arXiv subjects

Robert E. Zillich

Publications and source records attributed to Robert E. Zillich.

At least 19 recordsLinked to original sources

arXiv2026

Non-Additivity of Microwave-Shielded Interactions between Dipolar Molecules

Theoretical models of the effective interactions between microwave-shielded polar molecules typically rely on the assumption of pairwise additivity. In this work, we test the validity of this pairwise approximation by evaluating the exact many-body potential energy for configurations of three and four molecules. We demonstrate that this approximation fails for molecule configurations in the plane of the circularly polarized microwave field. In these planar geometries, many-body effects significantly increase the depth of the attractive potential well and shift the position of the repulsive barrier. Although out-of-plane interactions in three-dimensional arrangements weaken this non-additivity, the effective interactions between microwave-shielded dipoles are not a simple sum of pair interactions. In particular, their attractive well, crucial for self-bound clusters, can only be described by the full many-body potential energy.

cond-mat.quant-gas↗

arXiv2025

Phases of a Bose-Einstein condensate of microwave-shielded dipolar molecules

Bose-Einstein condensation of dipolar molecules can be achieved by shielding loss channels with microwave fields. The microwave coupling can be approximated by effective dipole-dipole interactions with a short-range repulsion. We study properties and stability of these molecular Bose gases with a many-body variational method, the hypernetted-chain Euler-Lagrange method for a wide range of densities and repulsion strengths of the microwave shield. We find a homogeneous gas-like phase which, however, is unstable at low density against density waves: at a critical density, which depends on the repulsion strength, the dipolar fluid undergoes a phase transition to a layer phase. Thus, if the molecular condensate is expanded adiabatically by decreasing the confinement strength, it will spontaneously form layers at the critical density. These quasi-two-dimensional layers can be self-bound, hence form two-dimensional liquids. By varying the microwave shield, the predicted equilibrium densities span more than an order of magnitude.

cond-mat.quant-gas↗

arXiv2025

The bridge function as a functional of the radial distribution function: Operator learning and application

Properties of classical molecular systems can be calculated with integral equation theories based on the Ornstein-Zernike (OZ) equation and a complementing closure relation. One such closure relation is the hyper netted chain (HNC) approximation, which neglects the so-called bridge function. We present a new way to use machine learning to train a deep operator network to predict the bridge function, based on the radial distribution function as input. Bridge functions for the Lennard-Jones fluid are calculated from Monte Carlo simulations in a wide range of densities and temperatures. These results are used to train the deep operator network. This network is employed to improve the HNC closure by the prediction for the bridge function, and the resulting set of equations is solved iteratively. For assessment, we compare the radial distribution function and the pressure, calculated by the viral expression, with Monte Carlo results and standard HNC. We demonstrate that incorporating the neural network based bridge function in the closure relation leads to substantially improved predictions. Universality of our method is demonstrated by comparing results for the hard sphere fluid, calculated with our model trained on the Lennard-Jones fluid, with exact hard sphere results, showing overall good agreement.

cond-mat.stat-mech↗

arXiv2025

Nonadiabatic laser-induced alignment dynamics of alkali dimers on the surface of a helium droplet

Alkali dimers, $\mathrm{Ak}_2$, located on the surface of a helium nanodroplet, are set into rotation through the polarizability interaction with a nonresonant 1-ps-long laser pulse. The time-dependent degree of alignment is recorded using femtosecond-probe-pulse-induced Coulomb explosion into a pair of $\mathrm{Ak}^+$ fragment ions. The results, obtained for $\mathrm{Na}_2$, $\mathrm{K}_2$, and $\mathrm{Rb}_2$ in both the ground state $1 ^1Σ_g^+$ and the lowest-lying triplet state $1 ^3Σ_u^+$, exhibit distinct, periodic revivals with a gradually decreasing amplitude. The dynamics differ from that expected for dimers had they behaved as free rotors. Numerically, we solve the time-dependent rotational Schrödinger equation, including an effective mean-field potential to describe the interaction between the dimer and the droplet. The experimental and simulated alignment dynamics agree well and their comparison enables us to determine the effective rotational constants of the alkali dimers with the exception of $\mathrm{Rb}_2$($1 ^3Σ_u^+$) that only exhibits a prompt alignment peak but no subsequent revivals. For $\mathrm{Na}_2$($1 ^3Σ_u^+$), $\mathrm{K}_2$($1 ^1Σ_g^+$), $\mathrm{K}_2$($1 ^3Σ_u^+$) and $\mathrm{Rb}_2$($1 ^1Σ_g^+$), the alignment dynamics are well-described by a 2D rotor model. We ascribe this to a significant confinement of the internuclear axis of these dimers, induced by the orientation-dependent droplet-dimer interaction, to the tangential plane of their residence point on the droplet.

