Gold-standard coupled-cluster accuracy for metals and small-gap solids · revision history
Revision 1
Accepted · first revision · record
- Title
- Gold-standard coupled-cluster accuracy for metals and small-gap solids
- Plain
- The method chemists trust most for molecules, coupled cluster with perturbative triples (an approximate correction for three-electron correlations), gives an infinite correlation energy for metals. A version that works for metals with the same reliability is needed to benchmark surface chemistry and catalysis.
- Precise
- The perturbative triples correction (T) of CCSD(T) diverges for the uniform electron gas and for metals in the thermodynamic limit because of the long-range Coulomb interaction (infrared divergence). Determine whether a modified triples treatment (for example CCSD(cT), 2023) or full CCSDT gives cohesive energies, lattice constants and adsorption energies of simple and noble metals (Li, Na, Al, Cu) within 1 kcal/mol per atom of experiment or of numerically exact quantum Monte Carlo, with finite-size errors controlled. An answer is a convergent method demonstrated on these metals.
- Settled by
- Thermodynamic-limit coupled-cluster calculations on metals and metal surfaces compared with quantum Monte Carlo and experimental cohesive and adsorption energies.
- Kind
- well-posed
- Answer type
- identification
- References
- (empty)
- Literature status
- partially-resolved
- Status note
- In 2023 Masios, Irmler, Schafer and Gruneis (Phys. Rev. Lett., https://doi.org/10.1103/PhysRevLett.131.186401) showed that the CCSD(cT) variant removes the divergence in the uniform electron gas; tests on real metals and surfaces are limited.
- Posed since
- (empty)