Stimulated X-ray Raman scattering – a critical assessment of the building block of nonlinear X-ray spectroscopy

Kimberg, Victor; Sánchez‐González, Álvaro; Mercadier, Laurent; Weninger, Clemens; Lutman, Alberto; Ratner, Daniel; Coffee, Ryan; Bucher, Maximilian; Mucke, Melanie; Agåker, Marcus; Såthe, Conny; Bostedt, Christoph; Nordgren, J.; Rubensson, Jan‐Erik; Rohringer, Nina

doi:10.1039/c6fd00103c

Cited by 27 publications

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“…This results in pulses of limited temporal coherence, thus impeding the experimental control and analysis. To measure stimulated emission driven by a stochastic source, high gain and optically dense samples are necessary [26,27]. In order to become a valuable spectroscopic technique, the spectral evolution at these high gain conditions have to be understood and examined.…”

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Stimulated X-Ray Emission Spectroscopy in Transition Metal Complexes

et al. 2018

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We report the observation and analysis of the gain curve of amplified Kα x-ray emission from solutions of Mn(II) and Mn(VII) complexes using an x-ray free electron laser to create the 1s core-hole population inversion. We find spectra at amplification levels extending over 4 orders of magnitude until saturation. We observe bandwidths below the Mn 1s core-hole lifetime broadening in the onset of the stimulated emission. In the exponential amplification regime the resolution corrected spectral width of ~1.7 eV FWHM is constant over 3 orders of magnitude, pointing to the buildup of transform limited pulses of ~1 fs duration. Driving the amplification into saturation leads to broadening and a shift of the line. Importantly, the chemical sensitivity of the stimulated x-ray emission to the Mn oxidation state is preserved at power densities of ~1020 W/cm2 for the incoming x-ray pulses. Differences in signal sensitivity and spectral information compared to conventional (spontaneous) x-ray emission spectroscopy are discussed. Our findings build a baseline for nonlinear x-ray spectroscopy for a wide range of transition metal complexes in inorganic chemistry, catalysis, and materials science.

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confidence: 99%

Stimulated X-Ray Emission Spectroscopy in Transition Metal Complexes

et al. 2018

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“…Normally, the reference spectrum is measured before inserting the sample and averaged for many shots, or even averaged for shots sorted in different bins as a function of one or two of the features28. However, this approach cannot be used to bin with respect to more than two variables, as then the number of samples per bin would become too small.…”

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Accurate prediction of X-ray pulse properties from a free-electron laser using machine learning

et al. 2017

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Free-electron lasers providing ultra-short high-brightness pulses of X-ray radiation have great potential for a wide impact on science, and are a critical element for unravelling the structural dynamics of matter. To fully harness this potential, we must accurately know the X-ray properties: intensity, spectrum and temporal profile. Owing to the inherent fluctuations in free-electron lasers, this mandates a full characterization of the properties for each and every pulse. While diagnostics of these properties exist, they are often invasive and many cannot operate at a high-repetition rate. Here, we present a technique for circumventing this limitation. Employing a machine learning strategy, we can accurately predict X-ray properties for every shot using only parameters that are easily recorded at high-repetition rate, by training a model on a small set of fully diagnosed pulses. This opens the door to fully realizing the promise of next-generation high-repetition rate X-ray lasers.

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“…Coherence properties are exploited in imaging techniques that aim to obtain atomic spatial resolution for weakly scattering systems, in part combined with a corresponding temporal resolution [16]. Finally, the very high X-ray pulse energies, which combined with ultrashort pulse durations correspond to very high peak powers of up to several tens of GW, promise to enable access to new information of excited solids through non-linear X-ray scattering [17].…”

Section: Overview European Xfelmentioning

confidence: 99%

“…Scientific objectives include, but are not limited to the understanding and control of complex materials [81][82][83], the investigation of ultrafast magnetization processes on the nanoscale [84,85], the real-time observation of chemical reactions at surfaces and in liquids [86,87], and the exploration of nonlinear X-ray spectroscopic techniques that are cornerstones at optical wavelengths [17,88].…”

Section: Scientific Scope and X-ray Techniquesmentioning

confidence: 99%

Photon Beam Transport and Scientific Instruments at the European XFEL

et al. 2017

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Featured Application: This article describes the layout of the European XFEL, a soft and hard X-ray free-electron laser user facility starting operation in 2017. Emphasis is put on the photon beam systems, scientific applications and the instrumentation of the scientific instruments of the European XFEL.Abstract: European XFEL is a free-electron laser (FEL) user facility providing soft and hard X-ray FEL radiation to initially six scientific instruments. Starting user operation in fall 2017 European XFEL will provide new research opportunities to users from science domains as diverse as physics, chemistry, geo-and planetary sciences, materials sciences or biology. The unique feature of European XFEL is the provision of high average brilliance in the soft and hard X-ray regime, combined with the pulse properties of FEL radiation of extreme peak intensities, femtosecond pulse duration and high degree of coherence. The high average brilliance is achieved through acceleration of up to 27,000 electron bunches per second by the super-conducting electron accelerator. Enabling the usage of this high average brilliance in user experiments is one of the major instrumentation drivers for European XFEL. The radiation generated by three FEL sources is distributed via long beam transport systems to the experiment hall where the scientific instruments are located side-by-side. The X-ray beam transport systems have been optimized to maintain the unique features of the FEL radiation which will be monitored using build-in photon diagnostics. The six scientific instruments are optimized for specific applications using soft or hard X-ray techniques and include integrated lasers, dedicated sample environment, large area high frame rate detector(s) and computing systems capable of processing large quantities of data.

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Stimulated X-ray Raman scattering – a critical assessment of the building block of nonlinear X-ray spectroscopy

Cited by 27 publications

References 29 publications

Stimulated X-Ray Emission Spectroscopy in Transition Metal Complexes

Stimulated X-Ray Emission Spectroscopy in Transition Metal Complexes

Accurate prediction of X-ray pulse properties from a free-electron laser using machine learning

Photon Beam Transport and Scientific Instruments at the European XFEL

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