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While carbon provides the basis for all of organic chemistry and biology, elemental carbon compounds themselves play vital roles in our world. Graphite, diamond, fullerenes, graphene, and amorphous carbon solids are used in myriad modern applications, and a number of new, metastable states of carbon with unusual and promising properties have recently been proposed and created. Furthermore, liquid carbon and warm dense carbon are of astrophysical interest, and been proposed to exist in the cores of large planets and stars (Ross, 1981) [1]. While much is known about the solid forms of carbon, its liquid state remains very poorly understood. Due to difficulties in preparing and studying this material, its structure and properties remain essentially unknown. In this review, we describe recent technological advances which have enabled new experiments on liquid carbon samples, prepared with laser melting and shock compression techniques.

We have examined the transmission of soft X-ray pulses from the FERMI free electron laser through carbon films of varying thickness, quantifying nonlinear effects of pulses above and below the carbon K-edge. At typical of soft X-ray free electron laser intensities, pulses exhibit linear absorption at photon energies above and below the K-edge, ∼308 and ∼260 eV, respectively; whereas two-photon absorption becomes significant slightly below the K-edge, ∼284.2 eV. The measured two-photon absorption cross section at 284.18 eV (∼6 × 10−48 cm4 s) is 7 orders of magnitude above what is expected from a simple theory based on hydrogen-like atoms - a result of resonance effects.

Nonlinear optical processes at soft x-ray wavelengths have remained largely unexplored due to the lack of available light sources with the requisite intensity and coherence. Here we report the observation of soft x-ray second harmonic generation near the carbon K edge (∼284  eV) in graphite thin films generated by high intensity, coherent soft x-ray pulses at the FERMI free electron laser. Our experimental results and accompanying first-principles theoretical analysis highlight the effect of resonant enhancement above the carbon K edge and show the technique to be interfacially sensitive in a centrosymmetric sample with second harmonic intensity arising primarily from the first atomic layer at the open surface. This technique and the associated theoretical framework demonstrate the ability to selectively probe interfaces, including those that are buried, with elemental specificity, providing a new tool for a range of scientific problems.