Attractive Dipolar Interactions Research Articles

Control of colloidal cohesive states in active chiral fluids

Ensembles of suspended spinning particles in liquids form a distinct category of active matter systems known as chiral fluids. Recent experimental instances of dense chiral fluids have comprised of spinning colloidal magnets powered by an external rotating magnetic field. These particles interact through both magnetic and hydrodynamic forces, organizing collectively into circulating clusters characterized by unidirectional edge flows. Here, we externally drive the collective behavior of spinning colloids by leveraging diffusiophoretic interactions among the geometrically anisotropic particles. We show that these nanoscale interfacial flows lead to the formation of bound states between spinning colloids that are stabilized through near-field hydrodynamic and chemical interactions. At a collective level, we demonstrate that added diffusiophoretic interactions cause a loss in structural cohesion of the circulating clusters and promote expansion, while preserving global cluster inter-connectivity. The expanded cluster state is characterized by the formation of a dynamic interconnected network promoted by axi-asymmetric interactions around particles with attractive dipolar interactions dominating along the direction of the magnetic moment. This process is observed to be entirely reversible, offering external control over the emergent dynamics in dense chiral fluids, paving the way for new self-organization routes in chiral fluids and broader forms of active matter.

Quantum phase transitions and cat states in cavity-coupled quantum dots

We study double quantum dots coupled to a quasistatic cavity mode with high mode-volume compression allowing for strong light-matter coupling. Besides the cavity-mediated interaction, electrons in different double quantum dots interact with each other via dipole-dipole (Coulomb) interaction. There is a first-order cavity-induced ferroelectric quantum phase transition when the attractive dipolar interaction is smaller than the critical value defined by the energy splitting in DQDs and a smooth transition, otherwise. We show that, in the smooth transition region, both the ground and the first excited states of an array of double quantum dots are cat states. Such states are actively discussed as high-fidelity qubits for quantum computing, and thus our proposal provides a platform for semiconductor implementation of such qubits. We also calculate gauge-invariant observables such as the net dipole moment, the optical conductivity, and the absorption spectrum beyond the semiclassical approximation. The results are robust against cavity losses and variations of system parameters. Published by the American Physical Society 2024

Observation of quadrupolar and dipolar excitons in a semiconductor heterotrilayer.

Van der Waals (vdW) materials have opened up many avenues for discovery through layer assembly, as epitomized by interlayer dipolar excitons that exhibit electrically tunable luminescence, lasing and exciton condensation. Extending interlayer excitons to more vdW layers, however, raises fundamental questions concerning coherence within excitons and coupling between moiré superlattices at multiple interfaces. Here, by assembling angle-aligned WSe2/WS2/WSe2 heterotrilayers, we demonstrate the emergence of quadrupolar excitons. We confirm the exciton's quadrupolar nature by the decrease in its energy of 12 meV from coherent hole tunnelling between the two outer layers, its tunable static dipole moment under an external electric field and the reduced exciton-exciton interactions. At high exciton density, we also see signatures of a phase of oppositely aligned dipolar excitons, consistent with a staggered dipolar phase predicted to be driven by attractive dipolar interactions. Our demonstration paves the way for discovering emergent exciton orderings for three vdW layers and beyond.

Effect of Transverse Confinement on a Quasi-One-Dimensional Dipolar Bose Gas

We study a gas of bosonic dipolar atoms in the presence of a transverse harmonic trapping potential by using an improved variational Bethe ansatz, which includes the transverse width of the atomic cloud as a variational parameter. Our calculations show that the system behavior evolves from quasi-one dimensional to a strictly one-dimensional one by changing the atom–atom interaction, or the axial density, or the frequency of the transverse confinement. Quite remarkably, in the droplet phase induced by the attractive dipolar interaction the system becomes sub-one dimensional when the transverse width is smaller than the characteristic length of the transverse harmonic confinement.

Numerical characterization of inter-core coalescence by AC dielectrophoresis in double-emulsion droplets.

