We investigate the role of nonlocal correlations in LiFeAs by exploring an ab initio–derived multiorbital Hubbard model for LiFeAs via the two-particle self-consistent (TPSC) approach. The multiorbital formulation of TPSC approximates the irreducible interaction vertex to be an orbital-dependent constant, which is self-consistently determined from local spin and charge sum rules. Within this approach, we disentangle the contribution of local and nonlocal correlations in LiFeAs and show that in the local approximation one recovers the dynamical mean field theory result. The comparison of our theoretical results to most recent angular-resolved photoemission spectroscopy and de Haas–van Alphen data shows that nonlocal correlations in LiFeAs are decisive to describe the measured spectral function $A(\overrightarrow{k},\omega )$, Fermi surface, and scattering rates. These findings underline the importance of nonlocal correlations and benchmark different theoretical approaches for iron-based superconductors.

• Received 3 July 2019
• Corrected 17 November 2020

DOI:https://doi.org/10.1103/PhysRevLett.123.256401