Neighboring Lattice Sites Research Articles

Fluoride Ion Storage and Conduction Mechanism in Fluoride Ion Battery Positive Electrode, Ruddlesden-Popper-Type Layered Perovskite La1.2Sr1.8Mn2O7 Crystal.

Structural characteristics on fluoride ion storage and conduction mechanism in La1.2Sr1.8Mn2O7, and its fluoridated materials, La1.2Sr1.8Mn2O7F and La1.2Sr1.8Mn2O7F2, for an all-solid-state fluoride ion battery positive electrode with a high volumetric capacity surpassing those of lithium-ion ones have been revealed using the Rietveld method and maximum entropy method. In La1.2Sr1.8Mn2O7, once the F- ions are taken into the NaCl slabs in its crystal through the charging process, it forms two stable fluoride compounds, La1.2Sr1.8Mn2O7F and La1.2Sr1.8Mn2O7F2, with the help of the Mn oxidation reaction. In these oxyfluorides, thermal vibrations of the F- ions inserted are much larger, especially in the a-b plane, than along the c axis. When surplus energy, such as an electric field for charging, is applied to these crystals at near room temperature or higher, the anions immediately begin to jump to their neighboring lattice sites, resulting in sufficiently rapid and large ionic conduction. The MEM analyses and density functional theory (DFT) calculations have revealed that the F- ions enable to easily travel along the ⟨110⟩ directions in the NaCl slabs of these crystals. These structural features thus make La1.2Sr1.8Mn2O7 and its fluorides possess both of two features incompatible with each other, ion storage and conduction, indispensable for rechargeable batteries.

Loss Difference Induced Localization in a Non-Hermitian Honeycomb Photonic Lattice.

Non-Hermitian systems with complex-valued energy spectra provide an extraordinary platform for manipulating unconventional dynamics of light. Here, we demonstrate the localization of light in an instantaneously reconfigurable non-Hermitian honeycomb photonic lattice that is established in a coherently prepared atomic system. One set of the sublattices is optically modulated to introduce the absorptive difference between neighboring lattice sites, where the Dirac points in reciprocal space are extended into dispersionless local flat bands, with two shared eigenstates: low-loss (high-loss) one with fields confined at sublattice B (A). When these local flat bands are broad enough due to larger loss difference, the incident beam with its tangential wave vector being at the K point in reciprocal space is effectively localized at sublattice B with weaker absorption, namely, the commonly seen power exchange between adjacent channels in photonic lattices is effectively prohibited. The current work unlocks a new capability from non-Hermitian two-dimensional photonic lattices and provides an alternative route for engineering tunable local flat bands in photonic structures.

Effects of long-range inter-particle interactions and isolated defect on quantum walks of two hard-core bosons in one-dimensional lattices

The quantum walk of two hard-core bosons in one-dimensional lattice under the effect of long-range inter-particle interaction is studied in detail. We also simulate the influence of an isolated defect that may exist in the lattice on the quantum walk of two particles by adding an additional potential energy to a certain lattice site. Using exact diagonalization method, the continuous-time quantum walk is directly simulated. The numerical simulations show that the range of interaction (long-range or short-range), the strength of the inter-particle interaction, the initial state of the two particles and the presence of the isolated defect have great influences on the quantum walk. Under the effect of strong long-range interaction, the particles initially located on the non-adjacent lattice sites have a co-walking behavior, while under the short-range interactions (nearest-neighbor interactions) only two particles initially located on the neighboring lattice sites can exhibit co-walking. After introducing the isolated defect into the system with strong interaction, two particles residing on the same side of the isolated defect keep co-walking, while two particles located on either sides of the isolated defect or one particle located on the isolated defect and the other particle staying on the side of the isolated defect, the two particles keep stationary or co-walking near the defect, displaying the characteristics of localization. By using the second-order perturbation theory of degenerate quantum system, a comprehensive theoretical analysis of the above numerical results is given. The theoretical analysis reveals the underlying physical law of quantum walks of two particles in one-dimensional lattice under the effects of strong long-range interaction and isolated defect in the lattice.

Effects of alkali ion dopants on the transport mechanisms and the thermal stabilities of imidazolium-based organic ionic plastic crystals.

