We use neutron time-of-flight scattering techniques to measure the low
-frequency vibrational density of states of solid cubane at 100 and 30
0 K. Debye-like behavior is observed up to similar to 60 cm(-1) at bot
h temperatures. At 100 K, the density of states exhibits three distinc
t peaks at 78, 94, and 114 cm(-1) before dropping to zero around 150 c
m(-1). We identify the 114 cm(-1) peak with the E(g) librational mode
of cubane based on the marked temperature dependence of its frequency
and a comparison to Raman measurements. In similar fashion we identify
the 94 cm(-1) peak with the A(g) librational mode. At 300 K, the libr
ational modes have softened to the extent that the density of states e
xhibits a plateau-like feature between 60 and 100 cm(-1). This is cons
istent with reports of two Raman-active lattice modes at 63 and 85 cm(
-1) having A(g) and E(g) symmetry, respectively. The energy scale asso
ciated with low-amplitude Librational excitations about an axis of 4-f
old symmetry, calculated from the NMR-measured activation energy for r
eorientation E(a) = 58 +/- 6 kJ/mol, is of order 94 +/- 5 cm(-1), whic
h is consistent with our observations. The heat capacity we calculate
from the measured density of states agrees well with recent calorimetr
ic data.