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Organic-inorganic hybrid perovskites have cemented their position as an exceptional class of optoelectronic materials thanks to record photovoltaic efficiencies of 22.1%, as well as promising demonstrations of light-emitting diodes, lasers, and light-emitting transistors. Perovskite materials with photoluminescence quantum yields close to 100% and perovskite light-emitting diodes with external quantum efficiencies of 8% and current efficiencies of 43 cd A(-1) have been achieved. Although perovskite light-emitting devices are yet to become industrially relevant, in merely two years these devices have achieved the brightness and efficiencies that organic light-emitting diodes accomplished in two decades. Further advances will rely decisively on the multitude of compositional, structural variants that enable the formation of lower-dimensionality layered and three-dimensional perovskites, nanostructures, charge-transport materials, and device processing with architectural innovations. Here, the rapid advancements in perovskite light-emitting devices and lasers are reviewed. The key challenges in materials development, device fabrication, operational stability are addressed, and an outlook is presented that will address market viability of perovskite light-emitting devices., (© 2016 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.)

Ultrafast spin manipulation for opto-spin logic applications requires material systems that have strong spin-selective light-matter interaction. Conventional inorganic semiconductor nanostructures [for example, epitaxial II to VI quantum dots and III to V multiple quantum wells (MQWs)] are considered forerunners but encounter challenges such as lattice matching and cryogenic cooling requirements. Two-dimensional halide perovskite semiconductors, combining intrinsic tunable MQW structures and large oscillator strengths with facile solution processability, can offer breakthroughs in this area. We demonstrate novel room-temperature, strong ultrafast spin-selective optical Stark effect in solution-processed (C6H4FC2H4NH3)2PbI4 perovskite thin films. Exciton spin states are selectively tuned by ~6.3 meV using circularly polarized optical pulses without any external photonic cavity (that is, corresponding to a Rabi energy of ~55 meV and equivalent to applying a 70 T magnetic field), which is much larger than any conventional system. The facile halide and organic replacement in these perovskites affords control of the dielectric confinement and thus presents a straightforward strategy for tuning light-matter coupling strength.

Semiconductors are ubiquitous gain media for coherent light sources. Solution-processed three-dimensional (3D) halide perovskites (e.g., CH3NH3PbI3) with their outstanding room temperature optical gain properties are the latest members of this family. Their two-dimensional (2D) layered perovskite counterparts with natural multiple quantum well structures exhibit strong light-matter interactions and intense excitonic luminescence. However, despite such promising traits, there have been no reports on room temperature optical gain in 2D layered perovskites. Herein, we reveal the challenges towards achieving amplified spontaneous emission (ASE) in the archetypal (C6H5C2H4NH3)2PbI4 (or PEPI) system. Temperature-dependent transient spectroscopy uncovers the dominant free exciton trapping and bound biexciton formation pathways that compete effectively with biexcitonic gain. Phenomenological rate equation modeling predicts a large biexciton ASE threshold of ∼1.4 mJ cm(-2), which is beyond the damage threshold of these materials. Importantly, these findings would rationalize the difficulties in achieving optical gain in 2D perovskites and provide new insights and suggestions for overcoming these challenges.

2D perovskites is one of the proposed strategies to enhance the moisture resistance, since the larger organic cations can act as a natural barrier. Nevertheless, 2D perovskites hinder the charge transport in certain directions, reducing the solar cell power conversion efficiency. A nanostructured mixed-dimensionality approach is presented to overcome the charge transport limitation, obtaining power conversion efficiencies over 9%., (© 2016 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.)

