Long-range Interatomic Interactions Research Articles

Nanoscale flow-induced nonlinear vibration of multilayer graphene based-resonators: Slip and transition flow regimes

This paper presents a nanoscale fluid-structure interaction (FSI) model for flow-induced nonlinear vibration of multilayer graphene based-resonators in the slip and transition regimes. Based on the multibeam interlayer shear model with von Kármán geometric nonlinearity and nonlocal modified couple stress theory, the size-dependent equations of motion are obtained for beam resonators laminated of NG-graphene layer and (NG−1) interlayer crosslinks. The small-scale effect on effective viscosity and slip boundary conditions of nanoscale flow is formulated by introducing the average velocity correction factor. For unbounded and bounded (by a rigid wall) nanoflows, the closed-form expressions of velocity correction factor in terms of Knudsen number, as a dimensionless discriminant parameter, are developed to correct the pressure distribution predicted by the potential theory. The present FSI model considers the size effects through the length scale parameter for microstructure local rotation, the nonlocal parameter for long-range interatomic interactions, and Knudsen number for slip condition of nanoscale flow. The Galerkin's method in conjunction with the multiple-scale perturbation technique is used to obtain closed-form solutions of frequency ratio and time-history response. The natural frequencies of cantilever multilayer graphene nanostrips are validated with the ones existing in the literature. Parametric studies are carried out to investigate the influences of small-scale, number of layers, interlayer shear modulus, and fluid characteristics on the linear and nonlinear natural frequencies. Findings show that the critical upstream speed for dynamic instability of the coupled system can change considerably by taking into account the size effects of nanoflow and nanostructures. Therefore, the classical FSI model is inadequate for analyzing nanoscale flow-induced vibration of nanoresonators. Also, it is seen that the effect of geometric nonlinearity becomes very significant for multilayer graphene beams with small interlayer shear modulus.

Optomechanics and quantum phase of the Bose-Einstein condensate with the cavity mediated spin-orbit coupling.

We investigated the optomechanical dynamics and explored the quantum phase of a Bose-Einstein condensate in a ring cavity. The interaction between the atoms and the cavity field in the running wave mode induces a semiquantized spin-orbit coupling (SOC) for the atoms. We found that the evolution of the magnetic excitations of the matter field resembles that of an optomechanical oscillator moving in a viscous optical medium, with very good integrability and traceability, regardless of the atomic interaction. Moreover, the light-atom coupling induces a sign-changeable long-range interatomic interaction, which reshapes the typical energy spectrum of the system in a drastic manner. As a result, a new quantum phase featuring a high quantum degeneracy was found in the transitional area for SOC. Our scheme is immediately realizable and the results are measurable in experiments.

Long-Range Interactions for Hydrogen Atoms in Excited D States

Pressure shifts inside an atomic beam are among the more theoretically challenging effects in high-precision measurements of atomic transitions. A crucial element in their theoretical analysis is the understanding of long-range interatomic interactions inside the beam. For excited reference states, the presence of quasi-degenerate states leads to additional challenges, due to the necessity to diagonalize large matrices in the quasi-degenerate hyperfine manifolds. Here, we focus on the interactions of hydrogen atoms in reference states composed of an excited nD state (atom A), and in the metastable 2S state (atom B). We devote special attention to the cases n=3 and n=8. For n=3, the main effect is generated by quasi-degenerate virtual P states from both atoms A and B and leads to experimentally relevant second-order long-range (van-der-Waals) interactions proportional to the sixth inverse power of the interatomic distance. For n=8, in addition to virtual states with two states of P symmetry, one needs to take into account combined virtual P and F states from atoms A and B. The numerical value of the so-called C6 coefficients multiplying the interaction energy was found to grow with the principal quantum number of the reference D state; it was found to be of the order of 1011 in atomic units. The result allows for the calculation of the pressure shift inside atomic beams while driving transitions to nD states.

