The performance of organometallic perovskite solar cells has rapidly surpassed those of both traditional dye-sensitized and organic photovoltaics, e.g. solar cells based on CH3NH3PbI3 have recently reached 18% conversion efficiency. We analyze its electronic structure and optical properties within the quasiparticle self-consistent GW approximation (QSGW ). Quasiparticle self-consistency is essential for an accurate description of the band structure: bandgaps are much larger than what is predicted by the local density approximation (LDA) or GW based on the LDA. Several characteristics combine to make the electronic structure of this material unusual. First, there is a strong driving force for ferroelectricity, as a consequence the polar organic moiety CH3NH3. The moiety is only weakly coupled to the PbI3 cage; thus it can rotate give rise to ferroelectric domains. This in turn will result in internal junctions that may aid separation of photoexcited electron and hole pairs, and may contribute to the current-voltage hysteresis found in perovskite solar cells. Second, spin orbit modifies both valence band and conduction band dispersions in a very unusual manner: both get split at the R point into two extrema nearby. This can be interpreted in terms of a large Dresselhaus term, which vanishes at R but for small excursions about R varies linearly in k. Conduction bands (Pb 6p character) and valence bands (I 5p) are affected differently; moreover the splittings vary with the orientation of the moiety. We will show how the splittings, and their dependence on the orientation of the moiety through the ferroelectric effect, have important consequences for both electronic transport and the optical properties of this material.

http://absimage.aps.org/image/MAR15/MWS_MAR15-2014-020499.pdf

Electronic structure of hybrid halide perovskite photovoltaic absorbers

Two-dimensional Ruddlesden–Popper phase (2DRP) perovskites are known to exhibit improved photostability and environmental stability compared with their three-dimensional (3D) counterparts. However, fundamental questions remain over the interaction between the bulky alkylammoniums and the 2DRP perovskite framework. Here, we unambiguously demonstrate that a sulfur–sulfur interaction is present for a new bulky alkylammonium, 2-(methylthio)ethylamine hydrochloride (MTEACl). In addition to a weaker van der Waals interaction, the interaction between sulfur atoms in two MTEA molecules enables a (MTEA)2(MA)4Pb5I16 (n = 5) perovskite framework with enhanced charge transport and stabilization. The result is 2DRP perovskite solar cells with significantly improved efficiency and stability. Cells with a power conversion efficiency as high as 18.06% (17.8% certified) are achieved, along with moisture tolerance for up to 1,512 h (under 70% humidity conditions), thermal stability for 375 h (at 85 °C) and stability under continuous light stress (85% of the initial efficiency retained over 1,000 h of operation at the maximum power point). Two-dimensional perovskite solar cells have been engineered to be robust against moisture, high temperatures and light stress.

Efficient and stable Ruddlesden–Popper perovskite solar cell with tailored interlayer molecular interaction

Two-dimensional (2D) perovskites have attracted considerable interest for their promising applications for solar cells and other optoelectronics, such as light-emitting diodes, spintronics, and photodetectors. Here, we review the recent achievements of 2D perovskites for various optoelectronic applications. First, we discuss the basic structure and optoelectronic properties of 2D perovskites, including band structure, optical properties, and charge transport. We then highlight recent achievements using 2D perovskites in solar cells and beyond solar cells, including progress on various synthesis strategies and their impact on structural and optoelectronic properties. Finally, we discuss current challenges and future opportunities to further develop 2D perovskites for various applications.

Advances in two-dimensional organic–inorganic hybrid perovskites

We report on nanoscale strain gradients in ferroelectric HoMnO3 epitaxial thin films, resulting in a giant flexoelectric effect. Using grazing-incidence in-plane x-ray diffraction, we measured strain gradients in the films, which were 6 or 7 orders of magnitude larger than typical values reported for bulk oxides. The combination of transmission electron microscopy, electrical measurements, and electrostatic calculations showed that flexoelectricity provides a means of tuning the physical properties of ferroelectric epitaxial thin films, such as domain configurations and hysteresis curves.