physics.atm-clus↗

arXiv2025

Interaction quenches in Bose gases studied with a time-dependent hypernetted-chain Euler-Lagrange method

We present a new variational method to study the dynamics of a closed bosonic many-body system, the time-dependent hypernetted-chain Euler-Lagrange method, tHNC . Based on the Jastrow ansatz, it accounts for quantum fluctuations in a non-perturbative way. tHNC scales well with the number of dimensions, as demonstrated by our results on one, two, and three dimensions. We apply the tHNC method to interaction quenches, i.e. sudden changes of the interaction strength, in homogeneous Bose gases. When the quench is strong enough that the final state has roton excitations (as found and predicted for dipolar and Rydberg-dressed Bose-Einstein condensates, respectively), the pair distribution function exhibits stable oscillations. For validation, we compare tHNC results with time-dependent variational Monte Carlo results in one and two dimensions.

cond-mat.quant-gas↗

arXiv2023

Suppression of polaron self-localization by correlations

We investigate self-localization of a polaron in a homogeneous Bose-Einstein condensate in one dimension. This effect, where an impurity is trapped by the deformation that it causes in the surrounding Bose gas, has been first predicted by mean field calculations, but has not been seen in experiments. We study the system in one dimension, where, according to the mean field approximation, the self-localization effect is particularly robust, and present for arbitrarily weak impurity-boson interactions. We address the question whether self-localization is a real effect by developing a variational method which incorporates impurity-boson correlations non-perturbatively and solving the resulting inhomogeneous correlated polaron equations. We find that correlations inhibit self-localization except for very strongly repulsive or attractive impurity-boson interactions. Our prediction for the critical interaction strength for self-localization agrees with a sharp drop of the inverse effective mass to almost zero found in quantum Monte Carlo simulations of polarons in one dimension.

cond-mat.quant-gas↗

arXiv2023

Nonadiabatic Laser-Induced Alignment Dynamics of Molecules on a Surface

We demonstrate that a sodium dimer, Na$_{2}$($1^3Σ_{u}^+$), residing on the surface of a helium nanodroplet, can be set into rotation by a nonresonant 1.0 ps infrared laser pulse. The time-dependent degree of alignment measured, exhibits a periodic, gradually decreasing structure that deviates qualitatively from that expected for gas phase dimers. Comparison to alignment dynamics calculated from the time-dependent rotational Schrödinger equation shows that the deviation is due to the alignment dependent interaction between the dimer and the droplet surface. This interaction confines the dimer to the tangential plane of the droplet surface at the point where it resides and is the reason that the observed alignment dynamics is also well-described by a 2D quantum rotor model.

physics.atm-clus↗

arXiv2023

Molecular Dynamics Study of the Sonic Horizon of Microscopic Laval Nozzles

A Laval nozzle can accelerate expanding gas above supersonic velocities, while cooling the gas in the process. This work investigates this process for microscopic Laval nozzles by means of non-equilibrium molecular dynamics simulations of statioary flow, using grand canonical Monte-Carlo particle reservoirs. We study the expansion of a simple fluid, a mono-atomic gas interacting via a Lennard-Jones potential, through an idealized nozzle with atomically smooth walls. We obtain the thermodynamic state variables pressure, density, and temperature, but also the Knudsen number, speed of sound, velocity, and the corresponing Mach number of the expanding gas for nozzles of different sizes. We find that the temperature is well-defined in the sense that the each velocity components of the particles obey the Maxwell-Boltzmann distribution, but it is anisotropic, especially for small nozzles. The velocity auto-correlation function reveals a tendency towards condensation of the cooled supersonic gas, although the nozzles are too small for the formation of clusters. Overall we find that microscopic nozzles act qualitatively like macroscopic nozzles in that the particles are accelerated to supersonic speeds while their thermal motion relative to the stationary flow is cooled. We find that, like macroscopic Laval nozzles, microscopic nozzles also exhibit a sonic horizon, which is well-defined on a microscopic scale. The sonic horizon is positioned only slightly further downstream compared to isentropic expansion through macroscopic nozzles, where it is situated in the most narrow part. We analyze the sonic horizon by studying spacetime density correlations, i.e.\ how thermal fluctuations at two positions of the gas density are correlated in time and find that after the sonic horizon there are indeed no upstream correlations on a microscopic scale.