Iron pyrite has received significant attention due to its high optical absorption. However, the loss of open circuit voltage (Voc) prevents its further application in photovoltaics. Herein, we have studied the photophysics of pyrite by ultrafast laser spectroscopy to understand fundamental limitation of low Voc by quantifying photocarrier losses in high quality, stoichiometric, and phase pure {100} faceted pyrite nanocubes. We found that fast carrier localization of photoexcited carriers to indirect band edge and shallow trap states is responsible for major carrier loss. Slow relaxation component reflects high density of defects within the band gap which is consistent with the observed Mott-variable range hopping (VRH) conduction from transport measurements. Magnetic measurements strikingly show the magnetic ordering associated with phase inhomogeneity, such as FeS2-δ (0 ≤ δ ≤ 1). This implies that improvement of iron pyrite solar cell performance lies in mitigating the intrinsic defects (such as sulfur vacancies) by blocking the fast carrier localization process. Photocarrier generation and relaxation model is presented by comprehensive analysis. Our results provide insight into possible defects that induce midgap states and facilitate rapid carrier relaxation before collection.

Perovskite semiconductors are actively investigated for high performance solar cells. Their large optical absorption coefficient and facile solution-based, low-temperature synthesis of thin films make perovskites also a candidate for light-emitting devices across the visible and near-infrared. Specific to their potential as optical gain medium for lasers, early work has demonstrated amplified spontaneous emission and lasing at attractively low thresholds of photoexcitation. Here, we take an important step toward practically usable perovskite lasers where a solution-processed thin film is embedded within a two-dimensional photonic crystal resonator. We demonstrate high degree of temporally and spatially coherent lasing whereby well-defined directional emission is achieved near 788 nm wavelength at optical pumping energy density threshold of 68.5 ± 3.0 μJ/cm(2). The measured power conversion efficiency and differential quantum efficiency of the perovskite photonic crystal laser are 13.8 ± 0.8% and 35.8 ± 5.4%, respectively. Importantly, our approach enables scalability of the thin film lasers to a two-dimensional multielement pixelated array of microlasers which we demonstrate as a proof-of-concept for possible projection display applications.

A high open circuit voltage (V(OC)) close to 1.4 V under AM 1.5, 100 mW cm(-2) conditions is achieved when carbon nanotubes (CNTs) are used as a hole conductor in methyl ammonium lead bromide (MAPbBr3) perovskite solar cells. Time-resolved photoluminescence and impedance spectroscopy investigations suggest that the observed high V(OC) is a result of the better charge extraction and lower recombination of the CNT hole conductor. Tandem solar cells with all perovskite absorbers are demonstrated with a MAPbBr3/CNT top cell and a MAPbI3 bottom cell, achieving a V(OC) of 2.24 V in series connection. The semitransparent and high voltage MAPbBr3/CNT solar cells show great potential for applications in solar cell windows, tandem solar cells and solar driven water splitting.

The temperature dependence of the principal photovoltaic parameters of perovskite photovoltaics is studied. The recombination activation energy is in good agreement with the perovskite's bandgap energy, thereby placing an upper bound on the open-circuit voltage. The photocurrent increases moderately with temperature and remains high at low temperature, reinforcing that the cells are not hindered by insufficient thermally activated mobility or carrier trapping by deep defects., (© 2016 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.)

The stunning rise of methylammonium lead iodide perovskite material as a light harvesting material in recent years has drawn much attention in the photovoltaic community. Here, we investigated in detail the uniform and void-free perovskite capping layer in the mesoscopic perovskite devices and found it to play a critical role in determining device performance and charge recombination process. Compared to the rough surface with voids of the perovskite layer, surface of the perovskite capping layer obtained from sequential deposition process is much more uniform with less void formation and distribution within the TiO2 mesoscopic scaffold is more homogeneous, leading to much improved photovoltaic parameters of the devices. The impact of void free perovskite capping layer surface on the charge recombination processes within the mesoscopic perovskite solar cells is further scrutinized via charge extraction measurement. Modulation of precursor solution concentrations in order to further improve the perovskite layer surface morphology leads to higher efficiency and lower charge recombination rates. Inhibited charge recombination in these solar cells also matches with the higher charge density and slower photovoltage decay profiles measured.

