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Inverted planar perovskite solar cells offer opportunities for a simplified device structure compared with conventional mesoporous titanium oxide interlayers. However, their lower open-circuit voltages result in lower power conversion efficiencies. Using mixed-cation lead mixed-halide perovskite and a solution-processed secondary growth method, Luo et al. created a surface region in the perovskite film that inhibited nonradiative charge-carrier recombination. This kind of solar cell had comparable performance to that of conventional cells. Science , this issue p. 1442 High open-circuit voltages were achieved for planar perovskite solar cells by creating a graded junction. The highest power conversion efficiencies (PCEs) reported for perovskite solar cells (PSCs) with inverted planar structures are still inferior to those of PSCs with regular structures, mainly because of lower open-circuit voltages ( V oc ). Here we report a strategy to reduce nonradiative recombination for the inverted devices, based on a simple solution-processed secondary growth technique. This approach produces a wider bandgap top layer and a more n-type perovskite film, which mitigates nonradiative recombination, leading to an increase in V oc by up to 100 millivolts. We achieved a high V oc of 1.21 volts without sacrificing photocurrent, corresponding to a voltage deficit of 0.41 volts at a bandgap of 1.62 electron volts. This improvement led to a stabilized power output approaching 21% at the maximum power point.

The performance of semiconductor devices is fundamentally governed by charge-carrier dynamics within the active materials 1 – 6 . Although advances have been made towards understanding these dynamics under steady-state conditions, the importance of non-equilibrium phenomena and their effect on device performances remains elusive 7 , 8 . In fact, the ballistic propagation of carriers is generally considered to not contribute to the mechanism of photovoltaics (PVs) and light-emitting diodes, as scattering rapidly disrupts such processes after carrier generation via photon absorption or electric injection 9 . Here we characterize the spatiotemporal dynamics of carriers immediately after photon absorption in methylammonium lead iodide perovskite films using femtosecond transient absorption microscopy (fs-TAM) with a 10 fs temporal resolution and 10 nm spatial precision. We found that non-equilibrium carriers propagate ballistically over 150 nm within 20 fs of photon absorption. Our results suggest that in a typical perovskite PV device operating under standard conditions, a large fraction of carriers can reach the charge collection layers ballistically. The ballistic transport distance appears to be limited by energetic disorder within the materials, probably due to disorder-induced scattering. This provides a direct route towards optimization of the ballistic transport distance via improvements in materials and by minimizing the energetic disorder. Our observations reveal an unexplored regime of carrier transport in perovskites, which could have important consequences for device performance. Charge-carrier dynamics are fundamental to the operation and performance of semiconductor devices. In methylammonium lead iodide perovskites, carriers in the non-equilibrium regime after excitation propagate ballistically over 150 nm within 20 fs.

Charge transport in conjugated polymer semiconductors has traditionally been thought to be limited to a low-mobility regime by pronounced energetic disorder. Much progress has recently been made in advancing carrier mobilities in field-effect transistors through developing low-disorder conjugated polymers. However, in diodes these polymers have to date not shown much improved mobilities, presumably reflecting the fact that in diodes lower carrier concentrations are available to fill up residual tail states in the density of states. Here, we show that the bulk charge transport in low-disorder polymers is limited by water-induced trap states and that their concentration can be dramatically reduced through incorporating small molecular additives into the polymer film. Upon incorporation of the additives we achieve space-charge limited current characteristics that resemble molecular single crystals such as rubrene with high, trap-free SCLC mobilities up to 0.2 cm 2 /Vs and a width of the residual tail state distribution comparable to k B T . Charge transport in organic diodes based on conjugated polymers is severely limited by the high water-related trap concentration and energetic disorder. Here, the authors report high-mobility trap-free charge transport in low-disorder conjugated polymers by incorporating small molecular additives.

