Optically reconfigurable quasi-phase-matching in silicon nitride microresonators

Quasi-phase-matching has long been a widely used approach in nonlinear photonics, enabling efficient parametric frequency conversions such as second-harmonic generation. However, in silicon photonics the task remains challenging, as materials best suited for photonic integration lack second-order susceptibility (χ(2)), and means for achieving momentum conservation are limited. Here we present optically reconfigurable quasi-phase-matching in large-radius silicon nitride microresonators, resulting in up to 12.5-mW on-chip second-harmonic generated power and a conversion efficiency of 47.6% W−1. Most importantly, we show that such all-optical poling can occur unconstrained from intermodal phase-matching, leading to broadly tunable second-harmonic generation. We confirm the phenomenon by two-photon imaging of the inscribed χ(2) grating structures within the microresonators as well as by in situ tracking of both the pump and second-harmonic mode resonances during all-optical poling. These results unambiguously establish that the photogalvanic effect, responsible for all-optical poling, can overcome phase mismatch constraints, even in resonant systems.

Real-space subfemtosecond imaging of quantum electronic coherences in molecules

Tracking electron motion in molecules is the key to understanding and controlling chemical transformations. Contemporary techniques in attosecond science are able to generate and trace the consequences of this motion in real time, but not in real space. Scanning tunnelling microscopy, on the other hand, can locally probe the valence electron density in molecules, but cannot alone provide dynamical information at this ultrafast timescale. Here we show that, by combining scanning tunnelling microscopy and attosecond technologies, quantum electronic coherences induced in molecules by <6-fs-long carrier-envelope-phase-stable near-infrared laser pulses can be directly visualized at ångström-scale spatial and subfemtosecond temporal resolutions. We demonstrate concurrent real-space and -time imaging of coherences involving the valence orbitals of perylenetetracarboxylic dianhydride molecules, and full control over the population of the involved orbitals. This approach opens the way to the unambiguous observation and manipulation of electron dynamics in complex molecular systems.