Lattice stability of ordered Au-Cu alloys in the warm dense matter regime

In the warm dense regime, where the electron temperature is increased to the same order of the Fermi temperature, the dynamical stability of elemental metals depends on its electronic band structure as well as its crystal structure. It has been known that phonon hardening occurs due to an enhanced internal pressure caused by electron excitations as in close-packed simple metals, whereas phonon softening occurs at a specific point in the Brillouin zone as in body-centered cubic metals. Here, we investigate the dynamical stability of binary ordered alloys (Au and Cu) in the L1$_0$ and L1$_2$ structures. By performing first principles calculations on phonon dispersions, we demonstrate that warm dense Au-Cu systems show phonon hardening behavior except the lowest frequency phonon mode at point R of AuCu in the L1$_0$ structure. We show that when a phonon mode is stabilized by long-range interatomic interactions at ambient condition, such a phonon will be destabilized by the short-range nature of the warm dense matters.

Nonaffine lattice dynamics with the Ewald method reveals strongly nonaffine elasticity of α-quartz.

A lattice dynamical formalism based on nonaffine response theory is derived for noncentrosymmetric crystals, accounting for long-range interatomic interactions using the Ewald method. The framework takes equilibrated static configurations as input to compute the elastic constants in excellent agreement with both experimental data and calculations under strain. Besides this methodological improvement, which enables faster evaluation of elastic constants without the need of explicitly simulating the deformation process, the framework provides insights into the nonaffine contribution to the elastic constants of α-quartz. It turns out that, due to the noncentrosymmetric lattice structure, the nonaffine (softening) correction to the elastic constants is very large, such that the overall elastic constants are at least 3-4 times smaller than the affine Born-Huang estimate.

The effects of trap-confinement and interatomic interactions on Josephson effects and macroscopic quantum self-trapping for a Bose–Einstein condensate

We theoretically study the effects of trap-confinement and interatomic interactions on Josephson oscillations (JO) and macroscopic quantum self-trapping (MQST) for a Bose–Einstein condensate confined in a trap which has a symmetric double-well potential along z-axis and 2D harmonic potentials along x- and y-axis. We consider three types of model interaction potentials: contact, long-range dipolar and finite-range potentials. Our results show that by changing the aspect ratio between the axial and radial trap sizes, one can induce a transition from JO to MQST for contact interactions with a small scattering length. For long-range dipolar interatomic interactions, we analyze transition from Rabi to Josephson regime and Josephson to MQST regime by changing the aspect ratio of the trap for a particular dipolar orientation. For a finite-range interaction, we study the effects of relatively large scattering length and effective range on JO and MQST. We show that JO and MQST are possible even if scattering length is relatively large, particularly near a narrow Feshbach resonance due to the finite-range effects.

Ultralow thermal conductivity in a two-dimensional material due to surface-enhanced resonant bonding

Crystalline materials with ultralow thermal conductivity are highly desirable for thermoelectric applications. Many known crystalline materials with low thermal conductivity, including PbTe and Bi2Te3, possess a special kind of chemical bond called ‘resonant bond’. Resonant bonds consist of superposition of degenerate bonding configurations that leads to structural instability, anomalous long-range interatomic interaction, and soft optical phonons. These factors contribute to large lattice anharmonicity and strong phonon-phonon scattering, which result in low thermal conductivity. In this work, we use first principles simulation to investigate the effect of resonant bonding in two dimensions (2D), where resonant bonds are in proximity to the surface. We find that the long-range interatomic interaction due to resonant bonding becomes more prominent in 2D because of reduced screening of the atomic displacement–induced charge density distortion. To demonstrate this effect, we analyze the phonon properties of quasi-2D Bi2PbTe4 with an ultralow thermal conductivity of 0.74 W/mK at 300 K. By comparing the interatomic force constants of quasi-2D Bi2PbTe4 and its bulk counterpart and the properties of resonant bonds near the surface and in the bulk, we conclude that resonant bonds are significantly enhanced in reduced dimensions and are more effective in reducing the lattice thermal conductivity. Our results will provide new clues to search for thermal insulators in low-dimensional materials.

