Photoemission Orbital Tomography Using a Robust Sparse PhaseLift.

Area of Science:

• Chemical Physics
• Materials Science
• Quantum Chemistry

Background:

• Photoemission Orbital Tomography (POT) visualizes molecular orbital (MO) shapes using photoelectron momentum maps (PMMs).
• Existing POT methods require further simplification and cost reduction for broader application.

Purpose of the Study:

• To develop a simple, low-cost, and accurate Photoemission Orbital Tomography (POT) method.
• To enable direct 3D reconstruction of molecular orbitals (MOs) and their phases from experimental data.

Main Methods:

• Introduced a novel POT method based on the PhaseLift algorithm (PhaseLift POT).
• Utilized a lifting procedure to transform PMMs into a first-order polynomial of lifted MO coefficients.
• Developed sparse PhaseLift POT to enhance phase retrieval accuracy from noisy PMM data by incorporating sparsity of MO coefficients.

Main Results:

• Successfully reconstructed three-dimensional MOs, including wave function phases, from single experimental PMMs.
• Achieved precise determination of adsorption-induced molecular deformations with 0.05 [Å] accuracy.
• Demonstrated the robustness of sparse PhaseLift POT against experimental noise through relaxed matching conditions.

Conclusions:

• PhaseLift POT offers an innovative and accessible tool for molecular orbital visualization.
• The method accurately determines molecular structures and is suitable for analyzing molecular dynamics during chemical reactions and excitation processes.