The study of the photophysical properties of organic-metallic lead halide perovskites, which demonstrate excellent photovoltaic performance in devices with electron- and hole-accepting layers, helps to understand their charge photogeneration and recombination mechanism and unravels their potential for other optoelectronic applications. We report surprisingly high photoluminescence (PL) quantum efficiencies, up to 70%, in these solution-processed crystalline films. We find that photoexcitation in the pristine CH3NH3PbI3-xClx perovskite results in free charge carrier formation within 1 ps and that these free charge carriers undergo bimolecular recombination on time scales of 10s to 100s of ns. To exemplify the high luminescence yield of the CH3NH3PbI3-xClx perovskite, we construct and demonstrate the operation of an optically pumped vertical cavity laser comprising a layer of perovskite between a dielectric mirror and evaporated gold top mirrors. These long carrier lifetimes together with exceptionally high luminescence yield are unprecedented in such simply prepared inorganic semiconductors, and we note that these properties are ideally suited for photovoltaic diode operation.

Metal-halide perovskite light-absorbers have risen to the forefront of photovoltaics research offering the potential to combine low-cost fabrication with high power-conversion efficiency. Much of the development has been driven by empirical optimisation strategies to fully exploit the favourable electronic properties of the absorber layer. To build on this progress, a full understanding of the device operation requires a thorough optical analysis of the device stack, providing a platform for maximising the power conversion efficiency through a precise determination of parasitic losses caused by coherence and absorption in the non-photoactive layers. Here we use an optical model based on the transfer-matrix formalism for analysis of perovskite-based planar heterojunction solar cells using experimentally determined complex refractive index data. We compare the modelled properties to experimentally determined data, and obtain good agreement, revealing that the internal quantum efficiency in the solar cells approaches 100%. The modelled and experimental dependence of the photocurrent on incidence angle exhibits only a weak variation, with very low reflectivity losses at all angles, highlighting the potential for useful power generation over a full daylight cycle

We present a material assembly route for the manufacture of dye-sensitized solar cells, coupling a high-surface mesoporous layer to a three-dimensional photonic crystal (PC). Material synthesis aided by self-assembly on two length scales provided electrical and pore connectivity at the mesoporous and the microporous level. This construct allows effective dye sensitization, electrolyte infiltration, and charge collection from both the mesoporous and the PC layers, opening up additional parameter space for effective light management by harvesting PC-induced resonances.KEYWORDS Photonic crystal, self-assembly, photovoltaics, dye-sensitized solar cell E ver since the pioneering work of O'Regan and Grät-zel, dye-sensitized solar cells (DSCs) have attracted great interest as a promising technology for future sustainable energy generation. 1 In DSCs, charge carrier generation takes place in a chemisorbed monolayer of photoactive dye which is sandwiched between a semiconductor oxide, usually mesoscopic anatase, and an electrolyte acting as electron and hole conducting materials, respectively. Using state-of-the-art ruthenium-based inorganic dyes, efficiencies higher than 11% have been reported. [2][3][4] DSCs are generally made from cheap and nontoxic components and can be designed in a variety of different colors and transparencies, which distinguishes them as an ideal photovoltaic concept for integrated architecture. It therefore seems only a matter of time before large scale production will follow. 5 In general, improvements in the overall power conversion efficiency have been centered on increasing the photovoltage through manipulation of the oxide, improving the photocurrent with new dyes, and increasing stability by better encapsulation. 5 While record-holding liquid electrolyte DSCs already achieve maximum quantum efficiency (photon-toelectron conversion) in the spectral range around 520 nm, light harvesting in the red and near-infrared (at the tail of the absorption spectra) is still relatively low. In solid-state devices, light absorption is generally limited by the film thickness, as thick mesoporous films prove difficult to infiltrate. 6 One way to successfully enhance light harvesting is the introduction of optical elements, such as highly scattering layers. These consist of large particles, that increase the photon path length in the cell. 7,8 This ubiquitous approach has the unfortunate effect of rendering the DSC opaque thus depriving it of one of its main advantages over competing technologies. As a result, photonic band gap materials in the form of 3D inverted TiO 2 opal or porous bragg stacks have been applied to DSCs to enhance light harvesting in specific partsofthespectrumwhileretainingthecelltransparency. 9-12 Several theoretical approaches report a variety of possible effects, including the localization of heavy photons near the edges of a photonic bandgap, 13 Bragg diffraction in a periodic lattice, 14 multiple scattering at disordered regions in the photonic crystal (PC), 15 and the for...

