Low-dimensional perovskites have-in view of their high radiative recombination rates-shown great promise in achieving high luminescence brightness and colour saturation. Here we investigate the ...effect of electron-phonon interactions on the luminescence of single crystals of two-dimensional perovskites, showing that reducing these interactions can lead to bright blue emission in two-dimensional perovskites. Resonance Raman spectra and deformation potential analysis show that strong electron-phonon interactions result in fast non-radiative decay, and that this lowers the photoluminescence quantum yield (PLQY). Neutron scattering, solid-state NMR measurements of spin-lattice relaxation, density functional theory simulations and experimental atomic displacement measurements reveal that molecular motion is slowest, and rigidity greatest, in the brightest emitter. By varying the molecular configuration of the ligands, we show that a PLQY up to 79% and linewidth of 20 nm can be reached by controlling crystal rigidity and electron-phonon interactions. Designing crystal structures with electron-phonon interactions in mind offers a previously underexplored avenue to improve optoelectronic materials' performance.
Perovskite nanocrystals (NCs) have attracted attention due to their high photoluminescence quantum yield (PLQY) in solution; however, maintaining high emission efficiency in the solid state remains a ...challenge. This study presents a solution‐phase synthesis of efficient green‐emitting perovskite NCs (CsPbBr3) embedded in robust and air‐stable rhombic prism hexabromide (Cs4PbBr6) microcrystals, reaching a PLQY of 90%. Theoretical modeling and experimental characterization suggest that lattice matching between the NCs and the matrix contribute to improved passivation, while spatial confinement enhances the radiative rate of the NCs. In addition, dispersing the NCs in a matrix prevents agglomeration, which explains their high PLQY.
Solution‐phase synthesis of efficient green‐emitting perovskite nanocrystal (NC) inclusions in rhombic prism microcrystals is presented. A theoretical model is built on the basis of experimental characterization of the material and further justified by means of density functional theory simulations. The potential of lattice‐matching between the NCs and the matrix strongly improves the interface, leading to high performance metrics in the solid‐state.
Store-operated Ca2+ entry (SOCE) is a major mechanism controlling Ca2+ signaling and Ca2+-dependent functions and has been implicated in immunity, cancer, and organ development. SOCE-dependent ...cytosolic Ca2+ signals are affected by mitochondrial Ca2+ transport through several competing mechanisms. However, how these mechanisms interact in shaping Ca2+ dynamics and regulating Ca2+-dependent functions remains unclear. In a recent issue, Yoast et al. shed light on these questions by defining multiple roles of the mitochondrial Ca2+ uniporter in regulating SOCE, Ca2+ dynamics, transcription, and lymphocyte activation.
Mitochondria are essential for proper cellular function through their critical roles in ATP synthesis, reactive oxygen species production, calcium (Ca
) buffering, and apoptotic signaling. In ...neurons, Ca
buffering is particularly important as it helps to shape Ca
signals and to regulate numerous Ca
-dependent functions including neuronal excitability, synaptic transmission, gene expression, and neuronal toxicity. Over the past decade, identification of the mitochondrial Ca
uniporter (MCU) and other molecular components of mitochondrial Ca
transport has provided insight into the roles that mitochondrial Ca
regulation plays in neuronal function in health and disease. In this review, we discuss the many roles of mitochondrial Ca
uptake and release mechanisms in normal neuronal function and highlight new insights into the Ca
-dependent mechanisms that drive mitochondrial dysfunction in neurologic diseases including epilepsy, Alzheimer's disease, Parkinson's disease, and amyotrophic lateral sclerosis. We also consider how targeting Ca
uptake and release mechanisms could facilitate the development of novel therapeutic strategies for neurological diseases.
Organo-metal halide perovskites are a promising platform for optoelectronic applications in view of their excellent charge-transport and bandgap tunability. However, their low photoluminescence ...quantum efficiencies, especially in low-excitation regimes, limit their efficiency for light emission. Consequently, perovskite light-emitting devices are operated under high injection, a regime under which the materials have so far been unstable. Here we show that, by concentrating photoexcited states into a small subpopulation of radiative domains, one can achieve a high quantum yield, even at low excitation intensities. We tailor the composition of quasi-2D perovskites to direct the energy transfer into the lowest-bandgap minority phase and to do so faster than it is lost to nonradiative centers. The new material exhibits 60% photoluminescence quantum yield at excitation intensities as low as 1.8 mW/cm2, yielding a ratio of quantum yield to excitation intensity of 0.3 cm2/mW; this represents a decrease of 2 orders of magnitude in the excitation power required to reach high efficiency compared with the best prior reports. Using this strategy, we report light-emitting diodes with external quantum efficiencies of 7.4% and a high luminescence of 8400 cd/m2.
