Discerning charge patterns in a cuprate Copper oxides are well known to be able to achieve the order required for superconductivity. They can also achieve another order—one that produces patterns in their charge density. Experiments using nuclear magnetic resonanceand resonant x-ray scattering have both detected this so-called charge density wave (CDW) in yttrium-based cuprates. However, the nature of the CDW appeared to be different in the two types of measurement. Gerber et al. used pulsed magnetic fields of up to 28 T, combined with scattering, to bridge the gap (see the Perspective by Julien). As the magnetic field increased, a two-dimensional CDW gave way to a three-dimensional one. Science , this issue p. 949 ; see also p. 914
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 demonstrate X-ray and optical sum-frequency generation. The underlying nonlinearity is a reciprocal-space probe of the optically induced charges and associated microscopic fields that arise in an illuminated material. To within the experimental errors, the measured efficiency is consistent with first-principles calculations of microscopic optical polarization in diamond. The ability to probe optical interactions on the atomic scale offers new opportunities in both basic and applied areas of science.Light-matter interactions have advanced our understanding of atoms, molecules and materials, and are also central to a number of areas of applied science. Although optical interactions have received a great deal of study, the microscopic details of how light manipulates matter are poorly understood in many circumstances. A material's optical response is complex, being determined by coupled many-body interactions that vary on the scale of atoms rather than on the scale of a long-wavelength applied field. Data are needed to combat this complexity, and so far it has not been possible to probe the microscopic details of light-matter interactions. X-ray and optical wave mixing, specifically sum-frequency generation (SFG), was proposed nearly half a century ago as an atomic-scale probe of light-matter interactions 1,2 . The process is, in essence, optically modulated X-ray diffraction: X-rays inelastically scatter from optically induced charge oscillations and probe optically polarized charge in direct analogy to how standard X-ray diffraction probes ground-state charge. Furthermore, the optically induced microscopic field is determined because it is closely related to the induced charge [3][4][5][6] . So far it has not been possible to measure these two quantities directly. X-ray and optical wave mixing has frequently been discussed 1,2,4,[7][8][9][10][11][12] , but it has not yet been demonstrated owing to a lack of sufficiently intense X-ray sources. More generally, although there have been theoretical studies of nonlinear X-ray scattering [13][14][15][16][17][18] , experimental observations have largely been confined to the spontaneous processes of X-ray parametric down-conversion [19][20][21][22][23] and resonant inelastic X-ray scattering 24,25 . X-ray free-electron lasers offer unprecedented brightness and new scientific opportunities 26 . Here we use an X-ray laser to demonstrate X-ray/optical SFG through the nonlinear interaction of the two fields in single-crystal diamond. Optically modulated X-ray diffract...
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