Analysis methodology of coherent oscillations in time- and angle-resolved photoemission spectroscopy

Oscillatory signals from coherently excited phonons are regularly observed in ultrafast pump-probe experiments on condensed matter samples. Electron-phonon coupling implies that coherent phonons also modulate the electronic band structure. These oscillations can be probed with energy and momentum resolution using time- and angle-resolved photoemission spectroscopy (trARPES), which reveals the orbital dependence of the electron-phonon coupling for a specific phonon mode. However, a comprehensive analysis remains challenging when multiple coherent phonon modes couple to multiple electronic bands. Complex spectral line shapes due to strong correlations in quantum materials add to this challenge. In this work, we examine how the frequency domain representation of trARPES data facilitates a quantitative analysis of coherent oscillations of the electronic bands. We investigate the frequency domain representation of the photoemission intensity and the first moment of the energy distribution curves. Both quantities provide complementary information and are able to distinguish oscillations of binding energy, linewidth, and intensity. We analyze a representative trARPES dataset of the transition metal dichalcogenide WTe2 and construct composite spectra, which intuitively illustrate how much each electronic band is affected by a specific phonon mode. We also show how a linearly chirped probe pulse can generate extrinsic artifacts that are distinct from the intrinsic coherent phonon signal.

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Publication Details

Journal
Review of Scientific Instruments
Published
2025-02-01
DOI
https://doi.org/10.1063/5.0234899
Primary Topic
Advanced Chemical Physics Studies
Type
article
Field-Weighted Citation Impact
0.00

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article

Analysis methodology of coherent oscillations in time- and angle-resolved photoemission spectroscopy

Zhi‐Xun Shen, Heike Pfau, P. S. Kirchmann, N. Gauthier et al.
Review of Scientific Instruments
Advanced Chemical Physics Studies
article

Analysis methodology of coherent oscillations in time- and angle-resolved photoemission spectroscopy

Zhi‐Xun Shen, Heike Pfau, P. S. Kirchmann, N. Gauthier, Jonathan A. Sobota, Hadas Soifer, Edbert J. Sie, Aaron M. Lindenberg
article en

Abstract

Oscillatory signals from coherently excited phonons are regularly observed in ultrafast pump-probe experiments on condensed matter samples. Electron-phonon coupling implies that coherent phonons also modulate the electronic band structure. These oscillations can be probed with energy and momentum resolution using time- and angle-resolved photoemission spectroscopy (trARPES), which reveals the orbital dependence of the electron-phonon coupling for a specific phonon mode. However, a comprehensive analysis remains challenging when multiple coherent phonon modes couple to multiple electronic bands. Complex spectral line shapes due to strong correlations in quantum materials add to this challenge. In this work, we examine how the frequency domain representation of trARPES data facilitates a quantitative analysis of coherent oscillations of the electronic bands. We investigate the frequency domain representation of the photoemission intensity and the first moment of the energy distribution curves. Both quantities provide complementary information and are able to distinguish oscillations of binding energy, linewidth, and intensity. We analyze a representative trARPES dataset of the transition metal dichalcogenide WTe2 and construct composite spectra, which intuitively illustrate how much each electronic band is affected by a specific phonon mode. We also show how a linearly chirped probe pulse can generate extrinsic artifacts that are distinct from the intrinsic coherent phonon signal.

Review of Scientific InstrumentsVol. 96(2)
Pennsylvania State University (US), Tel Aviv University (IL), SLAC National Accelerator Laboratory (US), Institut National de la Recherche Scientifique (CA), Stanford University (US)
Schweizerischer Nationalfonds zur Förderung der Wissenschaftlichen Forschung
Affordable and clean energy
Openalex Percentile: Top 97%
Advanced Chemical Physics Studies
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