(1. 云南冶金集團(tuán)總公司技術(shù)中心，昆明 650031；
2. 昆明理工大學(xué) 冶金與能源工程學(xué)院，昆明 650093；
3. 昆明冶研新材料股份有限公司，昆明 650031)
摘 要: 基于MP2/6-311G(d，p)方法，計(jì)算并得到SiCl4鋅還原各反應(yīng)通道上各駐點(diǎn)的幾何構(gòu)型、振動(dòng)頻率和能量。根據(jù)密度泛函理論，采用廣義密度梯度近似和總體能量平面波贗勢(shì)方法結(jié)合周期性平板模型，研究反應(yīng)駐點(diǎn)在Si(100)面上的吸附、解離及鋅還原過(guò)程。結(jié)果表明：襯底硅參與SiCl4鋅還原反應(yīng)，SiCl4易在頂位吸附解離成—SiCl3和—Cl自由基；當(dāng)硅基表面有—Cl自由基吸附時(shí)，氣相中的Zn原子或硅基面吸附的—ZnCl自由基更容易與—Cl自由基結(jié)合，而不是與含氯的硅自由基(—SiCln，n=1~3)結(jié)合。
關(guān)鍵字: 多晶硅；密度泛函理論；鋅還原；反應(yīng)機(jī)理
（1. The Technique Center of Yunnan Metallurgy Co., Ltd., Kunming 650031, China;
2. Faculty of Metallurgical and Energy Engineering, Kunming University of Science and Technology, Kunming 650093, China;
3. Kunming Yeyan New-Material Co., Ltd., Kunming 650031, China）
Abstract:The channel geometries, vibration frequencies and energy of all stagnations zinc reduction reaction for SiCl4 were calculated through the MP2/6-311G(d, p) method. According to density functional theory, the effects of adsorption, dissociation and zinc reduction of stagnation in the Si(100) surface were studied using the generalized gradient approximation density and total energy plane wave pseudo-potential method combined with periodic slab model. The results show that silicon substrate can participate in zinc reduction reaction of SiCl4, SiCl4 can be absorbed in top sites easily and dissociate into freed radical —SiCl3 and —Cl. When there is —Cl radical adsorbed on the surface of silicon, atom Zn or free radical —ZnCl, which is absorbed on the base silicon, tends to combine with —Cl rather silicon chloride (—SiCln, n=1-3).
Key words: polycrystalline silicon; density functional theory; zinc reduction; reaction mechanisms
