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Photoemission orbital tomography (POT) from photoelectron momentum maps(PMMs) has enabled detailed analysis of the shape and energy of molecularorbitals in the adsorbed state. This study proposes a new POT method based onthe PhaseLift. Molecular orbitals, including three-dimensional phases, can beidentified from a single PMM by actively providing atomic positions and basis.Moreover, our method is robust to noise and can perfectly discriminateadsorption-induced molecular deformations with an accuracy of 0.05 [angstrom].Our new method enables simultaneous analysis of the three-dimensional shapes ofmolecules and molecular orbitals and thus paves the way for advancedquantum-mechanical interpretation of adsorption-induced electronic statechanges and photo-excited inter-molecular interactions.

Photoemission Orbital Tomography Using Robust Sparse PhaseLift