Direct observation of concentration fluctuations in Au-Si eutectic liquid by small-angle neutron scattering

Yoshifumi Sakaguchi; Shin-Ichi Takata; Yukinobu Kawakita; Yuki Fujimura; Keietsu Kondo

doi:10.1088/1361-648X/ace577

Direct observation of concentration fluctuations in Au-Si eutectic liquid by small-angle neutron scattering

J Phys Condens Matter. 2023 Jul 17;35(41). doi: 10.1088/1361-648X/ace577.

Authors

Yoshifumi Sakaguchi¹, Shin-Ichi Takata², Yukinobu Kawakita², Yuki Fujimura³, Keietsu Kondo³

Affiliations

¹ Neutron Science and Technology Center, Comprehensive Research Organization for Science and Society, 162-1 Shirakata, Tokai, Ibaraki 319-1106, Japan.
² J-PARC Center, Japan Atomic Energy Agency, 2-4 Shirakata, Tokai, Ibaraki 319-1195, Japan.
³ Nuclear Science and Engineering Center, Japan Atomic Energy Agency, 2-4 Shirakata, Tokai, Ibaraki 319-1195, Japan.

PMID: 37419121
DOI: 10.1088/1361-648X/ace577

Abstract

It is well-known that eutectic gold-silicon (Au-Si) alloys exhibit anomalous melting point depression, which is more than 1000 °C from the melting point of elemental Si (1414 °C). The melting point depression in eutectic alloys is generally explained in terms of a decrease of the free energy by mixing. However, it is difficult to understand the anomalous melting point depression only from the stability of the homogeneous mixing. Some researchers suggest that there are concentration fluctuations in the liquids, where the atoms are inhomogeneously mixed. In this paper, we measure the small-angle neutron scattering (SANS) of Au_81.4Si_18.6(eutectic composition) and Au₇₅Si₂₅(off-eutectic composition) at temperatures from room temperature to 900 °C in both solid and liquid states to observe such concentration fluctuations directly. It is surprising that large SANS signals are observed in the liquids. This indicates that there are concentration fluctuations in the liquids. The concentration fluctuations are characterized by either the correlation lengths in multiple length scales or surface fractals. This finding yields new insight into the mixing state in the eutectic liquids. The mechanism of the anomalous melting point depression is discussed based on the concentration fluctuations.

Keywords: Au–Si system; anomalous melting point depression; concentration fluctuations; eutectic alloys; small-angle neutron scattering.