ABSTRACT
Combining high efficiency with good radiation tolerance, perovskite solar cells (PSCs) are promising candidates to upend expanding space photovoltaic (PV) technologies. Successful employment in a Near-Earth space environment, however, requires high resistance against atomic oxygen (AtOx). This work unravels AtOx-induced degradation mechanisms of PSCs with and without phenethylammonium iodide (PEAI) based 2D-passivation and investigates the applicability of ultrathin silicon oxide (SiO) encapsulation as AtOx barrier. AtOx exposure for 2 h degraded the average power conversion efficiency (PCE) of devices without barrier encapsulation by 40% and 43% (w/o and with 2D-PEAI-passivation) of their initial PCE. In contrast, devices with a SiO-barrier retained over 97% of initial PCE. To understand why 2D-PEAI passivated devices degrade faster than less efficient non-passivated devices, various opto-electrical and structural characterications are conducted. Together, these allowed to decouple different damage mechanisms. Notably, pseudo-J-V curves reveal unchanged high implied fill factors (pFF) of 86.4% and 86.2% in non-passivated and passivated devices, suggesting that degradation of the perovskite absorber itself is not dominating. Instead, inefficient charge extraction and mobile ions, due to a swiftly degrading PEAI interlayer are the primary causes of AtOx-induced device performance degradation in passivated devices, whereas a large ionic FF loss limits non-passivated devices.
ABSTRACT
Carbon quantum dots (CDs) have recently received a tremendous amount of interest owing to their attractive optical properties. However, CDs have broad absorption and emission spectra limiting their application ranges. We herein, for the first time, show synthesis of water-soluble red emissive CDs with a very narrow line width (â¼75 meV) spectral absorbance and hence demonstrate strong coupling of CDs and plasmon polaritons in liquid crystalline mesophases. The excited state dynamics of CDs has been studied by ultrafast transient absorption spectroscopy, and CDs display very stable and strong photoluminescence emission with a quantum yield of 35.4% and a lifetime of â¼2 ns. More importantly, we compare J-aggregate dyes with CDs in terms of their absorption line width, photostability, and ability to do strong coupling, and we conclude that highly fluorescent CDs have a bright future in the mixed light-matter states for emerging applications in future quantum technologies.
ABSTRACT
The advances in colloid chemistry and nanofabrication allowed us to synthesize noble monometallic and bimetallic nanocrystals with tunable optical properties in the visible and near infrared region of the electromagnetic spectrum. In the strong coupling regime, surface plasmon polaritons (SPPs) of metal nanoparticles interact with excitons of quantum dots or organic dyes and plasmon-exciton hybrid states called plexcitons are formed. Until now, various shaped metal nanoparticles such as nanorods, core-shell nanoparticles, hollow nanoparticles, nanoprisms, nanodisks, nanorings, and nanobipyramids have been synthesized to generate plasmon-exciton mixed states. However, in order to boost plasmon-exciton interaction at nanoscale dimensions and expand the application of plexcitonic nanocrystals in a variety of fields such as solar cells, light emitting diodes, and nanolasers, new plexcitonic nanocrystals with outstanding optical and chemical properties remain a key goal and challenge. Here we report laser-assisted synthesis of decahedral shaped noble metal nanocrystals, tuning optical properties of the decahedral shaped nanocrystals by galvanic replacement reactions, colloidal synthesis of bimetallic decahedral shaped plexcitonic nanocrystals, and strong plasmon-plasmon interaction in bimetallic decahedral shaped noble metal nanocrystals near a metal film. We photochemically synthesize decahedral Ag nanoparticles from spherical silver nanoparticles by using a 488 nm laser. The laser assisted synthesis of silver nanoparticles yields decahedral (bicolored) and prism (monocolored) shaped silver nanocrystals. The decahedral shaped nanoparticles were selectively separated from prism shaped nanoparticles by centrifugation. The optical properties of decahedral nanocrystals were tuned by the galvanic replacement reaction between gold ions and silver atoms. Excitons of J-aggregate dyes and SPPs of decahedral bimetallic nanoparticles strongly couple and hence decahedral shaped plexcitonic nanoparticles are prepared. In addition, localized SPPs of decahedral shaped bimetallic nanocrystals interact strongly with the propagating SPPs of a flat silver film and hence new hybrid plasmonic modes (plasmonic nanocavities) are generated. The experimental results are further fully corroborated by theoretical calculations including decahedral shaped plexcitonic nanoparticles and decahedral nanoparticles coupled to flat metal films.
