Electrostatic Correlations Lead to High Capacitance in Zwitterion-Containing Thin Films.

A novel zwitterion composed of an imidazolium tethered to an anionic sulfonyl(trifluoromethane sulfonyl)imide group was prepared as an alternative dielectric material to traditional ionic liquids. The zwitterion not only melted below 100 °C but also proved to be nonhygroscopic. High-capacitance organic dielectric materials were obtained by blending this compound with poly(methyl methacrylate) over a range of concentrations and thicknesses.

Physical Supercritical Fluid Deposition: Patterning Solution Processable Materials on Curved and Flexible Surfaces.

We provide the initial demonstration of a general thin film deposition technique that leverages the unique solubility properties of supercritical fluids. The technique is the solution-phase analogue of physical vapor deposition and allows thin films of a semiconducting polymer to be grown without the need for in situ chemical reactions. Film growth is approximately linear with time, indicating that film thickness can be controlled in a straightforward manner by varying the time of deposition.

Towards the Organic Double Heterojunction Solar Cell.

A perspective on the operating principles of organic bulk heterojunction solar cells is outlined and used to suggest an alternative device configuration, employing two type II semiconductor heterojunctions in series. Guiding principles to the implementation of this configuration, called a double heterojunction, are summarized. Assuming an exciton binding energy of 0.

Exploiting exciton coupling of ligand radical intervalence charge transfer transitions to tune NIR absorption.

We detail the rational design of a series of bimetallic bis-ligand radical Ni salen complexes in which the relative orientation of the ligand radical chromophores provides a mechanism to tune the energy of intense intervalence charge transfer (IVCT) bands in the near infrared (NIR) region. Through a suite of experimental (electrochemistry, electron paramagnetic resonance spectroscopy, UV-vis-NIR spectroscopy) and theoretical (density functional theory) techniques, we demonstrate that bimetallic Ni salen complexes form bis-ligand radicals upon two-electron oxidation, whose NIR absorption energies depend on the geometry imposed in the bis-ligand radical complex. Relative to the oxidized monomer [] ( = 4500 cm, = 27 700 M cm), oxidation of the cofacially constrained analogue to [] results in a blue-shifted NIR band ( = 4830 cm, = 42 900 M cm), while oxidation of to [], with parallel arrangement of chromophores, results in a red-shifted NIR band ( = 4150 cm, = 46 600 M cm); the NIR bands exhibit double the intensity in comparison to the monomer.

Ultrafast Charge Generation in an Organic Bilayer Film.

The dynamics of charge generation in a high performing molecular photovoltaic system, p-SIDT(FBTTh2)2 (see Figure 1 ) is studied with transient absorption. The optimized bulk heterojunction material shows behavior observed in many other systems; the majority of charges are generated at short time scales (<150 fs), and a slower contribution from incoherently diffusing excitons is observed at low pump fluence. In a separate experiment, the role of bulk heterojunction material morphology on the process of ultrafast charge generation was investigated with bilayers made with solution processed donor molecules on a photopolymerized C60 layer.

Effects of impurities on operational mechanism of organic bulk heterojunction solar cells.

Photoconductive atomic force microscopy in conjunction with transient absorption spectroscopy and charge transport study were used to investigate the effect of impurities (TCNQ and PC84 BM) on the performance of low band gap conjugated polymer and fullerene solar cells to gain insight into whether differing impurity shapes may lead to different loss mechanisms.

Photoinduced charge generation in a molecular bulk heterojunction material.

Understanding the charge generation dynamics in organic photovoltaic bulk heterojunction (BHJ) blends is important for providing the necessary guidelines to improve overall device efficiency. Despite more than 15 years of experimental and theoretical studies, a universal picture describing the generation and recombination processes operating in organic photovoltaic devices is still being forged. We report here the results of ultrafast transient absorption spectroscopy measurements of charge photogeneration and recombination processes in a high-performing solution-processed molecular BHJ.

Influence of Processing Additives on Charge-Transfer Time Scales and Sound Velocity in Organic Bulk Heterojunction Films.

The role of processing additives in organic bulk heterojunction thin films was investigated by means of transient absorption spectroscopy. The rate of ultrafast charge transfer was found to increase when a small amount of diiodooctane was used during film formation. In addition, coherent acoustic phonons were observed, and their velocity was determined.

Observing the multiexciton state in singlet fission and ensuing ultrafast multielectron transfer.

Multiple exciton generation (MEG) refers to the creation of two or more electron-hole pairs from the absorption of one photon. Although MEG holds great promise, it has proven challenging to implement, and questions remain about the underlying photo-physical dynamics in nanocrystalline as well as molecular media. Using the model system of pentacene/fullerene bilayers and femtosecond nonlinear spectroscopies, we directly observed the multiexciton (ME) state ensuing from singlet fission (a molecular manifestation of MEG) in pentacene.