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Register a new userRevealing Interfaces of Two-Dimensional Lateral Heterostructures by Second Harmonic Generation
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The interface between two different semiconductors is crucial in determining the electronic properties at the heterojunction, therefore novel techniques that can probe these regions are of particular interest. Recently it has been shown that heterojunctions of two-dimensional transition metal dichalcogenides have sharp and epitaxial interfaces that can be used to the next generation of flexible and on chip optoelectronic devices. Here, we show that second harmonic generation (SHG) can be used as an optical tool to reveal these atomically sharp interfaces in different lateral heterostructures. We observed an enhancement of the SH intensity at the heterojunctions, and showed that is due to a coherent superposition of the SH emission from each material. This constructive interference pattern reveals a phase difference arising from the distinct second-order susceptibilities of both materials at the interface. Our results demonstrate that SHG microscopy is a sensitive characterization technique to unveil nanometric features in layered materials and their heterostructures.
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We present a novel methodology to synthesize two-dimensional (2D) lateral heterostructures of graphene and MoS2 sheets with molecular carbon nanomembranes (CNMs), which is based on electron beam induced stitching. Monolayers of graphene and MoS2 were grown by chemical vapor deposition (CVD) on copper and SiO2 substrates, respectively, transferred onto gold/mica substrates and patterned by electron beam lithography or photolithography. Self-assembled monolayers (SAMs) of aromatic thiols were grown on the gold film in the areas where the 2D materials were not present. An irradiation with a low energy electron beam was employed to convert the SAMs into CNMs and simultaneously stitching the CNM edges to the edges of graphene and MoS2, therewith forming a heterogeneous but continuous film composed of two different materials. The formed lateral heterostructures possess a high mechanical stability, enabling their transfer from the gold substrate onto target substrates and even the preparation as freestanding sheets. We characterized the individual steps of this synthesis and the structure of the final heterostructures by complementary analytical techniques including optical microscopy, Raman spectroscopy, atomic force microscopy (AFM), helium ion microscopy (HIM), X-ray photoelectron spectroscopy (XPS) and high-resolution transmission electron microscopy (HRTEM) and find that they possess nearly atomically sharp boundaries.
The two-dimensional ferroelectrics GeS, GeSe, SnS and SnSe are expected to have large spontaneous in-plane electric polarization and enhanced shift-current response. Using density functional methods, we show that these materials also exhibit the largest effective second harmonic generation reported so far. It can reach magnitudes up to $10$ nm/V which is about an order of magnitude larger than that of prototypical GaAs. To rationalize this result we model the optical response with a simple one-dimensional two-band model along the spontaneous polarization direction. Within this model the second-harmonic generation tensor is proportional to the shift-current response tensor. The large shift current and second harmonic responses of GeS, GeSe, SnS and SnSe make them promising non-linear materials for optoelectronic applications.
An optical Second-Harmonic Generation (SHG) allows to probe various structural and symmetry-related properties of materials, since it is sensitive to the inversion symmetry breaking in the system. Here, we investigate the SHG response from a single layer of graphene disposed on an insulating hexagonal Boron Nitride (hBN) and Silicon Carbide (SiC) substrates. The considered systems are described by a non-interacting tight-binding model with a mass term, which describes a non-equivalence of two sublattices of graphene when the latter is placed on a substrate. The resulting SHG signal linearly depends on the degree of the inversion symmetry breaking (value of the mass term) and reveals several resonances associated with the band gap, van Hove singularity, and band width. The difficulty in distinguishing between SHG signals coming from the considered heterostrusture and environment (insulating substrate) can be avoided applying a homogeneous magnetic field. The latter creates Landau levels in the energy spectrum and leads to multiple resonances in the SHG spectrum. Position of these resonances explicitly depends on the value of the mass term. We show that at energies below the band-gap of the substrate the SHG signal from the massive graphene becomes resonant at physically relevant values of the applied magnetic field, while the SHG response from the environment stays off-resonant.
The second-order nonlinear optical susceptibility $Pi^{(2)}$ for second harmonic generation is calculated for gapped graphene. The linear and second-order nonlinear plasmon excitations are investigated in context of second harmonic generation (SHG). We report a red shift and an order of magnitude enhancement of the SHG resonance with growing gap, or alternatively, reduced electro-chemical potential.
Quantum geometry of the electron wave function plays a significant role in the linear and non-linear responses of crystalline materials. Here, we study quantum geometry induced second harmonic generation. We identify non-linear responses stemming from the quantum geometric tensor and the quantum geometric connection in systems with finite Fermi surfaces and disorder. In addition to the injection, shift, and anomalous currents we find two new contributions, which we term double resonant and higher-order pole contributions. Our findings can be tested in state-of-the-art devices in WTe2 (time-reversal symmetric system) and in CuMnAs (parity-time reversal symmetric systems).
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