Lifetime-broadening-suppressed/free XANES spectroscopy by high-resolution resonant inelastic x-ray scattering

Hayashi, Hisashi; Takeda, Rumi; Udagawa, Yasuo; Nakamura, Tetsuya; Miyagawa, Hayato; Shoji, Hironobu; Nanao, Susumu; Kawamura, N.

doi:10.1103/physrevb.68.045122

Cited by 56 publications

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“…(2) is the product of three functions having the energy of the excited electron, w, as a common variable: two Lorentzians, f1 centered at w1-Ω1s with a width of 1s (Γ1s) and f2 centered at w1-w2-Ω2p with a width of 2p (Γ2p); the oscillator strength distribution for K absorption is dg1s/dw, where dg1s/dw corresponds to the K-XAFS spectrum in the limit of vanishing lifetime broadenings, i.e., K LBS-XAFS. 8,23 The three functions can be depicted along the w axis, such as in Fig. 2b.…”

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confidence: 99%

“…However, although two attempts using laboratory x-ray sources can be found in the literature, 21,22 no substantiation of their prediction by using modern synchrotron sources was provided until recently. By our detailed RIXS experiments in 2003, 8,23 finally the basis of LBS-XAFS spectroscopy using RIXS (as well as PFY) spectra was established. The development of LBS-XAFS spectroscopy since then is rather remarkable.…”

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confidence: 99%

“…(1) is reduced to Eq. (2): 8,20,23,27 ∝ dw. (2) In deriving this equation, the emission process from | n〉 to | f〉 is assumed to be a one-electron transition between core levels, leaving all of the electronic states unchanged, but any other many-body effects can be included.…”

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confidence: 99%

“…In RIXS measurements, the incident x-ray energy, w1, is fixed and the scattering intensity (∂ 2 σ/∂w1∂w2) is monitored as a function of the emitted x-ray energy, w2, which is equivalent to sliding f2 along the w axis while keeping f1 and dg1s/dw fixed. 8,23 On the other hand, in PFY spectroscopy, 5 w1 is scanned and w2 is fixed to be Ω1s -Ω2p, which makes the center of f1 and f2…”

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confidence: 99%

“…[5][6][7][8][9][10][11][12] Here we loosely define RIXS as x-ray emissions excited with x-ray energies near an absorption edge. 6,7 Wide applications of RIXS have been so far hindered by its low intensity.…”

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Lifetime-Broadening-Suppressed Selective XAFS Spectroscopy

Hayashi

2008

ANAL. SCI.

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Every element has its characteristic absorption edge in the x-ray region, and x-ray absorption fine structure (XAFS) appears at the high-energy side. XAFS is sensitive to local electronic states and atomic environments around the absorbing atoms, and hence has been extensively employed over wide research fields as an element-specific characterization method. 1-3 XAFS spectroscopy is, however, not free from problems. One of them is that the natural widths (a few eV 4 in ordinary experiments) that originate from the finite lifetime of core holes determine the resolution of XAFS spectra.Lifetime-broadening often prevents detailed analyses, particularly, for the pre-edge region. 5 Another problem is that conventional XAFS does not have state selectivity, and therefore chemical state information is averaged, whereas in many instances, e.g. heterogeneous catalyst studies, it is of vital importance to selectively probe different forms of the elements.It is possible to circumvent these intrinsic shortcomings of XAFS spectroscopy by making use of resonant inelastic x-ray scattering (RIXS). [5][6][7][8][9][10][11][12] Here we loosely define RIXS as x-ray emissions excited with x-ray energies near an absorption edge. 6,7 Wide applications of RIXS have been so far hindered by its low intensity.However, the intensity problem in RIXS measurements is now being solved by developing highly sensitive emission spectrometers with high resolution, optimized for the use at third-generation synchrotron sources. [12][13][14][15] In the present review, we survey this novel technique, lifetimebroadening-suppressed (LBS) selective XAFS spectroscopy, while paying attention to basic aspects. Lifetime-broadening-suppressed XAFS and Resonant Inelastic X-ray ScatteringPioneer work to overcome the resolution limitation of XAFS has been made by Hämäläinen et al. at 1991. 5 They proposed partial fluorescent yield (PFY) spectroscopy to obtain LBS-XAFS, where highly monochromatic incident x-ray energy is scanned across an absorption edge while monitoring the characteristic x-rays with better resolution than the natural width. However, it was later suggested that PFY spectra cannot be viewed as genuine LBS-XAFS 16,17 (although for wide-band materials, where core-electron interactions are small, they can be a good approximation to LBS-XAFS). 6,16,18 Partially because of this indication, there were very few reports on succeeding PFY measurements. 19 An alternative method to obtain LBS-XAFS by using RIXS has been theoretically suggested by Tulkki and Åberg, 20 even before the proposition of the PFY spectroscopy (at 1982). They have stated that "the shape of the spectrum of the scattered photons may be used to disentangle bound-state excitations from continuous absorption more effectively than in ordinary Chemical and Biological Sciences, Faculty of Science, Japan Women's University, Bunkyo, Japan **PRESTO, Japan Science and Technology Agency, 5 Sanbancho, Chiyoda, Japan Lifetime-broadening-suppressed (LBS) state-selective XAFS spectra can be dedu...

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Lifetime-Broadening-Suppressed Selective XAFS Spectroscopy

Hayashi

2008

ANAL. SCI.

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Chemical Effects in Hard X‐ray Photon‐In Photon‐Out Spectra

Hayashi

2000

Encyclopedia of Analytical Chemistry

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Hard X‐ray photon‐in photon‐out techniques are targeted at applications where the sample environment cannot be freely chosen. The resultant X‐ray emission spectra are influenced by the chemical environments of the atoms involved. If high‐resolution measurements are possible, the chemical effects in the X‐ray emission spectra can provide information about the chemical states, complementary to that offered by other X‐ray spectroscopies. X‐ray emission is classified into six categories for convenience: X‐ray diagram lines, X‐ray valence‐band emission, radiative Auger effect, resonant X‐ray emission, Compton scattering, and X‐ray Raman scattering. After a brief description of the history of research on these types of emission, the chemical effects that they reveal and related topics, including high‐resolution absorption measurements and the static structure factor, are reviewed. An overview of the instrumentation employed in both laboratories and synchrotron radiation (SR) facilities is also given.

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Spectroscopic Techniques

2019

An Introduction to Synchrotron Radiation

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Lifetime-broadening-suppressed/free XANES spectroscopy by high-resolution resonant inelastic x-ray scattering

Cited by 56 publications

References 12 publications

Lifetime-Broadening-Suppressed Selective XAFS Spectroscopy

Lifetime-Broadening-Suppressed Selective XAFS Spectroscopy

Chemical Effects in Hard X‐ray Photon‐In Photon‐Out Spectra

Spectroscopic Techniques

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