Perovskite light-emitting diodes (PeLEDs) based on three-dimensional (3D) polycrystalline perovskites suffer from ion migration, which causes overshoot of luminance over time during operation and reduces its operational lifetime. Here, we demonstrate 3D/2D hybrid PeLEDs with extremely reduced luminance overshoot and 21 times longer operational lifetime than 3D PeLEDs. The luminance overshoot ratio of 3D/2D hybrid PeLED is only 7.4% which is greatly lower than that of 3D PeLED (150.4%). The 3D/2D hybrid perovskite is obtained by adding a small amount of neutral benzylamine to methylammonium lead bromide, which induces a proton transfer from methylammonium to benzylamine and enables crystallization of 2D perovskite without destroying the 3D phase. Benzylammonium in the perovskite lattice suppresses formation of deep-trap states and ion migration, thereby enhances both operating stability and luminous efficiency based on its retardation effect in reorientation. Ion migration can induce overshoot of luminance in normal 3D perovskite light-emitting diode devices and results in reduced lifetime. Here Kim et al. show that the ion migration and overshoot can be suppressed in 3D/2D hybrid perovskites, leading to 21 times longer operational lifetime.

Electroluminescence efficiencies of metal halide perovskite nanocrystals (PNCs) are limited by a lack of material strategies that can both suppress the formation of defects and enhance the charge carrier confinement. Here we report a one-dopant alloying strategy that generates smaller, monodisperse colloidal particles (confining electrons and holes, and boosting radiative recombination) with fewer surface defects (reducing non-radiative recombination). Doping of guanidinium into formamidinium lead bromide PNCs yields limited bulk solubility while creating an entropy-stabilized phase in the PNCs and leading to smaller PNCs with more carrier confinement. The extra guanidinium segregates to the surface and stabilizes the undercoordinated sites. Furthermore, a surface-stabilizing 1,3,5-tris(bromomethyl)-2,4,6-triethylbenzene was applied as a bromide vacancy healing agent. The result is highly efficient PNC-based light-emitting diodes that have current efficiency of 108 cd A−1 (external quantum efficiency of 23.4%), which rises to 205 cd A−1 (external quantum efficiency of 45.5%) with a hemispherical lens.Guanidinium doping is shown to enhance the operation of perovskite nanocrystal light-emitting diodes.

Metal-halide perovskites are at the frontier of optoelectronic research due to solution processability and excellent semiconductor properties. Here we use transient absorption spectroscopy to study hot-carrier distributions in CH 3 NH 3 PbI 3 and quantify key semiconductor parameters. Above bandgap, non-resonant excitation creates quasi-thermalized carrier distributions within 100 fs. During carrier cooling, a sub-bandgap transient absorption signal arises at ∼1.6 eV, which is explained by the interplay of bandgap renormalization and hot-carrier distributions. At higher excitation densities, a ‘phonon bottleneck’ substantially slows carrier cooling. This effect indicates a low contribution from inelastic carrier-impurity or phonon–impurity scattering in these polycrystalline materials, which supports high charge-carrier mobilities. Photoinduced reflectivity changes distort the shape of transient absorption spectra and must be included to extract physical constants. Using a simple band-filling model that accounts for these changes, we determine a small effective mass of m r =0.14 m o , which agrees with band structure calculations and high photovoltaic performance. The use of organic–inorganic metal-halide perovskites in hot-carrier devices depends on deepening the understanding of photoexcitations in these materials. Here, Price et al. use transient absorption spectroscopy to study hot-carrier distributions in CH 3 NH 3 PbI 3 and quantify key semiconductors parameters.

Organic-inorganic hybrid perovskites are emerging low-cost emitters with very high color purity, but their low luminescent efficiency is a critical drawback. We boosted the current efficiency (CE) of perovskite light-emitting diodes with a simple bilayer structure to 42.9 candela per ampere, similar to the CE of phosphorescent organic light-emitting diodes, with two modifications: We prevented the formation of metallic lead (Pb) atoms that cause strong exciton quenching through a small increase in methylammonium bromide (MABr) molar proportion, and we spatially confined the exciton in uniform MAPbBr₃ nanograins (average diameter = 99.7 nanometers) formed by a nanocrystal pinning process and concomitant reduction of exciton diffusion length to 67 nanometers. These changes caused substantial increases in steady-state photoluminescence intensity and efficiency of MAPbBr₃ nanograin layers.

