Polarized single-crystal Raman spectra at room temperature and 5 K and pola
rized infrared spectra at room temperature were obtained from four natural
cordierites of different compositions in the wave number region of the CO2
symmetric stretching vibration and the H2O stretching vibrations. The CO2 m
olecules are preferentially aligned parallel to the X axis, consistent with
results from Xray diffraction and optical studies. The CO2 contents of six
natural cordierites, previously studied by powder IR methods (Vry et al. 1
990), were determined via Raman spectroscopy. A linear relationship was fou
nd between CO2 content and the Raman intensity ratio of the normalized CO2
stretching mode against a Si-O stretching mode. This permits a determinatio
n of the CO2 contents in cordierite using micro-Raman measurements. The int
ernal stretching modes between 3500 and 3800 cm(-1) were assigned to variou
s types of H2O molecules occurring in the channel cavity. Three different o
rientations of H2O molecules that have no interactions with alkali cations
located at 0,0,0 in the six-membered tetrahedral rings are classified in a
static model as Class I H2O molecules. The H-H vector for two of them is pa
rallel to [001], and their molecular planes lie in the XZ and YZ crystal pl
anes. The third type has its HH vector directed along the X axis and its mo
lecular plane lies in the XZ plane. Two other types of H2O have interaction
s with the alkali cations located at 0,0,0. They are classified as Class II
H2O. They distinguish themselves by the number of H2O molecules bonded to
the alkali atoms, The formation of weak hydrogen bonds at low temperatures
may explain the appearance of some Raman stretching modes below 200 K. The
H2O molecules of Class I-Type I/II are probably dynamically disordered abou
t [001] hopping between orientations in the XY and XZ planes down to 5 K. C
lass II H2O may also be disordered, but more measurements are required to d
escribe its dynamic behavior.