3+ (LS: low spin; HS: high spin). Then the spin-state transition suppresses an electron hopping via a spin-blockade and gives rise to the insulating behavior of Sr1.5La0.5CoO4. A corresponding superexchange accounts for its ferromagnetism. Thus, spin state could provide a way to tune materials properties.

cond-mat.str-el↗

arXiv2012

Charge order at the frontier between the molecular and solid states in Ba3NaRu2O9

We show that the valence electrons of Ba3NaRu2O9, which has a quasi-molecular structure, completely crystallize below 210 K. Using an extended Hubbard model, we show that the charge ordering instability results from long-range Coulomb interactions. However, orbital ordering, metal-metal bonding and formation of a partial spin gap enforce the magnitude of the charge separation. The striped charge order and frustrated hcp lattice of Ru2O9 dimers lead to competition with a quasi-degenerate charge-melted phase under photo-excitation at low temperature. Our results establish a broad class of simple metal oxides as models for emergent phenomena at the border between the molecular and solid states.

cond-mat.str-el↗

arXiv2012

Is N-doped SrO magnetic? A first-principles view

N-doped SrO seems to be one of the model systems for d^0 magnetism, in which magnetism (or ideally, ferromagnetism) was ascribed to the localized N 2p spins mediated by delocalized O 2p holes. Here we offer a different view, using density functional calculations. We find that N-doped SrO with solely substitutional N impurities as widely assumed in the literature is unstable, and instead that a pairing state of substitutional and interstitial N impurities is significantly more stable and has a much lower formation energy than the former by 6.7 eV. The stable (N_{sub}-N_{int})^{2-} dimers behave like a charged (N_2)^{2-} molecule and have each a molecular spin=1. However, their spin-polarized molecular levels lie well inside the wide band gap of SrO and thus the exchange interaction is negligibly weak. As a consequence, N-doped SrO could not be ferromagnetic but paramagnetic.

cond-mat.mtrl-sci↗

arXiv2011

Electron spin ensemble strongly coupled to a three-dimensional microwave cavity

We demonstrate the strong coupling between an electron spin ensemble and a three-dimensional cavity in a reflection geometry. We also find that an anticrossing in the cavity/spin spectrum can be observed under conditions that the collective coupling strength $g_c$ is smaller than the spin linewidth $γ_s$ or the cavity linewidth. We identify a ratio of $g_c$ to $γ_s$ ($g_c/γ_s >$ 0.64) as a condition to observe a splitting in the cavity frequency. Finally, we confirm that $g_c$ scales with $\sqrt{N}$, where $N$ is the number of polarized spins.

quant-ph↗

arXiv2011

Orbital order in La0.5Sr1.5MnO4: beyond a common local Jahn-Teller picture

The standard way to find the orbital occupation of Jahn-Teller (JT) ions is to use structural data, with the assumption of a one-to-one correspondence between the orbital occupation and the associated JT distortion, e.g. in O6 octahedron. We show, however, that this approach in principle does not work for layered systems. Specifically, using the layered manganite La0.5Sr1.5MnO4 as an example, we found from our x-ray absorption measurements and theoretical calculations, that the type of orbital ordering strongly contradicts the standard local distortion approach for the Mn3+O6 octahedra, and that the generally ignored long-range crystal field effect and anisotropic hopping integrals are actually crucial to determine the orbital occupation. Our findings may open a pathway to control of the orbital state in multilayer systems and thus of their physical properties.

cond-mat.str-el↗

arXiv2011

Ab initio study of the giant ferroelectric distortion and pressure induced spin-state transition in BiCoO3

Using configuration-state-constrained electronic structure calculations based on the generalized gradient approximation plus Hubbard U method, we sought the origin of the giant tetragonal ferroelectric distortion in the ambient phase of the potentially multiferroic material BiCoO3 and identified the nature of the pressure induced spin-state transition. Our results show that a strong Bi-O covalency drives the giant ferroelectric distortion, which is further stabilized by an xy-type orbital ordering of the high-spin (HS) Co3+ ions. For the orthorhombic phase under 5.8 GPa, we find that a mixed HS and low-spin (LS) state is more stable than both LS and intermediate-spin (IS) states, and that the former well accounts for the available experimental results. Thus, we identify that the pressure induced spin-state transition is via a mixed HS+LS state, and we predict that the HS-to-LS transition would be complete upon a large volume decrease of about 20%.

cond-mat.str-el↗

arXiv2011

Shear-driven solidification of dilute colloidal suspensions

We show that the shear-induced solidification of dilute charge-stabilized (DLVO) colloids is due to the interplay between the shear-induced formation and breakage of large non-Brownian clusters. While their size is limited by breakage, their number density increases with the shearing-time. Upon flow cessation, the dense packing of clusters interconnects into a rigid state by means of grainy bonds, each involving a large number of primary colloidal bonds. The emerging picture of shear-driven solidification in dilute colloidal suspensions combines the gelation of Brownian systems with the jamming of athermal systems.

cond-mat.soft↗

arXiv2010

Magnetism in C or N-doped MgO and ZnO: density-functional study of impurity pairs

