High-resolution Valence and Core Excitation Spectra via First-Principles Calculations and Experiment

We calculate the optical and C K-edge near edge spectra of crystalline and molecular C$_{\mathrm{60}}$ measured with high-resolution electron energy-loss spectroscopy. The calculations are carried out using at least three different methods: Bethe-Salpeter calculations using the NIST Bethe-Salpeter Equation solver (NBSE) in the valence and OCEAN (Obtaining Core Excitation with Ab initio methods and NBSE) suite [Gilmore et al., Comp. Phys. Comm., (2015)]; excited-core-hole calculations using XCH [D. Prendergast and G. Galli, Phys. Rev. Lett. 96, 215502 (2006)]; and constrained occupancy using StoBe ( Stockholm-Berlin core-excitation code) [StoBe-deMon version 3.0, K. Hermann et al. (2009)]. They include self-energy effects, lifetime-damping, and Debye-Waller effects. A comparison of spectral features to those observed illustrates the sensitivity of certain features to computation details (e.g., self-energy corrections and core-hole screening). This may point to limitations of various approximations, e.g. in conventional BSE paradigm and/or the incomplete treatment of vibrational effects.