cond-mat.stat-mech↗

arXiv2023

Striped Ultradilute Liquid of Dipolar Bosons in Two Dimensions

We investigate the phases of a Bose-Einstein condensate of dipolar atoms restricted to move in a two-dimensional plane. The dipole moments are all aligned in a direction tilted with respect to the plane normal. As a result of the attractive and repulsive components of the dipole-dipole interaction, the dipolar gas has a self-bound phase, which is stabilized by quantum fluctuations. Furthermore, tilting the dipoles tunes the anisotropy of the dipole-dipole interaction, which can trigger a spatial density modulation. In this work we study these two aspects and investigate the conditions for the formation of a self-bound and striped phase, which has been realized in experiments with dipolar droplets. We use a variational method based on the hypernetted-chain Euler-Lagrange optimization of a Jastrow-Feenberg ansatz for the many-body wave function to study the ground state properties. This method takes into account quantum fluctuations in a non-perturbative way and thus can be used also for strongly correlated systems.

cond-mat.quant-gas↗

arXiv2022

Time-dependent variational Monte Carlo study of the dynamic response of bosons in an optical lattice

We study the dynamics of a one-dimensional Bose gas at unit filling in both shallow and deep optical lattices and obtain the dynamic structure factor ${S(k,ω)}$ by monitoring the linear response to a weak probe pulse. We introduce a new procedure, based on the time-dependent variational Monte Carlo method (tVMC), which allows to evolve the system in real time, using as a variational model a Jastrow-Feenberg wave function that includes pair correlations. Comparison with exact diagonalization results of ${S(k,ω)}$ obtained on a lattice in the Bose-Hubbard limit shows good agreement of the dispersion relation for sufficiently deep optical lattices, while for shallow lattices we observe the influence of higher Bloch bands. We also investigate non-linear response to strong pulses. From the power spectrum of the density fluctuations we obtain the excitation spectrum, albeit broadened, by higher harmonic generation after a strong pulse with a single low wave number. As a remarkable feature of our simulations we furthermore demonstrate that the full excitation spectrum can be retrieved from the power spectrum of the density fluctuations due to the stochastic noise inherent in any Monte Carlo method, without applying an actual perturbation.

cond-mat.quant-gas↗

arXiv2020

Rotational coherence spectroscopy of molecules in helium nanodroplets: Reconciling the time and the frequency domains

Alignment of OCS, CS$_2$ and I$_2$ molecules embedded in helium nanodroplets is measured as a function of time following rotational excitation by a non-resonant, comparatively weak ps laser pulse. The distinct peaks in the power spectra, obtained by Fourier analysis, are used to determine the rotational, B, and centrifugal distortion, D, constants. For OCS, B and D match the values known from IR spectroscopy. For CS$_2$ and I$_2$, they are the first experimental results reported. The alignment dynamics calculated from the gas-phase rotational Schrödinger equation, using the experimental in-droplet B and D values, agree in detail with the measurement for all three molecules. The rotational spectroscopy technique for molecules in helium droplets introduced here should apply to a range of molecules and complexes.

physics.atm-clus↗

arXiv2020

Rotons and Bose condensation in Rydberg-dressed Bose Gases

We investigate the ground-state properties and excitations of Rydberg-dressed bosons in both three and two dimensions, using the hypernetted-chain Euler-Lagrange approximation, which accounts for correlations and thus goes beyond the mean field approximation. The short-range behavior of the pair distribution function signals the instability of the homogeneous system towards the formation of droplet crystals at strong couplings and large soft-core radius. This tendency to spatial density modulation coexists with off-diagonal long-range order. The contribution of the correlation energy to the ground-state energy is significant at large coupling strengths and intermediate values of the soft-core radius while for a larger soft-core radius the ground-state energy is dominated by the mean-field (Hartree) energy. We have also performed path integral Monte Carlo simulations to verify the performance of our hypernetted-chain Euler-Lagrange results in three dimensions. In the homogeneous phase, the two approaches are in very good agreement. Moreover, Monte Carlo simulations predict a first-order quantum phase transition from a homogeneous superfluid phase to the quantum droplet phase with face-centered cubic symmetry for Rydberg-dressed bosons in three dimensions.

cond-mat.quant-gas↗

arXiv2018

Self-bound Bose mixtures

Recent experiments confirmed that fluctuations beyond the mean-field approximation can lead to self-bound liquid droplets of ultra-dilute binary Bose mixtures. We proceed beyond the beyond-mean-field approximation, and study liquid Bose mixtures using the variational hypernetted-chain Euler Lagrange method, which accounts for correlations non-perturbatively. Focusing on the case of a mixture of uniform density, as realized inside large saturated droplets, we study the conditions for stability against evaporation of one of the components (both chemical potentials need to be negative) and against liquid-gas phase separation (spinodal instability), the latter being accompanied by a vanishing speed of sound. Dilute Bose mixtures are stable only in a narrow range near an optimal ratio $ρ_1/ρ_2$ and near the total energy minimum. Deviations from a universal dependence on the s-wave scattering lengths are significant despite the low density.

