Resonant inelastic X-ray scattering and X-ray emission spectroscopy can be used to probe the energy and dispersion of the elementary low-energy excitations that govern functionality in matter: vibronic, charge, spin and orbital excitations1,2,3,4,5,6,7. A key drawback of resonant inelastic X-ray scattering has been the need for high photon densities to compensate for fluorescence yields of less than a per cent for soft X-rays8. Sample damage from the dominant non-radiative decays thus limits the materials to which such techniques can be applied and the spectral resolution that can be obtained. A means of improving the yield is therefore highly desirable. Here we demonstrate stimulated X-ray emission for crystalline silicon at photon densities that are easily achievable with free-electron lasers9. The stimulated radiative decay of core excited species at the expense of non-radiative processes reduces sample damage and permits narrow-bandwidth detection in the directed beam of stimulated radiation. We deduce how stimulated X-ray emission can be enhanced by several orders of magnitude to provide, with high yield and reduced sample damage, a superior probe for low-energy excitations and their dispersion in matter. This is the first step to bringing nonlinear X-ray physics in the condensed phase from theory10,11,12,13,14,15,16 to application.
Subscribe to Journal
Get full journal access for 1 year
only $3.90 per issue
All prices are NET prices.
VAT will be added later in the checkout.
Tax calculation will be finalised during checkout.
Rent or Buy article
Get time limited or full article access on ReadCube.
All prices are NET prices.
Kotani, A. & Shin, S. Resonant inelastic x-ray scattering spectra for electrons in solids. Rev. Mod. Phys. 73, 203–246 (2001)
Schlappa, J. et al. Collective magnetic excitations in the spin ladder Sr14Cu24O41 measured using high-resolution resonant inelastic x-ray scattering. Phys. Rev. Lett. 103, 047401 (2009)
Hennies, F. et al. Resonant inelastic scattering spectra of free molecules with vibrational resolution. Phys. Rev. Lett. 104, 193002 (2010)
Ament, L. J. P., van Veenendaal, M., Devereaux, T., Hill, J. P. & van den Brink, J. Resonant inelastic x-ray scattering studies of elementary excitations. Rev. Mod. Phys. 83, 705–767 (2011)
Le Tacon, M. et al. Intense paramagnon excitations in a large family of high-temperature superconductors. Nature Phys. 7, 725–730 (2011)
Pietzsch, A. et al. Spatial quantum beats in vibrational resonant inelastic soft x-ray scattering at dissociating states in oxygen. Phys. Rev. Lett. 106, 153004 (2011)
Schlappa, J. et al. Spin-orbital separation in the quasi-one-dimensional mott insulator Sr2CuO3 . Nature 485, 82–85 (2012)
Krause, M. O. Atomic radiative and radiationless yields for K and L shells. J. Phys. Chem. Ref. Data 8, 307 (1979)
McNeil, B. W. J. & Thompson, N. R. X-ray free-electron lasers. Nature Photon. 4, 814–821 (2010)
Tanaka, S. & Mukamel, S. Coherent x-ray Raman spectroscopy: a nonlinear local probe for electronic excitations. Phys. Rev. Lett. 89, 043001 (2002)
Mukamel, S. Multiple core-hole coherence in x-ray four-wave-mixing spectroscopies. Phys. Rev. B 72, 235110 (2005)
Schweigert, I. & Mukamel, S. Probing valence electronic wave-packet dynamics by all x-ray stimulated Raman spectroscopy: a simulation study. Phys. Rev. A 76, 012504 (2007)
Harbola, U. & Mukamel, S. Coherent stimulated x-ray Raman spectroscopy: attosecond extension of resonant inelastic x-ray Raman scattering. Phys. Rev. B 79, 085108 (2009)
Patterson, B. D. Resource letter on stimulated inelastic x-ray scattering at an XFEL. (SLAC Technical Note SLAC-TN-10-026, SLAC National Accelerator Laboratory, Menlo Park, California, 2010).