Various dopant alkali ions have been introduced into organic ionic plastic crystals (OIPCs) in order to design solid electrolytes with the desired thermal stability and ionic conductivity. We performed extensive molecular dynamics simulations to investigate at the molecular level how dopant alkali ions affect the rotational and the translational diffusion of ions and the thermal stability of OIPCs. We introduced lithium (Li+), sodium (Na+), and potassium (K+) ions as dopants into 1-methyl-3-methylimidazolium hexafluorophosphate ([MMIM][PF6]) OIPCs at the molecular level. We found that as smaller alkali ions are doped, larger domains of the crystals are disrupted. This makes it harder for OIPCs doped with smaller alkali ions to maintain their crystal structure such that the melting temperature of OIPCs decreases and phase transitions between rotator phases change. The size of dopant alkali ions also affects the rotational diffusion of matrix ions of [MMIM]+ and PF6-: the rotational diffusion of matrix ions near Li+ ions becomes more heterogeneous and facilitated than those near other kinds of alkali ions. We also find that alkali ions of different kinds diffuse translationally in OIPCs via different transport mechanisms: while the Li+ ion undergoes continuous (anion-associated) diffusion through an amorphous region, the K+ ion hops between neighbor lattice sites. To investigate the effects of the relative size between matrix cations and dopant ions on translational diffusions, we also simulate OIPCs with longer alkyl chains such as 1-ethyl-3-methylimidazolium hexafluorophosphate ([EMIM][PF6]) and 1-butyl-3-methylimidazolium hexafluorophosphate ([BMIM][PF6]) crystals. We find that as the size of imidazolium cations increases, the hopping diffusion of the K+ ion becomes suppressed and the K+ ion is more likely to diffuse through amorphous domains.

High-powered optical superlattice with robust phase stability for quantum gas microscopy.

Optical superlattice has a wide range of applications in the study of ultracold atom physics. Especially, it can be used to trap and manipulate thousands of atom pairs in parallel which constitutes a promising system for quantum simulation and quantum computation. In the present work, we report on a high-power optical superlattice formed by a 532-nm and 1064-nm dual-wavelength interferometer with a short lattice spacing of 630 nm. The short-term fluctuation (in 10 seconds) of the relative phase between the short lattice and the long lattice is measured to be 0.003π, which satisfies the needs for performing two-qubit gates among neighboring lattice sites. We further implement this superlattice in a 87Rb experiment with a quantum gas microscope of single-site resolution, where the high-power 532-nm laser is necessary for pinning atoms in the short lattice during imaging, providing a unique platform for engineering quantum states.

Probing the topology of the quantum analog of a classical skyrmion

In magnetism, skyrmions correspond to classical three-dimensional spin textures characterized by a topological invariant that keeps track of the winding of the magnetization in real space, a property that cannot be easily generalized to the quantum case since the orientation of a quantum spin is in general ill-defined. Moreover, as we show, the quantum skyrmion state cannot be directly observed in modern experiments that probe the local magnetization of the system. However, we show that this novel quantum state can still be identified and fully characterized by a special local three-spin correlation function defined on neighbouring lattice sites -- the scalar chirality -- which reduces to the classical topological invariant for large systems, and which is shown to be nearly constant in the quantum skyrmion phase.

Deducing transport properties of mobile vacancies from perovskite solar cell characteristics

The absorber layers in perovskite solar cells possess a high concentration of mobile ion vacancies. These vacancies undertake thermally activated hops between neighboring lattice sites. The mobile vacancy concentration N0 is much higher and the activation energy EA for ion hops is much lower than is seen in most other semiconductors due to the inherent softness of perovskite materials. The timescale at which the internal electric field changes due to ion motion is determined by the vacancy diffusion coefficient Dv and is similar to the timescale on which the external bias changes by a significant fraction of the open-circuit voltage at typical scan rates. Therefore, hysteresis is often observed in which the shape of the current–voltage, J–V, characteristic depends on the direction of the voltage sweep. There is also evidence that this defect migration plays a role in degradation. By employing a charge transport model of coupled ion-electron conduction in a perovskite solar cell, we show that EA for the ion species responsible for hysteresis can be obtained directly from measurements of the temperature variation of the scan-rate dependence of the short-circuit current and of the hysteresis factor H. This argument is validated by comparing EA deduced from measured J–V curves for four solar cell structures with density functional theory calculations. In two of these structures, the perovskite is MAPbI3, where MA is methylammonium, CH3NH3; the hole transport layer (HTL) is spiro (spiro-OMeTAD, 2,2′,7,7′- tetrakis[N,N-di(4-methoxyphenyl) amino]-9,9′-spirobifluorene) and the electron transport layer (ETL) is TiO2 or SnO2. For the third and fourth structures, the perovskite layer is FAPbI3, where FA is formamidinium, HC(NH2)2, or MAPbBr3, and in both cases, the HTL is spiro and the ETL is SnO2. For all four structures, the hole and electron extracting electrodes are Au and fluorine doped tin oxide, respectively. We also use our model to predict how the scan rate dependence of the power conversion efficiency varies with EA, N0, and parameters determining free charge recombination.