The utilization of an alternating current electric field provides a good means to achieve controlled coalescence between paired inner cores encapsulated in water-in-oil-in-water double-emulsion (DE) droplets. Although previous studies have experimentally determined the conditions under which inter-core electrokinetic fusion occurs, the transient interfacial dielectrophoretic (DEP) dynamics key to understand the underlying fluid mechanics is still unclear from a physical point of view. By coupling DEP motion of two-phase flow to phase-field formulation, bulk-coupled numerical simulations are conducted to characterize the spatial-temporal evolution of the surface charge wave and the resulting nonlinear electrical force induced at both the core/shell and medium/shell oil/water interfaces. The effect of interfacial charge relaxation and droplet geometry on inter-core attractive dipolar interaction is investigated within a wide parametric space, and four distinct device operation modes, including normal inter-core fusion, shell elongation, partial core leakage, and complete core release, are well distinguished from one another by flow regime argumentation. Our results herein reveal for the first time the hitherto unknown transient electrohydrodynamic fluid motion of DE droplet driven by Maxwell-Wagner structural polarization. The dynamic simulation method proposed in present study points out an effective outlet to predict the nonlinear electrokinetic behavior of multicore DE droplets for realizing a more controlled triggering of microscale reactions for a wide range of applications in drug discovery, skin care, and food industry.

Repulsive dynamics of strongly attractive one-dimensional quantum gases

We analyze the dynamics of one-dimensional quantum gases with strongly attractive contact interactions. We specify a class of initial states for which attractive forces effectively act as strongly repulsive ones during the time evolution. Our findings extend the theoretical results on the super-Tonks-Girardeau gas to a highly nonequilibrium dynamics. The novel mechanism is illustrated on the prototypical problem of the domain stability in a two-component Fermi gas. We also discuss nonlocal interactions and analyze universality of the presented results. Moreover, we use our conclusions to argue for the existence of metastable quantum droplets in the regime of strongly attractive contact and attractive dipolar interactions.

Attractive and repulsive dipolar interaction in bilayers of indirect excitons

We explore attractive dipolar interaction in indirect excitons (IXs). For one layer of IXs in a single pair of coupled quantum wells (CQW), the out-of-plane IX electric dipoles lead to repulsive dipolar interaction between IXs. The attractive dipolar interaction between IXs is realized in a 2-CQW heterostructure with two IX layers in two separated CQW pairs. We found both in experimental measurements and theoretical simulations that increasing density of IXs in one layer causes a monotonic energy reduction for IXs in the other layer. We also found an in-plane shift of a cloud of IXs in one layer towards a cloud of IXs in the other layer. This behaviour is qualitatively consistent with attractive dipolar interaction. The measured IX energy reduction and IX cloud shift are higher than the values given by the correlated liquid theory.

Attractive interactions, molecular complexes, and polarons in coupled dipolar exciton fluids

Dipolar (or spatially indirect) excitons (IXs) in semiconductor double quantum well (DQW) subjected to an electric field are neutral species with a dipole moment oriented perpendicular to the DQW plane. Here, we theoretically study interactions between IXs in stacked DQW bilayers, where the dipolar coupling can be either attractive or repulsive depending on the relative positions of the particles. By using microscopic band structure calculations to determine the electronic states forming the excitons, we show that the attractive dipolar interaction between stacked IXs deforms their electronic wave function, thereby increasing the inter-DQW interaction energy and making the IX electrically polarizable. Many-particle effects interaction are addressed by considering the coupling between a single IX in one of the DQWs to a cloud of IXs in the other DQW, which is modeled either as a closed-packed lattice or as a continuum IX fluid. We find that the lattice model yields IX interlayer binding energies decreasing with increasing lattice density. This behavior is due to the dominating role of the intra-DQW dipolar repulsion, which prevents more than one exciton from entering the attractive region of the inter-DQW coupling. Finally, both models shows that the single IX distorts the distribution of IXs in the adjacent DQW, thus inducing the formation of an IX polaron. While the interlayer binding energy reduces with IX density for lattice polarons, the continuous polaron model predicts a non-monotonous dependence on density in semi-quantitative agreement with a recent experimental study [cf. Hubert {\it et al.}, Phys. Rev. {\bf X}9, 021026 (2019)].

