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Journal articleCalado P, Telford AM, Bryant D, et al., 2016,
Evidence for ion migration in hybrid perovskite solar cells with minimal hysteresis
, Nature Communications, Vol: 7, ISSN: 2041-1723Ionic migration has been proposed as a possible cause of photovoltaic current-voltage hysteresis in hybrid perovskite solar cells. A major objection to this hypothesis is that hysteresis can be reduced by changing the interfacial contact materials; this is unlikely to significantly influence the behaviour of mobile ionic charge within the perovskite phase. Here we show that the primary effects of ionic migration can in fact be observed regardless of whether the contacts were changed to give devices with or without significant hysteresis. Transient optoelectronic measurements combined with device simulations indicate that electric-field screening, consistent with ionic migration, is similar in both high and low hysteresis CH3NH3PbI3 cells. Simulation of the photovoltage and photocurrent transients shows that hysteresis requires the combination of both mobile ionic charge and recombination near the perovskite-contact interfaces. Passivating contact recombination results in higher photogenerated charge concentrations at forward bias which screen the ionic charge, reducing hysteresis.
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Journal articleBarnes PRF, Vaissier V, Garcia Sakai V, et al., 2016,
How mobile are dye adsorbates and acetonitrile molecules on the surface of TiO2 nanoparticles? A quasi-elastic neutron scattering study
, Scientific Reports, Vol: 6, ISSN: 2045-2322Motions of molecules adsorbed to surfaces may control the rate of charge transport within monolayers in systems such as dye sensitized solar cells. We used quasi-elastic neutron scattering (QENS) to evaluate the possible dynamics of two small dye moieties, isonicotinic acid (INA) and bis-isonicotinic acid (BINA), attached to TiO2 nanoparticles via carboxylate groups. The scattering data indicate that moieties are immobile and do not rotate around the anchoring groups on timescales between around 10 ps and a few ns (corresponding to the instrumental range). This gives an upper limit for the rate at which conformational fluctuations can assist charge transport between anchored molecules. Our observations suggest that if the conformation of larger dye molecules varies with time, it does so on longer timescales and/or in parts of the molecule which are not directly connected to the anchoring group. The QENS measurements also indicate that several layers of acetonitrile solvent molecules are immobilized at the interface with the TiO2 on the measurement time scale, in reasonable agreement with recent classical molecular dynamics results.
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Journal articleLoheeswaran S, Thanihaichelvan M, Ravirajan P, et al., 2016,
Controlling recombination kinetics of hybrid poly-3-hexylthiophene (P3HT)/titanium dioxide solar cells by self-assembled monolayers
, JOURNAL OF MATERIALS SCIENCE-MATERIALS IN ELECTRONICS, Vol: 28, Pages: 4732-4737, ISSN: 0957-4522 -
Journal articleBaran D, Ashraf RS, Hanifi DA, et al., 2016,
Reducing the efficiency-stability-cost gap of organic photovoltaics with highly efficient and stable small molecule acceptor ternary solar cells
, Nature Materials, Vol: 16, Pages: 363-369, ISSN: 1476-4660Technological deployment of organic photovoltaic modules requires improvements in device light-conversion efficiency and stability while keeping material costs low. Here we demonstrate highly efficient and stable solar cells using a ternary approach, wherein two non-fullerene acceptors are combined with both a scalable and affordable donor polymer, poly(3-hexylthiophene) (P3HT), and a high-efficiency, low-bandgap polymer in a single-layer bulk-heterojunction device. The addition of a strongly absorbing small molecule acceptor into a P3HT-based non-fullerene blend increases the device efficiency up to 7.7 ± 0.1% without any solvent additives. The improvement is assigned to changes in microstructure that reduce charge recombination and increase the photovoltage, and to improved light harvesting across the visible region. The stability of P3HT-based devices in ambient conditions is also significantly improved relative to polymer:fullerene devices. Combined with a low-bandgap donor polymer (PBDTTT-EFT, also known as PCE10), the two mixed acceptors also lead to solar cells with 11.0 ± 0.4% efficiency and a high open-circuit voltage of 1.03 ± 0.01 V.
