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用密度泛函方法研究了ZrO2在羟基预处理的Si(100)-2×1表面原子层淀积(ALD)初始反应过程的反应机理,ZrO2的ALD过程包括两个前体反应物ZrCl4和H2O交替的半反应.两个半反应都经历一个相似的吸附中间体反应路径.比较单羟基Si表面反应的反应焓变,可以发现双羟基Si表面反应,由于相邻羟基的存在,对ZrCl4的半反应影响较大,尤其是化学吸附能增加明显.而对于H2O的半反应,单、双羟基Si表面反应的能量变化不是很明显.使用内禀反应坐标(IRC)方法,验证了两个半反应存在相似的过渡态结构和反应机理.另外,发现随着温度的升高,吸附络合物的稳定性降低,其向反应物方向的解吸附变得容易,而向产物方向的解离难度增加.
The reaction mechanism of ZrO2 on the initial reaction of atomic layer deposition (ALD) on Si (100) -2 × 1 surface was studied by means of density functional theory. The ALD process of ZrO2 includes two precursors, ZrCl4 and H2O Alternating half-reaction.All the two half-reactions all undergo a similar adsorption intermediate reaction pathway.Comparing the reaction enthalpy change of the mono-hydroxyl Si surface reaction, we can find that the surface of the bishydroxy Si reaction, due to the presence of adjacent hydroxyl, on the ZrCl4 half Especially the chemisorption.While for the half-reaction of H2O, the energy change of the surface reaction of mono-and bishydroxy Si is not obvious.Using the intrinsic reaction coordinate (IRC) method, the two half-reactions In addition, it was found that with the increase of temperature, the stability of the adsorbed complex decreased, its desorption in the reactant direction became easy and the dissociation in the product direction was more difficult .