cond-mat.quant-gas↗

arXiv2018

Quantum phases of dipolar rotors on two-dimensional lattices

The quantum phase transitions of dipoles confined to the vertices of two dimensional (2D) lattices of square and triangular geometry is studied using path integral ground state quantum Monte Carlo (PIGS). We analyze the phase diagram as a function of the strength of both the dipolar interaction and a transverse electric field. The study reveals the existence of a class of orientational phases of quantum dipolar rotors whose properties are determined by the ratios between the strength anisotropic dipole-dipole interaction, the strength of the applied transverse field, and the rotational constant. For the triangular lattice, the generic orientationally disordered phase found at zero and weak values of both dipolar interaction strength and applied field, is found to show a transition to a phase characterized by net polarization in the lattice plane as the strength of the dipole-dipole interaction is increased, independent of the strength of the applied transverse field, in addition to the expected transition to a transverse polarized phase as the electric field strength increases. The square lattice is also found to exhibit a transition from a disordered phase to an ordered phase as the dipole-dipole interaction strength is increased, as well as the expected transition to a transverse polarized phase as the electric field strength increases. In contrast to the situation with a triangular lattice, on square lattices the ordered phase at high dipole-dipole interaction strength possesses a striped ordering. The properties of these quantum dipolar rotor phases are dominated by the anisotropy of the interaction and provide useful models for developing quantum phases beyond the well-known paradigms of spin Hamiltonian models, realizing in particular a novel physical realization of a quantum rotor-like Hamiltonian that possesses an anisotropic long range interaction.

quant-ph↗

arXiv2017

Laser-induced rotation of iodine molecules in He-nanodroplets: revivals and breaking-free

Rotation of molecules embedded in He nanodroplets is explored by a combination of fs laser-induced alignment experiments and angulon quasiparticle theory. We demonstrate that at low fluence of the fs alignment pulse, the molecule and its solvation shell can be set into coherent collective rotation lasting long enough to form revivals. With increasing fluence, however, the revivals disappear -- instead, rotational dynamics as rapid as for an isolated molecule is observed during the first few picoseconds. Classical calculations trace this phenomenon to transient decoupling of the molecule from its He shell. Our results open novel opportunities for studying non-equilibrium solute-solvent dynamics and quantum thermalization.

physics.chem-ph↗

arXiv2016

The Multi-component Correlated Basis Function Method and its Application to Multilayered Dipolar Bose Gases

We present a method for calculating the dynamics of a bosonic mixture, the multi-component correlated basis function (CBF) method. For single components, CBF results for the excitation energies agree quite well with experimental results, even for highly correlated systems like $^4$He, and recent systematic improvements of CBF achieve perfect agreement. We give a full derivation of multi-component CBF, and apply the method to a dipolar Bose gas cut into two-dimensional layers by a deep optical lattice, with coupling between layers due to the long-ranged dipole-dipole interaction. We consider the case of strong coupling, leading to large positive interlayer correlations. We calculate the spectrum for a system of 8 layers and show that the strong coupling can lead to a simpler spectrum than in the uncoupled case, with a single peak carrying most of the spectral weight.

cond-mat.quant-gas↗

arXiv2016

Solvation of Mg in Helium-4: Are there Meta-stable Mg Dimers ?

Experiments on the formation of magnesium complexes in $^4$He nanodroplets were interpreted as the observation of the formation of weakly bound magnesium complexes. We present results for single Mg and Mg dimer solvation using the hypernetted chain / Euler-Lagrange method as well as path integral Monte Carlo simulations. We find that the phonon-mediated, indirect Mg-Mg interaction adds an oscillatory component to the direct Mg-Mg interaction. We undertake a step-by-step examination of the ingredients of the calculation of the phonon-induced interaction, comparing the results of semi-analytic HNC-EL calculations for bulk and single impurity results with experiments as well as Monte Carlo data. We do not find evidence for a sufficiently strong secondary minimum in the effective Mg-Mg interaction to support a metastable state.

physics.chem-ph↗

arXiv2015

Dipolar Bilayer with Antiparallel Polarization -- a Self-Bound Liquid

Dipolar bilayers with antiparallel polarization, i.e. opposite polarization in the two layers, exhibit liquid-like rather than gas-like behavior. In particular, even without external pressure a self-bound liquid puddle of constant density will form. We investigate the symmetric case of two identical layers, corresponding to a two-component Bose system with equal partial densities. The zero-temperature equation of state $E(ρ)/N$, where $ρ$ is the total density, has a minimum, with an equilibrium density that decreases with increasing distance between the layers. The attraction necessary for a self-bound liquid comes from the inter-layer dipole-dipole interaction that leads to a mediated intra-layer attraction. We investigate the regime of negative pressure towards the spinodal instability, where the bilayer is unstable against infinitesimal fluctuations of the total density, conformed by calculations of the speed of sound of total density fluctuations.

cond-mat.quant-gas↗