  We have performed thermal expansion and compressibility measurements on the
recently discovered superconducting material NaxCoO2*4xD2O (x=1/3) using
neutron powder diffraction over the temperature range 10-295 K and the pressure
range 0-0.6 GPa. Pressure measurements were done in a helium-gas pressure cell.
Both the thermal expansion and compressibility are very anisotropic, with the
largest effects along the c axis, as would be expected for a layered material
with weak hydrogen bonding nominally along the c axis. Near room temperature,
the anisotropies of the thermal expansion and compressibility of the hexagonal
crystal structure are nearly the same [(Dc/c)/(Da/a)=3-4], with a 100 C change
in temperature being roughly equivalent to 0.2 GPa pressure. This would imply
that changes in atom position parameters are also the same, but this is not the
case. While the effects of temperature on the atom positions are essentially
what one might expect, the effects of pressure are surprising. With increasing
pressure, the thickness of the CoO2 layer increases, due to the combined
effects of an increasing Co-O bond length and changes in the O-Co-O angles of
the CoO6 octahedra. We conclude that this unusual effect results from
pressure-induced strengthening of the hydrogen bonding between the Nax(D2O)4x
layers and the CoO2 layers. The strengthening of these hydrogen bonds requires
that charge be moved from the somewhere else in the structure; hence, there is
a pressure induced charge redistribution that weakens (lengthens) the Co-O
bonds and changes the electronic structure of the superconducting CoO2 layers.
