Circular dichroism in the photoelectron angular distribution of achiral molecules
arXiv:2507.12113 · doi:10.1103/6bkb-4rm3
Abstract
Circular dichroism in the angular distribution (CDAD) is the effect that the angular intensity distribution of photoemitted electrons depends on the handedness of the incident circularly polarized light. A CDAD may arise from intrinsic material properties like chirality, spin-orbit interaction, or quantum-geometrical effects on the electronic structure. In addition, CDAD has also been reported for achiral organic molecules at the interface to metallic substrates. For this latter case, we investigate two prototypical -conjugated molecules, namely tetracene and pentacene, whose frontier orbitals have a similar shape but exhibit distinctly different symmetries. By comparing experimental CDAD momentum maps with simulations within time-dependent density functional theory, we show how the final state of the photoelectron must be regarded as the source of the CDAD in such otherwise achiral systems. We gain additional insight into the mechanism by employing a simple scattering model for the final state, which allows us to decompose the CDAD signal into partial wave contributions.
References in corpus (29)
- NWChem: Past, Present, and Future
- Hidden spin polarization in inversion-symmetric bulk crystals
- Real-space grids and the Octopus code as tools for the development of new simulation approaches for electronic systems
- Octopus, a computational framework for exploring light-driven phenomena and quantum dynamics in extended and finite systems
- Chiral orbital-angular-momentum in the surface states of Bi2Se3
- Photo-electron momentum spectra from minimal volumes: the time-dependent surface flux method
- Electron spin polarization in strong-field ionization of Xenon atoms
- Local Berry curvature signatures in dichroic angle-resolved photoelectron spectroscopy
- Relaxation Dynamics in Photoexcited Chiral Molecules Studied by Time-Resolved Photoelectron Circular Dichroism: Toward Chiral Femtochemistry
- Simulating pump-probe photo-electron and absorption spectroscopy on the attosecond time-scale with time-dependent density-functional theory
- Selective probing of hidden spin-polarized states in inversion-symmetric bulk MoS2
- Experimental observation of hidden Berry curvature in inversion-symmetric bulk 2H-WSe2
- Modeling electron dynamics coupled to continuum states in finite volumes
- t-SURFF: Fully Differential Two-Electron Photo-Emission Spectra
- Ab-initio angle and energy resolved photoelectron spectroscopy with time-dependent density-functional theory
- Revealing Hidden Orbital Pseudospin Texture with Time-Reversal Dichroism in Photoelectron Angular Distributions
- Real-time probing of chirality during a chemical reaction
- A first principles TDDFT framework for spin and time-resolved ARPES in periodic systems
- How Circular Dichroism in time- and angle-resolved photoemission can be used to spectroscopically detect transient topological states in graphene
- Measurements of the quantum geometric tensor in solids
- Orbital tomography of hybridized and dispersing molecular overlayers
- Capturing electron-driven chiral dynamics in UV-excited molecules
- Efficient and accurate modeling of electron photoemission in nanostructures with TDDFT
- Efficient orbital imaging based on ultrafast momentum microscopy and sparsity-driven phase retrieval
- Polarization-Modulated Angle-Resolved Photoemission Spectroscopy: Towards Circular Dichroism without Circular Photons and Bloch Wavefunction Reconstruction
- Time-resolved chiral X-Ray photoelectron spectroscopy with transiently enhanced atomic site-selectivity: a Free Electron Laser investigation of electronically excited fenchone enantiomers
- The Huygens Principle of Angle-Resolved Photoemission
- A minimalist approach to 3D photoemission orbital tomography: algorithms and data requirements
- Reexamining Circular Dichroism in Photoemission From a Topological Insulator