Ab Initio 预测各种原子层沉积前体的蒸汽压力
Alexey Odinokov1, Won-Joon Son2, Alexander Yakubovich1
1Samsung Advanced Institute of Technology, Samsung Electronics, 130 Samsung-ro, Suwon 16678, Korea.
Journal of chemical theory and computation
|July 11, 2024
概括
现在可以在没有实验的情况下预测原子层沉积 (ALD) 前体的和蒸气压 (Pvap). 一种新的量子力学推导力场方法准确地估计了Pvap,有助于新型前体设计.
科学领域:
- 材料科学 材料科学 材料科学
- 计算化学计算化学
- 化学工程是化学工程的重要组成部分.
背景情况:
- 和蒸汽压力 (Pvap) 对于评估原子层沉积 (ALD) 前体,定义ALD温度窗口和可加工性至关重要.
- 预测Pvap对于早期新型前体设计至关重要,减少了实验合成需求.
- 目前用于Pvap预测的计算方法因缺乏适合分子动态的经验力场而受到限制,特别是对于包括金属,有机物和化物在内的各种化学物质.
研究的目的:
- 引入一种新的计算方法,用于预测原子层沉积 (ALD) 前体的和蒸气压 (Pvap).
- 开发一种可用于广泛的潜在ALD前体,包括具有新元素的潜在ALD前体的强大和多功能方法.
- 在不依赖实验数据的情况下实现准确的Pvap估计,从而加速新ALD前体的设计.
主要方法:
- 使用量子力学衍生力场进行分子动力学模拟.
- 开发了一种工作流来模拟液体和气体平衡阶段,用于Pvap计算.
- 使用基于单个分子的ab initio计算,参数化系统特定的力场.
主要成果:
- 对于各种ALD前体,在广泛的温度范围内实现了Pvap的稳健预测.
- 在对数尺度上验证了与比尔森相关系数 (R^2) 大于0.9的方法.
- 获得了自我溶解无能量的根平均平方偏差,低至1.3 kcal mol^-1.
结论:
- 开发的工作流提供了一个准确的,数据独立的方法来预测ALD前体的Pvap.
- 这种方法显著推进了新型ALD前体的计算机辅助设计.
- 通过实现更快的前体发现和过程优化,加速技术发展.
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