Photoemission Orbital Tomography Using Robust Sparse PhaseLift

TL;DR

This paper introduces a robust PhaseLift-based method for photoemission orbital tomography that accurately reconstructs 3D molecular orbitals from photoelectron momentum maps, even in noisy conditions.

Contribution

It presents a novel POT approach using PhaseLift that can identify 3D molecular orbitals from a single PMM with high noise robustness and precise deformation discrimination.

Findings

Achieves 0.05 Å accuracy in detecting molecular deformations.

Successfully reconstructs 3D molecular orbitals including phases.

Robustly discriminates adsorption-induced shape changes.

Abstract

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. Molecular orbitals, including three-dimensional phases, can be identified from a single PMM by actively providing atomic positions and basis. Moreover, our method is robust to noise and can perfectly discriminate adsorption-induced molecular deformations with an accuracy of 0.05 [angstrom]. Our new method enables simultaneous analysis of the three-dimensional shapes of molecules and molecular orbitals and thus paves the way for advanced quantum-mechanical interpretation of adsorption-induced electronic state changes and photo-excited inter-molecular interactions.