Energy-Efficient Solar Photochemistry with Luminescent Solar Concentrator Based Photomicroreactors.

The sun is the most sustainable light source available on our planet, therefore the direct use of sunlight for photochemistry is extremely appealing. Demonstrated here, for the first time, is that a diverse set of photon-driven transformations can be efficiently powered by solar irradiation with the use of solvent-resistant and cheap luminescent solar concentrator based photomicroreactors. Blue, green, and red reactors can accommodate both homogeneous and multiphase reaction conditions, including photochemical oxidations, photocatalytic trifluoromethylation chemistry, and metallaphotoredox transformations, thus spanning applications over the entire visible-light spectrum. To further illustrate the efficacy of these novel solar reactors, medicinally relevant molecules, such as ascaridole and an intermediate of artemisinin, were prepared as well.

An Automated Analysis of Homocoupling Defects Using MALDI-MS and Open-Source Computer Software.

Conjugated organic polymers have substantial potential for multiple applications but their properties are strongly influenced by structural defects such as homocoupling of monomer units and unexpected end-groups. Detecting and/or quantifying these defects requires complex experimental techniques, which hinder the optimization of synthesis protocols and fundamental studies on the influence of structural defects. Mass spectrometry offers a simple way to detect these defects but a manual analysis of many complex spectra is tedious and provides only approximate results. In this work, we develop a computational methodology for analyzing complex mass spectra of organic copolymers. Our method annotates spectra similarly to a human expert and provides quantitative information about the proportions of signal assigned to each ion. Our method is based on the open-source Masserstein algorithm, which we modify to handle large libraries of reference spectra required for annotating complex mass spectra of polymers. We develop a statistical methodology to analyze the quantitative annotations and compare the statistical distributions of structural defects in polymer chains between samples. We apply this methodology to analyze commercial and lab-made samples of a benchmark polymer and show that the samples differ both in the amount and in the types of structural defects.

A tetrathienopyrrole-based ladder-type donor polymer for high-performance organic near-infrared cavity detectors.

Organic semiconductors can afford detection at wavelengths beyond commercial silicon photodetectors. However, for each targeted near-infrared wavelength range, this requires individually optimized materials, which adds to the complexity and costs. Moreover, finding molecules with strong absorption beyond 1 µm that perform well in organic photodetectors remains a challenge. In microcavity devices, the detection window can be extended to wavelengths inaccessible for silicon without the need for new materials by adopting an intelligent design. Previous work has demonstrated the applicability of a dithienopyrrole-based donor polymer (PDTPQx) in such a cavity photodetector device, with a photoresponse up to 1200 nm. In this work, the π-conjugated backbone of the polymer is extended, affording higher hole mobility and better donor:acceptor intermixing. This leads to enhanced peak external quantum efficiencies up to 1450 nm. The (thermal noise limited) detectivities achieved with the PTTPQx polymer (1.07 × 1012 to 1.82 × 1010 Jones) are among the very best in the 900-1400 nm wavelength regime.