Equilibrium properties of two-species reactive lattice gases on random catalytic chains.

We focus here on the thermodynamic properties of adsorbates formed by two-species A+B→⊘ reactions on a one-dimensional infinite lattice with heterogeneous "catalytic" properties. In our model hard-core A and B particles undergo continuous exchanges with their reservoirs and react when dissimilar species appear at neighboring lattice sites in presence of a "catalyst." The latter is modeled by supposing either that randomly chosen bonds in the lattice promote reactions (Model I) or that reactions are activated by randomly chosen lattice sites (Model II). In the case of annealed disorder in spatial distribution of a catalyst we calculate the pressure of the adsorbate by solving three-site (Model I) or four-site (Model II) recursions obeyed by the corresponding averaged grand-canonical partition functions. In the case of quenched disorder, we use two complementary approaches to find exact expressions for the pressure. The first approach is based on direct combinatorial arguments. In the second approach, we frame the model in terms of random matrices; the pressure is then represented as an averaged logarithm of the trace of a product of random 3×3 matrices-either uncorrelated (Model I) or sequentially correlated (Model II).

Energy exchange in M-crowdion clusters in 2D Morse lattice

Dynamics of new class of M-solitons and M-crowdions, here M = 3 is the number of adjacent close-packed atomic rows where the atoms move, are studied in two-dimensional triangular Morse lattice using classical molecular dynamics simulations. 3-solitons/3-crowdions are excited by giving initial velocities to the three atoms in three neighboring close-packed atomic rows along the rows. Different relations between the initial velocities are considered: all three initial velocities are equal, initial velocity for the middle atom is lower than for the outermost atoms, and all three velocities are different. During propagation of a 3-soliton the atoms do not overcome potential barrier and relax back to their original lattice sites. Propagation of a 3-crowdion results in the shift of the atoms to the neighboring lattice sites along the direction of movement. It is found that propagation of 3-soliton/3-crowdion clusters is associated with the energy exchange between the adjacent atomic rows. The ratio between the initial energies, at which the maximum energy exchange occurs, is determined. The energy is transferred from the high-energy atomic rows to the low-energy one. In the case when initial velocities in all three rows are different, the dynamics of 3-soliton/3-crowdion clusters is unstable. Obtained results allow to better understand the dynamics of interstitial defect clusters.

Nonequilibrium magnetic phases in spin lattices with gain and loss

We study the magnetic phases of a non-equilibrium spin chain, where coherent interactions between neighboring lattice sites compete with alternating gain and loss processes. This competition between coherent and incoherent dynamics induces transitions between magnetically aligned and highly mixed phases, across which the system changes from a low- to an effective infinite-temperature state. We show that the origin of these transitions can be traced back to the dynamical effect of parity-time-reversal symmetry breaking, which has no counterpart in the theory of equilibrium phase transitions. This mechanism also results in very atypical features and we find first-order transitions without phase co-existence and mixed-order transitions which do not break the underlying $U(1)$ symmetry, even in the appropriate thermodynamic limit. Thus, despite its simplicity, the current model considerably extends the phenomenology of non-equilibrium phase transitions beyond that commonly assumed for driven-dissipative spins and related systems.

Ultrafast Creation of Overlapping Rydberg Electrons in an Atomic BEC and Mott-Insulator Lattice.

We study an array of ultracold atoms in an optical lattice (Mott insulator) excited with a coherent ultrashort laser pulse to a state where single-electron wave functions spatially overlap. Beyond a threshold principal quantum number where Rydberg orbitals of neighboring lattice sites overlap with each other, the atoms efficiently undergo spontaneous Penning ionization resulting in a drastic change of ion-counting statistics, sharp increase of avalanche ionization, and the formation of an ultracold plasma. These observations signal the actual creation of electronic states with overlapping wave functions, which is further confirmed by a significant difference in ionization dynamics between a Bose-Einstein condensate and a Mott insulator. This system is a promising platform for simulating electronic many-body phenomena dominated by Coulomb interactions in the condensed phase.

Robust Multiplexing with Topolectrical Higher-Order Chern Insulators

We explore an implementation of a higher-order Chern insulator in a topolectrical circuit as a platform to implement robust signal multiplexing. By utilizing basic circuit layouts that realize the required complex hopping between neighboring lattice sites, we demonstrate different topological phases in a three-dimensional topolectrical circuit, including a Wannier-based Chern insulator and a crystalline topological phase. The topological chiral hinge states supported by the circuit are nonreciprocal and avoid propagation to the hinge opposite the excitation. Such an unusual response can be explained in terms of a synthetic gauge field of the circuit lattice, enabling multiplexing inherently robust to defects.