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Journal articleFallon KJ, Wijeyasinghe N, Manley EF, et al., 2016,
Indolo-naphthyridine-6,13-dione Thiophene Building Block for Conjugated Polymer Electronics: Molecular Origin of Ultrahigh n-Type Mobility
, CHEMISTRY OF MATERIALS, Vol: 28, Pages: 8366-8378, ISSN: 0897-4756 -
Journal articleSandwell P, Chambon C, Saraogi A, et al., 2016,
Analysis of energy access and impact of modern energy sources in unelectrified villages in Uttar Pradesh
, Energy for Sustainable Development, Vol: 35, Pages: 67-79, ISSN: 0973-0826Bringingaccesstomodernenergysourcestothepoorestinsocietyisakeygoalofmanypolicymakers,businessesandcharities,butinorder tobea success projects and schemesmust be foundedonaccuratedata. We undertooka survey of energy demand and usage patterns in households in unelectrified villages in Uttar Pradesh, India toassess access to and utilisation of energy sources for lighting and cooking. The times of usage were recordedand analysed and the effect on usage patterns of transitioning from traditional to modern energy sourcesis assessed. We quantify the cost and greenhouse gas emissions of current energy use in order to provide abenchmark of potential mitigation through the use of renewable energy technologies: a typical householdwith kerosene lamps only for lighting spends INR 3243 (US$50.67) and emits 381 kgCO2eqper year; householdswithmoderncookingenergyspend17%morethroughincreasedusage,butemit28%lessgreenhousegasescom-pared to those with traditional stoves only. Cell phone ownership was found to be 50% amongst adults. We usedemographic and utilisation data to construct an hourly demand profile of basic electricity demand extrapolatedto each month of the year, and present an example of aspirational demand assess the impact of desirable appli-ances. A Monte Carlo simulation is used to highlight the daily and seasonal variation in total energy and powerdemand. A hybrid system, with solar power and battery storage meeting daytime demand and higher-capacitydiesel- or biomass-powered generation meeting the remainder during evening peaks and winter months,would satisfy demand most effectively.
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Journal articleMoia D, Szumska A, Vaissier V, et al., 2016,
Interdye Hole Transport Accelerates Recombination in Dye Sensitized Mesoporous Films
, Journal of the American Chemical Society, Vol: 138, Pages: 13197-13206, ISSN: 1520-5126Charge recombination between oxidized dyes attached to mesoporous TiO2 and electrons in the TiO2 was studied in inert electrolytes using transient absorption spectroscopy. Simultaneously, hole transport within the dye monolayers was monitored by transient absorption anisotropy. The rate of recombination decreased when hole transport was inhibited selectively, either by decreasing the dye surface coverage or by changing the electrolyte environment. From Monte Carlo simulations of electron and hole diffusion in a particle, modeled as a cubic structure, we identify the conditions under which hole lifetime depends on the hole diffusion coefficient for the case of normal (disorder free) diffusion. From simulations of transient absorption and transient absorption anisotropy, we find that the rate and the dispersive character of hole transport in the dye monolayer observed spectroscopically can be explained by incomplete coverage and disorder in the monolayer. We show that dispersive transport in the dye monolayer combined with inhomogeneity in the TiO2 surface reactivity can contribute to the observed stretched electron-hole recombination dynamics and electron density dependence of hole lifetimes. Our experimental and computational analysis of lateral processes at interfaces can be applied to investigate and optimize charge transport and recombination in solar energy conversion devices using electrodes functionalized with molecular light absorbers and catalysts.
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Conference paperEkins-Daukes NJ, Sandwell P, Nelson J, et al., 2016,
What does CPV need to achieve in order to succeed?