Topological supersolidity of dipolar Fermi gases in a spin-dependent optical lattice

We investigate the topological supersolid states of dipolar Fermi gases trapped in a spin-dependent 2D optical lattice. Our results show that topological supersolid states can be achieved via the combination of topological superfluid states with the stripe order. Different from the general held belief that supersolid state in fermionic system can only survive with simultaneous coexistence of the repulsive and attractive dipolar interaction. We demonstrate that it can be maintained when the dipolar interaction is attractive in both x and y direction. By adjusting the ratio of hopping amplitude between different directions and dipolar interaction strength U, the system will undergo a phase transition among px + ipy superfluid state, py-wave superfluid state, and the topological supersolid state. The supersolid state in the attractive environment is proved to be stable by the positive sign of the inverse compressibility. We also design an experimental protocol to realize the staggered next-next-nearest-neighbor hopping via the laser assisted tunneling technique, which is the key to simulate the spin-dependent potential.

Variational Bethe ansatz approach for dipolar one-dimensional bosons

We propose a variational approximation to the ground state energy of a one-dimensional gas of interacting bosons on the continuum based on the Bethe Ansatz ground state wavefunction of the Lieb-Liniger model. We apply our variational approximation to a gas of dipolar bosons in the single mode approximation and obtain its ground state energy per unit length. This allows for the calculation of the Tomonaga-Luttinger exponent as a function of density and the determination of the structure factor at small momenta. Moreover, in the case of attractive dipolar interaction, an instability is predicted at a critical density, which could be accessed in lanthanide atoms.

Formation of Colloidal Copper Indium Sulfide Nanosheets by Two-Dimensional Self-Organization.

Colloidal 2D semiconductor nanosheets (NSs) are an interesting new class of materials due to their unique properties. However, synthesis of these NSs is challenging, and synthesis procedures for materials other than the well-known Pb- and Cd-chalcogenides are still underdeveloped. In this paper, we present a new approach to make copper indium sulfide (CIS) NSs and study their structural and optical properties. The CIS NSs form via self-organization and oriented attachment of 2.5 nm chalcopyrite CuInS2 nanocrystals (NCs), yielding triangular- and hexagonal-shaped NSs with a thickness of ∼3 nm and lateral dimensions ranging from 20 to 1000 nm. The self-organization is induced by fast cation extraction, leading to attractive dipolar interactions between the NCs. Primary amines play a crucial role in the formation of the CIS NSs, both by forming in situ the cation extracting agent, and by preventing the attachment of NCs to the top and bottom facets of the NSs. Moreover, DFT calculations reveal that the amines are essential to stabilize the covellite crystal structure of the product CIS NSs. The NSs are indium-deficient and the off-stoichiometry gives rise to a plasmon resonance in the NIR spectral window.

Adiabatic Mach–Zehnder interferometer in a dipolar spin-1 condensate

We propose and analyze a realizable scheme for performing a Heisenberg-limited Mach–Zehnder interferometry with a dipolar spin-1 condensate. Based upon adiabatic processes of sweeping the transverse magnetic field, we demonstrate a perfect phase transition, which accomplishes the beam splitter, phase shifter and recombiner as for a Mach–Zehnder interferometer. The attractive dipolar interaction ensures the existence of a path-entangled state which enhances the phase measurement precision to the Heisenberg limit. We also study the spin squeezing of the state generated in the beam splitter and show that the spin squeezing exhibits an extremum near the critical point of phase transition.

Cooperative and Reversible Anisotropic Assembly of Gold Nanoparticles by Modulation of Noncovalent Interparticle Interactions

AbstractControlled and reversible anisotropic self‐assembly of gold nanoparticles (GNPs) is achieved by ligand exchange with concentrations of ligand below that needed for their complete capping, that is, using substoichiometric ligand coverages. A thoughtful rationale of the ligand chemical structure and control over exchange conditions have been pursued to foster a reversible process grounded on the cooperative balance between attractive, and repulsive interactions. The gradual replacement of the electrostatic and steric repulsions between the GNPs with attractive dipolar interactions and enhanced steric repulsions is accomplished by ligand exchange with an oligo (ethylene glycol) alkanethiol. The modulation of interparticle interactions is driven by the extent of ligand substitution and allows the reversible assembly of nanoparticles and tuning of their optical properties.

Nonlinear localized modes in dipolar Bose–Einstein condensates in two-dimensional optical lattices

We analyze the existence and properties of discrete localized excitations in a Bose–Einstein condensate loaded into a periodic two-dimensional optical lattice, when a dipolar interaction between atoms is present. The dependence of the Number of Atoms (Norm) on the energy of solutions is studied, along with their stability. Two important features of the system are shown, namely, the absence of the Norm threshold required for localized solutions to exist in finite 2D systems, and the existence of regions in the parameter space where two fundamental solutions are simultaneously unstable. This feature enables mobility of localized solutions, which is an uncommon feature in 2D discrete nonlinear systems. With attractive dipolar interaction, a non-trivial behavior of the Norm dependence is obtained, which is well described by an analytical model.