Interband resonant high-harmonic generation by valley polarized electron\u2013hole pairs

High-harmonic generation in solids is a unique tool to investigate the electron dynamics in strong light fields. The systematic study in monolayer materials is required to deepen the insight into the fundamental mechanism of high-harmonic generation. Here we demonstrated nonperturbative high harmonics up to 18th order in monolayer transition metal dichalcogenides. We found the enhancement in the even-order high harmonics which is attributed to the resonance to the band nesting energy. The symmetry analysis shows that the valley polarization and anisotropic band structure lead to polarization of the high-harmonic radiation. The calculation based on the three-step model in solids revealed that the electron–hole polarization driven to the band nesting region should contribute to the high harmonic radiation, where the electrons and holes generated at neighboring lattice sites are taken into account. Our findings open the way for attosecond science with monolayer materials having widely tunable electronic structures.

Thermodynamics of Liquid Solutions of Nitrogen in Chromium

A simple theory is proposed for the thermodynamic properties of nitrogen solutions in Fe–Cr melts. The theory is based on a lattice model of the solution. An fcc model lattice is adopted. Iron and chromium atoms are distributed at the lattice sites. Nitrogen atoms are located in octahedral interstices. The nitrogen atoms only interact with metal atoms at neighboring lattice sites. The energy of this interaction is assumed to depend neither on the composition nor on the temperature. The liquid Fe–Cr solutions are assumed perfect. Within this framework, the constant in the Sieverts law governing the solubility of nitrogen in liquid chromium may be expressed in terms of its value for the solubility of nitrogen in liquid iron and the value of the Wagner parameter for N–Cr interaction in liquid iron alloys. In addition, the partial enthalpy of solution of nitrogen in liquid chromium at infinite dilution is expressed in terms of the corresponding enthalpy for the solution of nitrogen in liquid iron and the Wagner parameter for N–Cr interaction in liquid iron alloys. A relation is also established between the Wagner parameter for N–Fe interaction in liquid chromium alloys and the Wagner parameter for N–Cr interaction in liquid iron alloys. On that basis, the constant in the Sieverts law governing the solubility of nitrogen in liquid chromium is calculated, along with enthalpy of solution of nitrogen in liquid chromium at infinite dilution and the Wagner parameter for N‒Fe interaction in liquid chromium alloys at 1873 K. The calculation results are compared with experimental data regarding the solubility of nitrogen in liquid chromium and Cr–Fe alloys obtained by various methods. The theoretical data are in best agreement with experimental data obtained by quenching. The values of the Wagner parameter for N–N interaction in liquid chromium alloys and iron alloys are discussed.

Correlated spin-flip tunneling in a Fermi lattice gas

We report the realization of correlated, density-dependent tunneling for fermionic 40K atoms trapped in an optical lattice. By appropriately tuning the frequency difference between a pair of Raman beams applied to a spin-polarized gas, simultaneous spin transitions and tunneling events are induced that depend on the relative occupations of neighboring lattice sites. Correlated spin-flip tunneling is spectroscopically resolved using gases prepared in opposite spin states, and the inferred Hubbard interaction energy is compared with a tight-binding prediction. We show that the laser-induced correlated tunneling process generates doublons via loss induced by light-assisted collisions. Furthermore, by controllably introducing vacancies to a spin-polarized gas, we demonstrate that correlated tunneling is suppressed when neighboring lattice sites are unoccupied.

(Invited) Electrochemistry of Solid-State Inorganic Polymer Electrolyte

Electrochemistry explores the charge transfer reaction across the interfaces, such as solid/liquid interface, liquid/liquid interface and also solid/solid interface. Most reported charge transfer behaviours across the “solid/solid” interface are involved liquid electrolyte. For example, in the lithium-ion batteries, the redox of cobalt-based active material is coupled by the heterogeneous intercalation/deintercalation of Li+ ions, which is existed in the electrolyte solution. In another words, the electron transfer occurs at the solid/solid interface while the ion transfer occurs at the solid/electrolyte solution. We employ SECM to construct the solid-solid interface and to study the electron transfer phenomena therein. That means there is no liquid electrolyte environment. When the electron transfer occurs at the solid/solid interface, the counterion transfer will occur in the crystal due to the crystalline defects. For example, we cultured the NaCl microcrystals, which are doped with iron oxides, between the pair electrodes on a microchip. The multi-step electron transfer processes of iron from Fe(0) to Fe(VI) through Fe(II) and Fe(III) were observed. The solid-state electrolyte solution just like an inorganic polymer. The electron transfer is wired through hopping between the neighboring redox lattice sites, coupling with the counterion transfer in the crystalline defects. The electrochemical behavior in the solid-state inorganic “polymer” electrolyte will be discussed in this presentation.