, 12th International Conference on Concentrator Photovoltaic Systems (CPV), Publisher: American Institute of Physics, ISSN: 0094-243XThe recent and dramatic reduction in flat-plate crystalline silicon (c-Si) technology has changed the competitive land-scape for concentrator PV (CPV) systems. Three system cost targets are considered, €1/Wp corresponding to the system cost of c-Si today, €0.75/Wp corresponding to the likely c-Si cost in 2020 and €0.5/Wp corresponding to a likely lower limit for c-Si in the long term. To compete successfully with c-Si, system efficiency needs to be raised from the present 30% to 40%, suggesting cell efficiencies of 50% and module efficiency of 44%. The module should be manufactured at an area cost below €275/m2 which implies a packaged cell cost of €3/cm2 and module + tracking cost €190/m2.
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Journal articleVella E, Li H, Grégoire P, et al., 2016,
Ultrafast decoherence dynamics govern photocarrier generation efficiencies in polymer solar cells
, Scientific Reports, Vol: 6, ISSN: 2045-2322All-organic-based photovoltaic solar cells have attracted considerable attention because of their lowcostprocessing and short energy payback time. In such systems the primary dissociation of an opticalexcitation into a pair of photocarriers has been recently shown to be extremely rapid and efficient,but the physical reason for this remains unclear. Here, two-dimensional photocurrent excitationspectroscopy, a novel non-linear optical spectroscopy, is used to probe the ultrafast coherent decayof photoexcitations into charge-producing states in a polymer:fullerene based solar cell. The twodimensionalphotocurrent spectra are interpreted by introducing a theoretical model for the descriptionof the coupling of the electronic states of the system to an external environment and to the appliedlaser fields. The experimental data show no cross-peaks in the twodimensional photocurrent spectra, aspredicted by the model for coherence times between the exciton and the photocurrent producing statesof 20fs or less.
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Journal articleSandwell P, Duggan G, Nelson J, et al., 2016,
The environmental impact of lightweight HCPV modules: efficient design and effective deployment
, Progress in Photovoltaics, Vol: 24, Pages: 1458-1472, ISSN: 1099-159XWe present a life cycle analysis of a lightweight design of high concentration photovoltaic module. The materials and processes used in construction are considered to assess the total environmental impact of the module construction in terms of the cumulative energy demand and embodied greenhouse gas emissions, which were found to be 355.3MJ and 27.9 kgCO2eq respectively. We consider six potential deployment locations and the system energy payback times are calculated to be 0.22–0.33 years whilst the greenhouse gas payback times are 0.29–0.88 years. The emission intensities over the life- times of the systems are found to be 6.5–9.8 g CO2eq/kWh, lower than those of other HCPV, PV and CSP technologies in similar locations.
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Journal articleVezie M, Few S, Meager I, et al., 2016,
Exploring the origin of high optical absorption in conjugated polymers
, Nature Materials, Vol: 15, Pages: 746-753, ISSN: 1476-4660The specific optical absorption of an organic semiconductor is critical to the performance of organic optoelectronic devices. For example, higher light-harvesting efficiency can lead to higher photocurrent in solar cells that are limited by sub-optimal electrical transport. Here, we compare over 40 conjugated polymers, and find that many different chemical structures share an apparent maximum in their extinction coefficients. However, a diketopyrrolopyrrole-thienothiophene copolymer shows remarkably high optical absorption at relatively low photon energies. By investigating its backbone structure and conformation with measurements and quantum chemical calculations, we find that the high optical absorption can be explained by the high persistence length of the polymer. Accordingly, we demonstrate high absorption in other polymers with high theoretical persistence length. Visible light harvesting may be enhanced in other conjugated polymers through judicious design of the structure.
