Delocalized Coupled-Cluster Theory for Polaron Structure and Dynamics
Polaron ground states and finite-temperature dynamics remain challenging to simulate because existing methods struggle to combine nonperturbative accuracy, systematic improvability, and scalability from models to materials-specific Hamiltonians. We introduce a translationally invariant variational coupled-cluster (CC) theory for polarons, termed delocalized CC (dCC), with closed-form energies at cost as low as $\mathcal{O}(N^3)$ and no phonon-number cutoff. dCC accurately describes the ground states of the one- and two-dimensional Holstein and Su--Schrieffer--Heeger (optical and bond) models and the Fr{ö}hlich model, in close agreement with density matrix renormalization group (DMRG) and diagrammatic Monte Carlo benchmarks. A projected tangent-space response formalism built on the same ansatz yields electron-addition spectral functions and optical conductivities at zero and finite temperature. The resulting spectra agree well with DMRG, Lanczos, and neural-network quantum-state benchmarks while retaining a physically interpretable excitation hierarchy, and extend to two-dimensional lattices at finite temperature beyond the practical reach of these methods. The same framework applies directly to \textit{ab initio} electron--phonon matrix elements, yielding LiF electron- and hole-polaron binding energies that match state-of-the-art many-body calculations. These results establish dCC as a unified variational framework for polaron ground states and dynamics, from model systems to real materials.