Out-of-equilibrium states and quasi-many-body localization in polar lattice gases

The absence of energy dissipation leads to an intriguing out-of-equilibrium dynamics for ultracold polar gases in optical lattices, characterized by the formation of dynamically-bound on-site and inter-site clusters of two or more particles, and by an effective blockade repulsion. These effects combined with the controlled preparation of initial states available in cold gases experiments can be employed to create interesting out-of-equilibrium states. These include quasi-equilibrated effectively repulsive 1D gases for attractive dipolar interactions and dynamically-bound crystals. Furthermore, non-equilibrium polar lattice gases can offer a promising scenario for the study of many-body localization in the absence of quenched disorder. This fascinating out-of-equilibrium dynamics for ultra-cold polar gases in optical lattices may be accessible in on-going experiments.

Quench dynamics of dipolar fermions in a one-dimensional harmonic trap

We study a system of few fermions in a one-dimensional harmonic trap, and focus on the case of dipolar majority particles in contact with a single impurity. The impurity is used both for quenching the system, and for tracking the system evolution after the quench. Employing exact diagonalization, we investigate relaxation and thermalization properties. In the absence of dipolar interactions, the system is near integrability, and the dynamics remains oscillatory even on long time scales. On the other hand, repulsive as well as attractive dipolar interactions lead to quick relaxation to the diagonal ensemble average which is significantly different from corresponding thermal averages. A Wigner-shaped level spacing distribution indicates level repulsion and thus chaotic dynamical behavior due to the presence of dipolar interactions.

Dual Stress and Thermally Driven Mechanical Properties of the Same Organic Crystal: 2,6-Dichlorobenzylidene-4-fluoro-3-nitroaniline.

An elastic organic crystal, 2,6-dichlorobenzylidine-4-fluoro-3-nitroaniline (DFNA), which also shows thermosalient behavior, is studied. The presence of these two distinct properties in the same crystal is unusual and unprecedented because they follow respectively from isotropy and anisotropy in the crystal packing. Therefore, while both properties lead from the crystal structure, the mechanisms for bending and thermosalience are quite independent of one another. Crystals of the low-temperature (α) form of the title compound are bent easily without any signs of fracture with the application of deforming stress, and this bending is within the elastic limit. The crystal structure of the α-form was determined (P21/c, Z = 4, a = 3.927(7) Å, b = 21.98(4) Å, c = 15.32(3) Å). There is an irreversible phase transition at 138 °C of this form to the high-temperature β-form followed by melting at 140 °C. Variable-temperature X-ray powder diffraction was used to investigate the structural changes across the phase transition and, along with an FTIR study, establishes the structure of the β-form. A possible rationale for strain build-up is given. Thermosalient behavior arises from anisotropic changes in the three unit cell parameters across the phase transition, notably an increase in the b axis parameter from 21.98 to 22.30 Å. A rationale is provided for the existence of both elasticity and thermosalience in the same crystal. FTIR studies across the phase transition reveal important mechanistic insights: (i) increased π···π repulsions along [100] lead to expansion along the a axis; (ii) change in alignment of C-Cl and NO2 groups result from density changes; and (iii) competition between short-range repulsive (π···π) interactions and long-range attractive dipolar interactions (C-Cl and NO2) could lie at the origin of the existence of two distinctive properties.

Trapping and chaining self-assembly of colloidal polystyrene particles over a floating electrode by using combined induced-charge electroosmosis and attractive dipole-dipole interactions.