Lead halide perovskite solar cells are presently the forerunner among the third generation solution-processed photovoltaic technologies. With efficiencies exceeding 20% and low production costs, they are prime candidates for commercialization. Critical insights into their light harvesting, charge transport, and loss mechanisms have been gained through time-resolved optical probes such as femtosecond transient absorption spectroscopy (fs-TAS), transient photoluminescence spectroscopy, and time-resolved terahertz spectroscopy. Specifically, the discoveries of long balanced electron-hole diffusion lengths and gain properties in halide perovskites underpin their significant roles in uncovering structure-function relations and providing essential feedback for materials development and device optimization. In particular, fs-TAS is becoming increasingly popular in perovskite characterization studies, with commercial one-box pump-probe systems readily available as part of a researcher's toolkit. Although TAS is a powerful probe in the study of charge dynamics and recombination mechanisms, its instrumentation and data interpretation can be daunting even for experienced researchers. This issue is exacerbated by the sensitive nature of halide perovskites where the kinetics are especially susceptible to pump fluence, sample preparation and handling and even degradation effects that could lead to disparate conclusions. Nonetheless, with end-users having a clear understanding of TAS's capabilities, subtleties, and limitations, cutting-edge work with deep insights can still be performed using commercial setups as has been the trend for ubiquitous spectroscopy instruments like absorption, fluorescence, and transient photoluminescence spectrometers. Herein, we will first briefly examine the photophysical processes in lead halide perovskites, highlighting their novel properties. Next, we proceed to give a succinct overview of the fundamentals of pump-probe spectroscopy in relation to the spectral features of halide perovskites and their origins. In the process, we emphasize some key findings of seminal photophysical studies and draw attention to the interpretations that remain divergent and the open questions. This is followed by a general description into how we prepare and conduct the TAS characterization of CH3NH3PbI3 thin films in our laboratory with specific discussions into the potential pitfalls and the influence of thin film processing on the kinetics. Lastly, we conclude with our views on the challenges and opportunities from the photophysical perspective for the field and our expectations for systems beyond lead halide perovskites.

Despite their extremely good performance in solar cells with efficiencies approaching 20% and the emerging application for light-emitting devices, organic-inorganic lead halide perovskites suffer from high content of toxic, polluting, and bioaccumulative Pb, which may eventually hamper their commercialization. Here, we present the synthesis of two-dimensional (2D) Cu-based hybrid perovskites and study their optoelectronic properties to investigate their potential application in solar cells and light-emitting devices, providing a new environmental-friendly alternative to Pb. The series (CH3NH3)2CuCl(x)Br(4-x) was studied in detail, with the role of Cl found to be essential for stabilization. By exploiting the additional Cu d-d transitions and appropriately tuning the Br/Cl ratio, which affects ligand-to-metal charge transfer transitions, the optical absorption in this series of compounds can be extended to the near-infrared for optimal spectral overlap with the solar irradiance. In situ formation of Cu(+) ions was found to be responsible for the green photoluminescence of this material set. Processing conditions for integrating Cu-based perovskites into photovoltaic device architectures, as well as the factors currently limiting photovoltaic performance, are discussed: among them, we identified the combination of low absorption coefficient and heavy mass of the holes as main limitations for the solar cell efficiency. To the best of our knowledge, this is the first demonstration of the potential of 2D copper perovskite as light harvesters and lays the foundation for further development of perovskite based on transition metals as alternative lead-free materials. Appropriate molecular design will be necessary to improve the material's properties and solar cell performance filling the gap with the state-of-the-art Pb-based perovskite devices.