Due to their low-temperature processing properties and inherent mechanical flexibility, conjugated polymer field-effect transistors (FETs) are promising candidates for enabling flexible electronic circuits and displays. Much progress has been made on materials performance; however, there remain significant concerns about operational and environmental stability, particularly in the context of applications that require a very high level of threshold voltage stability, such as active-matrix addressing of organic light-emitting diode displays. Here, we investigate the physical mechanisms behind operational and environmental degradation of high-mobility, p-type polymer FETs and demonstrate an effective route to improve device stability. We show that water incorporated in nanometre-sized voids within the polymer microstructure is the key factor in charge trapping and device degradation. By inserting molecular additives that displace water from these voids, it is possible to increase the stability as well as uniformity to a high level sufficient for demanding industrial applications. Small molecular additives incorporated into films of conjugate polymers are shown to fill the voids present in the polymer network. As a result, the stability of organic transistors based on these materials is significantly improved.

Measurements and simulations of several high-mobility conjugated polymers show that their charge transport properties reflect an almost complete lack of disorder in the polymers, despite their amorphous microstructures, resulting from the resilience of the planar polymer backbone conformations to side-chain disorder. Bringing order to disorder So-called 'conjugated polymers' have attracted much interest in recent decades. They are organic macromolecules with covalent-bond-containing backbone structures that combine the flexibility and processibility of plastics with the useful electronic properties of semiconductors. Polymeric materials tend to be naturally disordered however, and such disorder ultimately limits their electronic performance. Deepak Venkateshvaran and colleagues now show that several of the better-performing conjugated polymers are actually behaving electronically as if they were free of disorder, despite their amorphous microstructure. With the aid of simulations, the authors identify the molecular origins of this surprising 'disorder-free' behaviour, and offer guidelines for how this might be engineered into other conjugated polymeric systems. Conjugated polymers enable the production of flexible semiconductor devices that can be processed from solution at low temperatures. Over the past 25 years, device performance has improved greatly as a wide variety of molecular structures have been studied 1 . However, one major limitation has not been overcome; transport properties in polymer films are still limited by pervasive conformational and energetic disorder 2 , 3 , 4 , 5 . This not only limits the rational design of materials with higher performance, but also prevents the study of physical phenomena associated with an extended π-electron delocalization along the polymer backbone. Here we report a comparative transport study of several high-mobility conjugated polymers by field-effect-modulated Seebeck, transistor and sub-bandgap optical absorption measurements. We show that in several of these polymers, most notably in a recently reported, indacenodithiophene-based donor–acceptor copolymer with a near-amorphous microstructure 6 , the charge transport properties approach intrinsic disorder-free limits at which all molecular sites are thermally accessible. Molecular dynamics simulations identify the origin of this long sought-after regime as a planar, torsion-free backbone conformation that is surprisingly resilient to side-chain disorder. Our results provide molecular-design guidelines for ‘disorder-free’ conjugated polymers.

In lead halide perovskite solar cells, there is at least one recycling event of electron–hole pair to photon to electron–hole pair at open circuit under solar illumination. This can lead to a significant reduction in the external photoluminescence yield from the internal yield. Here we show that, for an internal yield of 70%, we measure external yields as low as 15% in planar films, where light out-coupling is inefficient, but observe values as high as 57% in films on textured substrates that enhance out-coupling. We analyse in detail how externally measured rate constants and photoluminescence efficiencies relate to internal recombination processes under photon recycling. For this, we study the photo-excited carrier dynamics and use a rate equation to relate radiative and non-radiative recombination events to measured photoluminescence efficiencies. We conclude that the use of textured active layers has the ability to improve power conversion efficiencies for both LEDs and solar cells. Recombinations govern losses in solar cells. Here, Richter et al . use transient spectroscopy to evaluate how re-absorption and re-emission of photons in perovskite absorbers affect intrinsic recombination coefficients, and to differentiate between external and internal photoluminescence quantum yields.