Sun, Y.-P., Liu, J.-C., Wang, C.-K. & Gel'mukhanov, F. Propagation of a strong x-ray pulse: pulse compression, stimulated raman scattering, amplified spontaneous emission, lasing without inversion, and four-wave mixing. Phys. Rev. A 81, 013812 (2010)
Biggs, J. D., Zhang, Y., Healion, D. & Mukamel, S. Two-dimensional stimulated resonance Raman spectroscopy of molecules with broadband x-ray pulses. J. Chem. Phys. 136, 174117 (2012)
Ackermann, W. et al. Operation of a free-electron laser from the extreme ultraviolet to the water window. Nature Photon. 1, 336–342 (2007)
Emma, P. et al. First lasing and operation of an angstrom-wavelength free-electron laser. Nature Photon. 4, 641–647 (2010)
Di Mitri, S. et al. in Advances in X-ray Free-Electron Lasers: Radiation Schemes, X-Ray Optics, and Instrumentation (eds Tschentscher, T. & Cocco, D. ) Vol. 8078, 807802, doi:10.1117/12.886491 (Proc. SPIE, 2011)
Pile, D. X-rays: first light from SACLA. Nature Photon. 5, 456–457 (2011)
Rohringer, N. et al. Atomic inner-shell x-ray laser at 1.46 nanometres pumped by an x-ray free-electron laser. Nature 481, 488–491 (2012)
Glover, T. E. et al. X-ray and optical wave mixing. Nature 488, 603–608 (2012)
Beye, M., Sorgenfrei, F., Schlotter, W. F., Wurth, W. & Föhlisch, A. The liquid-liquid phase transition in silicon revealed by snapshots of valence electrons. Proc. Natl Acad. Sci. USA 107, 16772–16776 (2010)
Wernet, P. Electronic structure in real time: mapping valence electron rearrangements during chemical reactions. Phys. Chem. Chem. Phys. 13, 16941–16954 (2011)
Salén, P. et al. Experimental verification of the chemical sensitivity of two-site double core-hole states formed by an x-ray free-electron laser. Phys. Rev. Lett. 108, 153003 (2012)
Yeh, J. J. & Lindau, I. Atomic subshell photoionization cross-sections and asymmetry parameters—1 ≤ z ≤ 103. Atom. Data Nucl. Data Tab. 32, 1–155 (1985)
Frühling, U. et al. Single-shot terahertz-field-driven x-ray streak camera. Nature Photon. 3, 523–528 (2009)
Martins, M. et al. Monochromator beamline for FLASH. Rev. Sci. Instrum. 77, 115108 (2006)
Tiedtke, K. et al. The soft x-ray free-electron laser FLASH at DESY: beamlines, diagnostics and end-stations. New J. Phys. 11, 023029 (2009)
Nordgren, J. Soft x-ray emission spectroscopy—preface. J. Electron Spectrosc. 110–111, ix– x (2000)
Henke, B. L., Gullikson, E. M. & Davis, J. C. X-ray interactions: photoabsorption, scattering, transmission, and reflection at E = 50-30,000 eV, Z = 1-92. Atom. Data Nucl. Data Tab. 54, 181–342 (1993)
Kunnus, K. et al. A setup for resonant inelastic soft x-ray scattering on liquids at free electron laser light sources. Rev. Sci. Instrum. 83, 123109 (2012)
Hricovini, K. et al. Electronic structure and its dependence on local order for H/Si(111)-(1x1) surfaces. Phys. Rev. Lett. 70, 1992–1995 (1993)
We thank N. Rohringer, A. Scherz and J. Stöhr for discussions. We acknowledge support from the FLASH staff. Financial support was given to M.B. by the VolkswagenStiftung. Further support was given by the German Federal Ministry of Education and Research through the priority programme FLASH: “Matter in the light of ultrashort and extremely intense X-ray pulses” and contract number 05K10PK2, and also by the Deutsche Forschungsgemeinschaft through the graduate school: “Physics with new advanced coherent radiation sources”.
The authors declare no competing financial interests.
About this article
Cite this article
Beye, M., Schreck, S., Sorgenfrei, F. et al. Stimulated X-ray emission for materials science. Nature 501, 191–194 (2013). https://doi.org/10.1038/nature12449
Scientific Reports (2020)
Nature Communications (2018)
Scientific Reports (2016)