Au Nanoparticle Formation from Amorphous Au/Si Multilayer

Abstract

By direct observations of transmission electron microscopy (TEM), irreversible morphological transformations of as-deposited amorphous Au/Si multilayer (a-Au/a-Si) were observed on heating. The well arrayed sequence of the multilayer changed to zigzag layered structure at 478 K (=T zig). Finally, the zigzag structure transformed to Au nanoparticles at 508 K. The distribution of the Au nanoparticles was random within the thin film. In situ X-ray diffraction during heating can clarify partial crystallization Si (c-Si) in the multilayer at 450 K (= T ML MIC), which corresponds to metal induced crystallization (MIC) from amorphous Si (a-Si) accompanying by Au diffusion. On further heating, a-Au started to crystallize at around 480 K (=T c) and gradually grew up to 3.2 nm in radius, although the volume of c-Si was almost constant. Continuous heating caused crystal Au (c-Au) melting into liquid AuSi (ℓ-AuSi) at 600 K (= T NP m), which was lower than bulk eutectic temperature (T B E = 636 5 K ±). Due to the AuSi eutectic effect, reversible phase transition between liquid and solid occurred once temperature is larger than T NP m. Proportionally to the maximum temperatures at each cycles (673, 873 and 1073 K), both T NP m and Au crystallization temperature approaches to T B E. Using a thermodynamic theory of the nanoparticle formation in the eutectic system, the relationship between T NP m and the nanoparticle size is explained.