SHNITSEL - Surface Hopping Nested Instances Training Set for Excited-state Learning
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SHNITSEL-dynamic K. Höllring, T. E. Röhrkasten & C. Müller The Surface Hopping Nested Instances Training Set for Excited-State Learning (SHNITSEL) is a comprehensive data repository designed to support the development and benchmarking of excited-state dynamics methods. SHNITSEL-dynamic contains datasets with comprehensive surface hopping trajectory data of five organic molecules: Alkenes: ethene (A01), propene (A02), 2-butene (A03) Ring structures: 1,3-cyclohexadiene (R02) The data are stored in xarray format using xarray.DataTree objects for efficient handling of multidimensional trajectory ensembles. Metadata such as units, electronic-structure method, charge, and number of electronic states are stored as attributes of the individual datasets within the tree. The datasets contain key electronic-structure quantities for singlet and triplet states, including energies, nuclear forces, dipole moments, transition dipole moments, nonadiabatic couplings, and spin-orbit couplings, computed at the multireference ab initio level. Two data representations are provided: Stacked (#271,700 data points in total): for each molecule, the DataTree contains a single dataset in which all trajectories are stacked along a trajectory dimension. Unstacked (#271,700 data points in total): for each molecule, the DataTree contains one dataset per trajectory, stored as individual leaves. These complementary formats allow users to choose between trajectory-resolved and ensemble-level data representations depending on their analysis needs. ---------------------------------------- Additional Datasets for I01 (CH2NH2+) S. Mai & J. C. B. Dietschreit a) About Two additional datasets for compound I01 are provided, aiming to sample the free energy surface around the S1/S0 conical intersection (I01_dietschreit_sa2-cas22_196_S1traj.nc) and sample the photoinduced dynamics (I01_dietschreit_sa2-cas22_500_fssh.nc). b) Computational Details Dynamics: NAMD method: SHARC4 surface hopping was turned off and a Langevin thermostat (1000K) was activated to sample the free energy surface around the S1/S0 conical intersection (I01_dietschreit_sa2-cas22_196_S1traj.nc) surface hopping (gradients for all states, NACs computed with nacdr, I01_dietschreit_sa2-cas22_500_fssh.nc) timestep: 0.5 fs, substeps: 25 total time: 5000 fs (10000 time steps, 01_dietschreit_sa2-cas22_196_S1traj.nc) 100 fs (200 time steps, I01_dietschreit_sa2-cas22_500_fssh.nc) number of trajectories: 196 (I01_dietschreit_sa2-cas22_196_S1traj.nc) 4999 (I01_dietschreit_sa2-cas22_500_fssh.nc) Electronic structure theory: engine: OpenMOLCAS (v24.06) reference method: SA(2)-CAS(2,2) (state-average CASSCF) basis set: cc-pVDZ charge: +1 states: two lowest singlets (S0 and S1) as active states ---------------------------------------- Data of Aza-Diarylethenes (R04 & R06) M. Hartinger & C. Müller a) About Aza-diarylethenes (aDAEs) are emerging photoswitches that undergo reversible light-induced C–N bond formation. This dataset contains surface-hopping trajectories for two representative aDAEs, R04 (corresponding to D-open in 10.1039/D6CP01330A) and