The Influence of Alkyl Spacers and Molecular Weight on the Charge Transport and Storage Properties of Oxy-Bithiophene-Based Conjugated Polymers.

Conjugated polymers (CPs) with polar side chains can conduct electronic and ionic charges simultaneously, making them promising for bioelectronics, electrocatalysis and energy storage. Recent work showed that adding alkyl spacers between CP backbones and polar side chains improved electronic charge carrier mobility, reduced swelling and enhanced stability, without compromising ion transport. However, how alkyl spacers impact polymer backbone conformation and, subsequently, electronic properties remain unclear.

Structure-Property Relationships for the Electronic Applications of Bis-Adduct Isomers of Phenyl-C Butyric Acid Methyl Ester.

Higher adducts of a fullerene, such as the bis-adduct of PCBM (bis-PCBM), can be used to achieve shallower molecular orbital energy levels than, for example, PCBM or C Substituting the bis-adduct for the parent fullerene is useful to increase the open-circuit voltage of organic solar cells or achieve better energy alignment as electron transport layers in, for example, perovskite solar cells. However, bis-PCBM is usually synthesized as a mixture of structural isomers, which can lead to both energetic and morphological disorder, negatively affecting device performance. Here, we present a comprehensive study on the molecular properties of 19 pure bis-isomers of PCBM using a variety of characterization methods, including ultraviolet photoelectron spectroscopy, thermal gravimetric analysis, differential scanning calorimetry, single crystal structure, and (time-dependent) density functional theory calculation.

Controlling swelling in mixed transport polymers through alkyl side-chain physical cross-linking.

Semiconducting conjugated polymers bearing glycol side chains can simultaneously transport both electronic and ionic charges with high charge mobilities, making them ideal electrode materials for a range of bioelectronic devices. However, heavily glycolated conjugated polymer films have been observed to swell irreversibly when subjected to an electrochemical bias in an aqueous electrolyte. The excessive swelling can lead to the degradation of their microstructure, and subsequently reduced device performance.

Impact of Side-Chain Hydrophilicity on Packing, Swelling, and Ion Interactions in Oxy-Bithiophene Semiconductors.

Exchanging hydrophobic alkyl-based side chains to hydrophilic glycol-based side chains is a widely adopted method for improving mixed-transport device performance, despite the impact on solid-state packing and polymer-electrolyte interactions being poorly understood. Presented here is a molecular dynamics (MD) force field for modeling alkoxylated and glycolated polythiophenes. The force field is validated against known packing motifs for their monomer crystals.

Influence of the Hole Transporting Layer on the Thermal Stability of Inverted Organic Photovoltaics Using Accelerated-Heat Lifetime Protocols.

High power conversion efficiency (PCE) inverted organic photovoltaics (OPVs) usually use thermally evaporated MoO as a hole transporting layer (HTL). Despite the high PCE values reported, stability investigations are still limited and the exact degradation mechanisms of inverted OPVs using thermally evaporated MoO HTL remain unclear under different environmental stress factors. In this study, we monitor the accelerated lifetime performance under the ISOS-D-2 protocol (heat conditions 65 °C) of nonencapsulated inverted OPVs based on the thiophene-based active layer materials poly(3-hexylthiophene) (P3HT), poly[[4,8-bis[(2-ethylhexyl)oxy]benzo[1,2-b:4,5-b']dithiophene-2,6-diyl][3-fluoro-2-[(2-ethylhexyl)carbonyl]thieno[3,4-b]thiophenediyl]] (PTB7), and thieno[3,2-b]thiophene-diketopyrrolopyrrole (DPPTTT) blended with [6,6]-phenyl C-butyric acid methyl ester (PC[70]BM).

Simultaneous topographical, electrical and optical microscopy of optoelectronic devices at the nanoscale.

Novel optoelectronic devices rely on complex nanomaterial systems where the nanoscale morphology and local chemical composition are critical to performance. However, the lack of analytical techniques that can directly probe these structure-property relationships at the nanoscale presents a major obstacle to device development. In this work, we present a novel method for non-destructive, simultaneous mapping of the morphology, chemical composition and photoelectrical properties with <20 nm spatial resolution by combining plasmonic optical signal enhancement with electrical-mode scanning probe microscopy.

Influence of polymer-blend morphology on charge transport and photocurrent generation in donor-acceptor polymer blends.

Monte Carlo algorithms are used to simulate the morphologies adopted by polymer chains in a polymer-blend film in the limits where the chains are mutually attractive (homophilic regime) and mutually repulsive (heterophilic regime) and then to simulate the drift transport of charges through the polymer chains. In the homophilic regime, chains aggregate into tangled domains resulting in a relatively high percolation threshold, a high density of configurational trap states, and slow, dispersive charge transport. In the heterophilic regime at the same polymer volume fraction, chains self-organize into a lacework pattern resulting in a low percolation threshold and efficient, trap-free charge transport.