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Journal articleLeguy AM, Goñi AR, Frost JM, et al., 2016,
Dynamic disorder, phonon lifetimes, and the assignment of modes to the vibrational spectra of methylammonium lead halide perovskites
, Physical Chemistry Chemical Physics, Vol: 18, Pages: 27051-27066, ISSN: 1463-9084We present Raman and terahertz absorbance spectra of methylammonium lead halide single crystals (MAPbX3, X = I, Br, Cl) at temperatures between 80 and 370 K. These results show good agreement with density-functional-theory phonon calculations. Comparison of experimental spectra and calculated vibrational modes enables confident assignment of most of the vibrational features between 50 and 3500 cm(-1). Reorientation of the methylammonium cations, unlocked in their cavities at the orthorhombic-to-tetragonal phase transition, plays a key role in shaping the vibrational spectra of the different compounds. Calculations show that these dynamic effects split Raman peaks and create more structure than predicted from the independent harmonic modes. This explains the presence of extra peaks in the experimental spectra that have been a source of confusion in earlier studies. We discuss singular features, in particular the torsional vibration of the C-N axis, which is the only molecular mode that is strongly influenced by the size of the lattice. From analysis of the spectral linewidths, we find that MAPbI3 shows exceptionally short phonon lifetimes, which can be linked to low lattice thermal conductivity. We show that optical rather than acoustic phonon scattering is likely to prevail at room temperature in these materials.
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Journal articleTuladhar SM, Azzouzi M, Delval F, et al., 2016,
Low Open-Circuit Voltage Loss in Solution Processed Small Molecule Organic Solar Cells
, ACS Energy Letters, Vol: 1, Pages: 302-308, ISSN: 2380-8195 -
Journal articleGambhir A, Sandwell P, Nelson J, 2016,
The future costs of OPV - A bottom-up model of material and manufacturing costs with uncertainty analysis
, Solar Energy Materials and Solar Cells, Vol: 156, Pages: 49-58, ISSN: 0927-0248Organic photovoltaic (OPV) technology has the potential to provide cheap solar electricity, given advances in low-cost production and module efficiency and lifetime. However, several uncertainties remain in terms of the future costs of OPV modules, which depend on future material and manufacturing costs, as well as key performance characteristics. This assessment takes an engineering-based approach to assessing the potential future cost of each component of OPV modules, as well as the future scale of OPV production plants and associated scale economies, using stochastic analysis to account for uncertainty. The analysis suggests that OPV module costs could fall within a (interquartile) range of US$0.23–0.34/Wp, with a median cost estimate of US$0.28/Wp in the near-term, with future costs most sensitive to manufacturing scale, cell efficiency and module fill factor. This compares to a projected range of module costs for more established PV technologies (crystalline silicon, cadmium telluride and copper indium gallium selenide) of US$0.35–0.6/Wp by 2020. In levelised cost of electricity terms, OPV could compete with the established technologies in both roof- and ground-mounted systems if it can achieve a 10-year lifetime.
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Journal articleGuilbert AA, Zbiri M, Jenart MV, et al., 2016,
New insights into the molecular dynamics of P3HT:PCBM bulk heterojunction: a time-of-flight quasi-elastic neutron scattering study
, Journal of Physical Chemistry Letters, Vol: 7, Pages: 2252-2257, ISSN: 1948-7185The molecular dynamics of organic semiconductor blend layers are likely to affect the optoelectronic properties and the performance of devices such as solar cells. We study the dynamics (5-50 ps) of the poly(3-hexylthiophene) (P3HT): phenyl-C61-butyric acid methyl ester (PCBM) blend by time-of-flight quasi-elastic neutron scattering, at temperatures in the range 250-360 K, thus spanning the glass transition temperature region of the polymer and the operation temperature of an OPV device. The behavior of the QENS signal provides evidence for the vitrification of P3HT upon blending, especially above the glass transition temperature, and the plasticization of PCBM by P3HT, both dynamics occurring on the picosecond time scale.
