Abstract

Second-harmonic generation (SHG) is a powerful measurement technique to analyze the symmetry properties of crystals. Mechanical strain can reduce the symmetry of a crystal and even weak strain can have a considerable impact on the SHG intensity along different polarization directions. The impact of strain on the SHG can be modeled with a second-order nonlinear photoelastic tensor. In this work, we determined the photoelastic tensors at a fundamental wavelength of 800 nm for four different transition metal dichalcogenide (TMD) monolayers: MoS2, MoSe2, WS2, and WSe2. Strain is applied using a three-point bending scheme, and the polarization-resolved SHG pattern is measured in backscattering geometry. Furthermore, we connected the strain dependent SHG with the strain dependence of the A-exciton energy. With the second-order nonlinear photoelastic tensor, full strain information can be accurately extracted from polarization-resolved SHG measurements. Accordingly, uniaxial strain, induced by polydimethylsiloxan (PDMS) exfoliation and transfer, is measured. We find that TMD monolayers fabricated with PDMS are strained by ∼0.2%. With the experimentally determined nonlinear photoelastic tensors, it will be possible to optically probe arbitrary strain fields in TMD monolayers.

Highlights

  • The availability of highly intense light, made possible by the development of short-pulse lasers, has allowed for the investigation of nonlinear optical processes.1 There is a wide range of nonlinear optical effects, spanning from frequency mixing2 to the optical Kerr effect.3 The first discovered nonlinear optical effect is second-harmonic generation (SHG),1 which has, together with the related phenomena of sum- and difference-frequency generation, many important applications

  • The photoelastic coefficients p1 and p2 for the relevant transition metal dichalcogenide (TMD) monolayers were determined by applying varying levels of strain and measuring the polarization-resolved SHG

  • In order to avoid slipping of the TMD monolayer on the bent substrate, we limited the applied strain to values below 0.5%

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Summary

Introduction

The availability of highly intense light, made possible by the development of short-pulse lasers, has allowed for the investigation of nonlinear optical processes. There is a wide range of nonlinear optical effects, spanning from frequency mixing to the optical Kerr effect. The first discovered nonlinear optical effect is second-harmonic generation (SHG), which has, together with the related phenomena of sum- and difference-frequency generation, many important applications. The availability of highly intense light, made possible by the development of short-pulse lasers, has allowed for the investigation of nonlinear optical processes.. There is a wide range of nonlinear optical effects, spanning from frequency mixing to the optical Kerr effect.. The first discovered nonlinear optical effect is second-harmonic generation (SHG), which has, together with the related phenomena of sum- and difference-frequency generation, many important applications. These effects are used, for example, in optical parametric oscillators, in quantum optics to generate entangled photons, or to produce femtosecond light pulses by Kerr-lens mode-locking.. Odd-ordered nonlinear processes, such as third-harmonic generation (THG), are allowed in all materials

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