Interaction between polar molecules subject to a far-off-resonant optical field: Entangled dipoles up- or down-holding each other

We show that the electric dipole-dipole interaction between a pair of polar molecules undergoes an all-out transformation when superimposed by a far-off resonant optical field. The combined interaction potential becomes tunable by variation of wavelength, polarization and intensity of the optical field and its dependence on the intermolecular separation exhibits a crossover from an inverse-power to an oscillating behavior. The ability thereby offered to control molecular interactions opens up avenues toward the creation and manipulation of novel phases of ultracold polar gases among whose characteristics is a long-range entanglement of the dipoles' mutual orientation. We devised an accurate analytic model of such optical-field-dressed dipole-dipole interaction potentials, which enables a straightforward access to the optical-field parameters required for the design of intermolecular interactions in the laboratory.Comment: 11 pages, 6 figures, 1 table. arXiv admin note: substantial text overlap with arXiv:1104.104

Diagrammatic Monte Carlo approach to angular momentum in quantum many-particle systems

We introduce a Diagrammatic Monte Carlo (DiagMC) approach to angular momentum properties of quantum many-particle systems possessing a macroscopic number of degrees of freedom. The treatment is based on a diagrammatic expansion that merges the usual Feynman diagrams with the angular momentum diagrams known from atomic and nuclear structure theory, thereby incorporating the non-Abelian algebra inherent to quantum rotations. Our approach is applicable at arbitrary coupling, is free of systematic errors and of finite size effects, and naturally provides access to the impurity Green function. We exemplify the technique by obtaining an all-coupling solution of the angulon model, however, the method is quite general and can be applied to a broad variety of systems in which particles exchange quantum angular momentum with their many-body environment.Comment: 6+5 pages, 2+2 figures, accepted for publication in Phys. Rev. Let

Strongly aligned molecules inside helium droplets in the near-adiabatic regime

Iodine (I$_2$) molecules embedded in He nanodroplets are aligned by a 160 ps long laser pulse. The highest degree of alignment, occurring at the peak of the pulse and quantified by $\langle \cos^2 \theta_{2D} \rangle$, is measured as a function of the laser intensity. The results are well described by $\langle \cos^2 \theta_{2D} \rangle$ calculated for a gas of isolated molecules each with an effective rotational constant of 0.6 times the gas-phase value, and at a temperature of 0.4 K. Theoretical analysis using the angulon quasiparticle to describe rotating molecules in superfluid helium rationalizes why the alignment mechanism is similar to that of isolated molecules with an effective rotational constant. A major advantage of molecules in He droplets is that their 0.4 K temperature leads to stronger alignment than what can generally be achieved for gas phase molecules -- here demonstrated by a direct comparison of the droplet results to measurements on a $\sim$ 1 K supersonic beam of isolated molecules. This point is further illustrated for more complex system by measurements on 1,4-diiodobenzene and 1,4-dibromobenzene. For all three molecular species studied the highest values of $\langle \cos^2 \theta_{2D} \rangle$ achieved in He droplets exceed 0.96.Comment: 11 pages, 8 figure

Collisions of paramagnetic molecules in magnetic fields: An analytic model based on Fraunhofer diffraction of matter waves

We investigate the effects of a magnetic field on the dynamics of rotationally inelastic collisions of open-shell molecules (² Σ, ³Σ, and ²Π) with closed-shell atoms. Our treatment makes use of the Fraunhofer model of matter wave scattering and its recent extension to collisions in electric [M. Lemeshko and B. Friedrich, J. Chem. Phys. 129, 024301 (2008)] and radiative fields [M. Lemeshko and B. Friedrich, Int. J. Mass. Spec. in press (2008)]. A magnetic field aligns the molecule in the space-fixed frame and thereby alters the effective shape of the diffraction target. This significantly affects the differential and integral scattering cross sections. We exemplify our treatment by evaluating the magnetic-field-dependent scattering characteristics of the He – CaH (X² Σ⁺), He – O₂ (X³Σ⁻) and He – OH (X²ΠΩ ) systems at thermal collision energies. Since the cross sections can be obtained fordifferent orientations of the magnetic field with respect to the relative velocity vector, the model also offers predictions about the frontal-versus-lateral steric asymmetry of the collisions. The steric asymmetry is found to be almost negligible for the He – OH system, weak for the He – CaH collisions, and strong for the He – O₂ . While odd ∆M transitions dominate the He – OH (J = 3/2, f → J′ , e/f ) integral cross sections in a magnetic field parallel to the relative velocity vector, even ∆M transitions prevail in the case of the He – CaH (X²Σ⁺) and He – O₂ (X³Σ⁻) collision systems. For the latter system, the magnetic field opens inelastic channels that are closed in the absence of the field. These involve the transitions N = 1, J = 0 → N′, J′ with J′ = N′

An analytic model of the stereodynamics of rotationally inelastic molecular collisions

We develop an analytic model of vector correlations in rotationally inelastic atom-diatom collisions and test it against the much examined Ar--NO (X²Π) system. Based on the Fraunhofer scattering of matter waves, the model furnishes complex scattering amplitudes needed to evaluate the polarization moments characterizing the quantum stereodynamics. The analytic polarization moments are found to be in an excellent agreement with experimental results and with close-coupling calculations available at thermal energies. The model reveals that the stereodynamics is governed by diffraction from the repulsive core of the Ar--NO potential, which can be characterized by a single Legendre moment

Quantum many-body dynamics of the Einstein-de Haas effect

In 1915, Einstein and de Haas and Barnett demonstrated that changing the magnetization of a magnetic material results in mechanical rotation, and vice versa. At the microscopic level, this effect governs the transfer between electron spin and orbital angular momentum, and lattice degrees of freedom, understanding which is key for molecular magnets, nano-magneto-mechanics, spintronics, and ultrafast magnetism. Until now, the timescales of electron-to-lattice angular momentum transfer remain unclear, since modeling this process on a microscopic level requires addition of an infinite amount of quantum angular momenta. We show that this problem can be solved by reformulating it in terms of the recently discovered angulon quasiparticles, which results in a rotationally invariant quantum many-body theory. In particular, we demonstrate that non-perturbative effects take place even if the electron--phonon coupling is weak and give rise to angular momentum transfer on femtosecond timescales.Comment: 15 pages, 5 figure

Exotic roton excitations in quadrupolar Bose-Einstein condensates

We investigate the occurrence of rotons in a quadrupolar Bose-Einstein condensate confined to two dimensions. Depending on the particle density, the ratio of the contact and quadrupole-quadrupole interactions, and the alignment of the quadrupole moments with respect to the confinement plane, the dispersion relation features two or four point-like roton minima, or one ring-shaped minimum. We map out the entire parameter space of the roton behavior and identify the instability regions. We propose to observe the exotic rotons by monitoring the characteristic density wave dynamics resulting from a short local perturbation, and discuss the possibilities to detect the predicted effects in state-of-the-art experiments with ultracold homonuclear molecules