Nanoscale dynamics by short-wavelength four wave mixing experiments

Abstract

Multi-dimensional spectroscopies with vacuum ultraviolet (VUV)/x-ray free-electron laser (FEL) sources would open up unique capabilities for dynamic studies of matter at the femtosecond–nanometer time–length scales. Using sequences of ultrafast VUV/x-ray pulses tuned to electron transitions enables element-specific studies of charge and energy flow between constituent atoms, which embody the very essence of chemistry and condensed matter physics. A remarkable step forward towards this goal would be achieved by extending the four wave mixing (FWM) approach at VUV/soft x-ray wavelengths, thanks to the use of fully coherent sources, such as seeded FELs. Here, we demonstrate the feasibility of VUV/soft x-ray FWM at Fermi@Elettra and we discuss its applicability to probe ultrafast intramolecular dynamics, charge injection processes involving metal oxides and electron correlation and magnetism in solid materials. The main advantage in using VUV/soft x-ray wavelengths is in adding element-sensitivity to FWM methods by exploiting the core resonances of selected atoms in the sample.