2D piezotronics : performance to functionality

includes bibliographical references and index

PhD; 2023; Centre for Nano Science and Engineering

In the pursuit of interactive electronic devices, there is a need for smart materials which can serve multiple functionalities. 2D (two-dimensional) layered materials have gained attention in semiconductor technology because of their versatile electrical and optical properties. Furthermore, some materials exhibit piezoelectricity at 2D scale and can withstand enormous strain. These properties make them suitable as smart materials involving electromechanical signals. In the literature, materials which are semiconducting and piezoelectric are termed piezotronic (piezo+electronic) materials. Theoretical studies have indicated many materials as piezoelectric in 2D form. However, experimental tools to investigate the extent of piezoelectric coupling in 2D materials are limited, and their relevance for piezotronics has not been studied in detail. This dissertation presents some key aspects of 2D Piezotronics for improved performance and to achieve additional functionalities with heterojunctions. The work constitutes proposing a technique to estimate piezoelectric coupling coefficients, choice of flexible substrates for piezotronics, methods to reduce the charge screening effects, measurement strategies to extract the actual piezoelectric output from the bending measurements, and the study of heterojunctions for rectifying behaviour. In this work, Molybdenum disulfide (MoS2) is used as active piezoelectric material. In the initial part of the work, I propose a technique to estimate in-plane piezoelectric coupling quantitatively for 2D materials. The method involves a novel approach for in-plane field excitation in lateral Piezo force microscopy (PFM). Contact resonance gain of the tip-sample system is leveraged to measure the piezoelectric coupling coefficients in a few pm/V to sub pm/V range. However, I have shown that operating PFM at contact resonance can cause pseudo piezoelectric signals. Therefore, a detailed methodology for signal calibration and electrostatic background subtraction is developed in this work. The technique is verified by estimating the in-plane piezoelectric coupling coefficients (d11) for freely suspended MoS2 of one to five atomic layers. The technique presented is useful in estimating the piezoelectric coupling strengths in emerging 2D materials. Piezotronic devices are made on flexible substrates for practical applications. Fabrication on flexible substrates often poses great difficulties in handling them, depositing inorganic materials, and carrying out lithography processes. I propose the commercially available nano flex film as a prospective substrate for piezotronics. Carrying out fabrication on these substrates is as seamless as that on rigid substrates. Substrates such as PET, Nano flex and TPU can be used for low-temperature (<150 deg C) applications. Kapton is one of the flexible substrates that can handle higher temperatures(>200 deg C). However, they tend to twist when heated, making the fabrication difficult. I have proposed a gel-based bonding for the Kapton substrates wherein the debonding process is automatic. The method is helpful for the fabrication of 2D material devices on Kapton. Besides selecting the substrates, suitable base layers and passivation techniques are studied to reduce the charge screening effects and thus improve the performance of piezotronic devices. It is verified that open circuit voltages and strain gauge factors obtained for the current monolayer MoS2 device on SiO2 are three folds higher than those presented in the literature. A simple measurement setup which does not require probe needles or wire bonding is developed for the bending strain measurements. The open circuit voltage and short circuit current signals obtained from a single 2D material device are very small. The noise signals that originate from various triboelectric and electrostatic sources of the measurement setup can be of similar magnitude. Consequently, the electrical outputs from these devices during bending measurements are often misinterpreted. Thus, it is essential to analyse various noise sources in bending measurements. I then discuss ways to reduce the background noise and identify the valid piezoelectric output. Finally, I have studied some homogeneous and heterogeneous junctions of MoS2 to achieve good rectifying junction behaviour, which can add extra functionalities for piezotronics. The rectification ratio values as high as 5000 could be achieved at 1 V bias. Besides the rectifying ratio, I have observed that the heterojunctions of MoS2 and MoTe2 have superior piezoelectric behaviour compared to other 2D material junctions reported so far with open circuit voltages as high as ~1 V and peak power density of ~200 mW/m2 at 0.44% bending strain. Formation of the p-n and Schottky junction hybrid in MoS2-MoTe2 heterojunction could achieve high rectification ratios and open circuit voltages and is fascinating for further study.