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The optical, electrochemical, morphological and transport properties of a series of thiadiazinone (acceptor) and (thienyl)carbazoles (donor) containing π-extended donor-acceptor-donors (D-A-D) are presented. Systematic variations in the number of the thienyl units, the choice of branched or straight alkyl side chains and the use of a processing additive demonstrate their use as electron donors in bulk heterojunction solar cells blended with fullerene acceptors. The best power conversion efficiency (PCE) of 2.7% is achieved by adding to the D-A-D 3:fullerene blend a polydimethylsiloxane (PDMS) additive, that improves the morphology and doubles the hole mobility within the D-A-D:fullerene blend. © The Royal Society of Chemistry. 3 10 2358 2365 Cited By :7

The photovoltaic performance of blends of a series of 4,4′-Difluoro-4-bora-3a,4a-diaza-s-indacenes)-based (BODIPY) conjugated polymers donors with fullerene electron acceptors is investigated. Despite the high Voc values observed, solar cell device yields relatively low power conversion efficiencies. Our study takes into account the materials’ structure-property relationship, light harvesting capabilities, charge transport, collection properties and morphological characteristics to elucidate factors affecting the photovoltaic performance in this class of polymers. We show that elimination of low molecular weight species and suitable electrodes for hole collection can be used to overcome some of the observed limitations on photovoltaic performance. © 2017 Elsevier B.V. 226 25 30

A systematic investigation of Förster resonant energy transfer (FRET) is reported within a hybrid prototype structure based on nitride single quantum well (SQW) donors and light emitting polymer acceptors. Self-consistent Schrödinger-Poisson modeling and steady-state and time-resolved photoluminescence experiments were initially employed to investigate the influence of a wide structural parameter space on the emission quantum yield of the nitride component. The optimized SQW heterostructures were processed into hybrid structures with spin-casted overlayers of polyfluorenes. The influence of important unexplored aspects of the inorganic heterostructure such as SQW confinement, content, and doping on the dipole-dipole coupling was probed. Competing mechanisms to the FRET process associated with interfacial recombination and charge transfer have been studied and their implications to device applications exploiting FRET across heterointerfaces have been discussed. © 2015 AIP Publishing LLC. 143 21 Cited By :2

We report an optical investigation of conjugated polymer (P3HT)/fullerene (PCBM) semiconductor blends sensitized by near-infrared absorbing quantum dots (PbS QDs). A systematic series of samples that include pristine, binary and ternary blends of the materials are studied using steadystate absorption, photoluminescence (PL) and ultrafast transient absorption. Measurements show an enhancement of the absorption strength in the near-infrared upon QD incorporation. PL quenching of the polymer and the QD exciton emission is observed and predominantly attributed to intermaterial photoinduced charge transfer processes. Pump-probe experiments show photo-excitations to relax via an initial ultrafast decay while longer-lived photoinduced absorption is attributed to charge transfer exciton formation and found to depend on the relative ratio of QDs to P3HT:PCBM content. PL experiments and transient absorption measurements indicate that interfacial charge transfer processes occur more efficiently at the fullerene/polymer and fullerene/nanocrystal interfaces compared to polymer/nanocrystal interfaces. Thus the inclusion of the fullerene seems to facilitate exciton dissociation in such blends. The study discusses important and rather unexplored aspects of exciton recombination and charge transfer processes in ternary blend composites of organic semiconductors and near-infrared quantum dots for applications in solution-processed photodetectors and solar cells. © 2011 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim. 1 5 802 812 Cited By :56

We report the processing conditions for inkjet-printed active layers of organic photovoltaic (OPV) devices comprising bulk-heterojunction blends of the low bandgap conjugated polymer poly[(4,4′-bis(2-ethylhexyl)dithieno[3,2-b: 2′,3′-d]silole)-2,6-diyl-alt-(4,7-bis(2-thienyl)-2,1, 3-benzothiadiazole)-5,5′-diyl] (Si-PCPDTBT) as well as poly[N-9′-hepta-decanyl-2,7-carbazole-alt-5,5-(4′, 7′-di-2-thienyl-2′,1′,3′-benzothiadiazole)] (PCDTBT) used as electron donors with [6,6]-phenyl-C71-butyric acid methyl ester (PC 70BM) as electron acceptor. By controlling the inkjet printing processing conditions, we gain a significant improvement in device power conversion efficiency (PCE) to previously reported work using these materials. We obtain Si-PCPDTBT:fullerene and PCDTBT:fullerene-based inkjet-printed OPVs with power conversion efficiency of ~3% and ~4%, respectively. © 2014 Elsevier B.V. 130 474 480 Cited By :10

