Determining the complex second-order optical susceptibility in macroscale van der Waals heterobilayers

TL;DR

This study experimentally measures the second-order optical susceptibility in MoSe2/WS2 heterobilayers using a novel heterodyne detection scheme, revealing insights into interlayer effects and complex phases relevant for nanophotonic design.

Contribution

Developed a heterodyne-detection method for second-harmonic generation to characterize complex susceptibilities in macroscale heterobilayers, distinguishing domain orientations and interlayer effects.

Findings

Heterodyne scheme successfully distinguished crystal domain orientations.

Interlayer effects on second-harmonic generation are within experimental uncertainty.

Provided quantitative data for nanophotonic system design based on stacking.

Abstract

We report on the experimental characterization of the second-order susceptibility in MoSe$_2$/WS$_2$ heterobilayers, including their hidden complex phases. To this end, we developed a heterodyne-detection scheme for second-harmonic generation and applied it to macroscale heterobilayer samples prepared using the gold-tape exfoliation method. The heterodyne scheme enabled us to distinguish the relative orientation of the crystal domains, and further, it allowed us to characterize the complex phases of the susceptibility relative to a reference quartz sample. By comparing the results from the monolayer regions and the heterobilayer region over several hundred microns of the sample area, we determined that the contribution of interlayer effects to second-harmonic generation is within the experimental uncertainty arising from the sample inhomogeneity. The results here provide fundamental quantitative information necessary for the precise design of nanophotonic systems based on stacking engineering.