Symmetry-Breaking Electron Dynamics Enable Ultrabroadband Optical-Field Sampling via Second-Harmonic Generation

Abstract

Optical-field sampling using second-harmonic generation (SHG) from strong-field ionization enables ultrabroadband terahertz detection, but the microscopic origin of the SHG signal and its ultrabroadband response have been unclear. Here we show that the target field lifts the half-cycle cancellation of photoelectron dipole emission, generating the SHG signal used for field sampling. Time-dependent Schrodinger-equation simulations, supported by classical-trajectory Monte Carlo analysis, demonstrate that the SHG yield directly encodes the instantaneous target electric field at the ionization time, enabling waveform retrieval by scanning the probe-target delay. Because the SHG response is gated by a subcycle ionization window rather than the probe envelope, the detection bandwidth can extend far beyond the probe duration. We further quantify practical constraints on retrieval, including intrinsic probe asymmetry and SHG back-action, providing a predictive framework to optimize sensitivity, temporal resolution, and fidelity through controlled electron dynamics.