A novel method for resonant inelastic soft X-ray scattering<i>via</i>photoelectron spectroscopy detection

Dakovski, Georgi L.; Lin, Ming Fu; Damiani, D. S.; Schlotter, W. F.; Turner, Joshua J.; Nordlund, Dennis; Ogasawara, Hirohito

doi:10.1107/s1600577517011869

Cited by 3 publications

(21 citation statements)

References 30 publications

(6 reference statements)

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“…For example, high-resolution time-resolved RIXS measurements probe dynamics of elementary excitations and can discriminate well between different states that occur in sample evolution (Wernet et al, 2015), but require recording many accurate spectra. Unfortunately, grating spectrometers detect only one X-ray photon for every $ 10 7 or more scattered RIXS photons (Qiao et al, 2017;Ghiringhelli & Braicovich, 2013;Dakovski et al, 2017), making such studies very challenging. Work has been done towards improving this.…”

Section: Introductionmentioning

confidence: 99%

“…Recently, Dakovski et al (2017) proposed doing exactly that to measure RIXS with hundreds of meV or better resolution through photoelectron spectrometry for analysis of X-rays (PAX) (Krause, 1965;Ebel, 1975). Fig.…”

Section: Introductionmentioning

confidence: 99%

“…While Dakovski et al (2017) demonstrated the possibility of recording PAX spectra for RIXS with moderate resolution and estimating the corresponding RIXS spectra as a sum of peaks, further development is required for PAX to be a proven high-resolution RIXS technique. First, a general algorithm for faithfully reconstructing X-ray spectra from PAX measurements is needed.…”

Section: Introductionmentioning

confidence: 99%

“…First, a general algorithm for faithfully reconstructing X-ray spectra from PAX measurements is needed. The algorithm proposed by Dakovski et al (2017) works when spectral line shapes and their photon energy distribution are priorly known in order to estimate the spectra as a sum of Gaussian functions. Without this information, spectral features will be poorly deconvoluted.…”

Section: Introductionmentioning

confidence: 99%

“…Finally, an experimental demonstration of the ability of PAX to perform a high-resolution RIXS study is needed. Here, we fill the first two of these gaps by proposing an algorithm for analyzing PAX data, then showing the capability of this algorithm on the data from Dakovski et al (2017) and finally showing the potential of PAX for estimating finer RIXS features through simulations. The algorithm we propose is a regularized maximum-likelihood estimation algorithm where the optimal regularization strength is estimated in a self-supervised manner from PAX data (summarized later in Algorithms 1 and 2).…”

Section: Introductionmentioning

confidence: 99%

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Using photoelectron spectroscopy to measure resonant inelastic X-ray scattering: a computational investigation

Higley¹,

Ogasawara²,

Zohar³

et al. 2022

J Synchrotron Radiat

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Resonant inelastic X-ray scattering (RIXS) has become an important scientific tool. Nonetheless, conventional high-resolution (few hundred meV or less) RIXS measurements, especially in the soft X-ray range, require low-throughput grating spectrometers, which limits measurement accuracy. Here, the performance of a different method for measuring RIXS, i.e. photoelectron spectrometry for analysis of X-rays (PAX), is computationally investigated. This method transforms the X-ray measurement problem of RIXS to an electron measurement problem, enabling use of high-throughput, compact electron spectrometers. X-rays to be measured are incident on a converter material and the energy distribution of the resultant photoelectrons, the PAX spectrum, is measured with an electron spectrometer. A deconvolution algorithm for analysis of such PAX data is proposed. It is shown that the deconvolution algorithm works well on data recorded with ∼0.5 eV resolution. Additional simulations show the potential of PAX for estimation of RIXS features with smaller widths. For simulations using the 3d levels of Ag as a converter material, and with 105 simulated detected electrons, it is estimated that features with a few hundred meV width can be accurately estimated in a model RIXS spectrum. For simulations using a sharp Fermi edge to encode RIXS spectra, it is estimated that one can accurately distinguish 100 meV FWHM peaks separated by 45 meV with 105 simulated detected electrons that were photoemitted from within 0.4 eV of the Fermi level.

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Section: Introductionmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

See 3 more Smart Citations

Using photoelectron spectroscopy to measure resonant inelastic X-ray scattering: a computational investigation

Higley¹,

Ogasawara²,

Zohar³

et al. 2022

J Synchrotron Radiat

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A compact approach to higher-resolution resonant inelastic x-ray scattering detection using photoelectrons

Schunck,

Buck,

Engel

et al. 2024

New J. Phys.

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The detection of inelastically scattered soft X-rays with high energy resolution usually requires large grating spectrometers. Recently, photoelectron spectrometry for analysis of X-rays (PAX) has been rediscovered for modern spectroscopy experiments at synchrotron light sources. By converting scattered photons to electrons and using an electron energy analyser, the energy resolution for resonant inelastic X-ray scattering (RIXS) becomes decoupled from the X-ray spot size and instrument length. In this work, we develop PAX towards high energy resolution using a modern photoemission spectroscopy setup studying Ba2Cu3O4Cl2 at the Cu L 3 edge. We measure a momentum transfer range of 24% of the first Brillouin zone simultaneously. Our results hint at the observation of a magnon excitation below 100 meV energy transfer and show intensity variations related to the dispersion of dd-excitations. With dedicated setups, PAX can complement the best and largest RIXS instruments, while at the same time opening new opportunities to acquire RIXS at a range of momentum transfers simultaneously and combine it with angle-resolved photoemission spectroscopy in a single instrument.

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Using photoelectron spectroscopy to measure resonant inelastic X-ray scattering: A computational investigation

Higley¹,

Ogasawara²,

Zohar³

et al. 2020

Preprint

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Resonant inelastic X-ray scattering (RIXS) has become an important scientific tool. Nonetheless, conventional high-resolution RIXS measurements (< 100 meV), especially in the soft x-ray range, require large and low-throughput grating spectrometers that limits measurement accuracy and simplicity. Here, we computationally investigate the performance of a different method for measuring RIXS, Photoelectron Spectrometry for Analysis of X-rays (PAX). This method transforms the Xray measurement problem of RIXS to an electron measurement problem, enabling use of compact, high-throughput electron spectrometers. In PAX, X-rays to be measured are incident on a converter material and the energy distribution of the resultant photoelectrons, the PAX spectrum, is measured with an electron spectrometer. The incident X-ray spectrum is then estimated through a deconvolution algorithm that leverages concepts from machine learning. We investigate a few example PAX cases. Using the 3d levels of Ag as a converter material, and with 10 5 detected electrons, we accurately estimate features with 100s of meV width in a model RIXS spectrum. Using a sharp Fermi edge to encode RIXS spectra, we accurately distinguish 100 meV FWHM peaks separated by 45 meV with 10 7 electrons detected that were photoemitted from within 0.4 eV of the Fermi level.

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A novel method for resonant inelastic soft X-ray scatteringviaphotoelectron spectroscopy detection

Cited by 3 publications

References 30 publications

Using photoelectron spectroscopy to measure resonant inelastic X-ray scattering: a computational investigation

Using photoelectron spectroscopy to measure resonant inelastic X-ray scattering: a computational investigation

A compact approach to higher-resolution resonant inelastic x-ray scattering detection using photoelectrons

Using photoelectron spectroscopy to measure resonant inelastic X-ray scattering: A computational investigation

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