  Recording molecular movies on ultrafast timescales has been a longstanding
goal for unravelling detailed information about molecular dynamics. We present
the direct experimental recording of very-high-resolution and -fidelity
molecular movies over more than one-and-a-half periods of the laser-induced
rotational dynamics of carbonylsulfide (OCS) molecules. Utilising the
combination of single-quantum-state selection and an optimised two-pulse
sequence to create a tailored rotational wavepacket, an unprecedented degree of
field-free alignment, $\langle \cos^{2}{\theta_{2D}}\rangle=0.96$ ($\langle
\cos^{2}{\theta}\rangle=0.94$) was achieved, exceeding the theoretical limit
for single-pulse alignment. The very rich experimentally observed quantum
dynamics is fully recovered by the angular probability distribution obtained
from solutions of the time-dependent Schr\"odinger equation with parameters
refined against the experiment. The populations and phases of rotational states
in the retrieved time-dependent three-dimensional wavepacket rationalised the
observed very high degree of alignment.