Effect of Fourier transform on the streaming in quantum lattice gas algorithms

ABSTRACTAll our previous quantum lattice gas algorithms for nonlinear physics have approximated the kinetic energy operator by streaming sequences to neighboring lattice sites. Here, the kinetic energy can be treated to all orders by Fourier transforming the kinetic energy operator with interlaced Dirac-based unitary collision operators. Benchmarking against exact solutions for the 1D nonlinear Schrodinger equation shows an extended range of parameters (soliton speeds and amplitudes) over the Dirac-based near-lattice-site streaming quantum algorithm.

Free energy change of a dislocation due to a Cottrell atmosphere

The free energy reduction of a dislocation due to a Cottrell atmosphere of solutes is computed using a continuum model. We show that the free energy change is composed of near-core and far-field components. The far-field component can be computed analytically using the linearized theory of solid solutions. Near the core the linearized theory is inaccurate, and the near-core component must be computed numerically. The influence of interactions between solutes in neighbouring lattice sites is also examined using the continuum model. We show that this model is able to reproduce atomistic calculations of the nickel–hydrogen system, predicting hydride formation on dislocations. The formation of these hydrides leads to dramatic reductions in the free energy. Finally, the influence of the free energy change on a dislocation’s line tension is examined by computing the equilibrium shape of a dislocation shear loop and the activation stress for a Frank–Read source using discrete dislocation dynamics.

Fission dynamics with microscopic level densities

Working within the Langevin framework of nuclear shape dynamics, we study the dependence of the evolution on the degree of excitation. As the excitation energy of the fissioning system is increased, the pairing correlations and the shell effects diminish and the effective potential-energy surface becomes ever more liquid-drop like. This feature can be included in the treatment in a formally well-founded manner by using the local level densities as a basis for the shape evolution. This is particularly easy to understand and implement in the Metropolis treatment where the evolution is simulated by means of a random walk on the five-dimensional lattice of shapes for which the potential energy has been tabulated. Because the individual steps between two neighboring lattice sites are decided on the basis of the ratio of the statistical weights, what is needed is the ratio of the local level densities for those shapes, evaluated at the associated local excitation energies. For this purpose, we adapt a recently developed combinatorial method for calculating level densities which employs the same single-particle levels as those that were used for the calculation of the pairing and shell contributions to the macroscopic-microscopic deformation-energy surface. For each nucleus under consideration, the level density (for a fixed total angular momentum) is calculated microscopically for each of the over five million shapes given in the three-quadratic-surface parametrization. This novel treatment, which introduces no new parameters, is illustrated for the fission fragment mass distributions for selected uranium and plutonium cases.

Distribution of randomly diffusing particles in inhomogeneous media.

Diffusion can be conceptualized, at microscopic scales, as the random hopping of particles between neighboring lattice sites. In the case of diffusion in inhomogeneous media, distinct spatial domains in the system may yield distinct particle hopping rates. Starting from the master equations (MEs) governing diffusion in inhomogeneous media we derive here, for arbitrary spatial dimensions, the deterministic lattice equations (DLEs) specifying the average particle number at each lattice site for randomly diffusing particles in inhomogeneous media. We consider the case of free (Fickian) diffusion with no steric constraints on the maximum particle number per lattice site as well as the case of diffusion under steric constraints imposing a maximum particle concentration. We find, for both transient and asymptotic regimes, excellent agreement between the DLEs and kinetic Monte Carlo simulations of the MEs. The DLEs provide a computationally efficient method for predicting the (average) distribution of randomly diffusing particles in inhomogeneous media, with the number of DLEs associated with a given system being independent of the number of particles in the system. From the DLEs we obtain general analytic expressions for the steady-state particle distributions for free diffusion and, in special cases, diffusion under steric constraints in inhomogeneous media. We find that, in the steady state of the system, the average fraction of particles in a given domain is independent of most system properties, such as the arrangement and shape of domains, and only depends on the number of lattice sites in each domain, the particle hopping rates, the number of distinct particle species in the system, and the total number of particles of each particle species in the system. Our results provide general insights into the role of spatially inhomogeneous particle hopping rates in setting the particle distributions in inhomogeneous media.