Bulk-sensitive XAS characterization of light elements: from X-ray Raman scattering to X-ray Raman spectroscopy

Bergmann, Uwe; Glatzel, Pieter; Cramer, Stephen P.

doi:10.1016/s0026-265x(02)00014-0

Cited by 144 publications

(106 citation statements)

References 43 publications

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“…This has been successfully used to study the bulk properties of low-Z systems under ambient and extreme conditions (Wernet et al, 2004;Mao et al, 2006;Bergmann et al, 2007), including oxygen Kedge EXAFS on water using the XRS technique . For a more detailed review of all the hard X-ray techniques described above, see Bergmann et al (2002) and .…”

Section: Introductionmentioning

confidence: 99%

Photon-in photon-out hard X-ray spectroscopy at the Linac Coherent Light Source

Alonso-Mori

Sokaras

Zhu

et al. 2015

J Synchrotron Radiat

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X-ray free-electron lasers (FELs) have opened unprecedented possibilities to study the structure and dynamics of matter at an atomic level and ultra-fast timescale. Many of the techniques routinely used at storage ring facilities are being adapted for experiments conducted at FELs. In order to take full advantage of these new sources several challenges have to be overcome. They are related to the very different source characteristics and its resulting impact on sample delivery, X-ray optics, X-ray detection and data acquisition. Here it is described how photon-in photon-out hard X-ray spectroscopy techniques can be applied to study the electronic structure and its dynamics of transition metal systems with ultra-bright and ultra-short FEL X-ray pulses. In particular, some of the experimental details that are different compared with synchrotron-based setups are discussed and illustrated by recent measurements performed at the Linac Coherent Light Source.

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Section: Introductionmentioning

confidence: 99%

Photon-in photon-out hard X-ray spectroscopy at the Linac Coherent Light Source

Alonso-Mori

Sokaras

Zhu

et al. 2015

J Synchrotron Radiat

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“…20 The XRS technique applies tuneable hard X-ray radiation. Hard X-ray (absorption) spectroscopies can be performed in situ and supply element-specific electronic structure information 20,21 and the main difficulty is that synchrotron radiation is required. In our previous paper 20 the presence of oxygen in the gas stream during the experiments had a huge impact on the spectral shape and influenced the interpretation of the results.…”

Section: Introductionmentioning

confidence: 99%

In situ X-ray Raman spectroscopy study of the hydrogen sorption properties of lithium borohydride nanocomposites

Miedema

Ngene

Eerden

et al. 2014

Phys. Chem. Chem. Phys.

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Nanoconfined alkali metal borohydrides are promising materials for reversible hydrogen storage applications, but the characterization of hydrogen sorption in these materials is difficult. Here we show that with in situ X-ray Raman spectroscopy (XRS) we can track the relative amounts of intermediates and final products formed during de-and re-hydrogenation of nanoconfined lithium borohydride (LiBH 4 ) and therefore we can possibly identify the de-and re-hydrogenation pathways. In the XRS of nanoconfined LiBH 4 at different points in the de-and re-hydrogenation, we identified phases that lead to the conclusion that de-and re-hydrogenation pathways in nanoconfined LiBH 4 are different from bulk LiBH 4 : intercalated lithium (LiC x ), boron and lithium hydride were formed during de-hydrogenation, but as well Li 2 B 12 H 12 was observed indicating that there is possibly some bulk LiBH 4 present in the nanoconfined sample LiBH 4 -C as prepared.Surprisingly, XRS revealed that the de-hydrogenated products of the LiBH 4 -C nanocomposites can be partially rehydrogenated to about 90% of Li 2 B 12 H 12 and 2-5% of LiBH 4 at a mild condition of 1 bar H 2 and 350 1C. This suggests that re-hydrogenation occurs via the formation of Li 2 B 12 H 12 . Our results show that XRS is an elegant technique that can be used for in and ex situ study of the hydrogen sorption properties of nanoconfined and bulk light-weight metal hydrides in energy storage applications.

