We recently developed a new method of preparing a parahydrogen crystal
which is suitable for experiments on nonlinear optical processes. The
crystal was grown slowly from pressurized liquid-phase in order to av
oid internal stress from the thermal constriction, and was cooled down
to 4.2 K. The obtained crystal was uncracked and perfectly transparen
t with a high damage threshold. To evaluate the quality, the vibration
al coherence decay was measured using the time-resolved coherent anti-
Stokes Raman spectroscopy (CARS) technique. The decay process showed a
nonexponential behavior, with an asymptotic limit characterized by a
single time constant of 2.6 mu s, which corresponds to a linewidth of
less than 0.1 MHz. This decay time is extremely slow compared to the p
reviously published work.