Amorphous oxide semiconductors such as indium zinc tin oxide (IZTO) are considered favorites to serve as channel materials for thin film transistors (TFTs) because they combine high charge carrier mobility with high optical transmittance, allowing for the development of transparent electronics. Although the influence of relative cationic concentrations in determining the electronic properties have been studied in sputtered and PLD films, the development of printed transparent electronics hinges on such dependencies being explored for solution-processed systems. Here, we study solution-processed indium zinc tin oxide thin film transistors (TFTs) to investigate variation in their electrical properties with change in cationic composition. Charge transport mobility ranging from 0.3 to 20.3 cm(2)/(V s), subthreshold swing ranging from 1.2 to 8.4 V/dec, threshold voltage ranging from -50 to 5 V, and drain current on-off ratio ranging from 3 to 6 orders of magnitude were obtained by examining different compositions of the semiconductor films. Mobility was found to increase with the incorporation of large cations such as In(3+) and Sn(4+) due to the vast s-orbital overlap they can achieve when compared to the intercationic distance. Subthreshold swing decreased with an increase in Zn(2+) concentration due to reduced interfacial state formation between the semiconductor and dielectric. The optimized transistor obtained at a compositional ratio of In/Zn/Sn = 1:1:1, exhibited a high field-effect mobility of 8.62 cm(2)/(V s), subthreshold swing of 1.75 V/dec, and current on-off ratio of 10(6). Such impressive performances reaffirm the promise of amorphous metal oxide semiconductors for printed electronics.

Lead-halide perovskites have transcended photovoltaics. Perovskite light-emitting diodes (PeLEDs) emerge as a new field to leverage on these fascinating semiconductors. Here, we report the first use of completely inorganic CsPbBr3 thin films for enhanced light emission through controlled modulation of the trap density by varying the CsBr-PbBr2 precursor concentration. Although pure CsPbBr3 films can be deposited from equimolar CsBr-PbBr2 and CsBr-rich solutions, strikingly narrow emission line (17 nm), accompanied by elongated radiative lifetimes (3.9 ns) and increased photoluminescence quantum yield (16%), was achieved with the latter. This is translated into the enhanced performance of the resulting PeLED devices, with lower turn-on voltage (3 V), narrow electroluminescence spectra (18 nm) and higher electroluminescence intensity (407 Cd/m(2)) achieved from the CsBr-rich solutions.

The advantages of employing an interconnected periodic ZnO morphology, i.e. an inverse opal structure, in electrodeposited ZnO/Cu2O devices are presented. The solar cells are fabricated using low cost solution based methods such as spin coating and electrodeposition. The impact of inverse opal geometry, mainly the diameter and thickness, is scrutinized. By employing 3 layers of an inverse opal structure with a 300 nm pore diameter, higher short circuit photocurrents (∼84% improvement) are observed; however the open circuit voltages decrease with increasing interfacial area. Optical simulation using a finite difference time domain method shows that the inverse opal structure modulates light propagation within the devices such that more photons are absorbed close to the ZnO/Cu2O junction. This increases the collection probability resulting in improved short circuit currents.

Low-temperature solution-processed CH3 NH3 PbI3 interfaced with TiO2 has recently been demonstrated as a highly successful type-II light harvesting heterojunction with ≈20% efficiency. Therefore, an efficient ultrafast photoexcited electron transfer from CH3 NH3 PbI3 to TiO2 is expected. However, by probing the photoexcited charge carrier dynamics in CH3 NH3 PbI3 /quartz, CH3 NH3 PbI3 /TiO2 (compact), and CH3 NH3 PbI3 /PCBM in a comparative study, an electron transfer potential barrier between CH3 NH3 PbI3 and the compact TiO2 (prepared with the spray pyrolysis method) formed by surface states is uncovered. Consequently, the CH3 NH3 PbI3 photoluminescence intensity and lifetime is enhanced when interfaced to compact TiO2 . The electron accumulation within CH3 NH3 PbI3 needed to overcome this interfacial potential barrier results in the undesirable large current-voltage hysteresis observed for CH3 NH3 PbI3 /TiO2 planar heterojunctions. The findings in this study indicate that careful surface engineering to reduce this potential barrier is key to pushing perovskite solar cell efficiencies toward the theoretical limit., (© 2015 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.)

