Physica B 284}288 (2000) 1157}1158

Density dependence of the boson peak of vitreous silica

Y. Inamura *, M. Arai , T. Otomo , N. Kitamura , U. Buchenau
Institute of Materials Structure Science, KEK, 1-1 Oho, Tsukuba 305-0801, Japan Government Industrial Research Institute of Osaka, 1-8-31 Midorigaoka, Ikeda, Japan Institut f ur Festkorperforschung, Forschungszentrum Julich, D-52425, Julich, Germany ( K ( (

Abstract Density dependence of low-energy dynamics of vitreous silica was investigated by means of neutron scattering measurements. On densi"cation, the intensity of the boson peak is drastically suppressed at the low-energy region, and eventually its position shifts toward higher energy. From this result we conclude that the origin of the boson peak is not a phonon scattering by local density #uctuations but a soft mode of void space in vitreous silica. 2000 Published by Elsevier Science B.V. All rights reserved.
Keywords: Glass; Boson peak; Intermediate range structure

The universal thermodynamic properties of noncrystalline systems have a close relation with the lowenergy dynamics of their intermediate range structure (IMRS) [1]. We reported the evolution in the structure and the low-energy dynamics, i.e. the boson peak, on densifying vitreous silica [2]. In the previous report, we studied the dynamics by Raman scattering, which has ambiguity in the photon}phonon coupling factor. In this report, we show more detailed and systematic results on the relation between the structural change and the lowenergy dynamics studied by inelastic neutron scattering. Densi"ed vitreous silica samples were prepared by an isotropic compression method using an octahedral anvil [3]. The four samples had densities of 2.20 (uncompressed), 2.32$0.02, 2.45$0.01 and 2.63$0.03 g cm\. We measured the dynamic structure factor by the inelastic neutron scattering performed on IN-6 at Institute of Laue Langevin, France. Fig. 1 shows the boson peak of vitreous silica at various densities measured at ambient temperature. The intensity was scaled by the mass of the samples, but no corrections were done on the sample shielding, etc. The boson peaks have sizable evolution on densi"cation. It

* Corresponding author. Tel.: #81-298-64-5628; fax: #81298-64-3202. E-mail address: yasuhiro.inamura@kek.jp (Y. Inamura)

shows clear suppression at lower energy region, and eventually the peak position shifts to higher energies on densi"cation. On the other hand, the tails of intensities above 15 meV do not depend on densi"cation. The small di!erence at the tails above 15 meV is likely attributed to the normalization by the sample mass. Therefore, in order to see the evolution in the low-energy dynamics, we took di!erence between the data at various densities. Fig. 2 shows the intensity of each sample subtracted by the intensity of the most densi"ed one. The subtracted intensity decreases on densi"cation, but the width and the peak position have only small density dependence. This result clearly indicates that the evolution of the boson peak is not a shift of the peak but a peculiar suppression in the density of states on densi"cation. In some reports, the origin of the boson peak has been explained by the phonon scattering by atomic-density #uctuations in non-crystalline system [4,5]. In these reports, they assumed the diameter of the density #uctuations, which appears as the position (Q ) or the width  ( Q ) of the "rst sharp di!raction peak (FSDP) in the  structure factor S(Q). It is also a characteristic length scale to satisfy the Io!e}Regel condition. As a result, they expected a linear relation between the maximum peak position of the boson peak and Q or Q , ex    pressed as "(v /3 )Q or "(v /2 c) Q ,       where is a constant, v is the sound velocity and c is the  speed of light. In the inset of Fig. 1, of the present 

0921-4526/00/$ - see front matter 2000 Published by Elsevier Science B.V. All rights reserved. PII: S 0 9 2 1 - 4 5 2 6 ( 9 9 ) 0 2 7 8 8 - X

1158

Y. Inamura et al. / Physica B 284}288 (2000) 1157}1158

Fig. 1. The density dependence of the boson peak. The inset shows the relation between FSDP position (Q ) and the boson  peak position ( ). 

work is plotted as a function of Q using values given in  our previous report [2]. Although the relation is linear, the extrapolated line to lower Q values does not go  through the origin. Therefore, it could not explain that the phonon scattering by density #uctuations is the origin of the boson peak. As we concluded in the previous paper, the structural evolution on densi"cation is associated with a drastic suppression of void space while keeping the SiO tet rahedron structure [2]. Therefore, the suppression in the density of state, as shown in Fig. 2, could be attributed to the suppression of a soft mode of an additional freedom in the void structure as proposed by Nakayama [6,7]. However, this scenario does not give a satisfactory explanation to the inset of Fig. 1, and further studies are needed.

Acknowledgements We acknowledge K. Anderson for his valuable help on performing the neutron scattering experiments on IN-6 at ILL, Grenoble.

References
[1] [2] [3] [4] [5] [6] [7] Fig. 2. The intensity of 2.20, 2.34 and 2.45 g cm\ samples subtracted by the intensity of the most dense sample (2.64 g cm\). Pohl, Zeller, Phys. Rev. B 5 (1971) 2029. Y. Inamura et al., Physica B 241}243 (1998) 903. N. Kitamura, K. Fukumi, Phys. Rev. B 50 (1994) 132. S.R. Elliott, Europhys. Lett. 19 (1992) 201. A.P. Sokolov et al., Phys. Rev. Lett. 69 (1992) 1540. T. Nakayama, Phys. Rev. Lett. 80 (1998) 1244. T. Nakayama, J. Phys.: Condens. Matter 10 (1998) L41.