A series of synthesized small organic molecules based on the 4H-1,2,6-thiadiazine moiety are studied using electrochemistry, to probe their potential as comonomer building blocks for solar-absorbing polymers for organic solar cells. This is the first instance of an electrochemical report for this family of heterocycles. Structure-physical property relationships are identified that can guide future synthetic efforts. Parameters that can influence the properties of the final copolymer such as the choice of electron donor comonomer and the energy level of the fullerene adduct acceptor are factored-in and discussed and the thiadiazines that can meet the requirements are singled-out. © 2013 Elsevier Ltd. All rights reserved. 107 448 453 Cited By :5

Electronic and interface properties of spin-coated poly(9,9- dioctylfluorenyl-2,7-diyl) (PFO) films on GaN have been investigated in terms of their potential for optoelectronic applications. The PFO/GaN interface was studied by photoemission spectroscopy showing a type-II energy alignment with band offsets suitable for efficient photocurrent generation. The light harvesting potential is further supported by fluorescence experiments that show evidence of photo-induced electron transfer from PFO to GaN. The impact of polymer film thickness was probed using emission anisotropy and ellipsometry, indicating the presence of an ordered planar phase of PFO. The study has implications to hybrid optoelectronic devices employing the two important materials. © 2013 American Institute of Physics. 102 6 Cited By :4

Five new polymers based on the 4,4'-difluoro-4-bora-3a,4a-diaza-s-indacene core (BODIPY) chromophore moiety have been synthesized as low bandgap polymers for optoelectronic applications. The polymers exhibited high solubility in common organic solvents and optical bandgaps ranging from 1.7-2 eV. The materials were characterized using NMR, UV-Vis, steady state and time-resolved photoluminescence and the energy levels were examined using electrochemistry and validated using quantum chemical calculations. Finally, a representative BODIPY derivative : PCBM blend was examined in terms of photovoltaic properties. Preliminary device performance parameters as a function of photo-active layer thickness and composition are reported and discussed, relating to power conversion efficiency values. © The Royal Society of Chemistry 2013. 3 26 10221 10229

1 online ID: 467 In: ADVANCED ENERGY MATERIALS volume 3 issue 11 page 1490. Summary: Abstract The photophysics of bulk heterojunctions of a high‐performance, low‐gap silicon‐bridged dithiophene polymer with oleic acid capped PbS quantum dots (QDs) are studied to assess the material potential for light harvesting in the visible‐ and IR‐light ranges. By employing a wide range of nanocrystal sizes, systematic dependences of electron and hole transfer on quantum‐dot size are established for the first time on a low‐gap polymer–dot system. The studied system exhibits type II band offsets for dot sizes up to ca. 4 nm, whch allow fast hole transfer from the quantum dots to the polymer that competes favorably with the intrinsic QD recombination. Electron transfer from the polymer is also observed although it is less competitive with the fast polymer exciton recombination for most QD sizes studied. The incorporation of a fullerene derivative provides efficient electron‐quenching sites that improve interfacial polymer‐exciton dissociation in ternary polymer–fullerene–QD blends. The study indicates that programmable band offsets that allow both electron and hole extraction can be produced for efficient light harvesting based on this low‐gap polymer‐PbS QD composite..

The photophysics of bulk heterojunctions of a high-performance, low-gap silicon-bridged dithiophene polymer with oleic acid capped PbS quantum dots (QDs) are studied to assess the material potential for light harvesting in the visible- and IR-light ranges. By employing a wide range of nanocrystal sizes, systematic dependences of electron and hole transfer on quantum-dot size are established for the first time on a low-gap polymer-dot system. The studied system exhibits type II band offsets for dot sizes up to ca. 4 nm, whch allow fast hole transfer from the quantum dots to the polymer that competes favorably with the intrinsic QD recombination. Electron transfer from the polymer is also observed although it is less competitive with the fast polymer exciton recombination for most QD sizes studied. The incorporation of a fullerene derivative provides efficient electron-quenching sites that improve interfacial polymer-exciton dissociation in ternary polymer-fullerene-QD blends. The study indicates that programmable band offsets that allow both electron and hole extraction can be produced for efficient light harvesting based on this low-gap polymer-PbS QD composite. © 2013 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim. 3 11 1490 1499 Cited By :18

