Shrayesh N. Patel

High‐Mobility Field‐Effect Transistors Fabricated with Macroscopic Aligned Semiconducting Polymers

A record high OFET hole mobility, as high as 23.7 cm(2) /Vs, is achieved in macroscopic aligned semiconducting polymers. The high mobility is insensitive to the polymer molecular weight. Polymer chains are aligned along the fiber to facilitate intrachain charge transport.

Power Factor Enhancement in Solution‐Processed Organic n‐Type Thermoelectrics Through Molecular Design

A new class of high-performance n-type organic thermoelectric materials, self-doping perylene diimide derivatives with modified side chains, is reported. These materials achieve the highest n-type thermoelectric performance of solution-processed organic materials reported to date, with power factors as high as 1.4 μW/mK(2). These results demonstrate that molecular design is a promising strategy for enhancing organic thermoelectric performance.

Simultaneous Conduction of Electronic Charge and Lithium Ions in Block Copolymers

The main objective of this work is to study charge transport in mixtures of poly(3-hexylthiophene)-b-poly(ethylene oxide) (P3HT-PEO) block copolymers and lithium bis(trifluoromethanesulfonyl) imide salt (LiTFSI). The P3HT-rich microphase conducts electronic charge, while the PEO-rich microphase conducts ionic charge. The nearly symmetric P3HT-PEO copolymer used in this study self-assembles into a lamellar phase. In contrast, the morphologies of asymmetric copolymers with P3HT as the major component are dominated by nanofibrils. A combination of ac and dc impedance measurements was used to determine the electronic and ionic conductivities of our samples. The ionic conductivities of P3HT-PEO/LiTFSI mixtures are lower than those of mixtures of PEO homopolymer and LiTFSI, in agreement with published data obtained from other block copolymer/salt mixtures. In contrast, the electronic conductivities of the asymmetric P3HT-PEO copolymers are significantly higher than those of the P3HT homopolymer. This is unexpected because of the presence of the nonelectronically conducting PEO microphase. This implies that the intrinsic electronic conductivity of the P3HT microphase in P3HT-PEO copolymers is significantly higher than that of P3HT homopolymers.

The Density of States and the Transport Effective Mass in a Highly Oriented Semiconducting Polymer: Electronic Delocalization in 1D

The determination of the band structure along k parallel to the chain direction demonstrates significant electronic delocalization. The small effective mass [m* = 0.106mo ] is consistent with the high measured mobility.

Morphology controls the thermoelectric power factor of a doped semiconducting polymer

The orientational correlation length of domains in a semiconducting polymer controls its thermoelectric performance. The electrical performance of doped semiconducting polymers is strongly governed by processing methods and underlying thin-film microstructure. We report on the influence of different doping methods (solution versus vapor) on the thermoelectric power factor (PF) of PBTTT molecularly p-doped with FnTCNQ (n = 2 or 4). The vapor-doped films have more than two orders of magnitude higher electronic conductivity (σ) relative to solution-doped films. On the basis of resonant soft x-ray scattering, vapor-doped samples are shown to have a large orientational correlation length (OCL) (that is, length scale of aligned backbones) that correlates to a high apparent charge carrier mobility (μ). The Seebeck coefficient (α) is largely independent of OCL. This reveals that, unlike σ, leveraging strategies to improve μ have a smaller impact on α. Our best-performing sample with the largest OCL, vapor-doped PBTTT:F4TCNQ thin film, has a σ of 670 S/cm and an α of 42 μV/K, which translates to a large PF of 120 μW m−1 K−2. In addition, despite the unfavorable offset for charge transfer, doping by F2TCNQ also leads to a large PF of 70 μW m−1 K−2, which reveals the potential utility of weak molecular dopants. Overall, our work introduces important general processing guidelines for the continued development of doped semiconducting polymers for thermoelectrics.