Abstract
Silicon polymorphs with exotic electronic and optical properties have recently attracted significant attention due to the wide range of useful bandgap characteristics1,2,3,4. They are typically formed by high pressure techniques, which put limitations on the sample volumes and their crystal structure5,6,7,8,9,10. This constitutes a major obstacle to study these polymorphs and their incorporation into existing technology. Here, we report on a new approach to create unusual crystal structures deep into the bulk of a silicon wafer by MeV-electrons generated by laser irradiation at ultra-relativistic intensity above ~2x10^18 W/cm2. Strong repulsion between the electrons, their branching due to self-generated magnetic field and nonlinear relativistic effects11,12,13 enhance deposition of their energy deep into the target and form high energy density conditions leading to ionisation, followed by fast quenching and restructuring into new crystal arrangements14,15,16,17,18. Analysis by Raman spectroscopy, synchrotron X-ray diffraction, and high-resolution transmission electron microscopy of nanocrystals formed in the irradiated samples provide compelling evidence of the formation of metastable Si phases. The unexplored domain of material transformations exposed to laser-produced MeV-electrons opens new pathways for the conversion into new crystal structures applicable to a wide range of materials at considerably larger quantity, all preserved for further studies and exploitation.