Low-temperature optical spectroscopy of guest-host molecular crystal s
ystems provides a very sensitive tool to study proton tunneling proces
ses. Examples include the light-induced creation and evolution of ''pr
oton defects', translational tunneling along hydrogen bonds as well as
rotational tunneling of methyl groups. Absorption spectra at 2 K of g
amma-picoline single crystals evolve over time scales of days due to t
he slow spin conversion of the methyl groups which leads to an orderin
g of the crystal.