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Radical-Enhanced Atomic Layer Deposition of a Tungsten Oxide Film with the Tunable Oxygen Vacancy Concentration
The Journal of Physical Chemistry C ( IF 3.3 ) Pub Date : 2020-07-24 , DOI: 10.1021/acs.jpcc.0c05446 Roman I. Romanov 1 , Maxim G. Kozodaev 1 , Yury Y. Lebedinskii 1 , Timofey V. Perevalov 2 , Aleksandr S. Slavich 1 , Cheol Seong Hwang 3 , Andrey M. Markeev 1
The Journal of Physical Chemistry C ( IF 3.3 ) Pub Date : 2020-07-24 , DOI: 10.1021/acs.jpcc.0c05446 Roman I. Romanov 1 , Maxim G. Kozodaev 1 , Yury Y. Lebedinskii 1 , Timofey V. Perevalov 2 , Aleksandr S. Slavich 1 , Cheol Seong Hwang 3 , Andrey M. Markeev 1
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This work reports a radical-enhanced atomic layer deposition (REALD) process using WH2(Cp)2–O*–H* reaction cycles (Cp = cyclopentadienyl group) to grow WO3–x films with a wide range of tunable oxygen vacancy (VO) concentrations where O* and H* represent oxygen and hydrogen radicals, respectively. The fundamental WH2(Cp)2–O* ALD process was characterized by saturation behavior for the W-precursor/O* dose, high deposition uniformity, and a short incubation period. The VO concentration could be limitedly controlled up to ∼0.7 at. % when the O* dose was appropriately decreased within the ALD saturation range. However, a further increase in the VO concentration could hardly be achieved by simply decreasing the O* dose, which accompanied the carbon-related impurities due to incomplete ligand release from the growing film. The addition of the H* pulse step in each ALD cycle rendered it possible to achieve a much higher VO concentration up to ∼5 at. % without disturbing the ALD saturation conditions and involving any carbon-containing impurities. Ab initio calculations of the valence band (VB) spectra, assuming oxygen-deficient WO3–x, showed good agreement with the experimental VB X-ray photoelectron spectroscopy (XPS) data, which corroborated the estimated VO concentrations based on the core-level XPS data. The increase in the VO concentration obtained in the new reaction cycle process was accompanied by a significant film resistivity decrease and a noticeable change in the crystalline structure. The VO concentration-controlled WO3–x films could be a viable material for diverse electronic applications, including resistive random-access memory devices.
中文翻译：
具有可调氧空位浓度的氧化钨膜的原子增强原子层沉积
这项工作报告了使用WH 2（Cp）2 –O * –H *反应周期（Cp =环戊二烯基）的自由基增强原子层沉积（REALD）工艺，以生长具有宽范围可调节氧空位的WO 3– x膜（V ø）的浓度其中O *和H *表示氧和氢自由基，分别。基本WH 2（Cp）2 -O * ALD工艺的特征在于W前体/ O *剂量的饱和行为，高沉积均匀性和较短的孵育时间。V O的浓度可以有限地控制在约0.7 at。当O *剂量在ALD饱和范围内适当降低时的％。但是，V进一步增加仅通过降低O *剂量很难达到O浓度，O *剂量伴随着与碳有关的杂质，这是由于从生长膜中释放的配体不完全。在每个ALD周期中增加H *脉冲步长，有可能获得更高的V O浓度，最高可达〜5 at。％，而不会干扰ALD饱和条件并且涉及任何含碳杂质。从头价带（VB）光谱，假定氧不足型的WO的计算3- X，表现出与实验VB X射线光电子能谱（XPS）数据，该数据证实了估计的V一致Ò基于所述核-浓度级XPS数据。V O的增加在新的反应循环过程中获得的浓度升高，则膜电阻率显着降低，晶体结构发生明显变化。V O浓度控制的WO 3 – x膜可能是多种电子应用的可行材料，包括电阻性随机存取存储设备。
更新日期：2020-08-20
中文翻译：
具有可调氧空位浓度的氧化钨膜的原子增强原子层沉积
这项工作报告了使用WH 2（Cp）2 –O * –H *反应周期（Cp =环戊二烯基）的自由基增强原子层沉积（REALD）工艺，以生长具有宽范围可调节氧空位的WO 3– x膜（V ø）的浓度其中O *和H *表示氧和氢自由基，分别。基本WH 2（Cp）2 -O * ALD工艺的特征在于W前体/ O *剂量的饱和行为，高沉积均匀性和较短的孵育时间。V O的浓度可以有限地控制在约0.7 at。当O *剂量在ALD饱和范围内适当降低时的％。但是，V进一步增加仅通过降低O *剂量很难达到O浓度，O *剂量伴随着与碳有关的杂质，这是由于从生长膜中释放的配体不完全。在每个ALD周期中增加H *脉冲步长，有可能获得更高的V O浓度，最高可达〜5 at。％，而不会干扰ALD饱和条件并且涉及任何含碳杂质。从头价带（VB）光谱，假定氧不足型的WO的计算3- X，表现出与实验VB X射线光电子能谱（XPS）数据，该数据证实了估计的V一致Ò基于所述核-浓度级XPS数据。V O的增加在新的反应循环过程中获得的浓度升高，则膜电阻率显着降低，晶体结构发生明显变化。V O浓度控制的WO 3 – x膜可能是多种电子应用的可行材料，包括电阻性随机存取存储设备。
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