In lead halide perovskites, organic A-site cations are generally introduced to fine-tune the properties. One of the questions under debate is whether organic A-site cations are essential for high-performance solar cells. In this study, we compare the band edge carrier dynamics and diffusion process in MAPbBr3 and CsPbBr3 single-crystal microplates. By transient absorption microscopy, the band-edge carrier diffusion constants are unraveled. With the replacement of inorganic A-site cations, the diffusion constant in CsPbBr3 increases almost 8 times compared to that in MAPbBr3. This work reveals that introducing inorganic A-site cations can lead to a much larger diffusion length and improve the performance of band-edge carriers.

The electron-phonon interaction is known as one of the major mechanisms determining electrical and thermal properties. In particular, it alters the carrier transport behaviors and sets fundamental limits to carrier mobility. Establishing how electrons interact with phonons and the resulting impact on the carrier transport property is significant for the development of high-efficiency electronic devices. Here, carrier transport behavior mediated by the electron-phonon coupling in BiFeO3 epitaxial thin films is directly observed. Acoustic phonons are generated by the inverse piezoelectric effect and coupled with photocarriers. Via the electron-phonon coupling, doughnut shape carrier distribution has been observed due to the coupling between hot carriers and phonons. The hot carrier quasi-ballistic transport length can reach 340 nm within 1 ps. The results suggest an effective approach to investigating the effects of electron-phonon interactions with temporal and spatial resolutions, which is of great importance for designing and improving electronic devices.

Various exciton species in transition metal dichalcogenides (TMDs), such as neutral excitons, trions (charged excitons), dark excitons, and biexcitons, have been individually discovered with distinct light-matter interactions. In terms of valley-spin locked band structures and electron-hole configurations, these exciton species demonstrate flexible control of emission light with degrees of freedom (DOFs) such as intensity, polarization, frequency, and dynamics. However, it remains elusive to fully manipulate different exciton species on demand for practical photonic applications. Here, we investigate the contrasting light-matter interactions to control multiple DOFs of emission light in a hybrid monolayer WSe2-Ag nanowire (NW) structure by taking advantage of various exciton species. These excitons, including trions, dark excitons, and biexcitons, are found to couple independently with propagating surface plasmon polaritons (SPPs) of Ag NW in quite different ways, thanks to the orientations of transition dipoles. Consistent with the simulations, the dark excitons and dark trions show extremely high coupling efficiency with SPPs, while the trions demonstrate directional chiral-coupling features. This study presents a crucial step towards the ultimate goal of exploiting the comprehensive spectrum of TMD excitons for optical information processing and quantum optics.

Perovskite solar cells have shown remarkable efficiencies beyond 22%, through organic and inorganic cation alloying. However, the role of alkali-metal cations is not well-understood. By using synchrotron-based nano-X-ray fluorescence and complementary measurements, we show that when adding RbI and/or CsI the halide distribution becomes homogenous. This homogenization translates into long-lived charge carrier decays, spatially homogenous carrier dynamics visualized by ultrafast microscopy, as well as improved photovoltaic device performance. We find that Rb and K phase-segregate in highly concentrated aggregates. Synchrotron-based X-ray-beam-induced current and electron-beam-induced current of solar cells show that Rb clusters do not contribute to the current and are recombination active. Our findings bring light to the beneficial effects of alkali metal halides in perovskites, and point at areas of weakness in the elemental composition of these complex perovskites, paving the way to improved performance in this rapidly growing family of materials for solar cell applications.

Formamidinium lead iodide (FAPbI₃) perovskites are promising emitters for near-infrared light-emitting diodes. However, their performance is still limited by defect-assisted nonradiative recombination and band offset-induced carrier aggregation at the interface. Herein, we introduce a couple of cadmium salts with acetate or halide anion into the FAPbI₃ perovskite precursors to synergistically passivate the material defects and optimize the device band structure. Particularly, the perovskite analogs, containing zero-dimensional formamidinium cadmium iodide, one-dimensional δ-FAPbI₃, two-dimensional FA₂FA_n-1Pb_nI_3n+1, and three-dimensional α-FAPbI₃, can be obtained in one pot and play a pivotal and positive role in energy transfer in the formamidinium iodide-rich lead-based perovskite films. As a result, the near-infrared FAPbI₃-based devices deliver a maximum external quantum efficiency of 24.1% together with substantially improved operational stability. Combining our findings on defect passivation and energy transfer, we also achieve near-infrared light communication with device twins of light emitting and unprecedented self-driven detection.

The role of the alkali metal cations in halide perovskite solar cells is not well understood. Using synchrotron-based nano-x-ray fluorescence and complementary measurements, we found that the halide distribution becomes homogenized upon addition of cesium iodide, either alone or with rubidium iodide, for substoichiometric, stoichiometric, and overstoichiometric preparations, where the lead halide is varied with respect to organic halide precursors. Halide homogenization coincides with long-lived charge carrier decays, spatially homogeneous carrier dynamics (as visualized by ultrafast microscopy), and improved photovoltaic device performance. We found that rubidium and potassium phase-segregate in highly concentrated clusters. Alkali metals are beneficial at low concentrations, where they homogenize the halide distribution, but at higher concentrations, they form recombination-active second-phase clusters.