We report on excitation dynamics in pristine and bulk heterojunction films of the low bandgap silicon-bridged dithiophene copolymer poly[(4,4′-bis(2- ethylhexyl)dithieno[3,2-b:2′, 3′-d]silole)-2,6-diyl-alt-(4,7-bis(2- thienyl)-2,1,3-benzothiadiazole)-5,5′-diyl] with methanofullerene derivatives. The combination of ultrafast transient transmission and photoluminescence allows us to probe the relaxation of both exciton and polaron states in a relatively wide spectral and temporal range. Measurements reveal that the majority of excitations undergo ultrashort non-radiative relaxation while a small fraction of the photoexcited species decays slowly within hundreds of ps. In the blend films, significantly longer decays are observed suggesting the presence of long lived holes and/or charged-transfer type of excitons. © 2012 American Institute of Physics. 100 15 Cited By :3

PbS quantum dots (QDs) of different sizes capped with short (NH4)(3)AsS3 inorganic ligands are produced via ligand exchange processes from oleate-capped PbS QDs. The solid-state photophysical properties of the control organic-capped and the inorganic-ligand-capped QDs are investigated to determine their potential for optoelectronic applications. Ultrafast transient transmission shows that in the oleate-capped QDs, carrier recombination at sub-nanosecond scales occurs via Auger recombination, traps, and surface states. At longer times, intense signals associated with radiative recombination are obtained. After ligand exchange, the QDs become decorated with (NH4)(3)AsS3 complexes and relaxation is dominated by efficient carrier transfer to the ligand states on timescales as fast as approximate to 2 ps, which competes with carrier thermalization to the QD band edge states. Recombination channels present in the oleate-capped QDs, such as radiative and Auger recombination, appear quenched in the inorganic-capped QDs. Evidence of efficient carrier trapping at shallow ligand states, which appears more intense under excitation above the (NH4)(3)AsS3 gap, is provided. A detailed band diagram of the various relaxation and recombination processes is proposed that comprehensively describes the photophysics of the QD systems studied. 4 7 1301547 1301547 PT: J TC: 8 J9: ADV ENERGY MATER

The dynamics of photoexcitations in hybrid blends of poly(3-hexylthiophene) (P3HT) conjugated polymer donor and oleic-acid capped lead sulfide (PbS) quantum dot (QD) acceptors of different concentrations - for light harvesting applications - were investigated using time-resolved transmission and photoluminescence spectroscopies. Following excitation at 400 nm and probing in the 500-1000 nm region, we find that geminate excitation recombination in the blend of P3HT/PbS QDs dominates the transient decays at sub-ns times while intermaterial interactions such as charge transfer processes appear at longer times in the 1-50 ns regime. For the hybrid blend films with lower QD concentrations (Cited By :4

We have introduced the pentafluorophenyl substituted benzimidazole as a building block of conjugated polymers for optoelectronic applications. We present the synthesis of a copolymer bearing fluorene as the comonomer. A detailed characterization of the novel material including structural, electrochemical and optical (using absorption, emission and time-resolved photoluminescence techniques) properties as well as computational modeling is described. The polymer exhibits highly efficient photoluminescence quenching when blended with fullerene derivatives (PCBM). The experimental results are compared with the alternating fluorene copolymer (APFO-3) in order to identify structure and property relations with the novel synthesized conjugated polymer. Early photovoltaic performance data are presented and compared with the well established APFO-3:PCBM material system. © 2012 The Royal Society of Chemistry. 3 8 2236 2243 Cited By :10

Progress toward electrically driven conjugated polymer lasers should benefit from the identification of materials that exhibit good charge transport properties coupled with large optical gain. Here, we report a detailed study of a blue-emitting fluorene-based polymer that combines a large hole mobility with desirable stimulated emission characteristics. Laser oscillation is achieved within distributed feedback structures and leads to low threshold, tunable lasers operating in the blue spectral region. Our results establish this material as an attractive gain medium with which to try and construct a polymer laser diode. © 2006 American Institute of Physics. 88 8 Cited By :22