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Abstract Tuning the properties of a pair of entangled electron and hole in a light-induced exciton is a fundamentally intriguing inquiry for quantum science. Here, using semiconducting hybrid perovskite as an exploratory platform, we discover that Nd²⁺-doped CH₃NH₃PbI₃(MAPbI₃) perovskite exhibits a Kondo-like exciton-spin interaction under cryogenic and photoexcitation conditions. The feedback to such interaction between excitons in perovskite and the localized spins in Nd²⁺is observed as notably prolonged carrier lifetimes measured by time-resolved photoluminescence, ~10 times to that of pristine MAPbI₃without Nd²⁺dopant. From a mechanistic standpoint, such extended charge separation states are the consequence of the trap state enabled by the antiferromagnetic exchange interaction between the light-induced exciton and the localized 4 fspins of the Nd²⁺in the proximity. Importantly, this Kondo-like exciton-spin interaction can be modulated by either increasing Nd²⁺doping concentration that enhances the coupling between the exciton and Nd²⁺4 fspins as evidenced by elongated carrier lifetime, or by using an external magnetic field that can nullify the spin-dependent exchange interaction therein due to the unified orientations of Nd²⁺spin angular momentum, thereby leading to exciton recombination at the dynamics comparable to pristine MAPbI₃. 

With the rapid development of perovskite solar cells (PSCs), lowering fabrication costs for PSCs has become a prominent challenge for commercialization. At present, gold is commonly used as the back metal electrode in state-of-the-art n-i-p structured PSCs due to its compatible work function, chemical inertness, and high conductivity. However, the high cost of gold and the expensive and time-consuming vacuum-based thin-film coating facilities may impede large-scale industrialization of PSCs. Here, we report a bilayer back electrode configuration consisting of an Ni-doped natural graphite layer with a fusible Bi-In alloy. This back electrode can be deposited in a vacuum-free approach and enables PSCs with a power conversion efficiency of 21.0%. These inexpensive materials and facile ambient fabrication techniques provide an appealing disruptive solution to low-cost PSC industrialization. 

Abstract In hybrid perovskite solar cells (PSCs), the reaction of hydrogens (H) located in the amino group of the organic A-site cations with their neighboring halides plays a central role in degradation. Inspired by the retarded biological activities of cells in heavy water, we replaced the light H atom with its abundant, twice-as-heavy, nonradioactive isotope, deuterium (D) to hamper the motion of H. This D substitution retarded the formation kinetics of the detrimental H halides in Pb-based PSCs, as well as the H bond-mediated oxidation of Sn2+ in Sn–Pb-based narrow-bandgap PSCs, evidenced by accelerated stability studies. A computational study indicated that the zero point energy of D-based formamidinium (FA) is lower than that of pristine FA. In addition, the smaller increase in entropy in D-based FA than in pristine FA accounts for the increased formation free energy of the Sn2+ vacancies, which leads to the retarded oxidation kinetics of Sn2+. In this study, we show that substituting active H with D in organic cations is an effective way to enhance the stability of PSCs without sacrificing photovoltaic (PV) performance. This approach is also adaptable to other stabilizing methods. 

High-performance optoelectronic devices, such as solar cells and light-emitting diodes, have been fabricated with lead halide perovskites owing to their superior carrier properties. However, charge transport in such optoelectronics is intrinsically directional due to the existence of p–n junctions, which thus lacks the potential to elucidate any perturbations in light or electricity during energy conversion. Here, with the presence of a LiCl additive in a formamidinium chloride (FACl) solution, the as-grown LiCl:FAPbCl 3 nanorods demonstrate greatly enhanced crystallinity and UV photoresponse as compared to pristine FAPbCl 3 nanostructures without the LiCl additive. Most importantly, the LiCl:FAPbCl 3 nanorod film exhibits unprecedented distinguishability to UV photons with different energies and oscillating intensities, in the form of bipolar and periodically oscillatory photocurrents. This work could advance the fundamental understanding of photoinduced carrier processes in halide perovskites and facilitate the development of novel UV-based optical communications.