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Atomic Layer Etching of AlF3 Using Sequential, Self-Limiting Thermal Reactions with Sn(acac)2 and Hydrogen Fluoride
The Journal of Physical Chemistry C ( IF 3.3 ) Pub Date : 2015-11-02 00:00:00 , DOI: 10.1021/acs.jpcc.5b07236 Younghee Lee 1 , Jaime W. DuMont 1 , Steven M. George 1
The Journal of Physical Chemistry C ( IF 3.3 ) Pub Date : 2015-11-02 00:00:00 , DOI: 10.1021/acs.jpcc.5b07236 Younghee Lee 1 , Jaime W. DuMont 1 , Steven M. George 1
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The atomic layer etching (ALE) of AlF3 was demonstrated using sequential thermal reactions with Sn(acac)2 and hydrogen fluoride (HF) as the reactants. AlF3 ALE is the first example of the thermal ALE of a metal fluoride. AlF3 ALE was investigated using in situ quartz crystal microbalance (QCM) and Fourier transform infrared (FTIR) measurements at temperatures from 150 to 250 °C. The QCM studies observed that AlF3 was etched linearly with atomic level precision versus number of sequential reactant cycles. QCM investigations also revealed that the sequential Sn(acac)2 and HF reactions were self-limiting versus reactant exposure. The FTIR spectroscopic analysis observed AlF3 etching by monitoring the loss of absorbance of Al–F stretching vibrations in the AlF3 film. The FTIR studies also suggested that the Sn(acac)2 reaction is self-limiting because of the buildup of acac-containing species on the AlF3 surface. The QCM measurements determined that the mass change per cycle (MCPC) increased with temperature from −2.0 ng/(cm2 cycle) at 150 °C to −18.2 ng/(cm2 cycle) at 250 °C. These MCPC values are equivalent to etch rates from 0.069 Å/cycle at 150 °C to 0.63 Å/cycle at 250 °C. In the proposed reaction mechanism for AlF3 ALE, the Sn(acac)2 reactant accepts fluorine from AlF3 and donates acac to the surface. This reaction is believed to yield SnF(acac) and AlF(acac)2 as volatile reaction products. The QCM and FTIR results suggest that the HF reaction converts AlF2(acac)* surface intermediates to AlF3* and volatile acacH reaction products. The ALE of other metal fluorides using Sn(acac)2 and HF should be possible by a similar mechanism.
中文翻译：
利用Sn（acac）2和氟化氢的顺序自限热反应对AlF 3进行原子层蚀刻
使用Sn（acac）2和氟化氢（HF）作为反应物的顺序热反应证明了AlF 3的原子层蚀刻（ALE）。AlF 3 ALE是金属氟化物的热ALE的第一个示例。使用原位石英晶体微天平（QCM）和傅立叶变换红外（FTIR）在150至250°C的温度下对AlF 3 ALE进行了研究。QCM研究发现，AlF 3以原子级精度相对于顺序反应物循环数线性蚀刻。QCM调查还显示，连续的Sn（acac）2和HF反应与反应物暴露是自限性的。FTIR光谱分析观察AlF通过监测AlF 3膜中Al–F拉伸振动的吸光度损失来进行3蚀刻。FTIR研究还表明，Sn（acac）2反应是自限性的，因为在AlF 3表面上会形成含acac的物质。QCM测量确定，每循环质量变化（MCPC）随着温度从150°C时的-2.0 ng /（cm 2循环）增加到250°C时的-18.2 ng /（cm 2循环）。这些MCPC值相当于从150°C的0.069Å/循环到250°C的0.63Å/循环的蚀刻速率。在拟议的AlF 3 ALE反应机理中，Sn（acac）2反应物从AlF 3接受氟并向表面捐赠acac。据信该反应产生作为挥发性反应产物的SnF（acac）和AlF（acac）2。QCM和FTIR结果表明，HF反应将AlF 2（acac）*表面中间体转化为AlF 3 *和挥发性acacH反应产物。采用类似的机制，使用Sn（acac）2和HF的其他金属氟化物的ALE应该是可能的。
更新日期：2015-11-02
中文翻译：
利用Sn（acac）2和氟化氢的顺序自限热反应对AlF 3进行原子层蚀刻
使用Sn（acac）2和氟化氢（HF）作为反应物的顺序热反应证明了AlF 3的原子层蚀刻（ALE）。AlF 3 ALE是金属氟化物的热ALE的第一个示例。使用原位石英晶体微天平（QCM）和傅立叶变换红外（FTIR）在150至250°C的温度下对AlF 3 ALE进行了研究。QCM研究发现，AlF 3以原子级精度相对于顺序反应物循环数线性蚀刻。QCM调查还显示，连续的Sn（acac）2和HF反应与反应物暴露是自限性的。FTIR光谱分析观察AlF通过监测AlF 3膜中Al–F拉伸振动的吸光度损失来进行3蚀刻。FTIR研究还表明，Sn（acac）2反应是自限性的，因为在AlF 3表面上会形成含acac的物质。QCM测量确定，每循环质量变化（MCPC）随着温度从150°C时的-2.0 ng /（cm 2循环）增加到250°C时的-18.2 ng /（cm 2循环）。这些MCPC值相当于从150°C的0.069Å/循环到250°C的0.63Å/循环的蚀刻速率。在拟议的AlF 3 ALE反应机理中，Sn（acac）2反应物从AlF 3接受氟并向表面捐赠acac。据信该反应产生作为挥发性反应产物的SnF（acac）和AlF（acac）2。QCM和FTIR结果表明，HF反应将AlF 2（acac）*表面中间体转化为AlF 3 *和挥发性acacH反应产物。采用类似的机制，使用Sn（acac）2和HF的其他金属氟化物的ALE应该是可能的。
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