Polarization-Modulated Angle-Resolved Photoemission Spectroscopy: Towards Circular Dichroism without Circular Photons and Bloch Wavefunction Reconstruction

TL;DR

This paper introduces a polarization modulation technique in ARPES that enables the extraction of phase information and reconstruction of Bloch wavefunctions without circular photons, advancing the analysis of topological materials.

Contribution

A novel ARPES methodology using polarization modulation to retrieve phase information and reconstruct Bloch wavefunctions, including orbital pseudospin, without circularly polarized light.

Findings

Successfully demonstrated phase retrieval in ARPES data.

Reconstructed Bloch wavefunctions in WSe2.

Provided a new approach to analyze topological properties.

Abstract

Angle-resolved photoemission spectroscopy (ARPES) is the most powerful technique to investigate the electronic band structure of crystalline solids. To completely characterize the electronic structure of topological materials, one needs to go beyond band structure mapping and access information about the momentum-resolved Bloch wavefunction, namely orbitals, Berry curvature, and topological invariants. However, because phase information is lost in the process of measuring photoemission intensities, retrieving the complex-valued Bloch wavefunction from photoemission data has yet remained elusive. We introduce a novel measurement methodology and associated observable in extreme ultraviolet angle-resolved photoemission spectroscopy, based on continuous modulation of the ionizing radiation polarization axis. Tracking the energy- and momentum-resolved amplitude and phase of the photoemission intensity modulation upon polarization axis rotation allows us to retrieve the circular dichroism in photoelectron angular distributions (CDAD) without using circular photons, providing direct insights into the phase of photoemission matrix elements. In case of two relevant bands, it is possible to reconstruct the orbital pseudospin (and thus the Bloch wavefunction) with moderate theory input, as demonstrated for the prototypical layered semiconducting transition metal dichalcogenide 2H-WSe$_2$. This novel measurement methodology in ARPES, which is articulated around the manipulation of the photoionization transition dipole matrix element, in combination with a simple tight-binding theory, is general and adds a new dimension to obtaining insights into the orbital pseudospin, Berry curvature, and Bloch wavefunctions of many relevant crystalline solids.