The miscibility and aggregation of PCBM ([6,6]-phenyl-C 61 -butyric acid methyl ester) in a polymer matrix is of great importance for the development of fullerene-based organic photovoltaic cells (OPVs). In this study we have systematically investigated the loading of PCBM in regioregular and regiorandom P3HT (poly(3-hexylthiophene-2,5-diyl). Using optical microscopy, we demonstrate the partial miscibility of PCBM in thermally annealed P3HT films and relate it to the relative crystallinity of P3HT. The low polydispersity and the nearly 100% regioregularity of a self-synthesized P3HT allowed a detailed X-ray characterization as a function of PCBM content, revealing a superstructure of periodic amorphous and crystalline lamellar domains of fully chain extended polymer chains. PCBM dissolves in the amorphous interlamellar P3HT regions (partially indexmatching the X-ray scattering contrast) up to a threshold, above which PCBM aggregates start to form. These results show that crystallization of P3HT into 10-nm-wide lamellar domains sets the main length scale in P3HT/PCBM structure formation. PCBM is displaced into the amorphous intralamellar regions, swelling the lamellar stack. This structure formation by crystallization, which is intrinsic to most semicrystalline polymers, followed by the enrichment, segregation, and crystallization of PCBM provides an interdigitated structure, which is conceptually ideal for excitonic solar cells.

following statement: These materials can be processed from solution and yet exhibit optoelectronic materials properties described in classic solid-state physics textbooks. This unprecedented combination has led to photovoltaic devices that can be processed at room temperature and achieve performance levels similar to industry giant polycrystalline silicon, from a starting point of 3.8% in 2009. [1][2][3][4] The first light-emitting electrochemical cells [5] and diodes [6][7][8] have also been introduced recently, leading to tunable light emission spectra and internal quantum efficiencies exceeding 15%.The road towards these achievements has been marked by a constant improvement of perovskite deposition techniques fueled by our increasing understanding of the crystallization processes. The choice of deposition technique, either from solution or vapor, and the composition and order in which precursor species are applied has a great influence on the crystallization kinetics. Here, one can distinguish one-step methods where the perovskite is formed from a precursor mixture dissolved in a common solution, and two-step methods where the inorganic compound is deposited first and transformed to the perovskite phase later by addition of the organic constituents. [9][10][11] Furthermore, many parameters during processing can have an effect on the crystallization mechanism and consequently on film morphology, such as the choice of solvents, concentrations and processing additives that are often not incorporated into the final product. [11][12][13] We discuss this aspect in Section 2, where we focus our attention on the most commonly employed solution-based techniques. Additionally, as for any new technology trying to displace an incumbent technology, higher efficiencies, lower costs, reproducibility, stability, and sustainability are paramount. In particular, reproducibility has been a major challenge in perovskite solar cells from the beginning: small variations in morphology, like crystal size, film roughness, and pinholes can have detrimental effects on photovoltaic performance. [14] On the other hand, current-voltage measurements often showed a hysteresis that is rarely seen in other photovoltaic technologies. [15] These topics are highlighted in Sections 3 and 4. Finally, in Section 5 we discuss the framework for market introduction, such as cost reduction by choosing low-cost charge transport layers, or how the lifetime of perovskite absorbers can be extended by the choice of materials composition.Hybrid metal halide perovskites have become one of the hottest topics in optoelectronic materials research in recent years. Not only have they surpassed everyone's expectations and achieved similar performance as tried and true polycrystalline silicon photovoltaic devices, but they are also finding applications in a variety of different fields, including lighting. The main advantages of hybrid metal halide perovskites are simple processability, compatible with large-scale solution processing such as roll-to-roll printing, a...

Proper percolation of charges in solar cells is possible with the self‐assembled nanostructure of a block‐copolymer film (see the TEM cross section of a solar cell). A photovoltaic device made from such a block copolymer exhibits a ten‐times higher short circuit current and a considerably larger photovoltage than its polymer‐blend analogue.

In this paper, we demonstrate a double nanoimprinting process that allows the formation of nanostructured polymer heterojunctions of composition and morphology that can be selected independently. We fabricated photovoltaic (PV) devices with extremely high densities (10(14)/mm(2)) of interpenetrating nanoscale columnar features in the active polymer blend layer. The smallest feature sizes are as small as 25 nm on a 50 nm pitch, which results in a spacing of heterojunctions at or below the exciton diffusion length. Photovoltaic devices based on double-imprinted poly((9,9-dioctylfluorene)-2,7-diyl-alt-[4,7-bis(3-hexylthien-5-yl)-2,1,3-benzothiadiazole]-2',2''-diyl) (F8TBT)/ poly(3-hexylthiophene) (P3HT) films are among the best polymer-polymer blend devices reported to date with a power conversion efficiency (PCE, eta(e)) of 1.9%.

Recently, solution-processable organic-inorganic metal halide perovskites have come to the fore as a result of their high power-conversion efficiencies (PCE) in photovoltaics, exceeding 17%. To attain reproducibility in the performance, one of the critical factors is the processing conditions of the perovskite film, which directly influences the photophysical properties and hence the device performance. Here we study the effect of annealing parameters on the crystal structure of the perovskite films and correlate these changes with its photophysical properties. We find that the crystal formation is kinetically driven by the annealing atmosphere, time and temperature. Annealing in air produces an improved crystallinity and large grain domains as compared to nitrogen. Lower photoluminescence quantum efficiency (PLQE) and shorter photoluminescence (PL) lifetimes are observed for nitrogen annealed perovskite films as compared to the air-annealed counterparts. We note that the limiting nonradiative pathways (i.e., maximizing PLQE) is important for obtaining the highest device efficiency. This indicates a critical impact of the atmosphere upon crystallization and the ultimate device performance.