发表机构
Westlake University; Westlake Institute for Advanced Study（西湖大学; 西湖高等研究院）
机构由 AI 辅助整理，请以论文原文为准。AI 中文总结
提出Aurora方法，结合神经量子态与连分数记忆核耦合理论，从变分基态直接重建电子和电子振动光谱，无需激发态，并在多个分子上验证了准确性。
AI 中文摘要
从可扩展的基态表示来模拟分子吸收光谱具有挑战性，因为传统方法通常需要显式的激发态或时间传播。在此，我们提出了一种通过递归算子响应与电子振动增强获得吸收光谱的方法（Aurora），该方法将神经量子态（NQSs）与连分数记忆核耦合理论（CF-MKCT）相结合。Aurora将零温Liouvillian响应层级映射为对偶极制备态重复施加移位哈密顿量的波函数空间操作，从而能够直接从变分基态重建光谱。该实现结合了变分蒙特卡罗、隐式重启Lanczos辅助的NQS优化、无矩阵哈密顿量应用以及自适应递归控制。对于易处理的分子，所得电子光谱与全组态相互作用和传统MKCT参考结果高度一致，重启Lanczos策略改善了困难的NQS情况。对于电子-声子哈密顿量，Aurora结合了Huang-Rhys模式选择与局部奇异值分解（SVD）声子编码器。H2基准表明，压缩保留了主要的电子振动包络，并优于裸局部基截断，而对N2、H2O、H2S和NH3的配对计算在有无编码的情况下均产生相似的主要特征。我们还获得了C6H6和10电子、10轨道C10H8活性空间的电子振动光谱。总体而言，Aurora提供了一条从变分分子基态到电子和电子振动光谱的统一路径，而无需构建激发态流形。
英文摘要
Modelling molecular absorption spectra from scalable ground-state representations is challenging because conventional approaches often require explicit excited states or time propagation. Here, we introduce a method to obtain Absorption Using Recursive Operator Response with vibronic Augmentation (Aurora), which combines neural quantum states (NQSs) with continued-fraction memory-kernel coupling theory (CF-MKCT). Aurora maps the zero-temperature Liouvillian response hierarchy onto repeated wavefunction-space applications of a shifted Hamiltonian to a dipole-prepared state, enabling direct spectral reconstruction from variational ground states. The implementation combines variational Monte Carlo, implicit-restarted-Lanczos-assisted NQS optimization, matrix-free Hamiltonian application, and adaptive recursion control. The resulting electronic spectra closely agree with full-configuration-interaction and conventional MKCT references for tractable molecules, with the restarted-Lanczos strategy improving difficult NQS cases. For electron-phonon Hamiltonians, Aurora combines Huang-Rhys mode selection with local singular-value-decomposition (SVD) phonon encoders. The H2 benchmark indicates that compression retains the dominant vibronic envelope and improves upon bare local-basis truncation, while paired calculations for N2, H2O, H2S, and NH3 yield similar principal features with and without encoding. We further obtain vibronic spectra for C6H6 and a 10-electron, 10-orbital C10H8 active space. Overall, Aurora provides a unified route from variational molecular ground states to electronic and vibronic spectra without constructing excited-state manifolds.