/pdf/giant-flexoelectric-effect-in-ferroelectric-epitaxial-thin-24sbqwd74x.pdf

Giant Flexoelectric Effect in Ferroelectric Epitaxial Thin Films

A series of ternary organic photovoltaics (OPVs) are fabricated with one wide bandgap polymer D18-Cl as donor, and well compatible Y6 and Y6-1O as acceptor. The open-circuit-voltage (VOC ) of ternary OPVs is monotonously increased along with the incorporation of Y6-1O, indicating that the alloy state should be formed between Y6 and Y6-1O due to their excellent compatibility. The energy loss can be minimized by incorporating Y6-1O, leading to the VOC improvement of ternary OPVs. By finely adjusting the Y6-1O content, a power conversion efficiency of 17.91% is achieved in the optimal ternary OPVs with 30 wt% Y6-1O in acceptors, resulting from synchronously improved short-circuit-current density (JSC ) of 25.87 mA cm-2, fill factor (FF) of 76.92% and VOC of 0.900 V in comparison with those of D18-Cl : Y6 binary OPVs. The JSC and FF improvement of ternary OPVs should be ascribed to comprehensively optimal photon harvesting, exciton dissociation and charge transport in ternary active layers. The more efficient charge separation and transport process in ternary active layers can be confirmed by the magneto-photocurrent and impedance spectroscopy experimental results, respectively. This work provides new insight into constructing highly efficient ternary OPVs with well compatible Y6 and its derivative as acceptor.

Approaching 18% efficiency of ternary organic photovoltaics with wide bandgap polymer donor and well compatible Y6 : Y6-1O as acceptor.

Uniform Permutation of Quasi-2D Perovskites by Vacuum Poling for Efficient, High-Fill-Factor Solar Cells

https://iopscience.iop.org/article/10.1088/1361-6463/aae2ab/pdf

Polymer assist crystallization and passivation for enhancements of open-circuit voltage and stability in tin-halide perovskite solar cells

Surface polarization and recombination in organic-inorganic hybrid perovskite solar cells based on photo- and electrically induced negative capacitance studies

Substrate‐Dependent Spin–Orbit Coupling in Hybrid Perovskite Thin Films

These days, organic-inorganic hybrid perovskites (OIHP) and non-fullerene acceptor (NFA) molecules are all at the frontiers of research and development in the domain of photovoltaics. A careful design and use of inorganic transparent metal oxides with wide band gaps as electron and hole transport layers are critically important for highly efficient and stable solar cells. As one of the most favorable electron transport materials, tin oxide (SnO2), which has been frequently utilized in highly efficient OIHP solar cells, is rarely seen in the application of NFA organic bulk heterojunction (BHJ) solar cells. To appropriately tailor an interface of SnO2 and an organic blend, while to make them compatible and useful may offer some opportunities for achieving higher efficiencies and longer lifetimes. In fact, there is still a lack of a method to solve the problem. Herein, a unique way is developed by implementing a surface decoration nanostructure such as low dimensional MAPbI3 perovskite nanowires (PeNWs) at the interface of SnO2 and the organic blend such as PBDB-T-SF:IT-4F. Such an interface functions well for the improvement of photovoltaic performance for the organic solar cell of the structure ITO(glass)/SnO2/PeNWs/PBDB-T-SF:IT-4F/MoO3/Ag. Experimental results indicate that the electron-hole dissociation, charge extraction, and photo-absorption ability of the organic solar cell can be improved significantly. The inside generation of the photocurrent is explored by the magneto-photocurrent method. Finally, the solar cell exhibits more than 80% power conversion efficiencies even after 20 days, which suggests the merits of having both SnO2 and PeNWs in the NFA-based organic solar cell.

Haomiao Yu

Papers

Uniform Permutation of Quasi-2D Perovskites by Vacuum Poling for Efficient, High-Fill-Factor Solar Cells

Polymer assist crystallization and passivation for enhancements of open-circuit voltage and stability in tin-halide perovskite solar cells

Surface polarization and recombination in organic-inorganic hybrid perovskite solar cells based on photo- and electrically induced negative capacitance studies

Substrate‐Dependent Spin–Orbit Coupling in Hybrid Perovskite Thin Films

Surface Modification of SnO2 via MAPbI3 Nanowires for a Highly Efficient Non-Fullerene Acceptor-Based Organic Solar Cell.