Publications by authors named "Pabitra Shakya-Tuladhar"

Article Synopsis
  • Recent advancements in organic photovoltaics (OPVs) have significantly improved device efficiency, particularly through the design of nonfullerene acceptors and reducing energy offset at the donor/acceptor interface.
  • Temperature-dependent transient absorption spectroscopy reveals that charge generation in these OPV blends has minimal activation energy (11-21 meV), indicating a highly efficient process that is largely independent of energy offset.
  • While geminate recombination also shows low activation energy, bimolecular charge recombination is significantly influenced by temperature, with an activation energy greater than 400 meV, suggesting that charge generation might be more of an adiabatic process than one governed by traditional Marcus theory.
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Herein, a new ternary strategy to fabricate efficient and photostable inverted organic photovoltaics (OPVs) is introduced by combining a bulk heterojunction (BHJ) blend and a fullerene self-assembled monolayer (C -SAM). Time-of-flight secondary-ion mass spectrometry - analysis reveals that the ternary blend is vertically phase separated with the C -SAM at the bottom and the BHJ on top. The average power conversion efficiency - of OPVs based on the ternary system is improved from 14.

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Fundamental mechanisms underlying exciton formation in organic semiconductors are complex and elusive as it occurs on ultrashort sub-100-fs timescales. Some fundamental aspects of this process, such as the evolution of exciton binding energy, have not been resolved in time experimentally. Here, we apply a combination of sub-10-fs Pump-Push-Photocurrent, Pump-Push-Photoluminescence, and Pump-Probe spectroscopies to polyfluorene devices to track the ultrafast formation of excitons.

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Additive engineering is emerging as a powerful strategy to further enhance the performance of perovskite solar cells (PSCs), with the incorporation of bulky cations and amino acid (AA) derivatives being shown as a promising strategy for enhanced device stability. However, the incorporation of such additives typically results in photocurrent losses owing to their saturated carbon backbones, hindering charge transport and collection. Here, we investigate the use of AAs with varying carbon chain lengths as zwitterionic additives to enhance the PSC device stability, in air and nitrogen, under illumination.

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Minimizing the energy offset between the lowest exciton and charge-transfer (CT) states is a widely employed strategy to suppress the energy loss () in polymer:non-fullerene acceptor (NFA) organic solar cells (OSCs). In this work, transient absorption spectroscopy is employed to determine CT state lifetimes in a series of low energy loss polymer:NFA blends. The CT state lifetime is observed to show an inverse energy gap law dependence and decreases as the energy loss is reduced.

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We analyse organic solar cells with four different photoactive blends exhibiting differing dependencies of short-circuit current upon photoactive layer thickness. These blends and devices are analysed by transient optoelectronic techniques of carrier kinetics and densities, air photoemission spectroscopy of material energetics, Kelvin probe measurements of work function, Mott-Schottky analyses of apparent doping density and by device modelling. We conclude that, for the device series studied, the photocurrent loss with thick active layers is primarily associated with the accumulation of photo-generated charge carriers in intra-bandgap tail states.

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Recent progress in organic photovoltaics (OPVs) has been enabled by optimization of the energetic driving force for charge separation, and thus maximization of open-circuit voltage, using non-fullerene acceptor (NFA) materials. In spite of this, the carrier dynamics and relative energies of the key states controlling the photophysics of these systems are still under debate. Herein, we report an in-depth ultrafast spectroscopic study of a representative OPV system based on a polymer donor PffBT4T-2OD and a small-molecule NFA EH-IDTBR.

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In this work we lay out design guidelines for catalytically more efficient organic photocathodes achieving stable hydrogen production in neutral pH. We propose an organic photocathode architecture employing a NiO hole selective layer, a PCDTBT:PCBM bulk heterojunction, a compact TiO2 electron selective contact and a RuO2 nanoparticle catalyst. The role of each layer is discussed in terms of durability and function.

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Article Synopsis
  • - The study compares the charge carrier dynamics and device performance of the low band gap polymer PBDTTT-CT when blended with two different acceptors: PC71BM (a fullerene) and a PDI derivative with similar electron affinities.
  • - Both blends show efficient and ultrafast charge separation, with time constants of 1.6 ps for PC71BM and 1.4 ps for the PDI derivative, indicating similar initial charge dynamics.
  • - However, the PDI acceptor leads to lower device performance (1.75%) compared to PC71BM (3.5%) due to slower charge transport and increased recombination losses during charge collection.
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Three organic or hybrid photovoltaic technologies are compared with respect to performance and stability under the harsh regime of concentrated light. Although all three technologies show surprisingly high (and linear) photocurrents, and better than expected stability, no golden apples are awarded.

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Thieno[3,2-b]thienobis(silolothiophene), a new electron rich hexacyclic monomer has been synthesized and incorporated into three novel donor-acceptor low-bandgap polymers. By carefully choosing the acceptor co-monomer, the energy levels of the polymers could be modulated and high power conversion efficiencies of 5.52% were reached in OPV devices.

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We report the synthesis and polymerization of a novel thieno[3,2-b]thiophene-diketopyrrolopyrrole-based monomer. Copolymerization with thiophene afforded a polymer with a maximum hole mobility of 1.95 cm(2) V(-1) s(-1), which is the highest mobility from a polymer-based OFET reported to date.

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