Abstract
When a biased electric/light field is applied to centrosymmetric crystals like silicon, the broken symmetry creates even-order harmonics radiation which can reveal key insights into the material. Recently, the second harmonic has been generated by THz-induced symmetry breaking, but the observation of higher-order radiation remains largely unexplored. Here, we demonstrate picosecond-level ultrafast, nondestructive symmetry manipulation of silicon crystal by using a 500 kV/cm intense terahertz (THz) electric field. The THz-induced fourth harmonic of the infrared probe is also observed and characterized for the first time. In addition, we find that the even-order harmonics show no dependence on the THz field direction thus it allows for sub-cycle symmetry manipulations. Our study paves the way toward ultrafast all-optical crystal symmetry control in the future high-speed electronics and photonics.