We report on the preparation of a series of solution-processed perovskite solar cells based on methylammonium (MA) lead halide derivatives, MAPbX3, which show tunable optical properties depending on the nature and ratio of the halides employed (X = Cl, Br, and I). Devices have been prepared with different cell architecture, thin film, and mesoporous scaffold (TiO2 and Al2O3). We have analyzed different sample sets focusing on the characterization of the charge recombination by means of impedance spectroscopy (IS). On the one hand, our study discloses that the insertion of both Cl and Br in the perovskite lattice reduces the charge recombination rates in the light absorber film, thus determining the open circuit voltage (Voc) of the device. The samples prepared on a mesoporous Al2O3 electrode present lower charge recombination rates than those devices prepared on mesoporous TiO2. Furthermore, the addition of Br in the perovskite structure was demonstrated to improve slightly the lifetime of the devices; in fact, the efficiencies of all devices tested remained at least at the 80% of the initial value 1 month after their preparation. These results highlight the crucial role of the charge-recombination processes on the performance of the perovskite solar cells and pave the way for further progress on this field.

Organic-inorganic hybrid perovskite solar cells have demonstrated unprecedented high power conversion efficiencies in the past few years. Now, the universal instability of the perovskites has become the main barrier for this kind of solar cells to realize commercialization. This situation can be even worse for those tin-based perovskites, especially for CsSnI, because upon exposure to ambient atmosphere the desired black orthorhombic phase CsSnI would promptly lose single crystallinity and degrade to the inactive yellow phase, followed by irreversible oxidation into metallic CsSnI. By alloying CsSnI with CsPbI, we herein report the synthesis of alloyed perovskite quantum dot (QD), CsSnPbI, which not only can be phase-stable for months in purified colloidal solution but also remains intact even directly exposed to ambient air, far superior to both of its parent CsSnI and CsPbI QDs. Ultrafast transient absorption spectroscopy studies reveal that the photoexcited electrons in the alloyed QDs can be injected into TiO nanocrystals at a fast rate of 1.12 × 10 s, which enables a high photocurrent generation in solar cells.

Frequently observed high V loss in tin-lead mixed perovskite solar cells is considered to be one of the serious bottle-necks in spite of the high attainable Jsc due to wide wavelength photon harvesting. An amicable solution to minimize the V loss up to 0.50 V has been demonstrated by introducing an n-type interface with spike structure between the absorber and electron transport layer inspired by highly efficient Cu(In,Ga)Se solar cells. Introduction of a conduction band offset of ∼0.15 eV with a thin phenyl-C61-butyric acid methyl ester layer (∼25 nm) on the top of perovskite absorber resulted into improved V of 0.75 V leading to best power conversion efficiency of 17.6%. This enhancement is attributed to the facile charge flow at the interface owing to the reduction of interfacial traps and carrier recombination with spike structure as evidenced by time-resolved photoluminescence, nanosecond transient absorption, and electrochemical impedance spectroscopy measurements.

In organic photovoltaic devices, outer interface structures play a significant role in establishing optimal contact conditions for efficient extraction (or blocking) of charge carriers. Buffer layers of different nature are currently employed to enhance both power conversion efficiency (PCE) and cell stability by improving contact performance. Several materials have been explored to enhance the electron selectivity of the cathode contact: alkali metal compounds (LiF, etc.), metal oxides (TiO x , ZnO, etc.), and low molecular weight organic compounds have been reported to contribute to the overall PCE and solar cell lifetime, as reviewed in recent reports.1À3 Among those approaches, the effect of the dipole moment associated with self-assembled monolayers (SAM) attached to the interface, which alter the energy level alignment between the cathode metal and the bulk of the blend, 4 is particularly interesting, as well as the inclusion of conjugated polyelectrolyte interlayers. 5 In all of these cases, the energy shift induced by the charge dipole built up at interface layers enables the use of air-stable high work function metals. It is then inferred that electrostatic mechanisms occurring at the nanometer scale, both in the active layer bulk and at interfaces, have a great influence on the overall device operation. 6,7 Interface dipole layers are regarded as a determining ingredient of the metal/organic contact equilibration. 8À12 Several models have been proposed to account for the energy level alignment at interfaces, depending on the degree of interaction between the metal contact and the deposited organic layer. When the chemical interaction between the metal and contacting conjugated molecules or polymers is not negligible, it is expected that molecules attached to the metal surface undergo both a shift and a broadening of their molecular energy levels. Energy distribution of the attached molecules should be modeled by a specific interfacial density of states (IDOS) which differs from that encountered in the bulk of the organic layer. The situation is

International audienceLead halide perovskites are attracting a great deal of interest for optoelectronic applications such as solar cells, LEDs, and lasers because of their unique properties. In solar cells, heat dissipation by hot carriers results in a major energy loss channel responsible for the Shockley–Queisser efficiency limit. Hot carrier solar cells offer the possibility to overcome this limit and achieve energy conversion efficiency as high as 66% by extracting hot carriers. Therefore, fundamental studies on hot carrier relaxation dynamics in lead halide perovskites are important. Here, we elucidated the hot carrier cooling dynamics in all-inorganic cesium lead iodide (CsPbI3) perovskite using transient absorption spectroscopy. We observe that the hot carrier cooling rate in CsPbI3 decreases as the fluence of the pump light increases and the cooling is as slow as a few 10 ps when the photoexcited carrier density is 7 × 1018 cm−3, which is attributed to phonon bottleneck for high photoexcited carrier densities. Our findings suggest that CsPbI3 has a potential for hot carrier solar cell applications