2012
DOI: 10.1038/nature11340
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X-ray and optical wave mixing

Abstract: Light-matter interactions are ubiquitous, and underpin a wide range of basic research fields and applied technologies. Although optical interactions have been intensively studied, their microscopic details are often poorly understood and have so far not been directly measurable. X-ray and optical wave mixing was proposed nearly half a century ago as an atomic-scale probe of optical interactions but has not yet been observed owing to a lack of sufficiently intense X-ray sources. Here we use an X-ray laser to de… Show more

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Cited by 216 publications
(193 citation statements)
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“…The brightness of XFELs is many orders of magnitude higher than that of synchrotron sources [12]. Unprecedentedly ultraintense x-ray pulses enable us to study nonlinear x-ray physics [13,14,15,16], including nonlinear two-photon x-ray Compton scattering [17,18]. The features of ultraintense and ultrashort XFEL pulses are useful to create warm dense matter [19], and the inelastic x-ray scattering technique has been developed to measure characteristics (density and temperature) of high energy density plasma [20,21,22,23].…”
Section: Introductionmentioning
confidence: 99%
“…The brightness of XFELs is many orders of magnitude higher than that of synchrotron sources [12]. Unprecedentedly ultraintense x-ray pulses enable us to study nonlinear x-ray physics [13,14,15,16], including nonlinear two-photon x-ray Compton scattering [17,18]. The features of ultraintense and ultrashort XFEL pulses are useful to create warm dense matter [19], and the inelastic x-ray scattering technique has been developed to measure characteristics (density and temperature) of high energy density plasma [20,21,22,23].…”
Section: Introductionmentioning
confidence: 99%
“…Prior to the development of free electron lasers (FELs), only parametric downconversion had been observed [17]. While the advent of XFELs has recently enabled second-and third-order nonlinear spectroscopies at hard x-ray energies, including SHG [2], SFG [1], two-photon absorption [4], and inelastic Compton scattering [18], current hard x-ray FELs lack the longitudinal and temporal coherence necessary for efficiently satisfying the phase-matching conditions required for nonlinear spectroscopies, thus, making the exploitation of some of these techniques difficult [19,20]. Furthermore, the shorter hard x-ray wavelengths (λ < 0.2 nm) induce second harmonic and sum frequency generation even within centrosymmetric media, as the observed response depends on material inhomogeneity on the length scale of the x-ray wavelength, similar to how SHG is seen in a plasma, and effectively making this method a bulk probe [21].…”
mentioning
confidence: 99%
“…At infrared, visible, and ultraviolet wavelengths, secondorder nonlinear spectroscopies have become important tools in surface science, as symmetry considerations within the dipole approximation constrain signal generation to regions lacking centrosymmetry, such as surfaces and interfaces [9][10][11][12]. In contrast, at hard x-ray wavelengths, second harmonic and sum frequency generation (SFG) have been observed in centrosymmetric materials with a nonuniform electron density and are essentially bulk probes [1,2]. As soft x-ray wavelengths fall in between the hard x-ray and UV regimes, there has been uncertainty regarding the interface specificity of soft x-ray SHG.…”
mentioning
confidence: 99%
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