Photoelectrochemical water splitting half reactions on semiconducting photoelectrodes have received much attention but efficient overall water splitting driven by a single photoelectrode has remained elusive due to stringent electronic and thermodynamic property requirements. Utilizing a tandem configuration wherein the total photovoltage is generated by complementary optical absorption across different semiconducting electrodes is a possible pathway to unassisted overall light-induced water splitting. Because of the low photovoltages generated by conventional photovoltaic materials (e.g., Si, CIGS), such systems typically consist of triple junction design that increases the complexity due to optoelectrical trade-offs and are also not cost-effective. Here, we show that a single solution processed organic-inorganic halide perovskite (CH3NH3PbI3) solar cell in tandem with a Fe2O3 photoanode can achieve overall unassisted water splitting with a solar-to-hydrogen conversion efficiency of 2.4%. Systematic electro-optical studies were performed to investigate the performance of tandem device. It was found that the overall efficiency was limited by the hematite's photocurrent and onset potential. To understand these limitations, we have estimated the intrinsic solar to chemical conversion efficiency of the doped and undoped Fe2O3 photoanodes. The total photopotential generated by our tandem system (1.87 V) exceeds both the thermodynamic and kinetic requirements (1.6 V), resulting in overall water splitting without the assistance of an electrical bias.

Solar cells based on organic-inorganic lead iodide perovskite (CH3NH3PbI3) exhibit remarkably high power conversion efficiency (PCE). One of the key issues in solution-processed films is that often the polycrystalline domain orientation is not well-defined, which makes it difficult to predict energy alignment and charge transfer efficiency. Here we combine ab initio calculations and photoelectron spectroscopy to unravel the electronic structure and charge redistribution at the interface between different surfaces of CH3NH3PbI3 and typical organic hole acceptor Spiro-OMeTAD and electron acceptor PCBM. We find that both hole and electron interfacial transfer depend strongly on the CH3NH3PbI3 surface orientation: while the (001) and (110) surfaces tend to favor hole injection to Spiro-OMeTAD, the (100) surface facilitates electron transfer to PCBM due to surface delocalized charges and hole/electron accumulation at the CH3NH3PbI3/organic interfaces. Molecular dynamic simulations indicate that this is due to strong orbital interactions under thermal fluctuations at room temperature, suggesting the possibility to further improve charge separation and extraction in perovskite-based solar cells by controlling perovskite film crystallization and surface orientation.

Low-temperature solution-processed organic-inorganic halide perovskite CH3NH3PbI3 has demonstrated great potential for photovoltaics and light-emitting devices. Recent discoveries of long ambipolar carrier diffusion lengths and the prediction of the Rashba effect in CH3NH3PbI3, that possesses large spin-orbit coupling, also point to a novel semiconductor system with highly promising properties for spin-based applications. Through circular pump-probe measurements, we demonstrate that highly polarized electrons of total angular momentum (J) with an initial degree of polarization Pini ∼90% (i.e., -30% degree of electron spin polarization) can be photogenerated in perovskites. Time-resolved Faraday rotation measurements reveal photoinduced Faraday rotation as large as 10°/μm at 200 K (at wavelength λ = 750 nm) from an ultrathin 70 nm film. These spin polarized carrier populations generated within the polycrystalline perovskite films, relax via intraband carrier spin-flip through the Elliot-Yafet mechanism. Through a simple two-level model, we elucidate the electron spin relaxation lifetime to be ∼7 ps and that of the hole is ∼1 ps. Our work highlights the potential of CH3NH3PbI3 as a new candidate for ultrafast spin switches in spintronics applications.

Organic-inorganic lead halide based perovskites solar cells are by far the highest efficiency solution-processed solar cells, threatening to challenge thin film and polycrystalline silicon ones. Despite the intense research in this area, concerns surrounding the long-term stability as well as the toxicity of lead in the archetypal perovskite, CH3NH3PbI3, have the potential to derail commercialization. Although the search for Pb-free perovskites have naturally shifted to other transition metal cations and formulations that replace the organic moiety, efficiencies with these substitutions are still substantially lower than those of the Pb-perovskite. The perovskite family offers rich multitudes of crystal structures and substituents with the potential to uncover new and exciting photophysical phenomena that hold the promise of higher solar cell efficiencies. In addressing materials beyond CH3NH3PbI3, this Perspective will discuss a broad palette of elemental substitutions, solid solutions, and multidimensional families that will provide the next fillip toward market viability of the perovskite solar cells.

