In the pursuit to better understand the mechanisms of perovskite solar cells we performed Raman and photoluminescence measurements of free-standing CH3NH3PbI3 films, comparing dark with working conditions. The films, grown on a glass substrate and sealed by a thin glass coverslip, were measured subsequent to dark and white-light pretreatments. The extremely slow changes we observe in both the Raman and photoluminescence cannot be regarded as electronic processes, which are much faster. Thus, the most probable explanation is of slow photoinduced structural changes. The CH3NH3PbI3 transformation between the dark and the light structures is reversible, with faster rates for the changes under illumination. The results seem to clarify several common observations associated with solar cell mechanisms, like performance improvement under light soaking. More important is the call for solar-cell-related investigation of CH3NH3PbI3 to take the photoinduced structural changes into consideration when measuring and interpreting the results.

With solar conversion efficiencies surpassing 20%, organometallic perovskites show tremendous promise for solar cell technology. Their high brightness has also led to demonstrations of lasing and power-efficient electroluminescence. Here we show that thin films of methylammonium lead iodide, prepared by solution processing at temperatures not exceeding 100 °C, exhibit a highly nonlinear intensity-dependent refractive index due to changes in the free-carrier concentration and for femtosecond excitation at higher intensities undergo saturation that can be attributed to the Pauli blocking effect. Nonlinear refractive index and nonlinear absorption coefficients were obtained by the Z-scan technique, performed simultaneously in open- and closed-aperture configurations. Both nanosecond- and femtosecond-pulsed lasers at multiple wavelengths were used in order to distinguish between the mechanisms inducing the nonlinearities. The magnitude and sign of the nonlinear refractive index n 2 were determined. For resonant excitation, free carrier generation is the dominant contribution to the nonlinear refractive index, with a large nonlinear refractive index of n 2 = 69 × 10–12 cm2/W being observed for resonant femtosecond pumping and n 2 = 34.4 × 10–9 cm2/W for resonant nanosecond pumping. For nonresonant femtosecond excitation, bound-charge-induced nonlinearity leads to n 2 = 36 × 10–12 cm2/W. These values are equivalent to the best reported metrics for conventional semiconductors, suggesting that organometallic perovskites are promising materials for optical switching and bistability applications.

All-oxide-based photovoltaics (PVs) encompass the potential for extremely low cost solar cells, provided they can obtain an order of magnitude improvement in their power conversion efficiencies. To achieve this goal, we perform a combinatorial materials study of metal oxide based light absorbers, charge transporters, junctions between them, and PV devices. Here we report the development of a combinatorial internal quantum efficiency (IQE) method. IQE measures the efficiency associated with the charge separation and collection processes, and thus is a proxy for PV activity of materials once placed into devices, discarding optical properties that cause uncontrolled light harvesting. The IQE is supported by high-throughput techniques for bandgap fitting, composition analysis, and thickness mapping, which are also crucial parameters for the combinatorial investigation cycle of photovoltaics. As a model system we use a library of 169 solar cells with a varying thickness of sprayed titanium dioxide (TiO2) as the window layer, and covarying thickness and composition of binary compounds of copper oxides (Cu–O) as the light absorber, fabricated by Pulsed Laser Deposition (PLD). The analysis on the combinatorial devices shows the correlation between compositions and bandgap, and their effect on PV activity within several device configurations. The analysis suggests that the presence of Cu4O3 plays a significant role in the PV activity of binary Cu–O compounds.

Hybridized polaritons are generated by simultaneously coupling two vibrational modes of two different organic materials to the resonance of a low-loss infrared optical microcavity. A thin film of poly methyl methacrylate with solvent molecules of dimethylformamide trapped inside provided two spectrally narrow, closely spaced carbonyl stretches with absorption peaks at 1731 and 1678 cm(-1). Situating this film in a microcavity based on Ge/ZnS distributed Bragg reflector mirrors produced three distinct polariton branches in the dispersion relation due to hybridization of the vibrational resonances. Two anticrossings were observed with Rabi splittings of 9.6 and 5.2 meV, between the upper-to-middle and middle-to-lower polariton branches, respectively. This system marks the first demonstration of polariton hybridization between a solid and solvent molecules and can open new paths toward chemical reaction modification and energy transfer studies in the mid-infrared spectral range.

Sublinear intensity dependence of photoluminescence from organic exciton-polariton microcavities under non-resonant excitation in two power regimes is shown. The sublinearity is attributed to exciton-exciton annihilation, which could compete with polariton-polariton scattering in these devices.