First-principles photoemission spectroscopy and orbital tomography in molecules from koopmans-compliant functionals

Ngoc Linh Nguyen, Giovanni Borghi, Andrea Ferretti, Ismaila Dabo, Nicola Marzari

Research output: Contribution to journalArticlepeer-review

31 Scopus citations

Abstract

The determination of spectral properties from first principles can provide powerful connections between microscopic theoretical predictions and experimental data, but requires complex electronic-structure formulations that fall outside the domain of applicability of common approaches, such as density-functional theory. We show here that Koopmans-compliant functionals, constructed to enforce piecewise linearity and the correct discontinuity derivative in energy functionals with respect to fractional occupation - i.e., with respect to charged excitations - provide molecular photoemission spectra and momentum maps of Dyson orbitals that are in excellent agreement with experimental ultraviolet photoemission spectroscopy and orbital tomography data. These results highlight the role of Koopmans-compliant functionals as accurate and inexpensive quasiparticle approximations to the spectral potential.

Original languageEnglish (US)
Article number166405
JournalPhysical Review Letters
Volume114
Issue number16
DOIs
StatePublished - Apr 24 2015

All Science Journal Classification (ASJC) codes

  • Physics and Astronomy(all)

Fingerprint Dive into the research topics of 'First-principles photoemission spectroscopy and orbital tomography in molecules from koopmans-compliant functionals'. Together they form a unique fingerprint.

Cite this