M\=oLe-{\Lambda}: Learning the Coupled-Cluster Response State for Energies, Gradients, and Properties
About
Coupled-cluster (CC) theory is often considered the gold standard of quantum chemistry, but its high computational cost limits routine access to accurate energies, forces and response properties. While the right-hand $T$-amplitudes determine the correlated wavefunction, many practically important observables additionally require the left-hand $\Lambda$-amplitudes. We introduce M\=oLe-$\Lambda$, an extension of Molecular Orbital Learning (M\=oLe) that predicts the full ground-state coupled-cluster singles and doubles (CCSD) response state by jointly learning right-hand amplitudes $(T_1,T_2)$ and left-hand amplitudes $(\Lambda_1,\Lambda_2)$ from localized Hartree--Fock molecular orbitals. Architecturally, M\=oLe-$\Lambda$ extends M\=oLe with $\Lambda_1$ and $\Lambda_2$ readouts that mirror the symmetry constraints of the $T_1$ and $T_2$ heads, while preserving the original equivariant orbital encoder, odd sign-equivariant decoding, locality and size-extensivity. The resulting model yields accurate CC-quality energies and forces, while simultaneously recovering dipoles, quadrupoles, polarizabilities, the electron density, and 2-electron observables such as the pair density. We show that M\=oLe-$\Lambda$ further extends the speed advantage of M\=oLe over full CCSD while substantially expanding the accessible properties, providing a route to wavefunction-level surrogate models for correlated quantum chemistry.
Related benchmarks
| Task | Dataset | Result | Rank | |
|---|---|---|---|---|
| Energy and force prediction | QM7 (val) | Energy (E)0.1 | 6 | |
| Energy and force prediction | Amino acids (size extrapolation) | Energy (E)0.37 | 6 | |
| Energy and force prediction | PubChem size extrapolation | Energy (E)0.63 | 6 | |
| Energy and force prediction | Diels-Alder (out-of-equilibrium) | Energy1.09 | 6 | |
| Energy and force prediction | Dihedral scan (out-of-equilibrium) | Energy0.29 | 6 | |
| Energy and force prediction | Chair-to-boat (out-of-equilibrium) | Energy (E)0.4 | 6 |