Quantum phases of dipolar rotors on two-dimensional lattices.

The quantum phase transitions of dipoles confined to the vertices of two-dimensional lattices of square and triangular geometry is studied using path integral ground state quantum Monte Carlo. 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 of the 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, implementing in particular a novel physical realization of a quantum rotor-like Hamiltonian that possesses an anisotropic long range interaction.

Excitations and stripe phase formation in a two-dimensional dipolar Bose gas with tilted polarization.

We present calculations of the ground state and excitations of an anisotropic dipolar Bose gas in two dimensions, realized by a nonperpendicular polarization with respect to the system plane. For sufficiently high density, an increase of the polarization angle leads to a density instability of the gas phase in the direction where the anisotropic interaction is strongest. Using a dynamic many-body theory, we calculate the dynamic structure function in the gas phase which shows the anisotropic dispersion of the excitations. We find that the energy of roton excitations in the strongly interacting direction decreases with increasing polarization angle and almost vanishes close to the instability. Exact path integral ground state Monte Carlo simulations show that this instability is indeed a quantum phase transition to a stripe phase, characterized by long-range order in the strongly interacting direction.

Roton-roton crossover in strongly correlated dipolar Bose-Einstein condensates.

We study the pair correlations and excitations of a dipolar Bose gas layer. The anisotropy of the dipole-dipole interaction allows us to tune the strength of pair correlations from strong to weak perpendicular and weak to strong parallel to the layer by increasing the perpendicular trap frequency. This change is accompanied by a roton-roton crossover in the spectrum of collective excitations, from a roton caused by the head-to-tail attraction of dipoles to a roton caused by the side-by-side repulsion, while there is no roton excitation for intermediate trap frequencies. We discuss the nature of these two kinds of rotons and the relation to instabilities of dipolar Bose gases. In both regimes of trap frequencies where rotons occur, we observe strong damping of collective excitations by decay into two rotons.

Dynamics of a two-dimensional system of quantum dipoles.

A detailed microscopic analysis of the dynamic structure function S(k,omega) of a two-dimensional Bose system of dipoles polarized along the direction perpendicular to the plane is presented and discussed. Starting from ground-state quantities obtained using a quantum diffusion Monte Carlo algorithm, the density-density response is evaluated in the context of the correlated basis functions (CBF) theory. CBF predicts a sharp peak and a multiexcitation component at higher energies produced by the decay of excitations. We discuss the structure of the phonon-roton peak and show that the Feynman and Bogoliubov predictions depart from the CBF result already at low densities. We finally discuss the emergence of a roton in the spectrum, but find the roton energy not low enough to make the system unstable under density fluctuations up to the highest density considered that is close to the freezing point.

OCS in para-hydrogen clusters: rotational dynamics and superfluidity.

We present a detailed analysis of the rotational excitations of the linear OCS molecule solvated by a variable number of para-hydrogen molecules (9 < or = N < or = 17). The effective rotational constant extracted from the fit of the rotational energy levels decreases up to N = 13, indicating near-rigid coupling between OCS rotations and para-hydrogen motion. Departure from rigidity is instead seen for larger clusters with 14 < or = N < or = 17. Path-integral Monte Carlo calculations show that the N dependence of the effective rotational constant can be explained in terms of a partial superfluid response of para-hydrogen to rotations about an axis perpendicular to the OCS axis. Complete para-hydrogen superfluid response to rotations about the OCS axis is found for N > or = 10.

Path integral methods for rotating molecules in superfluids.

We present a path integral Monte Carlo (PIMC) methodology for quantum simulation of molecular rotations in superfluid environments such as helium and para-hydrogen that combines the sampling of rotational degrees of freedom for a molecular impurity with multilevel Metropolis sampling of Bose permutation exchanges for the solvating species. We show how the present methodology can be applied to the evaluation of imaginary time rotational correlation functions of the molecular impurity, from which the effective rotational constants can be extracted. The combined rotation/permutation sampling approach allows for the first time explicit assessment of the effect of Bose permutations on molecular rotation dynamics, and the converse, i.e., the effect of molecular rotations on permutation exchanges and local superfluidity. We present detailed studies showing that the effect of Bose permutations in the solvating environment is more significant for the dynamics of heavy than light molecules in helium, and that Bose permutation exchanges are slightly enhanced locally by molecular rotation. Finally, the examples studied here reveal a size dependence of rotational excitations for molecules possessing a strongly anisotropic interaction with helium in 4HeN clusters between N approximately 20 and N approximately 10(3).

Roton-rotation coupling of acetylene in 4He.

Rotational absorption spectra of acetylene in superfluid 4He calculated using a path-integral correlation function approach are seen to result in an anomalously large distortion constant in addition to a reduced rotational constant, with values in excellent agreement with recent experiments. Semianalytic treatment of the dynamics with a combined correlated basis function-diffusion Monte Carlo method reveals that this anomalous behavior is due to strong coupling of the higher rotational states of the molecule with the roton and maxon excitations of 4He, and the associated divergence of the 4He density of states in this region.