Imaging the wave functions of adsorbed molecules

Area of Science:

• Quantum mechanics
• Molecular physics
• Surface science

Background:

• Electron wave functions, or orbitals, are fundamental to describing matter.
• Experimentally, only electron densities and energy levels are directly observable, with orbital phase information typically lost.

Purpose of the Study:

• To develop a method for retrieving lost phase information from molecular orbitals.
• To reconstruct real-space orbitals from experimental momentum maps.

Main Methods:

• Utilizing angle-resolved photoemission spectroscopy to obtain experimental momentum maps.
• Applying an iterative procedure to transform momentum maps into real-space orbitals, including phase retrieval.

Main Results:

• Successfully retrieved phase information and reconstructed real-space orbitals for pentacene and perylene-3,4,9,10-tetracarboxylic dianhydride molecules.
• Obtained experimental images in excellent agreement with ab initio calculations.
• Demonstrated the procedure's robustness and lack of requirement for a priori orbital knowledge.

Conclusions:

• The developed iterative procedure effectively retrieves lost orbital phase information.
• This method enables the visualization of real-space molecular orbitals from photoemission data.
• Advances the experimental and theoretical understanding of electron wave functions in molecules.