We propose a novel low-frequency strategy to trap 10 μm colloidal polystyrene (PS) particles of small buoyancy velocity on the surface of a floating electrode, on the basis of combined induced-charge electroosmotic (ICEO) flow and dipole-dipole chaining phenomenon. For field frequencies of 5-50 Hz, much lower than the reciprocal RC time scale, double-layer polarization makes electric field lines pass around the 'insulating' surface of the ideally polarizable floating electrode. Once the long-range ICEO convective micro-vortexes transport particles quickly from the bulk fluid to the electrode surface, neighbouring particles aligned along the local horizontal electric field attract one another by attractive dipolar interactions, and form arrays of particle chains that are almost parallel with the applied electric field. Most importantly, this low-frequency trapping method takes advantage of the dielectrophoretic (DEP) particle-particle interaction to enhance the downward buoyancy force of this dipolar chaining assembly structure, in order to overcome the upward ICEO fluidic drag and realize stable particle trapping around the flow stagnation region. For the sake of comparison, the field frequency is further raised far above the DC limit. At the intermediate frequencies of 200 Hz-2 kHz, this trapping method fails to work, since the normal electric field component emanates from the conducting electrode surface. Besides, at high field frequencies (>3 kHz), particles can be once again effectively trapped at the electrode center, though with a compact (3 kHz) or disordered (10 kHz) 2D packing state on the electrode surface and mainly governed by the short-range negative DEP force field, resulting in requiring a much longer trapping time. To gain a better interpretation of the various particle behaviours observed in experiments, we develop a theoretical framework that takes into account both Maxwell-Wagner interfacial charge relaxation at the particle/electrolyte interface and the field-induced double-layer polarization at the electrode/electrolyte interface, and apply it to quantify the particle-particle electrokinetic interactions. With this simple geometrical configuration of a floating electrode, our results provide a new way to realize trapping of colloidal particles with a small buoyancy velocity under the combined action of ICEO flow and an attractive dipole-dipole interaction.

Polymer-Filler Interphase Dynamics and Reinforcement of Elastomer Nanocomposites

The effect of polymer-filler interaction on interphase dynamics between filler particles in elastomer nanocomposites and the mechanisms of rubber reinforcement by carbon black (CB) are investigated with different techniques. To determine how polymer-filler interface influences the properties of the system, CB black was modified with the ionic liquid (IL) 1-allyl-3-methylimidazolium chloride (AMIC) and mixed with different, more or less, polar elastomers. For typical diene-elastomers (EPDM, SBR), this modification leads to a decreased polymer-filler coupling strength due to the coverage of active sites at the CB surface by AMIC. This is demonstrated by evaluating the energy site distribution from static gas adsorption isotherms with the polymer analogues gas 1-Butene. However, an improvement of polymer filler coupling was determined in the case of saturated, polar rubbers (HNBR) due to attractive dipolar interactions between the polar units of the polymer and the strongly adsorbed IL at the CB surface. The different couplings affect the polymer-filler interphase dynamics between filler particles, which determines the properties of the filler network and filler-filler bonds. To describe the effect of CB surface modification quantitatively, the Dynamic Flocculation Model (DFM) has been used to calculate polymer- and filler-specific material parameters from cyclic stress-strain measurements. The fitted data deliver a coherent picture of filler-filler- and polymer-filler couplings showing a characteristic dependence on rubber polarity. A confirmation of the effect of surface modification on the strength of filler-filler bonds is obtained by nonequilibrium molecular dynamics (MD) simulations of bond rupture under tension. They also provide indications for a glassy-like behavior of strongly confined polymer layers between attractive walls.

Stable colloids at the isoelectric point: Dipolar vs. electrostatic interactions

HypothesisThe strange stability of some colloid systems at the isoelectric point may be explained by interparticle electrostatic interactions (attractive and repulsive) of different electric charge patches on the particles’ surface, related to differences of their surface structure and possibly to adsorption of charged species on them. The coincidence of the minimum colloid stability with the electro-optically observed minimum of the particle electric polarizability (EP) is not in favor of attractive interparticle dipolar interactions playing a major role for the stability as stated before [1]. ExperimentsAqueous dispersions of rod-like palygorskite particles+surfactant cetyl pyridinium chloride (CPC) were studied at different CPC concentrations by optic, electro-optic and microelectrophoretic methods. Thus the CPC concentration dependences of the stability, EP and ζ-potential were established. FindingsLowest colloid stability at considerable ζ-potentials (about −30mV) well below the isoelectric point was found in Ref. [1]. The CPC concentrations, at which the lowest stability was observed experimentally, corresponded well to that of a minimum value of the EP. The new hypothesis and interpretation for the major importance of electrostatic interactions are in good accord with the present day knowledge in Colloid Science for deviations from the Derjaguin–Landau–Verway–Overbeek (DLVO) theory of colloid stability.