Lead free perovskite solar cells based on a CsSnI3 light absorber with a spectral response from 950 nm is demonstrated. The high photocurrents noted in the system are a consequence of SnF2 addition which reduces defect concentrations and hence the background charge carrier density., (© 2014 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.)

Iron pyrite has been the material of interest in the solar community due to its optical properties and abundance. However, the progress is marred due to the lack of control on the surface and intrinsic chemistry of pyrite. In this report, we show iron pyrite as an efficient counter electrode (CE) material alternative to the conventional Pt and poly(3,4-ethylenedioxythiophene (PEDOT) CEs in dye-sensitized solar cells (DSSCs). Pyrite film CEs prepared by spray pyrolysis are utilized in I3(-)/I(-) and Co(III)/Co(II) electrolyte-mediated DSSCs. From cyclic voltammetry and impedance spectroscopy studies, the catalytic activity is found to be comparable with that of Pt and PEDOT in I3(-)/I(-) and Co(III)/Co(II) electrolyte, respectively. With the I3(-)/I(-) electrolyte, photoconversion efficiency is found to be 8.0% for the pyrite CE and 7.5% for Pt, whereas with Co(III)/Co(II) redox DSSCs, efficiency is found to be the same for both pyrite and PEDOT (6.3%). The excellent performance of the pyrite CE in both the systems makes it a distinctive choice among the various CE materials studied.

The origins of performance enhancement in hybrid plasmonic organic photovoltaic devices are often embroiled in a complex interaction of light scattering, localized surface plasmon resonances, exciton-plasmon energy transfer and even nonplasmonic effects. To clearly deconvolve the plasmonic contributions from a single nanostructure, we herein investigate the influence of a single silver nanowire (NW) on the charge carriers in bulk heterojunction polymer solar cells using spatially resolved optical spectroscopy, and correlate to electrical device characterization. Polarization-dependent photocurrent enhancements with a maximum of ∼ 36% over the reference are observed when the transverse mode of the plasmonic excitations in the Ag NW is activated. The ensuing higher absorbance and light scattering induced by the electronic motion perpendicular to the NW long axis lead to increased exciton and polaron densities instead of direct surface plasmon-exciton energy transfer. Finite-difference time-domain simulations also validate these findings. Importantly, our study at the single nanostructure level explores the fundamental limits of plasmonic enhancement achievable in organic solar cells with a single plasmonic nanostructure.

Free-standing, ultrathin manganese dioxide nanoflakes were synthesized by cationic surfactant controlled reduction of KMnO4. MnO2 nanoflakes showed a much higher mass activity than other manganese based oxides as well as B and N doped nano carbons. The approach here demonstrates a facile chemical route towards efficient manganese dioxide catalysts.

Organic-inorganic metal halide perovskite solar cells were fabricated by laminating films of a carbon nanotube (CNT) network onto a CH3NH3PbI3 substrate as a hole collector, bypassing the energy-consuming vacuum process of metal deposition. In the absence of an organic hole-transporting material and metal contact, CH3NH3PbI3 and CNTs formed a solar cell with an efficiency of up to 6.87%. The CH3NH3PbI3/CNTs solar cells were semitransparent and showed photovoltaic output with dual side illuminations due to the transparency of the CNT electrode. Adding spiro-OMeTAD to the CNT network forms a composite electrode that improved the efficiency to 9.90% due to the enhanced hole extraction and reduced recombination in solar cells. The interfacial charge transfer and transport in solar cells were investigated through photoluminescence and impedance measurements. The flexible and transparent CNT network film shows great potential for realizing flexible and semitransparent perovskite solar cells.