It is shown that substitution of C or N for O recently proposed as a way to create ferromagnetism in otherwise nonmagnetic oxide insulators is curtailed by formation of impurity pairs, and the resultant C2 spin=1 dimers as well as the isoelectronic N2^{2+} interact antiferromagneticallly in p-type MgO. For C-doped ZnO, however, we demonstrate using the HSE hybrid functional that a resonance of the spin-polarized C2 ppπ* states with the host conduction band results in a long-range ferromagnetic interaction. Magnetism of open-shell impurity molecules is proposed as a possible route to d0-ferromagnetism in oxide spintronic materials.

cond-mat.mtrl-sci↗

arXiv2010

Orbital occupation and magnetic moments of tetrahedrally coordinated iron in CaBaFe4O7

CaBaFe4O7 is a mixed-valent transition metal oxide having both Fe2+ and Fe3+ ions in tetrahedral coordination. Here we characterize its magnetic properties by magnetization measurements and investigate its local electronic structure using soft x-ray absorption spectroscopy at the Fe L2,3 edges, in combination with multiplet cluster and spin-resolved band structure calculations. We found that the Fe2+ ion in the unusual tetrahedral coordination is Jahn-Teller active with the high-spin e^2 (up) t2^3 (up) e^1 (down) configuration having a x^2-y^2-like electron for the minority spin. We deduce that there is an appreciable orbital moment of about L_z=0.36 caused by multiplet interactions, thereby explaining the observed magnetic anisotropy. CaBaFe4O7, a member of the '114' oxide family, offers new opportunities to explore charge, orbital and spin physics in transition metal oxides.

cond-mat.str-el↗

arXiv2010

The spin states of Co ions in La1.5Ca0.5CoO4 from first-principles

The spin states and electronic structure of layered perovskite La1.5Ca0.5CoO4 are investigated using fullpotential linearized augmented plane-wave method. All the computational results indicate that the Co2+ ion is in a high-spin state and the Co3+ in a low-spin state. The Co2+ t2g orbitals with a small crystal-field splitting are mixed by spin-orbit coupling, which accounts for the observed easy in-plane magnetism. The nonmagnetic LS-Co3+ state, which is stabilized by a strong crystal field, provides a natural explanation for the observed low magnetic ordering temperature and a spin-blockade phenomenon of the electron hopping. Furthermore, we find that the intermediate-spin state of Co3+ has a large multiplet splitting. But the lowest-lying IS state of Co3+ is still higher in energy than the LS ground state by a few hundred millielectron volts and the HS state of Co3+ is even less stable, both in sharp contrast to a recent experimental study which suggested the HS+IS mixed Co3+ ground state. We note that either the IS-Co3+ or HS-Co3+ states or their mixture would produce a wrong out-of-plane magnetic anisotropy and a much higher magneticordering temperature than observed. Thus, the present work sheds light on this material concerning its electronic and magnetic structure, and it would stimulate different experiments to settle this intriguing spin-state issue.

cond-mat.str-el↗

arXiv2010

Electronic structure, spin state, and magnetism of the square-lattice Mott insulator La2Co2Se2O3 from first principles

Electronic and magnetic structures of the newly synthesized cobalt oxyselenide La2Co2Se2O3 (structurally similar to the superconducting iron pnictides) are studied through density functional calculations. The obtained results show that this material is a Mott insulator, and that it has a very stable Co2+ high-spin ground state with a t2g-like orbital ordering, which is substantiated by the calculated crystal-field excitation energies. The square lattice of the Co2+ spins is found to have a strong antiferro (a weak ferro) magnetic coupling for the second nearest neighbors (2nn) via O (Se2) and an intermediate antiferro one for the 1nn, with the strength ratio about 10:1:3. The present results account for the available experimental data of magnetism, and the prediction of a planar frustrated (2x2) antiferromagnetic structure would motivate a new experiment.

cond-mat.str-el↗

arXiv2010

Storage of multiple coherent microwave excitations in an electron spin ensemble

Electron and nuclear spins have good coherence times and an ensemble of spins is a promising candidate for a quantum memory. By employing holographic techniques via field gradients a single ensemble may be used to store many bits of information. Here we present a coherent memory using a pulsed magnetic field gradient, and demonstrate the storage and retrieval of up to 100 weak 10 GHz coherent excitations in collective states of an electron spin ensemble. We further show that such collective excitations in the electron spin can then be stored in nuclear spin states, which offer coherence times in excess of seconds.

quant-ph↗

arXiv2010

Shear-induced reaction-limited aggregation kinetics of Brownian particles at arbitrary concentrations

The aggregation of interacting Brownian particles in sheared concentrated suspensions is an important issue in colloid and soft matter science per se. Also, it serves as a model to understand biochemical reactions occurring in vivo where both crowding and shear play an important role. We present an effective medium approach within the Smoluchowski equation with shear which allows one to calculate the encounter kinetics through a potential barrier under shear at arbitrary colloid concentrations. Experiments on a model colloidal system in simple shear flow support the validity of the model in the range considered. By generalizing Kramers' rate theory to the presence of collective hydrodynamics, our model explains the significant increase in the shear-induced reaction-limited aggregation kinetics upon increasing the colloid concentration.

cond-mat.soft↗