Moderately intense, nonresonant laser pulses can be used to accurately control how gas phase molecules are oriented in space. This topic, driven by intense experimental and theoretical efforts, has been ever growing and developed for more than 20 years, and laser-induced alignment methods are used routinely in a number of applications in physics and chemistry. Starting in 2013, we have demonstrated that laser-induced alignment also applies to molecules dissolved in helium nanodroplets. Here we present an overview of this new work discussing alignment in both the nonadiabatic (short-pulse) and adiabatic (long-pulse) limit. We show how femtosecond or picosecond pulses can set molecules into coherent rotation that lasts for a long time and reflects the rotational structure of the helium-solvated molecules, provided the pulses are weak or, conversely, results in desolvation of the molecules when the pulses are strong. For long pulses we show that the 0.4 K temperature of the droplets, shared with the molecules or molecular complexes, leads to exceptionally high degrees of alignment. Upon rapid truncation of the laser pulse, the strong alignment can be made effectively field-free, lasting for about 10 ps thanks to slowing of molecular rotation by the helium environment. Finally, we discuss how the combination of strongly aligned molecular dimers and laser-induced Coulomb explosion imaging enables determination of the structure of the dimers. As a background and reference point, the first third of the article introduces some of the central concepts of laser-induced alignment for isolated molecules, illustrated by numerical and experimental examples.