In this work, we report a new cobalt(III) complex, tris[2-(1H-pyrazol-1-yl)pyrimidine]cobalt(III) tris[bis(trifluoromethylsulfonyl)imide] (MY11), with deep redox potential (1.27 V vs NHE) as dopant for 2,2',7,7'-tetrakis-(N,N-di-p-methoxyphenylamine)-9,9'-spirobifluorene (spiro-OMeTAD). This dopant possesses, to the best of our knowledge, the deepest redox potential among all cobalt-based dopants used in solar cell applications, allowing it to dope a wide range of hole-conductors. We demonstrate the tuning of redox potential of the Co dopant by incorporating pyrimidine moiety in the ligand. We characterize the optical and electrochemical properties of the newly synthesized dopant and show impressive spiro-to-spiro(+) conversion. Lastly, we fabricate high efficiency perovskite-based solar cells using MY11 as dopant for molecular hole-conductor, spiro-OMeTAD, to reveal the impact of this dopant in photovoltaic performance. An overall power conversion efficiency of 12% is achieved using MY11 as p-type dopant to spiro-OMeTAD., (© 2014 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.)

Low-temperature solution-processed materials that show optical gain and can be embedded into a wide range of cavity resonators are attractive for the realization of on-chip coherent light sources. Organic semiconductors and colloidal quantum dots are considered the main candidates for this application. However, stumbling blocks in organic lasing include intrinsic losses from bimolecular annihilation and the conflicting requirements of high charge carrier mobility and large stimulated emission; whereas challenges pertaining to Auger losses and charge transport in quantum dots still remain. Herein, we reveal that solution-processed organic-inorganic halide perovskites (CH3NH3PbX3 where X = Cl, Br, I), which demonstrated huge potential in photovoltaics, also have promising optical gain. Their ultra-stable amplified spontaneous emission at strikingly low thresholds stems from their large absorption coefficients, ultralow bulk defect densities and slow Auger recombination. Straightforward visible spectral tunability (390-790 nm) is demonstrated. Importantly, in view of their balanced ambipolar charge transport characteristics, these materials may show electrically driven lasing.

Mass transport has been identified as a limiting problem in the photovoltaic performance of dye-sensitized solar cells based on electrolytes consisting of ionic liquids or cobalt complexes. A mixed TiO2 macroporous-mesoporous morphology employed as photoanode is demonstrated to assist the diffusion of electrolytes with higher viscosity or consisting of bulky redox mediators, such as cobalt di-tert-butyl bipyridine [Co(dtb)3](2+/3+). This morphology with large pores improves the non-linearity of photocurrent response to light intensity indicating better diffusion. The incorporated sub-micrometer pores also reduce recombination and decrease diffusion resistance, as revealed by electrochemical impedance spectroscopy., (© 2014 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.)

The good electrical and morphological characteristics of TiO₂ nanofibers and the high extinction coefficient of CH₃NH₃PbI₃ perovskite are combined to obtain a solar cell with a power conversion efficiency of 9.8%. The increase of the film thickness dramatically diminishes the performance due to the reduction in porosity of the TiO₂ nanofiber framework. The optimum device (∼413 nm film thickness) is compared to a planar device, where the latter produces higher V(oc) but lower J(sc), and consequently lower efficiency at all measured light intensities.

The optical band gap of the light absorber and the alignment of its bands with the underlying wide band gap metal oxide are critical for efficient light harvesting and charge separation in semiconductor-sensitized solar cells (SSCs). In practice, these two requirements are however not always fulfilled concomitantly in SSCs. Favourable band alignment in CdSe-sensitized TiO2 requires utilization of quantum sized CdSe, which causes great losses in the harvesting of long wavelength photons due to quantum confinement effects. In the present study, ternary cadmium sulfoselenide (CdSxSe1-x), which has a tunable band gap between those of CdSe and CdS without reducing the dimension, was proposed as a sensitizer for TiO2. CdSxSe1-x was successfully synthesized by alternately depositing CdS and CdSe layers under ambient conditions. SSCs utilizing CdSxSe1-x-sensitized TiO2 yielded a power conversion efficiency of 4.05% under simulated AM1.5 100 mW cm(-2) illumination, rivalling the well-studied cascaded CdS/CdSe electrodes when an aqueous polysulfide solution was used as the electrolyte and Cu2S as the counter electrode. The findings of the present study provide an alternative and viable approach for optimizing the energetics of semiconductor sensitizers for efficient charge separation, while also maintaining good light harvesting.