Adiabatic Field-Free Alignment of Asymmetric Top Molecules with an Optical Centrifuge.

Theoretical description of adiabatic laser alignment and mixed-field orientation: the need for a non-adiabatic model.

We present a theoretical study of recent laser-alignment and mixed-field-orientation experiments of asymmetric top molecules. In these experiments, pendular states were created using linearly polarized strong ac electric fields from pulsed lasers in combination with weak electrostatic fields. We compare the outcome of our calculations with experimental results obtained for the prototypical larg...

Field-free molecular alignment of asymmetric top molecules using elliptically polarized laser pulses

Measurement of field-free alignment of jet-cooled molecules by nonresonant femtosecond degenerate four-wave mixing

A femtosecond degenerate four-wave mixing (fs-DFWM) technique for probing the alignment of molecules is described. The rotational wave packet generated by a strong pump beam modulates the nonresonant third-order susceptibility of the gas and this modulation is observed using a noncollinear background-free setup. As a demonstration of the technique, we measure the alignment of a linear molecule ...

Field-free three dimensional molecular axis alignment.

We investigate strategies for field-free three dimensional molecular axis alignment using strong nonresonant laser fields under experimentally realistic conditions. Using the polarizabilites and rotational constants of an asymmetric top rotor molecule (ethene, C2H4), we consider three different methods for axis alignment of a Boltzmann distribution of rotors at 4 K. Specifically, we compare the...

Field-free three-dimensional alignment of polyatomic molecules.

We experimentally demonstrate field-free, three-dimensional alignment (FF3DA) of polyatomic asymmetric top molecules. We achieve FF3DA in sulfur dioxide gas using two time-delayed, orthogonally polarized, nonresonant, femtosecond laser pulses. Our method avoids the use of rotational revivals and is therefore more robust to temperature. The alignment is probed using time-delayed coincidence Coul...