Silencing and enhancement of second-harmonic generation in optical gap antennas

Amplifying local electromagnetic fields by engineering optical interactions between individual constituents of an optical antenna is considered fundamental for efficient nonlinear wavelength conversion in nanometer-scale devices. In contrast to this general statement we show that high field enhancement does not necessarily lead to an optimized nonlinear activity. In particular, we demonstrate that second-harmonic responses generated at strongly interacting optical gap antennas can be significantly suppressed. Numerical simulations are confirming silencing of second-harmonic in these coupled systems despite the existence of local field amplification. We then propose a simple approach to restore and amplify the second-harmonic signal by changing the manner in which electrically-connected optical antennas are interacting in the charge-transfer plasmon regime. Our observations provide critical design rules for realizing optimal structures that are essential for a broad variety of nonlinear surface-enhanced characterizations and for realizing the next generation of electrically-driven optical antennas.