AVS 64th International Symposium & Exhibition
    2D Materials Focus Topic Friday Sessions
       Session 2D+MI+NS+SS+TF-FrM

Paper 2D+MI+NS+SS+TF-FrM7
Imaging Nanoscale Heterogeneity at the Two-dimensional Semiconductor-Metal Heterointerface by Correlated Scanning Probe Microscopy

Friday, November 3, 2017, 10:20 am, Room 15

Session: Nanostructures including Heterostructures and Patterning of 2D Materials
Presenter: Deep Jariwala, California Institute of Technology
Authors: D.J. Jariwala, California Institute of Technology
A. Krayev, AIST-NT Inc.
E. Robinson, AIST-NT Inc.
M.C. Sherrott, California Institute of Technology
M. Terrones, Pennsylvania State University
H.A. Atwater, California Institute of Technology
Correspondent: Click to Email

Transition metal dichalcogenides (TMDCs) of molybdenum and tungsten have recently attracted significant attention due to their band gaps in visible part of the spectrum for optoelectronic device applications. The ability to isolate these materials down to a monolayer with direct band-gap make TMDCs very attractive alternatives to graphene.

While a lot of investigation has been devoted to understanding of crystalline and electronic quality of TMDCs in devices, little is known about the spatial distribution of electronic quality and interfaces with metals. Conventional Raman spectroscopy and confocal Raman microscopy have proved to be useful tools in this regard. However, the spatial resolution of these techniques is diffraction limited to a few hundred nanometers only. Tip enhanced Raman scattering (TERS) provides spatial resolution down to few nanometers, along with increased sensitivity due to dramatic enhancement of the Raman signal by the plasmonic tip and is therefore a suitable technique to probe nanoscale heterogeneity in TMDC samples.

Here, we report observation of nanoscale heterogeneity in exfoliated WSe2 flakes on plasmonic Au and Ag substrates using a combination of spatial mapping with TERS, contact potential difference, topography and conductance measurements. In TERS mapping of exfoliated WSe2 flakes, we observe the presence of domains with enhanced or depreciated Raman signal compared to adjacent material. We also observe that WSe2 demonstrates a resonant Raman response with 638nm excitation, the TERS spectra of these domains feature a single peak at around 250 cm-1, typical for non-resonant conditions. Distribution of these domains correlates extremely well with surface potential map, non-resonant areas being negatively charged compared to adjacent areas of WSe2 that demonstrate a resonant Raman response.

We further correlate the TERS maps with concurrently recorded photocurrent maps, where we observe that domains showing both resonant and non-resonant Raman response, generated significant photocurrent, but of opposite polarities. Based on this observation, we conclude that in exfoliated layers of WSe2, there exist nanoscale semiconducting domains with opposite doping types when in contact with the underlying metal. This hitherto unobserved heterogeneity is therefore critical to understanding of the metal-two dimensional (2D) semiconductor contact and important for optoelectronic device design and performance. The results presented here show that cross-correlation of TERS with local conductivity, surface potential and photocurrent is a vital characterization technique for nanoscale in-homogenities in 2D semiconductors and devices.