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Physical Review Letters

Resonance-Enhanced Optical Reorientation of Molecules in Liquids via Intermolecular Interaction

Thai V. Truong, Y. R. Shen

Published Nov 2, 2007• 10 citations
Publisher

Abstract

Enhanced optical reorientation of molecules in a pure liquid was observed when the optical field was in resonance with the molecular electronic transition. The enhancement comes from photoinduced change in intermolecular interaction. Experimental results agree well with the time-dependent theory based on a mean-field model of intermolecular interaction.

DOI
10.1103/physrevlett.99.187802

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Enhanced optical reorientation of molecules in a pure liquid was observed when the optical field was in resonance with the molecular electronic transition. The enhancement comes from photoinduced change in intermolecular interaction. Experimental results agree well with the time-dependent theory based on a mean-field model of intermolecular interaction.
We show that dressing polar molecules with a far-off-resonant optical field leads to new types of intermolecular potentials, which undergo a crossover from the inverse power to oscillating behavior depending on the intermolecular distance, and whose parameters can be tuned by varying the laser intensity and wavelength. We present analytic expressions for the potential energy surfaces, thereby providing direct access to the parameters of an optical field required to design intermolecular interactions experimentally.
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, polarisation and intensity of the optical field and its dependence on the intermolecular separation exhibits a crossover from an inverse-power to an oscillating behaviour. 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.
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, polarisation and intensity of the optical field and its dependence on the intermolecular separation exhibits a crossover from an inverse-power to an oscillating behaviour. 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.
Abstract Molecular reorientation and laser heating induced by an optical field can yield significant changes in the refractive indices in a nematic liquid crystal. A c.w. laser beam is intense enough to induce a phase retardation much larger than 2pi in a nematic film less than 100 pm thick. Optical bistability in such a film sandwiched between mirrors can be readily observed. Coupling between the two mechanisms for induced refractive indices can lead to interesting results in the bistable operation.
A Stokes shifted superbroadening stimulated scattering has been studied in a CS2{\mathrm{CS}}_{2}CS2​ liquid-core hollow fiber system with a long gain length (2.5 m) by using \ensuremath{\approxeq}10-ns laser pulses with a pump intensity range of (106{10}^{6}106--5\ifmmode\times\else\texttimes\fi{}108{10}^{8}108 W/cm2{\mathrm{cm}}^{2}cm2). The salient features of this stimulated scattering are that the spectral broadening range is very large (\ensuremath{\ge}700 ${\mathrm{cm}}^{\mathrm{\ensuremath{-}}1}$) and no detectable shift of the spectral maximum or periodical modulation structure is observed. In order to interpret our experimental results, various possible mechanisms and processes are discussed. A model based on stimulated Kerr scattering of anisotropic molecules in liquid is suggested to explain the observation. This model assumes a single-step reorientation of anisotropic molecules induced by an intense optical field.
It is shown that the optical-field-induced first-order molecular reorientation and intrinsic optical bistability in a nemiatic liquid crystal can always be enhanced or suppressed by a low magneitc field (typically <1 kG) and hence can be seen in all existing nematics at a low optical power (typically <1 kW/cm2{\mathrm{cm}}^{2}cm2).