We demonstrate the synthesis of a new copolymer which is composed of dialkyl thienylated benzodithiophene and perfluororalkyl-carbonyl thienothiophene (DTBDT-TTFO) and the characterization of its optoelectronic properties. The introduction of thienyl groups enabled the extended delocalization of π electrons in the DTBDT-TTFO backbone and efficient intermolecular charge transport as proved by the fairly high field effect mobility of 0.02 cm(2)/(V s). The introduction of perfluororalkyl-carbonyl side chains resulted in a significant red-shift of DTBDT-TTFO in the absorption spectra and a decrease in the HOMO and LUMO levels. The resulting energy levels of DTBDT-TTFO were not satisfactory for solar cell applications, especially in terms of charge separation at the polymer/PCBM interfaces. Rather, the DTBDT-TTFO showed better energy level matching with the colloidal nanocrystals (NCs) of CdSe. A photodetector based on the bulkheterojunction of DTBDT-TTFO and CdSe NCs with coplanar device geometry resulted in a high photoconductive gain (responsivity higher than 1A/W under a low operating voltage of 1 V), possibly arising from electron trapping at CdSe NCs such that the hole can travel along the detector and its surrounding circuit. More importantly, the photodetector revealed a time constant of a few hundreds of microseconds, which means that the response speed of the photodetector is fast enough for lag-free imaging applications.
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Nano Lett
January 2025
Department of Chemistry, University of California, Berkeley, California 94720, United States.
The utilization of excited charge carriers in semiconductor nanocrystals (NCs) for optoelectronic technologies has been a long-standing goal in the field of nanoscience. Experimental efforts to extend the lifetime of excited carriers have therefore been a principal focus. To understand the limits of these lifetimes, in this work, we theoretically study the time scales of pure electron relaxation in negatively charged NCs composed of two prototypical materials: CdSe and CdS.
View Article and Find Full Text PDFInorg Chem
December 2024
Department of Chemistry and Biochemistry, University of Notre Dame, Notre Dame, Indiana 46556, United States.
Neutral metal salts coordinate to the surfaces of colloidal semiconductor nanocrystals (NCs) by acting as Lewis acid acceptors for the NC surface anions. This ligand coordination has been associated with increased emission due to the passivation of surface hole traps. Here, variation of the anionic ligands of metal salts is used to study anion effects on metal complex Lewis acidity and surface coordination at CdSe and InP NCs.
View Article and Find Full Text PDFSpectrochim Acta A Mol Biomol Spectrosc
November 2024
Hubei Key Laboratory of Low Dimensional Optoelectronic Materials and Devices, Hubei University of Arts and Science, Xiangyang, China. Electronic address:
Owing to the long-lived decay of triplet excited state, extensive efforts have been devoted to efficient triplet generation for applications covering triplet-triplet annihilation for photon upconversion, photocycloaddition and photoredox catalysis. Among the candidates, nanocrystal-molecule complexes have received tremendous attention for triplet generation because of easier spin flip and negligible energy loss during intersystem crossing. However, the triplet energy transfer (TET) from nanocrystals (NCs) to molecules can be very complicated in actual situation due to intricate energy level alignment and inevitable defect states, which often involves various decay pathes of the excited state competing with TET.
View Article and Find Full Text PDFACS Omega
February 2024
Department of Chemistry, SRM University AP-Andhra Pradesh, Mangalagiri, Andhra Pradesh 522 240, India.
Semiconductor quantum dots (QDs) have been used in a variety of applications ranging from optoelectronics to biodiagnostic fields, primarily due to their size dependent fluorescent nature. CdSe nanocrystals (NCs) are generally synthesized via a hot injection method in an organic solvent. However, such NCs are insoluble in water and therefore preclude the direct usage toward biological systems.
View Article and Find Full Text PDFJ Am Chem Soc
February 2024
Department of Chemistry, Northwestern University, Evanston, Illinois 60208, United States.
Semiconductor nanocrystals (NCs) offer prospective use as active optical elements in photovoltaics, light-emitting diodes, lasers, and photocatalysts due to their tunable optical absorption and emission properties, high stability, and scalable solution processing, as well as compatibility with additive manufacturing routes. Over the course of experiments, during device fabrication, or while in use commercially, these materials are often subjected to intense or prolonged electronic excitation and high carrier densities. The influence of such conditions on ligand integrity and binding remains underexplored.
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