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

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.

arXiv commentThis is the revised version that has been accepted in PRX

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• Time- and Angle-Resolved Photoemission Studies of Quantum Materials
• Orbital Hall effect in bilayer transition metal dichalcogenides: From the intra-atomic approximation to the Bloch states orbital magnetic moment approach
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• Advancing time- and angle-resolved photoemission spectroscopy: The role of ultrafast laser development
• Ultrafast Polarization-Tunable Monochromatic Extreme Ultraviolet Source at High-Repetition-Rate
• Spin- and time-resolved photoelectron spectroscopy and diffraction studies using time-of-flight momentum microscopes
• Controlling the orbital Hall effect in gapped bilayer graphene in the terahertz regime
• Geometry-induced spin-filtering in photoemission maps from WTe${}_2$ surface states
• High harmonic generation light source with polarization selectivity and sub-100-$\mu$m beam size for time- and angle-resolved photoemission spectroscopy
• Reexamining Circular Dichroism in Photoemission From a Topological Insulator
• Spinor ice correlation in flat-band electronic states on kagome and pyrochlore lattices with spin-orbit coupling
• Circular dichroism in the photoelectron angular distribution of achiral molecules