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Journal articleSandwell P, Chan NLA, Foster S, et al., 2016,
Off-grid solar photovoltaic systems for rural electrification and emissions mitigation in India
, Solar Energy Materials and Solar Cells, Vol: 156, Pages: 147-156, ISSN: 0927-0248Over one billion people lack access to electricity and many of them in rural areas far from existing infrastructure. Off-grid systems can provide an alternative to extending the grid network and using renewable energy, for example solar photovoltaics (PV) and battery storage, can mitigate greenhouse gas emissions from electricity that would otherwise come from fossil fuel sources. This paper presents a model capable of comparing several mature and emerging PV technologies for rural electrification with diesel generation and grid extension for locations in India in terms of both the levelised cost and lifecycle emissions intensity of electricity. The levelised cost of used electricity, ranging from $0.46–1.20/kWh, and greenhouse gas emissions are highly dependent on the PV technology chosen, with battery storage contributing significantly to both metrics. The conditions under which PV and storage becomes more favourable than grid extension are calculated and hybrid systems of PV, storage and diesel generation are evaluated. Analysis of expected price evolutions suggest that the most cost-effective hybrid systems will be dominated by PV generation around 2018.
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Journal articleKirchartz T, Nelson J, Rau U, 2016,
Reciprocity between Charge Injection and Extraction and Its Influence on the Interpretation of Electroluminescence Spectra in Organic Solar Cells
, PHYSICAL REVIEW APPLIED, Vol: 5, ISSN: 2331-7019 -
Journal articleLeguy AMA, Azarhoosh P, Alonso MI, et al., 2016,
Experimental and theoretical optical properties of methylammonium lead halide perovskites
, Nanoscale, Vol: 8, Pages: 6317-6327, ISSN: 2040-3372The optical constants of methylammonium lead halide single crystals CH3NH3PbX3 (X = I, Br, Cl) are interpreted with high level ab initio calculations using the relativistic quasiparticle self-consistent GW approximation (QSGW). Good agreement between the optical constants derived from QSGW and those obtained from spectroscopic ellipsometry enables the assignment of the spectral features to their respective inter-band transitions. We show that the transition from the highest valence band (VB) to the lowest conduction band (CB) is responsible for almost all the optical response of MAPbI3 between 1.2 and 5.5 eV (with minor contributions from the second highest VB and the second lowest CB). The calculations indicate that the orientation of [CH3NH3]+ cations has a significant influence on the position of the bandgap suggesting that collective orientation of the organic moieties could result in significant local variations of the optical properties. The optical constants and energy band diagram of CH3NH3PbI3 are then used to simulate the contributions from different optical transitions to a typical transient absorption spectrum (TAS).
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Journal articleEmmott CJM, Moia D, Sandwell P, et al., 2016,
In-situ, long-term operational stability of organic photovoltaics for off-grid applications in Africa
, Solar Energy Materials and Solar Cells, Vol: 149, Pages: 284-293, ISSN: 0927-0248 -
Journal articleBen Dkhil S, Gaceur M, Dachraoui W, et al., 2016,
P-type semiconductor surfactant modified zinc oxide nanorods for hybrid bulk heterojunction solar cells
, Solar Energy Materials and Solar Cells, Vol: 159, Pages: 608-616, ISSN: 0927-0248In this work, hybrid bulk heterojunction solar cells based on surfactant-modified zinc oxide nanorods (ZnO NRs) blended with poly-(3-hexylthiophene) (P3HT) are presented. (E)-2-cyano-3-(5′-(4-(dibutylamino)styryl)-2,2′-bithiophen-5-yl)acrylic acid (1), a p-type semiconductor, is used as grafted interfacial surfactant on ZnO NRs, named 1-ZnO NRs, in order to improve simultaneously the nanoscale morphology of the hybrid polymer blend as well as the electronic properties of the heterojunction interface. Our studies reveal that the ligand modification of ZnO NRs leads to strongly improved aggregate free P3HT/ZnO blends that show five time increased power conversion efficiency and corresponding photo-generated charge carrier transport compared to untreated ZnO NRs. From transient absorption spectroscopy, it was found that recombination kinetics were similar in the device using untreated ZnO and modified 1-ZnO NRs, respectively, pointing to a major impact of the ligand in the improvement of the blend morphology. Corresponding device optimization led to improvements of FF and Voc to values comparable to P3HT blends using fullerene acceptors, but photocurrent density of the P3HT/1-ZnO solar cells was found low even after optimization. The latter could be addressed to destruction of long range organization of P3HT induced by the presence of the ZnO NRs as well as low electron transport inside the blend.
