Many-body Interactions Research Articles

Collective dynamics of active dumbbells near a circular obstacle.

In this article, we present the collective dynamics of active dumbbells in the presence of a static circular obstacle using Brownian dynamics simulation. The active dumbbells aggregate on the surface of a circular obstacle beyond a critical radius. The aggregation is non-uniform along the circumference, and the aggregate size increases with the activity (Pe) and the curvature radius (Ro). The dense aggregate of active dumbbells displays persistent rotational motion with a certain angular speed, which linearly increases with activity. Furthermore, we show a strong polar ordering of the active dumbbells within the aggregate. The polar ordering exhibits long-range correlation, with the correlation length corresponding to the aggregate size. Additionally, we show that the residence time of an active dumbbell on the obstacle surface increases rapidly with area fraction due to many-body interactions that lead to a slowdown of the rotational diffusion. This article further considers the dynamical behavior of a tracer particle in the solution of active dumbbells. Interestingly, the speed of the passive tracer particle displays a crossover from monotonically decreasing to increasing with the size of the tracer particle upon increasing the dumbbells' speed. Furthermore, the effective diffusion of the tracer particle displays non-monotonic behavior with the area fraction; the initial increase in diffusivity is followed by a decrease for a larger area fraction.

High density electron doping in boron-doped twisted bilayer graphene: a ladder to extended flat-band

Realizing Von Hove singularity (VHS) and extended flat bands of graphene near the Fermi level (EF) to explore many-body interactions with a high tendency towards superconductivity.

Pattern and waves on 2D-Kuramoto model with many-body interactions

In this paper, the 2D-Kuramoto model with many-body interactions is studied. The study found that a certain oscillator will generate a spiral spin wave centered on itself after a natural frequency mutation occurs. The interaction of spiral spin waves produced by multiple such oscillators will produce a new waveform. In order to analyze the cause of this spiral spin wave, we constructed a minimal model. In this minimal model, the nature of the fixed point is analyzed, and the saddle-node bifurcation will occur in the system. We describe the process of this saddle-node bifurcation in detail. Finally, it is concluded that the many-body interactions promote the generation of spiral spin waves.

Analysis of phase stability and chemical segregation in the Mo-V alloys using a generalized embedded atom method potential

A new interatomic potential for the Mo-V system is introduced to facilitate the study of phase stability and mechanical properties at lower temperatures. This potential is based on a generalization of the embedded atom method and includes contributions from embedding energy, explicit two- and three-body interactions and nonlocal many-body interaction terms. The parameters of the potential are optimized by using data from ab initio density functional theory (DFT) calculations. The potential is rigorously validated across a range of physical properties, such as elastic constants, equation of states, phonon dispersion curves, point defect properties and melting temperatures for different compositions. Even though our potential is trained on a small dataset, its accuracy is comparable to available machine learning potentials for Mo and V. Our results show that an ordered B2 phase is stable at low temperatures in alloys containing 50% V, but the solid solution phase is stable above 800 K. However, such long-range ordering is not observed in V-rich or Mo-rich alloys. In addition, our results show that V segregates to dislocation cores and grain boundaries.

High-order exciton complexes induced by an interlayer carrier transfer in 2D van der Waals heterostructures.

High-order correlated excitonic states, such as biexciton, charged biexciton, and polaron, hold a promising platform in contemporary quantum and nonlinear optics due to their large Bohr radii and thus strong nonlinear interactions. The recently found 2D TMDs further give such excitonic states additional valley properties, with bound state of excitons in opposite valleys in momentum spaces. Despite great efforts that have been made on emission properties of excitonic states, their absorption features, especially the ultrafast absorption dynamics, are rarely reported. Here, we reported the enhanced optical absorption of the high-order charged-excitonic states in monolayer WS2, including singlet, triplet, and semidark trions (3-particle state), and charged biexcitons (5-particle state), by utilizing the interlayer charge transfer-induced photo-doping effect in the graphene-WS2 heterostructure. Depending on recombination rates of doping electrons, absorption intensities of charged complexes exhibit ultrafast decay dynamics, with lifetimes of several picoseconds. Due to many-body interaction, both increasing pump intensity and lattice temperature can broaden these fine excitonic absorption peaks and even reverse the shape of the transient absorption spectrum.

