Datasets

The tarball datasets.tar.gz contains all data, including XYZ files, property CSV files, extended XYZ files (for MACE), and dataset splits. It includes three datasets: TM-GSspin+, tmPHOTO, and OctaKulik.

TM-GSspin+

The TM-GSspinPlus/directory contains:

• 0-xyz/: DFT-optimized geometries with only hydrogen atoms optimized in the lowest-spin state (singlet or doublet)
• 1-extended_xyz/: Extended XYZ files for MACE with 10 train/test splits for 10-fold cross-validation (CV)
• 2-cv10-splits/: 10-fold CV index files (indices correspond to row numbers starting from 0 in TM-GSspinPlus_property.csv)
• TM-GSspinPlus_property.csv: Dataset properties, including:
  • refcode: Cambridge Structural Database (CSD) refcode
  • total_charge: Total molecular charge
  • multiplicity: Ground-state spin multiplicity
  • splitting: Vertical spin-splitting energy (kcal/mol)
  • HOMO: HOMO energy (eV)
  • LUMO: LUMO energy (eV)
  • gap: HOMO-LUMO gap (eV)
  • dipole_moment_Debye: Dipole moment magnitude (Debye)

tmPHOTO

The tmPHOTO/ directory contains:

• 0-xyz/: GFN2-xTB optimized geometries (singlet state)
• 1-extended_xyz/: Extended XYZ files for MACE with 10 train/test splits for 10-fold CV
• 2-cv10-splits/: 10-fold CV index files (indices correspond to row numbers starting from 0 in tmPHOTO_property.csv)
• tmPHOTO_property.csv: Dataset properties, including:
  • refcode: CSD refcode
  • total_charge: Total molecular charge
  • multiplicity: Spin multiplicity used in DFT computations (all singlet, 1)
  • HOMO: HOMO energy (Hartree)
  • LUMO: LUMO energy (Hartree)
  • gap: HOMO-LUMO gap (Hartree)
  • dipole_moment_Debye: Dipole moment magnitude (Debye)

OctaKulik

The OctaKulik/ directory contains:

• 0-xyz/: DFT-optimized geometries in low-spin (*_ls.xyz) or high-spin (*_hs.xyz) states

• 1-extended_xyz/: Extended XYZ files for MACE

  • HOMO_LUMO_gap/: 10 train/test splits for HOMO, LUMO, and HOMO-LUMO gap
  • splitting/: 10 train/test splits for spin-splitting energy; low-spin optimized geometries and low-spin multiplicities are used
  • train_valid/: Train/validation split from the reference paper
    (DOI: 10.1088/2632-2153/ad9f22, repository); files with LS correspond to spin-splitting energy targets

• 2-dataset_splits/: contains two subdirectories

  • HOMO_LUMO_gap/: indices corresponding to rows (0-based) in OctaKulik_property_HOMO_LUMO_gap.csv
  • splitting/: indices corresponding to rows (0-based) in OctaKulik_property_splitting.csv
    Each subdirectory contains the directories 2-cv10-splits/ (10-fold CV indices) and 3-train-valid-meyer/ (train/validation indices from the reference paper)

• OctaKulik_train_valid_merged_clean.csv:
  The training data and validation data from the reference paper were merged into a single dataset.
  Refcodes were assigned in this work for convenience. For example, the complex cr_3_[O-]#[C+]_[O-]#[C+]_[O-]#[C+]_[O-]#[C+]_[O-]#[C+]_[O-]#[C+] in the original training set is assigned the refcode train_0116, with geometries train_0116_ls.xyz (low-spin optimized) and train_0116_hs.xyz (high-spin optimized).

• OctaKulik_property_HOMO_LUMO_gap.csv:

  • refcode: Refcode assigned in this work
  • total_charge: Total molecular charge
  • multiplicity: Spin multiplicity used in the computation
  • HOMO: HOMO energy (eV)
  • LUMO: LUMO energy (eV)
  • gap: HOMO-LUMO gap (eV)

• OctaKulik_property_splitting.csv:

  • refcode: Refcode assigned in this work
  • total_charge: Total molecular charge
  • multiplicity: Lowest spin multiplicity among low-spin and high-spin states
  • splitting: Adiabatic spin-splitting energy (kcal/mol)
  • low_spin: Low-spin multiplicity
  • high_spin: High-spin multiplicity

Note: To prepare extended XYZ files for MACE, all energy values are converted to eV.
The following conversion factors are used:

• 1 kcal/mol = 0.0434 eV
• 1 Hartree = 27.2114 eV