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“…X-ray free electron lasers (XFELs) [5][6][7] with pulse durations in the fs range and unprecedented high intensities, hold the potential for transferring these techniques to the x-ray domain, to ultimately study the coherent interplay of electronic and vibrational degrees of freedom with high temporal and spatial resolution [8][9][10]. The high penetration depth of x rays, combined with the element and chemical sensitivity of inelastic x-ray scattering [11][12][13] could open pathways to temporally resolve complex dynamical processes such as energy transfer in light harvesting complexes or reaction dynamics of catalytic processes [14,15]. However, the cross section for x-ray Raman scattering is small compared to that in the visible spectral domain.…”

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Stimulated Electronic X-Ray Raman Scattering

Weninger

Purvis²,

Ryan³

et al. 2013

Phys. Rev. Lett.

135

111

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We demonstrate strong stimulated inelastic x-ray scattering by resonantly exciting a dense gas target of neon with femtosecond, high-intensity x-ray pulses from an x-ray free-electron laser (XFEL). A small number of lower energy XFEL seed photons drive an avalanche of stimulated resonant inelastic x-ray scattering processes that amplify the Raman scattering signal by several orders of magnitude until it reaches saturation. Despite the large overall spectral width, the internal spiky structure of the XFEL spectrum determines the energy resolution of the scattering process in a statistical sense. This is demonstrated by observing a stochastic line shift of the inelastically scattered x-ray radiation. In conjunction with statistical methods, XFELs can be used for stimulated resonant inelastic x-ray scattering, with spectral resolution smaller than the natural width of the core-excited, intermediate state. [5][6][7] with pulse durations in the fs range and unprecedented high intensities, hold the potential for transferring these techniques to the x-ray domain, to ultimately study the coherent interplay of electronic and vibrational degrees of freedom with high temporal and spatial resolution [8][9][10]. The high penetration depth of x rays, combined with the element and chemical sensitivity of inelastic x-ray scattering [11][12][13] could open pathways to temporally resolve complex dynamical processes such as energy transfer in light harvesting complexes or reaction dynamics of catalytic processes [14,15]. However, the cross section for x-ray Raman scattering is small compared to that in the visible spectral domain. Therefore, even at XFELs, single shot measurements are challenging, especially in dilute samples in the gas or liquid phase.This difficulty could be overcome by stimulating the Raman scattering process to produce a strong coherent amplification of the signal. We present the first demonstration of stimulated resonant electronic x-ray Raman scattering (SRXRS) in an atomic gas. Resonant x-ray Raman scattering, also referred to as resonant inelastic x-ray scattering [12], was discovered in 1974 [11] and since then has developed into a standard tool to study electronic and vibrational excitations in solids [16][17][18], liquids [19], gases [20], and on surfaces and interfaces [21,22]. Although several theoretical feasibility studies of SRXRS have been presented [23][24][25][26], no experiment has yet demonstrated this effect.SRXRS would ideally be realized by a narrow-band, tuneable two-color x-ray source: one frequency to excite an electronic inner-shell transition and the other, lower frequency to dump an electron into the short-lived core hole. Although the production of narrow-band x rays has been realized [27,28], and schemes for two-color self seeded sources have been proposed [29], there are currently no tunable, two-color, coherent sources available to perform such an experiment. Instead of this ideal, presently unrealizable approach, we report the demonstration of SRXRS in neon with a self-amplified...

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Bulk-sensitive XAS characterization of light elements: from X-ray Raman scattering to X-ray Raman spectroscopy

Cited by 144 publications

References 43 publications

Photon-in photon-out hard X-ray spectroscopy at the Linac Coherent Light Source

Photon-in photon-out hard X-ray spectroscopy at the Linac Coherent Light Source

In situ X-ray Raman spectroscopy study of the hydrogen sorption properties of lithium borohydride nanocomposites

Stimulated Electronic X-Ray Raman Scattering

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