Influence of long-range interatomic and interlayer interactions on dispersion of acoustic waves by multilayer graphene

In this study, effects of the long-range interatomic and interlayer interactions on the dispersion of acoustic waves by multilayer graphene are investigated. A hybrid model that accounts for the long-range interatomic and interlayer interactions is developed. In the context of this model, the interatomic interactions are modeled based on the general nonlocal theory. The general nonlocal theory effectively models the dispersions of acoustic waves where it defines two independent nonlocal fields for the longitudinal and transverse acoustic waves. Interlayer interactions are defined to model the van der Waals interaction between the graphene layers. A new approach is proposed to determine the mechanical properties and the equivalent thickness of a single-layer graphene. The Young's modulus and Poisson's ratio of a single-layer graphene is obtained by ∼345MPa and ∼0.08, respectively. The equivalent thickness of a graphene sheet is determined by ∼0.057nm. An experimental validation for the dispersions of four-layer graphene is carried out where a good assent is observed. A parametric study is then presented to demonstrate the significant influence of the long-rang interatomic and interlayer interactions on the dispersion of incident acoustic waves by multilayer graphene.

Resonance dispersion interaction of alkali metal atoms in Rydberg states

With the use of second-order perturbation theory in the long-range interatomic interaction for the degenerate states of two Rydberg atoms we have obtained a general formula for the dependence of atomic interaction energy on the interatomic distance R in the presence of the Förster resonance. Inside of the ‘Förster sphere’ (R < RF) this dependence transforms to the formula for electric dipole interaction energy ΔEd − d = C3/R3 and for R > RF it transforms to the formula for the van der Waals interaction energy ΔEVdW = −C6/R6. The van der Waals constant C6 is represented as an expansion in terms of irreducible components which define the dependence on the interatomic axis orientation relative to the quantisation axis of projections M of the total angular momentum J. The numerical values of the irreducible components of tensor C6 were calculated for rubidium atoms in the same Rydberg states |nlJM〉 with large quantum numbers n. We present the calculated resonance interaction energy of two rubidium atoms in the states |43D5/2M〉, whose total energy exceeds by only 8 MHz the total energy of one of the atoms in the state |45P3/2M〉 and of the other in the state |41F7/2M〉.

Retardation effects in induced atomic dipole-dipole interactions

We present mean-field calculations of azimuthally averaged retarded dipole-dipole interactions in a Bose-Einstein condensate induced by a laser, at both long and short wavelengths. Our calculations demonstrate that dipole-dipole interactions become significantly stronger at shorter wavelengths, by as much as 30-fold, due to retardation effects. This enhancement, along with inclusion of the dynamic polarizability, indicate a method of inducing long-range interatomic interactions in neutral atom condensates at significantly lower intensities than previously realized.

Phonon transport in a one-dimensional harmonic chain with long-range interaction and mass disorder.

Atomic mass and interatomic interaction are the two key quantities that significantly affect the heat conduction carried by phonons. Here, we study the effects of long-range (LR) interatomic interaction and mass disorder on the phonon transport in a one-dimensional harmonic chain with up to 10^{5} atoms. We find that while LR interaction reduces the transmission of low-frequency phonons, it enhances the transmission of high-frequency phonons by suppressing the localization effects caused by mass disorder. Therefore, LR interaction is able to boost heat conductance in the high-temperature regime or in the large size regime, where the high-frequency modes are important.

Reconciling simulated melting and ground-state properties of metals with a modified embedded-atom method potential

We propose a modification of the embedded-atom method-type potential aiming at reconciling simulated melting and ground-state properties of metals by means of classical molecular dynamics. Considering titanium, magnesium, gold, and platinum as case studies, we demonstrate that simulations performed with the modified force field yield quantitatively correctly both the melting temperature of the metals and their ground-state properties. It is shown that the accounting for the long-range interatomic interactions noticeably affects the melting point assessment. The introduced modification weakens the interaction at interatomic distances exceeding the equilibrium one by a characteristic vibration amplitude defined by the Lindemann criterion, thus allowing for the correct simulation of melting, while keeping its behavior in the vicinity of the ground state minimum. The modification of the many-body potential has a general nature and can be applicable to metals with different characteristics of the electron structure as well as for many different molecular and solid state systems experiencing phase transitions.

