We introduce analytical models of torsional alignment by moderately intense laser pulses that are applicable to the limiting cases of the torsional barrier heights. Using these models, we explore in detail the role that the laser intensity and pulse duration play in coherent torsional dynamics, addressing both experimental and theoretical concerns. Our results suggest strategies for minimizing the risk of off-resonant ionization, noting the qualitative differences between the case of torsional alignment subject to a field-free torsional barrier and that of torsional alignment of a barrier-less system (equivalent to a 2D rigid rotor). We also investigate several interesting torsional phenomena, including the onset of impulsive alignment of torsions, field-driven oscillations in quantum number space, and the disappearance of an alignment upper bound observed for a rigid rotor in the impulsive torsional alignment limit.

We present a model for strong field coherent control of torsional modes of molecules with a focus on exploring the controllability of molecular torsions subject to dissipative media and understanding how phase information is exchanged between torsional modes and a dissipative environment. Our theory is based on a density matrix formalism, wherein dissipation is accounted for within a multilevel Bloch equation model. Our results point to new and interesting phenomena in wavepacket dissipation dynamics that are unique to torsions and also enrich our general understanding of wavepacket phenomena. In addition, we suggest guidelines for designing torsional control experiments for molecules interacting with a dissipative bath.

We discuss several interesting phenomena in the dynamics of strong field-triggered torsional wavepackets, which carry implications for the problem of torsional alignment in nonrigid molecules. Our results point to the origin and consequences of the fundamental differences between rotational and torsional coherences. In addition, we provide design guidelines for torsional control experiments by illustrating the role played by the laser intensity, pulse width, temperature, and molecular parameters. Specifically, as an example of several classes of molecules expected to make suitable candidates for laboratory experiments, we explore the torsional control of 9-[2-(anthracen-9-yl)ethynyl]anthracene and contrast it with that of biphenyl. Finally, we propose several potential applications for coherent torsional control in chemistry, physics, and material science.