用物理化学约束神经网络,实时预测ALD表面覆盖率并反演反应动力学。
A Physics-Chemistry-Informed Neural Network (PCINN) for Real-Time Spatial-ALD Coverage Prediction and Reliable Kinetics Inversion

- 构建融合流体与表面反应机理的神经网络,仅需30组数据即实现高精度预测。
- 预测速度达7毫秒/次,比传统仿真快五万倍,对数决定系数达0.998。
- 模型可解释且支持动力学参数反演,适合工业过程控制与机理研究者。
空间原子层沉积(SALD)是工业级常压、高通量ALD的核心技术,但其设计与调控受限于表面覆盖率预测的高成本:高保真计算流体力学(CFD)过于缓慢,而解析模型忽略如气体帘幕等传质调制效应。本文提出物理-化学信息神经网络(PCINN),一种兼具CFD精度与实时速度的混合代理模型:单次查询仅需约7毫秒,较单次CFD求解快约5×10⁴倍;在仅30个训练样本覆盖四数量级覆盖率的情况下,测试集对数决定系数达R²_log = 0.998(留一法原始决定系数R²_raw = 0.974)。该架构非黑箱:小型网络仅学习操作条件至近壁浓度闭合关系,而已知表面动力学以可训练化学层形式沿基底轨迹硬编码。此单标量瓶颈使模型在稀疏数据下仍保持高精度、可解释性与可逆性。我们引入完整可辨识性分析(费雪信息矩阵、轮廓似然)。吸附能E_ads与脱附速率k_des可稳健辨识;单一温度下,k_ads无法独立辨识(仅可辨识k_ads·c_wall)。跨四个温度下,预指数因子ν与E_ads沿斜率为0.065 eV/decade的弱辨识退化谷关联,该值由k_B T_eff ln(10)解析导出,并转化为可靠性诊断:七化学不匹配矩阵显示其对任意单一阿伦尼乌斯失配不变,仅当出现第二个热激活过程时发生偏移,因此斜率偏离可标志未建模的位点异质性。数据源自已知真实动力学的仿真,通过相同动力学形式反演,验证了流程自洽性与辨识边界,而非真实参数估计。
原文摘要 · Abstract (English)
Spatial atomic layer deposition (SALD) is a leading atmospheric-pressure, high-throughput route to industrial ALD, but design and control are limited by the cost of predicting surface coverage: high-fidelity CFD is far too slow for operating-window scans, while analytic models miss transport modulation such as the gas curtain. We present a physics-chemistry-informed neural network (PCINN), a hybrid surrogate with CFD-level accuracy at real-time speed: a query returns coverage in about 7 ms, roughly 5x10^4 times faster than a CFD solve, reaching a test R^2_log = 0.998 (leave-one-out R^2_raw = 0.974) from only 30 training cases spanning four orders of magnitude in coverage. The architecture is not a black box: a small network learns only the operating-condition to near-wall concentration closure, while the known surface kinetics is a hard-coded, trainable chemistry layer integrated along the substrate trajectory. This single-scalar bottleneck keeps it accurate under sparse data, interpretable and invertible. We add a full identifiability analysis (Fisher information, profile likelihood). The adsorption energy E_ads and desorption rate k_des are robustly identifiable; k_ads is not separately identifiable at a single temperature (only k_ads*c_wall is). Across four temperatures the prefactor nu and E_ads bind along a weakly identifiable degeneracy valley of slope 0.065 eV/decade, derived analytically as k_B T_eff ln(10) and turned into a reliability diagnostic: a seven-chemistry mismatch matrix shows it is invariant under any single-Arrhenius mismatch and shifts only when a second thermally activated process appears, so a slope departure flags unmodelled site heterogeneity. Data come from simulation with known ground truth inverted by the same kinetic form, so the study verifies pipeline self-consistency and the identifiability boundary, not real parameters.
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