Optimizing Nonlinear Optical Visibility of Two-Dimensional Materials.

Two-dimensional (2D) materials have attracted broad research interests across various nonlinear optical (NLO) studies, including nonlinear photoluminescence (NPL), second harmonic generation (SHG), transient absorption (TA), and so forth. These studies have unveiled important features and information of 2D materials, such as in grain boundaries, defects, and crystal orientations. However, as most research studies focused on the intrinsic NLO processes, little attention has been paid to the substrates underneath. Here, we discovered that the NLO signal depends significantly on the thickness of SiO2 in SiO2/Si substrates. A 40-fold enhancement of the NPL signal of graphene was observed when the SiO2 thickness was varied from 270 to 125 nm under 800 nm excitation. We systematically studied the NPL intensity of graphene on three different SiO2 thicknesses within a pump wavelength range of 800-1100 nm. The results agreed with a numerical model based on back reflection and interference. Furthermore, we have extended our measurements to include TA and SHG of graphene and MoS2, confirming that SiO2 thickness has similar effects on all of the three major types of NLO signals. Our results will serve as an important guidance for choosing the optimum substrates to conduct NLO research studies on 2D materials.