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R. J. Nemanich Department of Physics and Department of Materials Science and Engineering, North Carolina State University, Raleigh, North Carolina 27695-8202 (Received 16 February 1990; accepted 20 August 1990) Silicide formation due to thermal treatment of thin (5-10 nm) molybdenum films on single-crystal, polycrystalline, and hydrogenated amorphous silicon substrates in the temperature range of 100 to 1000 °C was studied, with an emphasis on the initial interactions. The molybdenum deposition, annealing, and characterization using Raman scattering and Auger electron spectroscopy was carried out in UHV in order to minimize the effects of contaminants. Raman spectroscopy is used to distinguish between tetragonal (f-MoSi2) and hexagonal MoSi2 (h-MoSi2). The Raman spectrum of bulk tetragonal MoSi2 exhibits two prominent lines which are associated with theylig (325 cm"1) and Eg (440 cm"1) modes. The only silicide phases detected in the thin film experiments were £-MoSi2 and h-MoSi2- While hexagonal MoSi2 does not appear in the bulk phase diagram, it is the first silicide phase formed in thin film reactions at a temperature between 300 and 400 °C. The nucleation temperature of /z-MoSi2 was the same for Si(100), Si(lll), and amorphous Si. Indirect evidence for disordered intermixing of silicon and molybdenum before nucleation of /i-MoSi2 is found. Annealing at approximately 800 °C causes the silicide to transform from the hexagonal phase to the tetragonal phase for all substrates. Contaminants interfere with the formation of /i-MoSi2 and also retard the transformation of /i-MoSi2 to £-MoSi2. For the thin films considered here, the transformation to ?-MoSi2 is accompanied by islanding of the silicide film. A lower interfacial energy between the silicon and silicide for /i-MoSi2 has been proposed to explain the nucleation of /z-MoSi2 before f-MoSi2.

I. INTRODUCTION

The formation of a silicide film by the thermal treatment of a thin metal film on a silicon substrate is of technological and scientific interest. The steady decrease in the typical feature size of integrated circuits has led to interest in alternative materials for interconnects and contacts. Metal silicides are one class of materials of interest for these applications.1"6 As a result, the structure, properties, and the formation of metal silicides have been studied. There is scientific interest in these materials, as well, since the formation of a silicide film on a silicon substrate can be viewed as a model solidstate thin-film reaction. This particular system is an ideal model to study, since well characterized singlecrystal silicon substrates are readily available. The use of a thin film facilitates the study of the initial interactions involved in a solid-state reaction, since diffusion aspects can be minimized. Although bulk thermodynamics can provide predictions of the course of solid-state reactions, these predictions are not always successful for thin-film reactions.7'8 This implies that other factors need to be considered. In addition to 2854

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