Coherent Phonon Assisted Ultrafast Order-Parameter Reversal and Hidden Metallic State in Ta_{2}NiSe_{5}.

The nonequilibrium dynamics during photoinduced insulator-to-metal transition (IMT) in the excitonic insulator (EI) candidate Ta_{2}NiSe_{5} have been investigated, which reproduce the timescale and spectral features of the ultrafast switch and reveal intricate many-body interactions involving multidegrees of freedom. The key role of lattice order parameter (OP) reversal, occurring on a timescale comparable to that of purely electronic processes (<100 fs), is identified. This reversal is enabled by the anharmonic interactions between EI-OP-coupled phonons and the conventional coherent phonons, leading to a modified potential energy landscape and a high-frequency mode up-conversion. The phonon excitation depends on the dynamics of photocarriers distributed around the Fermi level, and thus intertwines with the excitonic quenching and the complete gap collapse. These findings provide a comprehensive understanding of exciton-phonon dynamics in correlated quantum materials.

Superradiant Detection of Microscopic Optical Dipolar Interactions.

The interaction between light and cold atoms is a complex phenomenon potentially featuring many-body resonant dipole interactions. A major obstacle toward exploring these quantum resources of the system is macroscopic light propagation effects, which not only limit the available time for the microscopic correlations to locally build up, but also create a directional, superradiant emission background whose variations can overwhelm the microscopic effects. In this Letter, we demonstrate a method to perform "background-free" detection of the microscopic optical dynamics in a laser-cooled atomic ensemble. This is made possible by transiently suppressing the macroscopic optical propagation over a substantial time, before a recall of superradiance that imprints the effect of the accumulated microscopic dynamics onto an efficiently detectable outgoing field. We apply this technique to unveil and precisely characterize a density-dependent, microscopic dipolar dephasing effect that generally limits the lifetime of optical spin-wave order in ensemble-based atom-light interfaces.

Quantitative measure of correlation strength among intertwined many-body interactions

Quantitative measure of correlation strength among intertwined many-body interactions

Circular dichroism in two-dimensional BC6N and B3C2N3 in absence of intervalley excitonic coupling

Two-dimensional (2D) noncentrosymmetric systems offer potential opportunities for exploiting the valley degrees of freedom for advanced information processing, owing to non-zero Berry curvature. However, such valley polarization in 2D materials is crucially governed by the intervalley excitonic scattering in momentum space due to reduced electronic degrees of freedom and consequent enhanced electronic correlation. Here, we study the valley excitonic properties of two 2D noncentrosymmetric complementary structures, namely, BC6N and B3C2N3 using first principles-based GW calculations combined with the Bethe–Salpeter equation, that brings the many-body interactions among the quasiparticles. The k-resolved oscillator strength of their first bright exciton indicates their ability to exhibit valley polarization under the irradiation of circularly polarized light of different chiralities. Both the systems show significant singlet excitonic binding energies of 0.74 eV and 1.31 eV, respectively. Higher stability of dark triplet excitons as compared to the singlet one can lead to higher quantum efficiency in both the systems. The combination of large excitonic binding energies and the valley polarization ability with minimal intervalley scattering make them promising candidates for applications in advanced optical devices and information storage technologies.