An efficient Laplace transform-wave packet method hybrid with substructure technique

By virtue of substructure technique, the wave packet method can be applied to efficiently evaluate the thermal conduction of each phonon mode in the large periodic harmonic lattice. The substructures are connected by the inter-belts due to the long-range interatomic interaction. A parallel dynamic substructure method is presented in the Laplace transform domain, without any approximation in the condensation process. The validity and efficiency of the proposed method is demonstrated by the one- and three-dimensional cases. By launching a wide band wave packet, the whole given phonon branch can be studied by a one-time calculation. Defined as the ratio between square of Fourier transform of the transmitted and incident wave packets, the resulted transmission coefficient agrees with that obtained by the atomistic Green’s function method. Moreover the time evolution of the wave field can be given by the method, and the multilevel substructure technique can also be used.

On ordering in solid solutions of Cu-25 at % Au and Cu-75 at % Au

Based on the X-ray diffuse scattering (XRDS) method, a methodology for experimental determination of the parameters of short-range order in disordered polycrystalline solid solutions is developed. The method is based on accounting for static displacements in the corresponding coordination spheres. Static displacements are described by introducing parameter \(\beta = \frac{1} {\nu }\frac{{d\nu }} {{dc}} \), where v is the unit-cell volume, and c is the solid-solution concentration. The short-range order parameters of polycrystalline Cu-25 at % Au and Cu-75 at % Au solid solutions are calculated for a large number of coordination spheres using experimental values of the XRDS intensity and a refined methodology. It is established that the values of the short-range order parameters of a polycrystalline solid solution are close to analogous values for the Cu3Au superstructure, despite the different character of the XRDS intensity. This points to the presence of long-range interatomic interactions in these solid solutions.

Precise study of asymptotic physics with subradiant ultracold molecules

Weakly bound molecules have physical properties without atomic analogues, even as the bond length approaches dissociation. In particular, the internal symmetries of homonuclear diatomic molecules result in formation of two-body superradiant and subradiant excited states. While superradiance has been demonstrated in a variety of systems, subradiance is more elusive due to the inherently weak interaction with the environment. Here we characterize the properties of deeply subradiant molecular states with intrinsic quality factors exceeding $10^{13}$ via precise optical spectroscopy with the longest molecule-light coherent interaction times to date. We find that two competing effects limit the lifetimes of the subradiant molecules, with different asymptotic behaviors. The first is radiative decay via weak magnetic-dipole and electric-quadrupole interactions. We prove that its rate increases quadratically with the bond length, confirming quantum mechanical predictions. The second is nonradiative decay through weak gyroscopic predissociation, with a rate proportional to the vibrational mode spacing and sensitive to short-range physics. This work bridges the gap between atomic and molecular metrology based on lattice-clock techniques, yielding new understanding of long-range interatomic interactions and placing ultracold molecules at the forefront of precision measurements.

First-principles theory, coarse-grained models, and simulations of ferroelectrics.

