The low efficiency triplet emission of hybrid copper(I) iodide clusters is a critical obstacle to their further practical optoelectronic application. Herein, we present an efficient hybrid copper(I) iodide cluster emitter (DBA)4Cu4I4, where the cooperation of excited state structure reorganization and the metallophilicity interaction enables ultra‐bright triplet yellow‐orange emission with a photoluminescence quantum yield over 94.9 %, and the phonon‐assisted de‐trapping process of exciton induces the negative thermal quenching effect at 80–300 K. We also investigate the potential of this emitter for X‐ray imaging. The (DBA)4Cu4I4 wafer demonstrates a light yield higher than 104 photons MeV−1 and a high spatial resolution of ≈5.0 lp mm−1, showing great potential in practical X‐ray imaging applications. Our new copper(I) iodide cluster emitter can serve as a model for investigating the thermodynamic mechanism of photoluminescence in hybrid copper(I) halide phosphorescence materials.
However, these devices can only be operated at cryogenic temperature. As temperature increases, the spin polarizations are quickly randomized by thermal fluctuation with the thermal energy (25 meV at 293 K) much larger than the Zeeman energy splitting. [6,10] Great efforts have been made to promote the room temperature (RT) spin-polarization, and few studies successfully used spin diffusion from a RT ferromagnet to semiconductor epitaxy layers-the so-called extrinsic MFE, to realize RT spin-polarization. [11][12][13] But the strict conditions such as elaborate device structure, high electric field, materials with high carrier mobility, and long spin diffusion length required limit their application. Semiconductors with RT intrinsic MFE could naturally avoid those problems and therefore are extremely desirable for advancing the spintronic applications. However, no such material has been reported to date.Lead halide perovskites (LHPs) offer opportunities to achieve RT intrinsic MFE because of the strong orbital moment carried by the heavy lead atoms, and further because of the σ-type direct orbital bonding in the [PbX 6 ] 4− octahedra lattice that may induce orbital ordering among electrons on excited states. The orbital interaction is often one or two orders of magnitude stronger than the spin interaction [14] and could contest with Magnetic-field-enhanced spin-polarized electronic/optical properties in semiconductors are crucial for fabricating various spintronic devices. However, this spin polarization is governed by weak spin exchange interactions and easily randomized by thermal fluctuations; therefore, it is only produced at cryogenic temperatures, which severely limits the applications. Herein, a room-temperature intrinsic magnetic field effect (MFE) on excitonic photoluminescence is achieved in CsPbX 3 :Mn (X = Cl, Br) perovskite nanocrystals. Through moderate Mn doping, the MFE is enhanced by exciton-Mn interactions, and through partial Br substitution, the MFE is stabilized at room temperature by exciton orbital ordering. The orbital ordering significantly enhances the g-factor difference between electrons and holes, which is evidenced by a parallel orbit-orbit interaction among excitons generated by circular polarized laser excitation. This study provides a clear avenue for engineering spintronic materials based on orbital interactions in perovskites.The ORCID identification number(s) for the author(s) of this article can be found under
Metal halide perovskites show considerable optical nonlinearity and could be used for cost-effective nonlinear optical devices if their nonlinear susceptibilities can be improved. Here, we report large optical nonlinearity, including third-order nonlinear absorption, refraction, and two-photon absorption excited luminescence, of CsPbBr3 nanoplatelets with a thickness of two or three atomic layers and a plane size of about 60 nm. Specifically, the nonlinear absorption was mainly induced by two-photon absorption at low incident powers, and the nonlinear absorption cross section reached 2.15 × 107 GM. It is two orders of magnitude larger than that of CsPbBr3 nanocrystals, which makes them an ideal optical limiting material. Furthermore, the nanoplatelets exhibited large self-phase modulation-induced nonlinear refraction, and the figures of merit W and T satisfied W >1 and T <1, which allow for optical switching. The large optical nonlinearity of CsPbBr3 nanoplatelets provides a basis for multifunctional applications in nonlinear optical devices.
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