Domingo, Ester; Vandewal, Koen; Fei, Zhuping; Watkins, Scott E.; Scholes, Fiona H.; Bannock, James H; de Mello, John; Richter, Lee J.; DeLongchamp, Dean M.; Amassian, Aram; Heeney, Martin; Salleo, Alberto; Stingelin, Natalie(Journal of the American Chemical Society, American Chemical Society (ACS), 2015-04-16)[Article]
We show that the Charge Transfer (CT) absorption signal in bulk-heterojunction (BHJ) solar cell blends, measured by photothermal deflection spectroscopy (PDS), is directly proportional to the density of molecular donor/acceptor interfaces. Since the optical transitions from ground state to the interfacial CT state are weakly allowed at photon energies below the optical gap of both donor and acceptor, we can exploit the use of this sensitive linear absorption spectroscopy for such quantification. Moreover, we determine the absolute molar extinction coefficient of the CT transition for an archetypical polymer-fullerene interface. The latter is ~100 times lower than the extinction coefficient of the donor chromophore involved, allowing us to experimentally estimate the transition dipole moment (0.3 D) and the electronic coupling between ground state and CT state to be on the order of 30 meV.
Nielsen, Christian B.; Giovannitti, Alexander; Sbircea, Dan-Tiberiu; Bandiello, Enrico; Niazi, Muhammad Rizwan; Hanifi, David A.; Sessolo, Michele; Amassian, Aram; Malliaras, George G.; Rivnay, Jonathan; McCulloch, Iain(Journal of the American Chemical Society, American Chemical Society (ACS), 2016-08-08)[Article]
The organic electrochemical transistor (OECT), capable of transducing small ionic fluxes into electronic signals in an aqueous envi-ronment, is an ideal device to utilize in bioelectronic applications. Currently, most OECTs are fabricated with commercially availa-ble conducting poly(3,4-ethylenedioxythiophene) (PEDOT)-based suspensions and are therefore operated in depletion mode. Here, we present a series of semiconducting polymers designed to elucidate important structure-property guidelines required for accumulation mode OECT operation. We discuss key aspects relating to OECT performance such as ion and hole transport, elec-trochromic properties, operational voltage and stability. The demonstration of our molecular design strategy is the fabrication of accumulation mode OECTs that clearly outperform state-of-the-art PEDOT based devices, and show stability under aqueous oper-ation without the need for formulation additives and cross-linkers.
Quan, Li Na; Yuan, Mingjian; Comin, Riccardo; Voznyy, Oleksandr; Beauregard, Eric M.; Hoogland, Sjoerd; Buin, Andrei; Kirmani, Ahmad R.; Zhao, Kui; Amassian, Aram; Kim, Dong Ha; Sargent, Edward H.(Journal of the American Chemical Society, American Chemical Society (ACS), 2016-02-17)[Article]
Metal halide perovskites have rapidly advanced thin film photovoltaic performance; as a result, the materials’ observed instabilities urgently require a solution. Using density functional theory (DFT), we show that a low energy of formation, exacerbated in the presence of humidity, explains the propensity of perovskites to decompose back into their precursors. We find, also using DFT, that intercalation of phenylethylammonium between perovskite layers introduces quantitatively appreciable van der Waals interactions; and these drive an increased formation energy and should therefore improve material stability. Here we report the reduced-dimensionality (quasi-2D) perovskite films that exhibit improved stability while retaining the high performance of conventional three-dimensional perovskites. Continuous tuning of the dimensionality, as assessed using photophysical studies, is achieved by the choice of stoichiometry in materials synthesis. We achieved the first certified hysteresis-free solar power conversion in a planar perovskite solar cell, obtaining a 15.3% certified PCE, and observe greatly improved performance longevity.
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