Colloidal quantum dot (CQD) solar cells are solution-processed photovoltaics with broad spectral absorption tunability. Major advances in their efficiency have been made via improved CQD surface ...passivation and device architectures with enhanced charge carrier collection. Herein, we demonstrate a new strategy to improve further the passivation of CQDs starting from the solution phase. A cosolvent system is employed to tune the solvent polarity in order to achieve the solvation of methylammonium iodide (MAI) and the dispersion of hydrophobic PbS CQDs simultaneously in a homogeneous phase, otherwise not achieved in a single solvent. This process enables MAI to access the CQDs to confer improved passivation. This, in turn, allows for efficient charge extraction from a thicker photoactive layer device, leading to a certified solar cell power conversion efficiency of 10.6%, a new certified record in CQD photovoltaics.
Organometallic trihalide perovskites are solution-processed semiconductors that have made great strides in third-generation thin film light-harvesting and light-emitting optoelectronic devices. ...Recently, it has been demonstrated that large, high-purity single crystals of these perovskites can be synthesized from the solution phase. These crystals’ large dimensions, clean bandgap, and solid-state order have provided us with a suitable medium to observe and quantify two-photon absorption in perovskites. When CH3NH3PbBr3 single crystals are pumped with intense 800 nm light, we observe band-to-band photoluminescence at 572 nm, indicative of two-photon absorption. We report the nonlinear absorption coefficient of CH3NH3PbBr3 perovskites to be 8.6 cm GW–1 at 800 nm, comparable to epitaxial single-crystal semiconductors of similar bandgap. We have leveraged this nonlinear process to electrically autocorrelate a 100 fs pulsed laser using a two-photon perovskite photodetector. This work demonstrates the viability of organometallic trihalide perovskites as a convenient and low-cost nonlinear absorber for applications in ultrafast photonics.
Efficient wide-bandgap perovskite solar cells (PSCs) enable high-efficiency tandem photovoltaics when combined with crystalline silicon and other low-bandgap absorbers. However, wide-bandgap PSCs ...today exhibit performance far inferior to that of sub-1.6-eV bandgap PSCs due to their tendency to form a high density of deep traps. Here, we show that healing the deep traps in wide-bandgap perovskites-in effect, increasing the defect tolerance via cation engineering-enables further performance improvements in PSCs. We achieve a stabilized power conversion efficiency of 20.7% for 1.65-eV bandgap PSCs by incorporating dipolar cations, with a high open-circuit voltage of 1.22 V and a fill factor exceeding 80%. We also obtain a stabilized efficiency of 19.1% for 1.74-eV bandgap PSCs with a high open-circuit voltage of 1.25 V. From density functional theory calculations, we find that the presence and reorientation of the dipolar cation in mixed cation-halide perovskites heals the defects that introduce deep trap states.
Bandtail states in disordered semiconductor materials result in losses in open-circuit voltage (V
) and inhibit carrier transport in photovoltaics. For colloidal quantum dot (CQD) films that promise ...low-cost, large-area, air-stable photovoltaics, bandtails are determined by CQD synthetic polydispersity and inhomogeneous aggregation during the ligand-exchange process. Here we introduce a new method for the synthesis of solution-phase ligand-exchanged CQD inks that enable a flat energy landscape and an advantageously high packing density. In the solid state, these materials exhibit a sharper bandtail and reduced energy funnelling compared with the previous best CQD thin films for photovoltaics. Consequently, we demonstrate solar cells with higher V
and more efficient charge injection into the electron acceptor, allowing the use of a closer-to-optimum bandgap to absorb more light. These enable the fabrication of CQD solar cells made via a solution-phase ligand exchange, with a certified power conversion efficiency of 11.28%. The devices are stable when stored in air, unencapsulated, for over 1,000 h.
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