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Conference paperHayes SC, Pieridou G, Vezie M, et al., 2016,
Effect of molecular weight on the vibronic structure of a diketopyrrolopyrrole polymer
, Conference on Physical Chemistry of Interfaces and Nanomaterials XV, Publisher: SPIE-INT SOC OPTICAL ENGINEERING, ISSN: 0277-786X -
Journal articleVaissier V, Frost JM, Barnes PRF, et al., 2015,
Influence of Intermolecular Interactions on the Reorganization Energy of Charge Transfer between Surface-Attached Dye Molecules
, JOURNAL OF PHYSICAL CHEMISTRY C, Vol: 119, Pages: 24337-24341, ISSN: 1932-7447The parameters controlling the kinetics ofintermolecular charge transfer are traditionally estimatedfrom electronic structure calculations on the charge donorand charge acceptor in isolation. Here, we show that thisprocedure results in inaccuracies for hole transfer between apair of organic dye molecules by comparing charge-constraineddensity functional theory (DFT) calculations on a dyecation/neutral dye pair to the conventional DFT calculationson the isolated molecules. We quantify the error made in thereorganization energy of hole exchange between dye molecules(λi). We choose three indolene-based organic dyes with application to dye-sensitized solar cells, namely, D149, D102, and D131,for which experimental values of λ are available. We find that, although highly system dependent, the intermolecular interactionbetween the charge donor and acceptor can lead to a 0.25 eV change in λi, illustrating the limitations of the widely used originalmethod in predicting the rate of charge transfer.
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Journal articleGuilbert AAY, Urbina A, Abad J, et al., 2015,
Temperature-dependent dynamics of polyalkylthiophene conjugated polymers: a combined neutron scattering and simulation study
, Chemistry of Materials, Vol: 27, Pages: 7652-7661, ISSN: 1520-5002The dynamics of conjugated polymers are known to influence the performance of optoelectronic devices. Polyalkylthiophenes are a widely studied class of conjugated polymers, which exhibit a glass transition around room temperature and consequently are sensitive to temperature variations. We studied the dynamics of two polyalkylthiophenes of different side chain lengths (hexyl and octyl) as a function of temperature, by comparing their quasi-elastic neutron scattering (QENS) with molecular dynamics simulations (MD). We found a good agreement between the simulated and experimental data within the explored time window (of ∼4 ns), demonstrating that the force fields used in MD simulations are appropriate and that the QENS technique can be used as a validation of such force fields. Using MD allows us to identify and to assign contributions to the QENS signal from different parts of the polymers and to determine the activation energies of the different motions.
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Journal articleMoia D, Leijtens T, Noel N, et al., 2015,
Dye Monolayers Used as the Hole Transporting Medium in Dye-Sensitized Solar Cells
, ADVANCED MATERIALS, Vol: 27, Pages: 5889-5894, ISSN: 0935-9648- Author Web Link
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- Citations: 20
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Journal articleWheeler, Deledalle F, Tokmoldin N, et al., 2015,
Influence of Surface Recombination on Charge-Carrier Kinetics in Organic Bulk Heterojunction Solar Cells with Nickel Oxide Interlayers
, Physical review applied, Vol: 4, ISSN: 2331-7019The choice of electrode for organic photovoltaics is known to be of importance to both device stability and performance, especially regarding the open-circuit voltage (VOC). Here we show that the work function of a nickel oxide anode, varied using an O2 plasma treatment, has a considerable influence on the open-circuit voltage VOC of an organic solar cell. We probe recombination in the devices using transient photovoltage and charge extraction to determine the lifetime as a function of charge-carrier concentration and compare the experimental results with numerical drift-diffusion simulations. This combination of experiment and simulations allows us to conclude that the variations in VOC are due to a change in surface recombination, localized at the NiO anode, although only a small change in carrier lifetime is observed.
