Carrier Transport in PbS and PbSe QD Films Measured by Photoluminescence Quenching
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Transient photoconductivity measurements carried out on bulk heterojunction (BHJ) solar cells demonstrate the competition between carrier sweep-out by the internal field and the loss of photogenerated carriers by recombination. The transient photoconductance data imply the existence of a well-defined internal field; carrier sweep-out is proportional to the magnitude of the internal field and limited by the carrier mobility. At external voltages near open circuit where the internal field approaches zero, the photocurrent decays because of the recombination of photogenerated mobile carriers. Mobility and recombination lifetimes are evaluated for carriers in poly[3-hexylthiophene] (P3HT): [6,6]-phenyl-C 61 -butyric acid methyl ester (PC 60 BM) and poly[N -9''-hepta-decanyl-2,7-carbazole-alt-5,5-(4',7'-di-2-thienyl-2',1',3'-benzothiadiazole)] (PCDTBT): [6,6]-phenyl-C 71 -butyric acid methyl ester (PC 71 BM) solar cells.
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Here, a high performance solar absorber using a 2D tantalum superlattice photonic crystal (PhC) is proposed and its design is optimized for high-temperature energy conversion. In contrast to the simple lattice PhC, which is limited by diffraction in the short wavelength range, the superlattice PhC achieves solar absorption over broadband spectral range due to the contribution from two superposed lattices with different cavity radii. The superlattice PhC geometry is tailored to achieve maximum thermal transfer efficiency for a low concentration system of 250 suns at 1500 K reaching 85.0% solar absorptivity. In the high concentration case of 1000 suns, the superlattice PhC absorber achieves a solar absorptivity of 96.2% and a thermal transfer efficiency of 82.9% at 1500 K, amounting to an improvement of 10% and 5%, respectively, versus the simple square lattice PhC absorber. In addition, the performance of the superlattice PhC absorber is studied in a solar thermophotovoltaic system which is optimized to minimize absorber re-emission by reducing the absorber-to-emitter area ratio and using a highly reflective silver aperture.
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Following the calculation of optimal energy transfer in thermal environment in our first paper [J. L. Wu, F. Liu, Y. Shen, J. S. Cao, and R. J. Silbey, New J. Phys. 12, 105012 (2010)], full quantum dynamics and leading-order 'classical' hopping kinetics are compared in the seven-site Fenna-Matthews-Olson (FMO) protein complex. The difference between these two dynamic descriptions is due to higher-order quantum corrections. Two thermal bath models, classical white noise (the Haken-Strobl-Reineker (HSR) model) and quantum Debye model, are considered. In the seven-site FMO model, we observe that higher-order corrections lead to negligible changes in the trapping time or in energy transfer efficiency around the optimal and physiological conditions (2% in the HSR model and 0.1% in the quantum Debye model for the initial site at BChl 1). However, using the concept of integrated flux, we can identify significant differences in branching probabilities of the energy transfer network between hopping kinetics and quantum dynamics (26% in the HSR model and 32% in the quantum Debye model for the initial site at BChl 1). This observation indicates that the quantum coherence can significantly change the distribution of energy transfer pathways in the flux network with the efficiency nearly the same. The quantum-classical comparison of the average trapping time with the removal of the bottleneck site, BChl 4, demonstrates the robustness of the efficient energy transfer by the mechanism of multi-site quantum coherence. To reconcile with the latest eight-site FMO model which is also investigated in the third paper [J. Moix, J. L. Wu, P. F. Huo, D. F. Coker, and J. S. Cao, J. Phys. Chem. Lett. 2, 3045 (2011)], the quantum-classical comparison with the flux network analysis is summarized in Appendix C. The eight-site FMO model yields similar trapping time and network structure as the seven-site FMO model but leads to a more disperse distribution of energy transfer pathways.
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