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Register a new userField-free long-lived alignment of molecules in extreme rotational states
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We introduce a new optical tool - a two-dimensional optical centrifuge, capable of aligning molecules in extreme rotational states. Unlike the conventional centrifuge, which confines the molecules in the plane of their rotation, its two-dimensional version aligns the molecules along a well-defined axis, similarly to the effect of a single linearly polarized laser pulse, but at a much higher level of rotational excitation. The increased robustness of ultra-high rotational states with respect to collisions results in a longer life time of the created alignment in dense media, offering new possibilities for studying and utilizing aligned molecular ensembles under ambient conditions.
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We analyze theoretically the interplay between the torsional and the rotational motion of an aligned biphenyl-like molecule. To do so, we consider a transition between two electronic states with different internal torsional potentials, induced by means of a resonant laser pulse. The change in the internal torsional potential provokes the motion of the torsional wavepacket in the excited electronic state, modifying the structure of the molecule, and hence, its inertia tensor. We find that this process has a strong impact on the rotational wave function, displaying different behavior depending on the electronic states involved and their associated torsional potentials. We describe the dynamics of the system by considering the degree of alignment and the expectations values of the angular momentum operators for the overall rotation of the molecule.
We combine experimental and theoretical approaches to explore excited rotational states of molecules embedded in helium nanodroplets using CS$_2$ and I$_2$ as examples. Laser-induced nonadiabatic molecular alignment is employed to measure spectral lines for rotational states extending beyond those initially populated at the 0.37 K droplet temperature. We construct a simple quantum mechanical model, based on a linear rotor coupled to a single-mode bosonic bath, to determine the rotational energy structure in its entirety. The calculated and measured spectral lines are in good agreement. We show that the effect of the surrounding superfluid on molecular rotation can be rationalized by a single quantity -- the angular momentum, transferred from the molecule to the droplet.
The mixed-field orientation of an asymmetric-rotor molecule with its permanent dipole moment non-parallel to the principal axes of polarizability is investigated experimentally and theoretically. We find that for the typical case of a strong, nonresonant laser field and a weak static electric field complete 3D orientation is induced if the laser field is elliptically polarized and if its major and minor polarization axes are not parallel to the static field. For a linearly polarized laser field solely the dipole moment component along the most polarizable axis of the molecule is relevant resulting in 1D orientation even when the laser polarization and the static field are non parallel. Simulations show that the dipole moment component perpendicular to the most-polarizable axis becomes relevant in a strong dc electric field combined with the laser field. This offers an alternative approach to 3D orientation by combining a linearly-polarized laser field and a strong dc electric field arranged at an angle equal to the angle between the most polarizable axis of the molecule and its permanent dipole moment.
We analyze the alignment of molecules generated by a pair of crossed ultra-short pump pulses of different polarizations by a technique based on the induced time-dependent gratings. Parallel polarizations yield an intensity grating, while perpendicular polarizations induce a polarization grating. We show that both configurations can be interpreted at moderate intensity as an alignment induced by a single polarized pump pulse. The advantage of the perpendicular polarizations is to give a signal of alignment that is free from the plasma contribution. Experiments on femtosecond transient gratings with aligned molecules were performed in CO2 at room temperature in a static cell and at 30 K in a molecular expansion jet.
Dipole-dipole interactions are at the origin of long-lived collective atomic states, often called subradiant, which are explored for their potential use in novel photonic devices or in quantum protocols. Here, we study subradiance beyond linear optics and experimentally demonstrate a two hundred-fold increase in the population of these modes, as the saturation parameter of the driving field is increased. We attribute this enhancement to a mechanism similar to optical pumping through the well-coupled superradiant states. The lifetimes are unaffected by the pump strength, as the system is ultimately driven toward the single-excitation sector.
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