A. Brodin et Lm. Torell, RELAXATIONAL AND LOW-WAVE-NUMBER VIBRATIONAL DYNAMICS OF STRONG GLASSFORMERS B2O3 AND GEO2 PROBED BY RAMAN-SCATTERING, Journal of Raman spectroscopy, 27(10), 1996, pp. 723-730
Low-wavenumber Raman scattering results are presented on the structura
l dynamics of two network-forming glasses: the moderately strong glass
former B2O3 and the extremely strong GeO2. Studies were performed fro
m temperatures ca. 10 It to above their respective glass transition te
mperatures (T-g approximate to 526 K for B2O3 and 800 K for GeO2). Two
distinct spectral contributions were detected, related to vibrational
and fast relaxational dynamics, respectively, and conventionally refe
rred to as the boson peak (BP) and quasi-elastic scattering (QS). The
fast relaxation spectrum is discussed in terms of the mode coupling th
eory (MCT), which has been shown to describe fragile glass formers suc
cessfully. A quantity proportional to the fast relaxation strength may
be deduced from the integral intensity of QS relative to BP of the sp
ectra. It turns out that for T < T-g, the so-obtained QS intensity of
the two glasses is similar and smoothly temperature dependent. As T-g
is passed, there is a pronounced change in behaviour and dramatic diff
erences between the two systems are observed. Thus, the fast relaxatio
nal dynamics are clearly affected by T-g, in contrast to the MCT predi
ctions of a single crossover temperature T-c > T-g. Moreover, the expe
rimentally obtained value of the MCT exponent a, describing the shape
of the fast dynamics, greatly exceeds the limiting value (a = 0.395) o
f the theory, the deviation increasing with increasing strength of the
system (a approximate to 0.7 for B2O3 and 0.9 for Ge0(2)). The differ
ence between the two glasses is discussed in terms of their difference
s in fragility as manifested in the behaviour of the specific heat aro
und T-g.