相关论文: Tomographic identification of all molecular orbita…
In the past decade, photoemission orbital tomography (POT) has evolved into a powerful tool to investigate the electronic structure of organic molecules adsorbed on (metallic) surfaces. By measuring the angular distribution of…
Photoemission orbital tomography (POT) from photoelectron momentum maps (PMMs) has enabled detailed analysis of the shape and energy of molecular orbitals in the adsorbed state. This study proposes a new POT method based on the PhaseLift.…
Photoemission orbital tomography (POT) is a powerful tool for investigating the orbitals and electronic band structure of oriented layers of organic molecules. In many cases, POT allows conclusions to be drawn regarding the geometric…
Driven by recent developments in time-resolved photoemission spectroscopy, we extend the successful method of photoemission orbital tomography (POT) to excitons. Our theory retains the intuitive orbital picture of POT, while respecting both…
Following electronic processes in molecules and materials at the level of the quantum mechanical electron wavefunction with angstrom-level spatial resolution and with full access to its femtosecond temporal dynamics is at the heart of…
In transitions between different environmental settings, a molecular system inevitably undergoes a range of detectable changes, and the ability to accurately simulate such responses, e.g., in the form of shifts to molecular energies,…
Conventional photoemission orbital tomography based on Fourier iterative method enables us to extract a projected two-dimensional (2D) molecular orbital from a 2D photoelectron momentum map (PMM) of planar $\pi$-conjugated molecules in a…
The energy positions of frontier orbitals in organic electronic materials are often studied experimentally by (inverse) photoemission spectroscopy and theoretically within density functional theory. However, standard exchange-correlation…
We quantify the accuracy of different non-self-consistent and self-consistent spin-orbit coupling (SOC) treatments in Kohn-Sham and hybrid density-functional theory by providing a band structure benchmark set for the valence and low-lying…
In this paper, we demonstrate that atom probe tomography (APT) can be applied to small-molecule organic materials. We show that APT can provide an unprecedented combination of mass resolution of $\lt 1~\mathrm{Da}$, spatial resolution of…
The momentum-space signatures of excitons can be experimentally accessed through time-resolved (pump-probe) photoelectron spectroscopy. In this work, we develop a computational framework for exciton photoemission orbital tomography (exPOT)…
The development and first applications of a new periodic energy decomposition analysis (pEDA) scheme for extended systems based on the Kohn-Sham approach to density functional theory are described. The pEDA decomposes the binding energy…
With angle resolved photoemission experiments and \emph{ab-initio} electronic structure calculations, the pentacene monolayers on Ag(110) and Cu(110) are compared and contrasted allowing the molecular orientation and an unambiguous…
The exchange-correlation energy in Kohn-Sham density functional theory is expressed as a functional of the electronic density and the Kohn-Sham orbitals. An alternative to Kohn-Sham theory is to express the energy as a functional of the…
Absolute binding energies of core electrons in molecules and bulk materials can be efficiently calculated by spin paired density-function theory employing a $\Delta$ Kohn-Sham ($\Delta$KS) scheme corrected by offsets that are highly…
We present a first-principles-based multiscale simulation framework for quantitative predictions of the high-energy part of the Ultraviolet Photoelectron Spectroscopy (UPS) spectra of amorphous molecular solids. The approach combines a…
The constrained electron density method of embedding a Kohn-Sham system in a substrate system (first described by P. Cortona, Phys. Rev. B {\bf 44}, 8454 (1991) and T.A. Wesolowski and A. Warshel, J. Phys. Chem {\bf 97}, 8050 (1993)) is…
Using angle-resolved photoemission spectroscopy, we show the direct evidence of charge transfer between adsorbed molecules and metal substrate, i.e. chemisorption of CO on Pt(111) and Pt-Sn/Pt(111) 2x2 surfaces. The observed band structure…
Exchange-correlation potentials vxc and energy densities exc are derived for integer and fractional electron counts using an orbital-averaged Kohn-Sham inversion procedure. The reference densities for inversion come from full configuration…
The accurate prediction of electronic response properties of extended molecular systems has been a challenge for conventional, explicit density functionals. We demonstrate that a self-interaction correction implemented rigorously within…