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Journal articleBaran D, Vezie MS, Gasparini N, et al., 2015,
Role of Polymer Fractionation in Energetic Losses and Charge Carrier Lifetimes of Polymer: Fullerene Solar Cells
, JOURNAL OF PHYSICAL CHEMISTRY C, Vol: 119, Pages: 19668-19673, ISSN: 1932-7447- Author Web Link
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- Citations: 20
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Journal articleMoia D, Cappel UB, Leijtens T, et al., 2015,
The Role of Hole Transport between Dyes in Solid-State Dye-Sensitized Solar Cells
, Journal of Physical Chemistry C, Vol: 119, Pages: 18975-18985, ISSN: 1932-7447 -
Journal articleYao J, Kirchartz T, Vezie MS, et al., 2015,
Quantifying losses in open-circuit voltage in solution-processable solar cells
, Physical Review Applied, Vol: 4, ISSN: 2331-7019The maximum open-circuit voltage of a solar cell can be evaluated in terms of its ability to emit light. We herein verify the reciprocity relation between the electroluminescence spectrum and subband-gap quantum efficiency spectrum for several photovoltaic technologies at different stages of commercial development, including inorganic, organic, and a type of methyl-ammonium lead- halide CH3NH3PbI3−xClx perovskite solar cells. Based on the detailed balance theory and reciprocity relations between light emission and light absorption, voltage losses at open circuit are quantified and assigned to specific mechanisms, namely, absorption edge broadening and nonradiative recombination. The voltage loss due to nonradiative recombination is low for inorganic solar cells (0.04–0.21 V), while for organic solar cell devices it is larger but surprisingly uniform, with values of 0.34–0.44 V for a range of material combinations. We show that, in CH3NH3PbI3−xClx perovskite solar cells that exhibit hysteresis, the loss to nonradiative recombination varies substantially with voltage scan conditions. We then show that for different solar cell technologies there is a roughly linear relation between the power conversion efficiency and the voltage loss due to nonradiative recombination.
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Journal articleLeguy AMA, Frost JM, McMahon AP, et al., 2015,
Corrigendum: The dynamics of methylammonium ions in hybrid organic–inorganic perovskite solar cells
, Nature Communications, Vol: 6, ISSN: 2041-1723 -
Journal articleLeguy AMA, Frost JM, McMahon AP, et al., 2015,
The dynamics of methylammonium ions in hybrid organic-inorganic perovskite solar cells
, Nature Communications, Vol: 6, ISSN: 2041-1723Methylammonium lead iodide perovskite can make high-efficiency solar cells, which also show an unexplained photocurrent hysteresis dependent on the device-poling history. Here we report quasielastic neutron scattering measurements showing that dipolar CH3NH3+ ions reorientate between the faces, corners or edges of the pseudo-cubic lattice cages in CH3NH3PbI3 crystals with a room temperature residence time of ~14 ps. Free rotation, π-flips and ionic diffusion are ruled out within a 1–200-ps time window. Monte Carlo simulations of interacting CH3NH3+ dipoles realigning within a 3D lattice suggest that the scattering measurements may be explained by the stabilization of CH3NH3+ in either antiferroelectric or ferroelectric domains. Collective realignment of CH3NH3+ to screen a device’s built-in potential could reduce photovoltaic performance. However, we estimate the timescale for a domain wall to traverse a typical device to be ~0.1–1 ms, faster than most observed hysteresis.
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