Halide perovskites possess enormous potential for various optoelectronic applications. Presently, a clear understanding of the interplay between the lattice and electronic effects is still elusive. Specifically, the weakly absorbing tail states and dual emission from perovskites are not satisfactorily described by existing theories based on the Urbach tail and reabsorption effect. Herein, through temperature-dependent and time-resolved spectroscopy on metal halide perovskite single crystals with organic or inorganic A-site cations, we confirm the existence of indirect tail states below the direct transition edge to arise from a dynamical Rashba splitting effect, caused by the PbBr6 octahedral thermal polar distortions at elevated temperatures. This dynamic effect is distinct from the static Rashba splitting effect, caused by non-spherical A-site cations or surface induced lattice distortions. Our findings shed fresh perspectives on the electronic-lattice relations paramount for the design and optimization of emergent perovskites, revealing broad implications for light harvesting/photo-detection and light emission/lasing applications.
additional analog converters, imposing issues with scalability and power consumption. [2][3][4][5] Development of next-generation materials and devices for neuromorphic electronics entails detailed understanding of the fundamental device characteristics and their possible emulation capabilities at an elemental level. Ionically gated transistors harness diffusive mechanics to achieve continuous modulation of channel conductance at low-power, but require coupling of two disparate electronically and ionically active material sets. [6,7] Solutions based on drift-memristors are inherently disadvantaged due to digital-like abrupt switching transitions, which limit their plasticity. [8] Very recently, second-order drift memristors, [9,10] electrochemical metallization cells, [11] and diffusive memristors [8] have been engineered to approximate the biological Ca 2+ dynamics based on metal atom diffusion, thermal dissipation, [9] mobility decay, [12] and spontaneous nanoparticle formation, but often require additional nonvolatile elements in series for long-term memory storage. An ionic semiconductor which intimately combines rapid electronic transitions with slow drift-diffusive ionic kinetics will enable dynamic tuning of metastable memristive conductance states, allowing efficient emulation of synaptic characteristics and catering for novel low-power architectures that exploit electronic properties of the semiconductor.Emulation of brain-like signal processing is the foundation for development of efficient learning circuitry, but few devices offer the tunable conductance range necessary for mimicking spatiotemporal plasticity in biological synapses. An ionic semiconductor which couples electronic transitions with drift-diffusive ionic kinetics would enable energy-efficient analog-like switching of metastable conductance states. Here, ionic-electronic coupling in halide perovskite semiconductors is utilized to create memristive synapses with a dynamic continuous transition of conductance states. Coexistence of carrier injection barriers and ion migration in the perovskite films defines the degree of synaptic plasticity, more notable for the larger organic ammonium and formamidinium cations than the inorganic cesium counterpart. Optimized pulsing schemes facilitates a balanced interplay of short-and longterm plasticity rules like paired-pulse facilitation and spike-time-dependent plasticity, cardinal for learning and computing. Trained as a memory array, halide perovskite synapses demonstrate reconfigurability, learning, forgetting, and fault tolerance analogous to the human brain. Network-level simulations of unsupervised learning of handwritten digit images utilizing experimentally derived device parameters, validates the utility of these memristors for energy-efficient neuromorphic computation, paving way for novel ionotronic neuromorphic architectures with halide perovskites as the active material. Artificial SynapsesThe ORCID identification number(s) for the author(s) of this article can be found under https://doi.C...
Perovskite–perovskite core–shell type nanoparticles with a high photoluminescence quantum yield and long term ambient stability.
The incorporation of phenylethylammonium bromide (PEABr) into a fully inorganic CsPbBr perovskite framework led to the formation of mixed-dimensional perovskites, which enhanced the photoluminescence due to efficient energy funnelling and morphological improvements. With a PEABr : CsPbBr ratio of 0.8 : 1, PeLEDs with a current efficiency of 6.16 cd A and an EQE value of 1.97% have been achieved.
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