A minimalist approach to 3D photoemission orbital tomography: algorithms and data requirements
arXiv:2402.10929 · doi:10.1088/1367-2630/ad3e22
Abstract
Photoemission orbital tomography provides direct access from laboratory measurements to the real-space molecular orbitals of well-ordered organic semiconductor layers. Specifically, the application of phase retrieval algorithms to photon-energy- and angle-resolved photoemission data enables the direct reconstruction of full 3D molecular orbitals without the need for simulations using density functional theory or the like. A major limitation for the direct approach has been the need for densely-sampled, well-calibrated 3D photoemission patterns. Here, we present an iterative projection algorithm that completely eliminates this challenge: for the benchmark case of the pentacene frontier orbitals, we demonstrate the reconstruction of the full orbital based on a dataset containing only four simulated photoemission momentum measurements. We discuss the algorithm performance, sampling requirements with respect to the photon energy, optimal measurement strategies, and the accuracy of orbital images that can be achieved.
arXiv comment27 pages, 10 figures, 44 references
References in corpus (15)
- X-ray image reconstruction from a diffraction pattern alone
- A unified evaluation of iterative projection algorithms for phase retrieval
- Probing the Low-Energy Electronic Structure of Complex Systems by ARPES
- Time- and momentum-resolved photoemission studies using time-of-flight momentum microscopy at a free-electron laser
- Alternating Projections and Douglas-Rachford for Sparse Affine Feasibility
- Orbital-resolved Observation of Singlet Fission
- Tracing orbital images on ultrafast time scales
- Time-Resolved Momentum Microscopy with a 1 MHz High-Harmonic Extreme Ultraviolet Beamline
- Quantitative convergence analysis of iterated expansive, set-valued mappings
- Efficient orbital imaging based on ultrafast momentum microscopy and sparsity-driven phase retrieval
- Ultrafast molecular orbital tomography of a pentacene thin film using time-resolved momentum microscopy at a free-electron laser
- Optimization on Spheres: Models and Proximal Algorithms with Computational Performance Comparisons
- Algorithms and image formation in orbital tomography
- Multiorbital exciton formation in an organic semiconductor
- Multispectral time-resolved energy-momentum microscopy using high-harmonic extreme ultraviolet radiation