用智能代理检测并修正材料激发态计算中的数值错误,提升精度。
Agentic multi-fidelity learning of quasiparticle and excitonic properties

- 通过智能代理评估计算可靠性,筛选高精度参考点
- 修复长波长屏蔽导致的能隙塌陷与异常,误差降低60%以上
- 适用于强量子限制纳米材料,如二维半导体、量子点等
多体GW-玻色-萨尔皮特方程计算对现代低维纳米材料电子结构和光学性质模拟至关重要,但计算成本高且易出现局部数值不稳定性或收敛失败,难以在高通量流程中察觉。本文提出一种代理引导的多保真度框架,用于修正应变MoS2-WS2双层中的激发态能带结构。该工作在不同堆叠构型、应变分支及倒空间采样下识别出尖峰状异常、近零能隙坍缩以及跨保真度不一致现象,这些均与脆弱的长波长介电屏蔽有关。结构代理通过赋予置信权重,选择性使用少量高精度参考点。机器学习模型则在相关体系间传递信息,并利用高斯过程修正,恢复更优的准粒子能隙与激子结合能,同时提供校准的不确定性估计。该方法在不抹除物理应变依赖性的前提下,显著改善与高保真参考结果的一致性,相较无代理基线提升明显。结果表明,可靠的激发态材料代理学习需显式诊断数值脆弱性,而非直接插值原始第一性原理数据点。该框架可推广至其他具有强量子限制的光电器件纳米材料,如量子点、纳米带、二维半导体及杂化钙钛矿纳米结构。
原文摘要 · Abstract (English)
Many-body GW-Bethe-Salpeter equation calculations are essential for accurate simulations of electronic structure and optical properties in modern low-dimensional nanomaterials. However, these methods are computationally demanding and can exhibit localized numerical instabilities or convergence failures that are difficult to detect within high-throughput workflows. We introduce an agent-guided multi-fidelity framework for correcting GW-Bethe-Salpeter excited-state landscapes in strained MoS2-WS2 bilayers. Across stacking registries, strain branches and reciprocal-space samplings, the workflow identifies spike-like excursions, near-zero-gap collapse and cross-fidelity inconsistencies associated with fragile long-wavelength dielectric screening. A structural agent evaluates calculations by assigning confidence weights and selectively using a small number of high-accuracy reference points. Machine learning models then transfer information across related systems and apply Gaussian process corrections to recover improved quasiparticle gaps and exciton binding energies, with calibrated uncertainty estimates. The approach corrects numerically induced artifacts without erasing physical strain dependence and substantially improves agreement with higher-fidelity references relative to a no-agent baseline. These results show that reliable surrogate learning for excited-state materials requires explicit diagnosis of numerical fragility, not direct interpolation of raw first-principles data points. The proposed framework is readily transferable to other optoelectronic nanomaterials characterized by strong quantum confinement, such as quantum dots, nanoribbons, layered two-dimensional semiconductors, and hybrid perovskite nanostructures.
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