Investigating ultrafast carrier dynamics in perovskite solar cells with an extended π-conjugated polymeric diketopyrrolopyrrole layer for hole transportation.

Here, we show a new diketopyrrole based polymeric hole-transport material (PBDTP-DTDPP, (poly[[2,5-bis(2-hexyldecyl)-2,3,5,6-tetrahydro-3,6-dioxopyrrolo[3,4-c]pyrrole-1,4-diyl]-alt-[[2,2'-(4,8-bis(4-ethylhexyl-1-phenyl)-benzo[1,2-b:4,5-b']dithiophene)bis-thieno[3,2-b]thiophen]-5,5'-diyl]])) for application in perovskite solar cells. The material performance was tested in a solar cell with an optimized configuration, FTO/SnO2/perovskite/PBDTP-DTDPP/Au, and the device showed a power conversion efficiency of 14.78%. The device charge carrier dynamics were investigated using transient absorption spectroscopy. The charge separation and recombination kinetics were determined in a device with PBDTP-DTDPP and the obtained results were compared to a reference device. We find that PBDTP-DTDPP enables similar charge separation time (<∼4.8 ps) to the spiro-OMeTAD but the amount of nongeminate recombination is different. Specifically, we find that the polymeric PBDTP-DTDPP hole-transport layer (HTL) slows-down the second-order recombination much less than spiro-OMeTAD. This effect is of particular importance in studying the charge transportation in optimized solar cell devices with diketopyrrole based HTL materials.

Systematic control of experimental inconsistency in combinatorial materials science.

We developed a method to systematically control experimental inconsistency, which is one of the most troublesome and difficult problems in high-throughput combinatorial experiments. The topic of experimental inconsistency is never addressed, even though all scientists in the field of combinatorial materials science face this very serious problem. Experimental inconsistency and material property were selected as dual objective functions that were simultaneously optimized. Specifically, in an attempt to search for promising phosphors with high reproducibility, photoluminescence (PL) intensity was maximized, and experimental inconsistency was minimized by employing a multiobjective evolutionary optimization-assisted combinatorial materials search (MOEO combinatorial material search) strategy. A tetravalent manganese-doped alkali earth germanium/titanium oxide system was used as a model system to be screened using MOEO combinatorial materials search. As a result of MOEO reiteration, we identified a halide-detached deep red phosphor with improved PL intensity and reliable reproducibility.

Lithium barium silicate, Li(2)BaSiO(4), from synchrotron powder data.

The structure of lithium barium silicate, Li(2)BaSiO(4), has been determined from synchrotron radiation powder data. The title compound was synthesized by high-temperature solid-state reaction and crystallizes in the hexagonal space group P6(3)cm. It contains two Li atoms, one Ba atom (both site symmetry ..m on special position 6c), two Si atoms [on special positions 4b (site symmetry 3..) and 2a (site symmetry 3.m)] and four O atoms (one on general position 12d, and three on special positions 6c, 4b and 2a). The basic units of the structure are (Li(6)SiO(13))(5-) units, each comprising seven tetrahedra sharing edges and vertices. These basic units are connected by sharing corners parallel to [001] and through sharing (SiO(4))(4-) tetrahedra in (001). The relationship between the structures and luminescence properties of Li(2)SrSiO(4), Li(2)CaSiO(4) and the title compound is discussed.

Minimizing Trap Charge Density towards an Ideal Diode in Graphene-Silicon Schottky Solar Cell.

Photovoltaic device performance of graphene/n-Si Schottky diodes is largely affected by inhomogeneous oxide formation at the interface that suppresses the tunneling current of injected and photoexcited charges. The accumulated trap charges at low current induce charge recombination at the interface and degrade the ideality factor of the diode and the fill factor (FF) of the solar cell. This consequently gives rise to a nonlinear current-voltage ( I- V) feature in solar cells, commonly known as an S-shaped kink, which can be engineered by optimizing the interface barrier thickness or by increasing the carrier mobility. Here, we present chemical and electrochemical doping methods to increase the conductivity of graphene that transforms nonlinear kink photodiodes with a low FF and solar cell efficiency towards trap-free linear photovoltaic I- V. Space-charge-limited-current manifested Ohmic I- V diode behavior with enhanced conductance in graphene by injecting homogeneous ionic liquid; confirming the significant reduction of trap charge density. This was further congruent with the disappearance of the nonlinear kink in photodiodes with a high FF and nearly ideal diodes. The solar cell efficiency obtained with our strategy is around 13.6% and suggests possibilities to reach the theoretical limit of 19% by tailoring parameters such as conductance of graphene, carrier density of Si, and oxidation of the interfaces.

Search for new red phosphors using genetic algorithm-assisted combinatorial chemistry.

A genetic algorithm was employed in association with high-throughput synthesis and characterization in an attempt to search for red phosphors with high photoluminescent intensity. A tetravalent manganese-doped alkali earth germanium oxide system, with an emission color close to a desirable deep red, was screened with the assistance of a genetic algorithm to pinpoint the phosphor exhibiting the highest photoluminescence. As the genetic algorithm was in progress, the PL intensity increased and maximized in the fourth generation. The highest and the average PL intensity of the fourth generation improved by 23 and 120%, respectively, compared with that of the first generation.

Excitation Intensity Dependent Carrier Dynamics of Chalcogen Heteroatoms in Medium-Bandgap Polymer Solar Cells.

The excitation intensity dependent carrier dynamics of blends with PC[70]BM of three new medium-band gap conjugated polymers with central chalcogen heteroatoms, PBDTfDTBX (X = O, T(Sulphur), Se) were studied. The PBDTfDTBX polymers (Poly[4,8-bis(5-(2-butyloctyl)thiophene-2-yl)benzo[1,2-b;4,5-b']dithiophene-alt-4,7-bis(4-(2-ethylhexyl)-2-thienyl)-dithieno[3',2':3,4;2″,3″:5,6]benzo[1,2-c][1,2,5] furazan or thiadiazole or selenadiazole]) have symmetrical structures but exhibit different solar cell performances. In this study, we determined how the photogenerated charge carrrier dynamics of the PBDTfDTBX:PC[70]BM blends varies with the heteroatom by performing transient absorption measurements at various excitation intensities. It was found that the charge carrier dynamics of the PBDTfDTBX blends with X = T or Se heteroatoms are dependent on the excitation intensity whereas that of the PBDTfDTBO blend is independent of the intensity. The photogenerated charge carrier dynamics of the PBDTfDTBO:PCBM, PBDTfDTBT:PCBM, and PBDTfDTBSe:PCBM blends were all modeled globally and rates were estimated for different photophysical processes occurring on different time scales.

Photoluminescent and decay behaviors of Mn2+ and Ce3+ coactivated MgSiN2 phosphors for use in light-emitting-diode applications.

We examined the photoluminescent behaviors of MgSiN2:Mn2+ and MgSiN2:Ce3+,Mn2+ phosphors for use in white-light-emitting diodes. The red emission from MgSiN2:Mn2+ phosphors consisted of two Gaussian components, P1 from a single Mn2+ ion and P2 from either Mn2+ pairs or clusters. Decay analysis based on the Yokota and Tanimoto equation identified long decay for P1 and fast decay for P2. Most importantly, Ce3+ codoping enhanced Mn2+ emission intensity; in particular, emission at 460 nm excitations was promoted by the Ce3+ codoping.