Many-body potential for simulating the self-assembly of polymer-grafted nanoparticles in a polymer matrix

Many-body interactions between polymer-grafted nanoparticles (NPs) play a key role in promoting their assembly into low-dimensional structures within polymer melts, even when the particles are spherical and isotropically grafted. However, capturing such interactions in simulations of NP assembly is very challenging because explicit modeling of the polymer grafts and melt chains is highly computationally expensive, even using coarse-grained models. Here, we develop a many-body potential for describing the effective interactions between spherical polymer-grafted NPs in a polymer matrix through a machine-learning approach. The approach involves using permutationally invariant polynomials to fit two- and three-body interactions derived from the potential of mean force calculations. The potential developed here reduces the computational cost by several orders of magnitude, thereby, allowing us to explore assembly behavior over large length and time scales. We show that the potential not only reproduces previously known assembled phases such as 1D strings and 2D hexagonal sheets, which generally cannot be achieved using isotropic two-body potentials, but can also help discover interesting phases such as networks, clusters, and gels. We demonstrate how each of these assembly morphologies intrinsically arises from a competition between two- and three-body interactions. Our approach for deriving many-body effective potentials can be readily extended to other colloidal systems, enabling researchers to make accurate predictions of their behavior and dissect the role of individual interaction energy terms of the overall potential in the observed behavior.

Second quantization of many-body dispersion interactions for chemical and biological systems

The many-body dispersion (MBD) framework is a successful approach for modeling the long-range electronic correlation energy and optical response of systems with thousands of atoms. Inspired by field theory, here we develop a second-quantized MBD formalism (SQ-MBD) that recasts a system of atomic quantum Drude oscillators in a Fock-space representation. SQ-MBD provides: (i) tools for projecting observables (interaction energy, transition multipoles, polarizability tensors) on coarse-grained representations of the atomistic system ranging from single atoms to large structural motifs, (ii) a quantum-information framework to analyze correlations and (non)separability among fragments in a given molecular complex, and (iii) a path toward the applicability of the MBD framework to molecular complexes with even larger number of atoms. The SQ-MBD approach offers conceptual insights into quantum fluctuations in molecular systems and enables direct coupling of collective plasmon-like MBD degrees of freedom with arbitrary environments, providing a tractable computational framework to treat dispersion interactions and polarization response in intricate systems.

Coion exclusion properties of cation exchange membranes in 2:1 divalent salt solutions

The selectivity of ion exchange membranes hinges on their capacity to exclude coions. Yet, understanding how they reject coions in multivalent salt solutions remains challenging. This study presents a new molecular theory to understand coion exclusion. It examines counterion and coion condensation, including electrosteric effects. Supported by experimental data [Gokturk et al., Nat. Commun., 13 (2022)], we analyze cation exchange membrane potential in a 2:1 salt solution, revealing insights into coion selectivity and exclusion mechanisms. Notably, our theory deviates from earlier research by accommodating condensed divalent counterions that bind to one or two fixed-charged monomers. Additionally, we account for many-body electrostatic interactions, allowing the former to bind to sorbed coions. Our findings highlight the importance of coion condensation, especially in low-concentration salt conditions where coions are mainly condensed. This effect becomes less significant as the external solution concentration rises. These findings clarify the suitability of the ideal Donnan model in high-concentration salts, but its accuracy decreases in low-concentration situations. To summarize, our study emphasizes the need to account for counterion and coion condensation to understand membrane selectivity in low-concentration multivalent salt solutions.

Tipping the Balance Between the bcc and fcc Phase Within the Alkali and Coinage Metal Groups.

Why the Group 1 elements crystallize in the body-centered cubic (bcc) structure, and the iso-electronic Group 11 elements in the face-centered cubic (fcc) structure, remains a mystery. Here we show that a delicate interplay between many-body effects, vibrational contributions and dispersion interactions obtained from relativistic density functional theory offers an answer to this long-standing controversy. It also sheds light on the Periodic Table of Crystal Structures. A smooth diffusionless transition through cuboidal lattices gives a detailed insight into the bcc→fcc phase transition for the Groups 1 and 11 elements.

Coarse-Grained Many-Body Potentials of Ligand-Stabilized Nanoparticles from Machine-Learned Mean Forces.

