HomeMachine LearningarXiv:2605.29622

M\=oLe-{\Lambda}: Learning the Coupled-Cluster Response State for Energies, Gradients, and Properties

Machine Learningphysics.chem-ph2026-05v1license

Abstract

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 TT-amplitudes determine the correlated wavefunction, many practically important observables additionally require the left-hand Λ\Lambda-amplitudes. We introduce M\=oLe-Λ\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 (T1,T2)(T_1,T_2) and left-hand amplitudes (Λ1,Λ2)(\Lambda_1,\Lambda_2) from localized Hartree--Fock molecular orbitals. Architecturally, M\=oLe-Λ\Lambda extends M\=oLe with Λ1\Lambda_1 and Λ2\Lambda_2 readouts that mirror the symmetry constraints of the T1T_1 and T2T_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-Λ\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.

Comments: ICML 2026 AI4Physics

Cite

@article{arxiv.2605.29622,
  title  = {M\=oLe-{\Lambda}: Learning the Coupled-Cluster Response State for Energies, Gradients, and Properties},
  author = {Andreas Burger and Luca Thiede and Abdulrahman Aldossary and Jorge A. Campos-Gonzalez-Angulo and Alex Zook and Jérôme Florian Gonthier and Alán Aspuru-Guzik},
  journal= {arXiv preprint arXiv:2605.29622},
  year   = {2026}
}