R06 (corresponding to K-open in 10.1039/D6CP01330A), generated to investigate the mechanistic origin of their distinct photochemical outcomes. This dataset contains surface-hopping trajectories classified according to their photochemical outcome. Trajectories are categorized as productive (leading to formation of the closed isomer), unproductive (returning to the open isomer or forming rare side products), and still excited (remaining in an excited electronic state at the end of the simulation). R04: 45% productive, 43% unproductive, 11% still excited R06: 29% productive, 66% unproductive, 5% still excited b) Computational Details Dynamics: NAMD method: trajectory surface hopping with Zhu-Nakamura algorithm in PyRAI2MD timestep: 0.5 fs total time: up to 1 ps for R06 and up to 2 ps for R04 number of trajectories: 97 trajectories each for R04 and R06 Electronic structure theory: engine: OpenQP reference method: MRSF-TD-DTCAM-AEE (mixed-reference spin-flip TD-DFT) basis set: 6-31G* charge: 0 states: three lowest singlets (S0, S1 and S2) as active states
SHNITSEL-dynamic K. Höllring、T. E. Röhrkasten 与 C. Müller 激发态学习用表面跳跃嵌套实例训练集（Surface Hopping Nested Instances Training Set for Excited-State Learning，SHNITSEL）是一套综合性数据资源库，旨在支撑激发态动力学方法的开发与基准测试。 SHNITSEL-dynamic 包含五种有机分子的全面表面跳跃轨迹数据集： 烯烃类：乙烯（ethene，A01）、丙烯（propene，A02）、2-丁烯（2-butene，A03） 环结构类：1,3-环己二烯（1,3-cyclohexadiene，R02） 数据以xarray格式存储，采用xarray.DataTree 对象（xarray.DataTree）实现多维轨迹集合的高效处理。元数据（如单位、电子结构方法、电荷与电子态数目）存储于树内各独立数据集的属性中。 数据集涵盖单重态与三重态的关键电子结构参量，包括能量、核力、偶极矩、跃迁偶极矩、非绝热耦合以及自旋轨道耦合，所有数据均通过多参考从头算方法计算得到。 本次提供两种数据表示形式： 堆叠式（总计271700个数据点）：针对每个分子，xarray.DataTree 包含单个数据集，所有轨迹沿轨迹维度堆叠存储。 非堆叠式（总计271700个数据点）：针对每个分子，xarray.DataTree 为每条轨迹分别存储一个数据集，作为独立叶节点。 这两种互补格式可让用户根据分析需求，选择轨迹分辨或系综级的数据表示形式。 ---------------------------------------- 针对化合物I01的附加数据集 S. Mai 与 J. C. B. Dietschreit a) 概述 本次提供针对化合物I01的两套附加数据集，旨在采样S1/S0锥形交叉点附近的自由能面（I01_dietschreit_sa2-cas22_196_S1traj.nc）以及光诱导动力学过程（I01_dietschreit_sa2-cas22_500_fssh.nc）。 b) 计算细节 动力学设置： 非绝热分子动力学（Nonadiabatic Molecular Dynamics，NAMD）方法：SHARC4 对于I01_dietschreit_sa2-cas22_196_S1traj.nc：关闭表面跳跃，启用朗之万恒温器（1000K）以采样S1/S0锥形交叉点附近的自由能面。 对于I01_dietschreit_sa2-cas22_500_fssh.nc：启用表面跳跃（所有态的梯度，使用nacdr程序计算非绝热耦合）。 时间步长：0.5 fs，子步数：25 总模拟时长： 5000 fs（10000个时间步，对应I01_dietschreit_sa2-cas22_196_S1traj.nc） 100 fs（200个时间步，对应I01_dietschreit_sa2-cas22_500_fssh.nc） 轨迹数目： 196条（对应I01_dietschreit_sa2-cas22_196_S1traj.nc） 4999条（对应I01_dietschreit_sa2-cas22_500_fssh.nc） 电子结构理论： 计算引擎：OpenMOLCAS（v24.06） 参考方法：态平均完全活性空间自洽场（state-average CASSCF，SA(2)-CAS(2,2)） 基组：cc-pVDZ 电荷：+1 活性电子态：两个最低单重态（S0与S1） ---------------------------------------- 氮杂二芳基乙烯（Aza-Diarylethenes，R04与R06）数据集 M. Hartinger 与 C. Müller a) 概述 氮杂二芳基乙烯（aDAEs）是一类新兴的光开关分子，可发生可逆光诱导C-N键形成反应。本数据集包含两种代表性aDAE的表面跳跃轨迹：R04（对应文献10.1039/D6CP01330A中的D-open构型）与R06（对应文献10.1039/D6CP01330A中的K-open构型），用于探究其不同光化学产物的机理起源。 本数据集根据轨迹的光化学结果进行分类：轨迹可分为有效轨迹（生成闭环异构体）、无效轨迹（返回开环异构体或生成罕见副产物）以及仍处于激发态的轨迹（模拟结束时仍保留在激发电子态）。 R04：45%有效轨迹、43%无效轨迹、11%仍处于激发态的轨迹 R06：29%有效轨迹、66%无效轨迹、5%仍处于激发态的轨迹 b) 计算细节 动力学设置： 非绝热分子动力学方法：采用PyRAI2MD中的Zhu-Nakamura算法实现轨迹表面跳跃 时间步长：0.5 fs 总模拟时长：R06最长1 ps，R04最长2 ps 轨迹数目：R04与R06各包含97条轨迹 电子结构理论： 计算引擎：OpenQP 参考方法：混合参考自旋翻转含时密度泛函（mixed-reference spin-flip TD-DFT，MRSF-TD-DTCAM-AEE） 基组：6-31G* 电荷：0 活性电子态：三个最低单重态（S0、S1与S2）