Colloidal nanoparticles self-assemble into a variety of superstructures with distinctive optical, structural, and electronic properties. These nanoparticles are usually stabilized by a capping layer of organic ligands to prevent aggregation in the solvent. When the ligands are sufficiently long compared to the dimensions of the nanocrystal cores, the effective coarse-grained forces between pairs of nanoparticles are largely affected by the presence of neighboring particles. In order to efficiently investigate the self-assembly behavior of these complex colloidal systems, we propose a machine-learning approach to construct effective coarse-grained many-body interaction potentials. The multiscale methodology presented in this work constitutes a general bottom-up coarse-graining strategy where the coarse-grained forces acting on coarse-grained sites are extracted from measuring the vectorial mean forces on these sites in reference fine-grained simulations. These effective coarse-grained forces, i.e., gradients of the potential of mean force or of the free-energy surface, are represented by a simple linear model in terms of gradients of structural descriptors, which are scalar functions that are rotationally invariant. In this way, we also directly obtain the free-energy surface of the coarse-grained model as a function of all coarse-grained coordinates. We expect that this simple yet accurate coarse-graining framework for the many-body potential of mean force will enable the characterization, understanding, and prediction of the structure and phase behavior of relevant soft-matter systems by direct simulations. The key advantage of this method is its generality, which allows it to be applicable to a broad range of systems. To demonstrate the generality of our method, we also apply it to a colloid-polymer model system, where coarse-grained many-body interactions are pronounced.

Topology and dynamics of higher-order multiplex networks

Higher-order networks are gaining significant scientific attention due to their ability to encode the many-body interactions present in complex systems. However, higher-order networks have the limitation that they only capture many-body interactions of the same type. To address this limitation, we present a mathematical framework that determines the topology of higher-order multiplex networks and illustrates the interplay between their topology and dynamics. Specifically, we examine the diffusion of topological signals associated not only to the nodes but also to the links and to the higher-dimensional simplices of multiplex simplicial complexes. We leverage on the ubiquitous presence of the overlap of the simplices to couple the dynamics among multiplex layers, introducing a definition of multiplex Hodge Laplacians and Dirac operators. We show that the spectral properties of these operators determine higher-order diffusion on higher-order multiplex networks and encode their multiplex Betti numbers. Our numerical investigation of the spectral properties of synthetic and real (connectome, microbiome) multiplex simplicial complexes indicates that the coupling between the layers can either speed up or slow down the higher-order diffusion of topological signals. This mathematical framework is very general and can be applied to study generic higher-order systems with interactions of multiple types. In particular, these results might find applications in brain networks which are understood to be both multilayer and higher-order.

GAABind: a geometry-aware attention-based network for accurate protein-ligand binding pose and binding affinity prediction.

Protein-ligand interactions are increasingly profiled at high-throughput, playing a vital role in lead compound discovery and drug optimization. Accurate prediction of binding pose and binding affinity constitutes a pivotal challenge in advancing our computational understanding of protein-ligand interactions. However, inherent limitations still exist, including high computational cost for conformational search sampling in traditional molecular docking tools, and the unsatisfactory molecular representation learning and intermolecular interaction modeling in deep learning-based methods. Here we propose a geometry-aware attention-based deep learning model, GAABind, which effectively predicts the pocket-ligand binding pose and binding affinity within a multi-task learning framework. Specifically, GAABind comprehensively captures the geometric and topological properties of both binding pockets and ligands, and employs expressive molecular representation learning to model intramolecular interactions. Moreover, GAABind proficiently learns the intermolecular many-body interactions and simulates the dynamic conformational adaptations of the ligand during its interaction with the protein through meticulously designed networks. We trained GAABind on the PDBbindv2020 and evaluated it on the CASF2016 dataset; the results indicate that GAABind achieves state-of-the-art performance in binding pose prediction and shows comparable binding affinity prediction performance. Notably, GAABind achieves a success rate of 82.8% in binding pose prediction, and the Pearson correlation between predicted and experimental binding affinities reaches up to 0.803. Additionally, we assessed GAABind's performance on the severe acute respiratory syndrome coronavirus 2 main protease cross-docking dataset. In this evaluation, GAABind demonstrates a notable success rate of 76.5% in binding pose prediction and achieves the highest Pearson correlation coefficient in binding affinity prediction compared with all baseline methods.

