Pristine, undoped graphene has a constant absorption of 2.3 % across the visible to near-infrared (VIS-NIR) region of the electromagnetic spectrum. Under certain conditions, such as nanostructuring and intense gating, graphene can interact more robustly with VIS-NIR light and exhibit a large nonlinear optical response. Here, we explore the optical properties of graphene/LaAlO3/SrTiO3 nanostructures, where nanojunctions formed at the LaAlO3/SrTiO3 interface enable large (~10 8 V/m) electric fields to be applied to graphene over a scale of ~10 nm. Upon illumination with ultrafast VIS-NIR light, graphene/LaAlO3/SrTiO3 nanostructures produce broadband THz emission as well as a sum-frequency generated (SFG) response. Strong spectrally sharp, gate-tunable extinction features (>99.99%) are observed in both the VIS-NIR and SFG regions alongside significant intensification of the nonlinear response. The observed gate-tunable strong graphene-light interaction and nonlinear optical response are of fundamental interest and open the way for future exploitation in graphene-based optical devices.Because graphene typically lacks a plasmonic response in the VIS-NIR regime, such behavior is difficult to achieve at higher frequencies 13 . However, the interaction between graphene and VIS-NIR light can be enhanced by creating graphene-based metamaterials or surfaces in which the CNP is modulated at the nanoscale, for example, using AFM 14 or STM 15 , by creating arrays of graphene nanodisks or nanoribbons [10][11][12]16 , or by placing graphene near plasmonic metasurfaces or nanoscale metal gratings [17][18][19][20] .Recently, a technique to control the CNP of graphene-both reversibly and locally-has been developed using graphene integrated with LaAlO3/SrTiO3 (LAO/STO) heterostructures 21,22 . LAO/STO has a tunable conductive interface 23 with a variety of interesting physical properties 24 . When the LAO thickness is close to the critical thickness for a metal-insulator transition, ∼3-4 unit cells 25 , the conductivity of the LAO/STO interface can be controlled using conductive atomic force microscope (c-AFM) lithography 14,26 .A wide range of optoelectronic devices can be fabricated at the LAO/STO interface in this fashion, such as a 10 nm-scale photodetector 27 and nanoscale, terahertz (THz) sources and detectors 28,29 with a bandwidth of more than 100 THz. LAO/STO nanostructures can be placed within two nanometers of an active graphene device and used, for example, to create reconfigurable edge channels in graphene 22 .
EXPERIMENTAL SETUPThe nonlinear optical properties of graphene/LAO/STO (G/LAO/STO) nanojunctions (illustrated in Figure 1(b)) are measured through a broadband THz spectroscopy technique (Figure 2) that takes advantage of strong optical nonlinearities in STO 28,29,30 . The G/LAO/STO nanojunctions are created using c-AFM lithography, described in detail elsewhere 14 and summarized in the Materials and Methods section. A nanojunction (Figure 1(b)) consists of a conducting LAO/STO nanowire with a nanoscale (~10 nm) i...