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Fullerene-derivatives based bulk heterojunctions hold an exceptionally important role on the roadmap of highly efficient organic solar cells (OSCs). In recent years, the utilization of the non-fused ring acceptors based OSCs has further improved photovoltaic power conversion efficiencies. Among these, one of the fundamental issues is to explore and to understand the spin-related polaron dissociation at charge transfer states because they act as the central unit for the photovoltaic action. It is also eagerly important to quantify some internal fields, such as hyperfine fields and the spin–orbit coupling. The aim of the work is to develop a method for unraveling the photoexcited spin states, particularly for the fullerene-derivative based OSC. Furthermore, it helps to elucidate a long-standing issue regarding the relatively high production of photocurrent for the P3HT:PC71BM system, which is indeed contrary to its counterpart the P3HT:PC61BM system. Their corresponding Jablonski diagrams have been determined in order to understand interior spin dynamics. The method of the study offers an alternative route for an understanding of device performance from the spin-related aspect. [ABSTRACT FROM AUTHOR]

Layer‐by‐layer all‐polymer solar cells (LbL all‐PSCs) are prepared with PM6 and PY‐IT by using sequential spin coating method. The exciton dissociation efficiency in acceptor layer near electrode is rather low due to the limited exciton diffuse distance and impossible energy transfer from narrow bandgap acceptor to wide bandgap donor. In this study, less PM6 is incorporated into PY‐IT layer to enhance exciton dissociation in PY‐IT layer near electrode. A power conversion efficiency (PCE) of 17.45% is achieved in the LbL all‐PSCs incorporating 10 wt% PM6 into PY‐IT layer, which is much larger than 16.04% PCE of PM6/PY‐IT‐based LbL all‐PSCs. Over 8% PCE enhancement can be realized by incorporating 10 wt% PM6 into PY‐IT layer, which is attributed to the enhanced exciton utilization efficiency in PY‐IT layers near electrode. The enhanced exciton utilization efficiency in PY‐IT layer can be confirmed from the quenched photoluminescence (PL) emission in PY‐IT:PM6 films. Meanwhile, charge transport in acceptor layers can be optimized by incorporating less PM6, as confirmed from the optimized molecular arrangement. This study indicates that the strategy of incorporating less donor into acceptor layer has great potential in fabricating efficient LbL all‐PSCs by improving exciton utilization efficiency in acceptor layer near electrode. [ABSTRACT FROM AUTHOR]

Abstract Recent studies have shown that organic-inorganic hybrid perovskites (OIHPs) exhibit unprecedented optoelectronic properties for photovoltaic applications. Complete realizations of photo- and electrically induced surface polarization and recombination are critically important for extensively upgrading solar cell performance. We have explored such effects in a planar solar cell comprising ITO(glass)/PEDOT:PSS/CH 3 NH 3 PbI 3-x Cl x /PC 60 BM/PEI/Ag with a maximum power conversion efficiency (PCE) of 15.4%. A remarkable frequency-dependence of surface polarization was observed for the operating device under illumination (i.e. short-circuit current J s c condition) and at steady state (i.e. open-circuit voltage V o c condition). A sign reversal of the capacitance (i.e. negative capacitance) associated with the surface polarization and recombination was detected at some specific steady states. Based on capacitance-voltage (C - V) spectroscopic measurements and theoretical fittings, they can be understood that, (i) a naturally formed surface depletion region due to energy mismatch can be fully suppressed at a very low fluence and moderate forward bias voltage; (ii) a surface capacitance (C s) appears at lower ac -modulation frequencies only; (iii) remarkable trap-assist and band to band surface recombination may play the dominant roles for generating the negative capacitive effect in the CH 3 NH 3 PbI 3-x Cl x based photovoltaic system. Graphical abstract Image Highlights • Surface depletion region can be fully suppressed at low fluence and moderate bias voltage. • Surface capacitance (C s) appears at lower ac -modulation frequencies only. • Trap-assist and band to band surface recombination play dominant roles for negative capacitive effect in perovskite solar cells. [ABSTRACT FROM AUTHOR]