CONSPECTUS: A ferroelectric crystal exhibits macroscopic electric dipole or polarization arising from spontaneous ordering of its atomic-scale dipoles that breaks inversion symmetry. Changes in applied pressure or electric field generate changes in electric polarization in a ferroelectric, defining its piezoelectric and dielectric properties, respectively, which make it useful as an electromechanical sensor and actuator in a number of applications. In addition, a characteristic of a ferroelectric is the presence of domains or states with different symmetry equivalent orientations of spontaneous polarization that are switchable with large enough applied electric field, a nonlinear property that makes it useful for applications in nonvolatile memory devices. Central to these properties of a ferroelectric are the phase transitions it undergoes as a function of temperature that involve lowering of the symmetry of its high temperature centrosymmetric paraelectric phase. Ferroelectricity arises from a delicate balance between short and long-range interatomic interactions, and hence the resulting properties are quite sensitive to chemistry, strains, and electric charges associated with its interface with substrate and electrodes. First-principles density functional theoretical (DFT) calculations have been very effective in capturing this and predicting material and environment specific properties of ferroelectrics, leading to fundamental insights into origins of ferroelectricity in oxides and chalcogenides uncovering a precise picture of electronic hybridization, topology, and mechanisms. However, use of DFT in molecular dynamics for detailed prediction of ferroelectric phase transitions and associated temperature dependent properties has been limited due to large length and time scales of the processes involved. To this end, it is quite appealing to start with input from DFT calculations and construct material-specific models that are realistic yet simple for use in large-scale simulations while capturing the relevant microscopic interactions quantitatively. In this Account, we first summarize the insights obtained into chemical mechanisms of ferroelectricity using first-principles DFT calculations. We then discuss the principles of construction of first-principles model Hamiltonians for ferroelectric phase transitions in perovskite oxides, which involve coarse-graining in time domain by integrating out high frequency phonons. Molecular dynamics simulations of the resulting model are shown to give quantitative predictions of material-specific ferroelectric transition behavior in bulk as well as nanoscale ferroelectric structures. A free energy landscape obtained through coarse-graining in real-space provides deeper understanding of ferroelectric transitions, domains, and states with inhomogeneous order and points out the key role of microscopic coupling between phonons and strain. We conclude with a discussion of the multiscale modeling strategy elucidated here and its application to other materials such as shape memory alloys.

Single-photon emitter based on an ensemble of lattice-trapped interacting atoms

Precisely controlling the atom number challenges the single-photon generation based on an individual neutral atom in experiments. A straightforward solution is to directly produce single photons via a number of atoms. We theoretically investigate such a single-photon emitter in which a bunch of Sr atoms are tightly confined in a blue-detuned optical lattice and weakly driven by an external field. The strong long-range interatomic interactions inducing large excitation-energy shifts results in a significant suppression of multiphoton emission. We consider two common approaches, which are widely used in experiments to generate single photons, in detail. The results indicate a potential to built up a single-photon source based on an ensemble of interacting atoms.

Titania nanorods curve to lower their energy

Spontaneous formation of curved nanorods is generally unexpected, since curvature introduces strain energy. However, electron microscopy shows that under hydrothermal conditions, some nanorods grown by oriented attachment of small anatase particles on {101} surfaces are curved and dislocation free. Molecular dynamics simulations show that the lattice energy of a curved anatase rod is actually lower than that of a linear rod due to more attractive long-range interatomic Coulombic interactions among atoms in the curved rod. The thermodynamic driving force stemming from lattice energy could be harnessed to produce asymmetric morphologies unexpected from classical Ostwald ripening with unusual shapes and properties.

Energy Calculations Predict Nanoparticle Attachment Orientations and Asymmetric Crystal Formation

Novel nanomaterials properties can stem from unusual morphologies that arise via oriented attachment (OA)-based crystal growth. However, the currently understood thermodynamic driving force of surface energy reduction for OA cannot predict experimental observation of attachment on relatively low energy surfaces in some crystals or sequential OA events that result in nanocrystals with morphology not predicted by symmetry. In this work, using molecular energetic calculations, we show that orientation-specific long-range interatomic interactions, in addition to surface energy reduction, predict morphology development and explain how OA produces crystals with lower symmetry than the initial material. Results also show that Coulombic interactions, rather than van der Waals interactions, control OA of ionic nanocrystals. Our computational approach and results can guide the selection or design of nanomaterials to achieve desired morphology as well as new physical and chemical properties.

Ideal mean-field transition in a modulated cold atom system

We show that an atomic system in a periodically modulated optical trap displays an ideal mean-field symmetry-breaking transition. The symmetry is broken with respect to time translation by the modulation period. We describe experimental observations and develop a full microscopic theory of the observed critical phenomena. The transition is explained as resulting from the interplay of the long-range interatomic interaction and nonequilibrium fluctuations in the strongly modulated system. The observations, including anomalous fluctuations in the symmetry broken phase, are fully described by the theory.