Polarization-Modulated Angle-Resolved Photoemission Spectroscopy: Toward Circular Dichroism without Circular Photons and Bloch Wave-function Reconstruction
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 abou...
| Main Authors: | , , , , , , , |
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| Format: | Article |
| Language: | English |
| Published: |
American Physical Society
2022-01-01
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| Series: | Physical Review X |
| Online Access: | http://doi.org/10.1103/PhysRevX.12.011019 |
| _version_ | 1818333521282859008 |
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| author | Michael Schüler Tommaso Pincelli Shuo Dong Thomas P. Devereaux Martin Wolf Laurenz Rettig Ralph Ernstorfer Samuel Beaulieu |
| author_facet | Michael Schüler Tommaso Pincelli Shuo Dong Thomas P. Devereaux Martin Wolf Laurenz Rettig Ralph Ernstorfer Samuel Beaulieu |
| author_sort | Michael Schüler |
| collection | DOAJ |
| description | 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 wave function, 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 wave function 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 the case of two relevant bands, it is possible to reconstruct the orbital pseudospin (and thus the Bloch wave function) 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 wave functions of many relevant crystalline solids. |
| first_indexed | 2024-12-13T13:52:57Z |
| format | Article |
| id | doaj.art-95630c284b264bd0b342991a99b45c6b |
| institution | Directory Open Access Journal |
| issn | 2160-3308 |
| language | English |
| last_indexed | 2024-12-13T13:52:57Z |
| publishDate | 2022-01-01 |
| publisher | American Physical Society |
| record_format | Article |
| series | Physical Review X |
| spelling | doaj.art-95630c284b264bd0b342991a99b45c6b2022-12-21T23:43:03ZengAmerican Physical SocietyPhysical Review X2160-33082022-01-0112101101910.1103/PhysRevX.12.011019Polarization-Modulated Angle-Resolved Photoemission Spectroscopy: Toward Circular Dichroism without Circular Photons and Bloch Wave-function ReconstructionMichael SchülerTommaso PincelliShuo DongThomas P. DevereauxMartin WolfLaurenz RettigRalph ErnstorferSamuel BeaulieuAngle-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 wave function, 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 wave function 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 the case of two relevant bands, it is possible to reconstruct the orbital pseudospin (and thus the Bloch wave function) 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 wave functions of many relevant crystalline solids.http://doi.org/10.1103/PhysRevX.12.011019 |
| spellingShingle | Michael Schüler Tommaso Pincelli Shuo Dong Thomas P. Devereaux Martin Wolf Laurenz Rettig Ralph Ernstorfer Samuel Beaulieu Polarization-Modulated Angle-Resolved Photoemission Spectroscopy: Toward Circular Dichroism without Circular Photons and Bloch Wave-function Reconstruction Physical Review X |
| title | Polarization-Modulated Angle-Resolved Photoemission Spectroscopy: Toward Circular Dichroism without Circular Photons and Bloch Wave-function Reconstruction |
| title_full | Polarization-Modulated Angle-Resolved Photoemission Spectroscopy: Toward Circular Dichroism without Circular Photons and Bloch Wave-function Reconstruction |
| title_fullStr | Polarization-Modulated Angle-Resolved Photoemission Spectroscopy: Toward Circular Dichroism without Circular Photons and Bloch Wave-function Reconstruction |
| title_full_unstemmed | Polarization-Modulated Angle-Resolved Photoemission Spectroscopy: Toward Circular Dichroism without Circular Photons and Bloch Wave-function Reconstruction |
| title_short | Polarization-Modulated Angle-Resolved Photoemission Spectroscopy: Toward Circular Dichroism without Circular Photons and Bloch Wave-function Reconstruction |
| title_sort | polarization modulated angle resolved photoemission spectroscopy toward circular dichroism without circular photons and bloch wave function reconstruction |
| url | http://doi.org/10.1103/PhysRevX.12.011019 |
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