Predicted Ordered Assembly of Ethylene Molecules Induced by Polarized Off-Resonance Laser Pulses

We illustrate a new phenomenon in the dynamics of molecular ensembles subjected to moderately intense, far-off-resonance laser fields, namely, field-driven formation of perfectly ordered, defect-free assembly. Interestingly, both the arrangement of the constituting molecules within the individual assembly and the long-range order of the assembly with respect to one another are subject to control through choice of the field polarization. Relying on strong induced dipole-induced dipole interactions that are established in dense molecular media, the effect is expected to be general.

Figure 1

Alignment and 3D alignment produced by linearly (cyan, squares), circularly (blue, circles), and elliptically (red, triangles) polarized fields. The field intensity is maintained at the peak value of $110\mathrm{TW}{\mathrm{cm}}^{-2}$ after the 440 ps turn-on time.

Figure 2

Time evolution of the mean Lennard-Jones and the interaction energy between induced dipoles in the course of laser alignment induced by linearly (cyan, squares), circularly (blue, circles), and elliptically (red, triangles) polarized fields. The time profile of the field intensity is as in Fig. 1.

Figure 3

A snapshot of a simulation box with 384 molecules at the end of the simulation. The field is elliptically polarized with a peak intensity of $110\mathrm{TW}{\mathrm{cm}}^{-2}$ maintained for the rest of the simulation.

Figure 4

As in Fig. 1, but for a linearly polarized field.