All-optical control of second-harmonic generation in β-BaB₂O₄ via coherent, terahertz-driven acentric lattice displacement.

Abstract

Dynamical control of the nonlinear optical properties of solids - with light itself - will be essential for future ultrafast photonic technologies. Previously, methods to modulate nonlinear processes including second-harmonic generation (SHG) have relied primarily on non-resonant light-matter interaction or photo-generation of hot electrons in nanoscale materials. However, these approaches are typically constrained by limited interaction lengths and the initial frequency conversion is relatively weak under equilibrium conditions. Here, a ~ 30% modulation of efficient phase-matched SHG in bulk beta-barium borate (β-BaB₂O₄) is achieved through transient lattice deformation by intense terahertz (THz) pulses that are tuned to resonance with an infrared-active phonon mode. The effect originates from modification of the index of refraction ellipsoid and the corresponding nonlinear phase-matching conditions, rather than from direct modulation of the nonlinear susceptibility through THz-mediated <math xmlns="http://www.w3.org/1998/Math/MathML"><msup><mrow><mi>χ</mi></mrow><mrow><mrow><mo>(</mo><mrow><mn>3</mn></mrow><mo>)</mo></mrow></mrow></msup></math> processes. This mechanism, of resonant selective lattice excitation, points toward novel THz-control schemes to tune the nonlinear optical response in materials.