Salt Effects on Caffeine across Concentration Regimes.

Salts affect the solvation thermodynamics of molecules of all sizes; the Hofmeister series is a prime example in which different ions lead to salting-in or salting-out of aqueous proteins. Early work of Tanford led to the discovery that the solvation of molecular surface motifs is proportional to the solvent accessible surface area (SASA), and later studies have shown that the proportionality constant varies with the salt concentration and type. Using multiscale computer simulations combined with vapor-pressure osmometry on caffeine-salt solutions, we reveal that this SASA description captures a rich set of molecular driving forces in tertiary solutions at changing solute and osmolyte concentrations. Central to the theoretical work is a new potential energy function that depends on the instantaneous surface area, salt type, and concentration. Used in, e.g., Monte Carlo simulations, this allows for a highly efficient exploration of many-body interactions and the resulting thermodynamics at elevated solute and salt concentrations.

Time, momentum, and energy resolved pump-probe tunneling spectroscopy of two-dimensional electron systems

Real-time probing of electrons can uncover intricate relaxation mechanisms and many-body interactions in strongly correlated materials. Here, we introduce time, momentum, and energy resolved pump-probe tunneling spectroscopy (Tr-MERTS). The method allows the injection of electrons at a particular energy and observation of their subsequent decay in energy-momentum space. Using Tr-MERTS, we visualize electronic decay processes, with lifetimes from tens of nanoseconds to tens of microseconds, in Landau levels formed in a GaAs quantum well. Although most observed features agree with simple energy-relaxation, we discovered a splitting in the nonequilibrium energy spectrum in the vicinity of a ferromagnetic state. An exact diagonalization study suggests that the splitting arises from a maximally spin-polarized state with higher energy than a conventional equilibrium skyrmion. Furthermore, we observe time-dependent relaxation of the splitting, which we attribute to single-flipped spins forming skyrmions. These results establish Tr-MERTS as a powerful tool for studying the properties of a 2DES beyond equilibrium.

Enhanced optical conductivity and many-body effects in strongly-driven photo-excited semi-metallic graphite

The excitation of quasi-particles near the extrema of the electronic band structure is a gateway to electronic phase transitions in condensed matter. In a many-body system, quasi-particle dynamics are strongly influenced by the electronic single-particle structure and have been extensively studied in the weak optical excitation regime. Yet, under strong optical excitation, where light fields coherently drive carriers, the dynamics of many-body interactions that can lead to new quantum phases remain largely unresolved. Here, we induce such a highly non-equilibrium many-body state through strong optical excitation of charge carriers near the van Hove singularity in graphite. We investigate the system’s evolution into a strongly-driven photo-excited state with attosecond soft X-ray core-level spectroscopy. We find an enhancement of the optical conductivity of nearly ten times the quantum conductivity and pinpoint it to carrier excitations in flat bands. This interaction regime is robust against carrier-carrier interaction with coherent optical phonons acting as an attractive force reminiscent of superconductivity. The strongly-driven non-equilibrium state is markedly different from the single-particle structure and macroscopic conductivity and is a consequence of the non-adiabatic many-body state.

Emergence and Control of Synchronization in Networks with Directed Many-Body Interactions.

The emergence of collective behaviors in networks of dynamical units in pairwise interaction has been explained as the effect of diffusive coupling. How does the presence of higher-order interaction impact the onset of spontaneous or induced synchronous behavior? Inspired by actuation and measurement constraints typical of physical and engineered systems, we propose a diffusion mechanism over hypergraphs that explains the onset of synchronization through a clarifying analogy with signed graphs. Our findings are mathematically backed by general conditions for convergence to the synchronous state.