Supporting data for Low Scaling MBE(3)-OSV-MP2 Analytical Gradient Theory and Application

Supporting data for the thesis entitled "Low Scaling MBE(3)-OSV-MP2 Analytical Gradient Theory and Application", composed of results for 1) OSV-MP2 gradients, 2) MBE(3)-OSV-MP2 gradients 3) and Criegee intermediate. We present a many-body expansion (MBE) formulation and implementation for efficient computation of analytical energy gradients from the orbital-specific-virtual second-order Møllet-Plesset perturbation theory (OSV-MP2). The third-order MBE(3) expansion of OSV-MP2 amplitudes and density matrices was developed to adopt the orbital-specific clustering and long-range termination schemes, which avoids term-by term differentiations of the MBE energy bodies.  For an illustrative application, number-adaptive MBE(3)-OSV-MP2/molecular mechanical Born-Oppenheimer molecular dynamics simulations are conducted for Criegee intermediates (CIs) CH2OO and anti-CH3CHOO, important short-lived intermediates generated from ozonolysis in the troposphere, at the surface of a large water microdroplet.

本数据集为题为《基于低标度MBE(3)-OSV-MP2分析梯度理论及其应用》的论文提供支持性数据，包括以下内容：1) OSV-MP2梯度，2) MBE(3)-OSV-MP2梯度，3) 及Criegee中间体。本数据集展示了针对轨道特定-虚二阶Møllet-Plesset微扰理论（OSV-MP2）的解析能量梯度的有效多体展开（MBE）公式的构建与实现。为采用轨道特定聚类和长程终止方案，以避免对MBE能量体的逐项微分，我们对OSV-MP2振幅和密度矩阵进行了三阶MBE(3)展开。为阐明应用实例，我们对大气对流层中臭氧分解产生的两种重要短寿命中间体CH2OO和反CH3CHOO，在大型水微滴表面的分子力学Born-Oppenheimer分子动力学模拟中，进行了数量自适应MBE(3)-OSV-MP2模拟。