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1.
Nature ; 550(7674): 87-91, 2017 10 04.
Artigo em Inglês | MEDLINE | ID: mdl-28980632

RESUMO

Medical X-ray imaging procedures require digital flat detectors operating at low doses to reduce radiation health risks. Solution-processed organic-inorganic hybrid perovskites have characteristics that make them good candidates for the photoconductive layer of such sensitive detectors. However, such detectors have not yet been built on thin-film transistor arrays because it has been difficult to prepare thick perovskite films (more than a few hundred micrometres) over large areas (a detector is typically 50 centimetres by 50 centimetres). We report here an all-solution-based (in contrast to conventional vacuum processing) synthetic route to producing printable polycrystalline perovskites with sharply faceted large grains having morphologies and optoelectronic properties comparable to those of single crystals. High sensitivities of up to 11 microcoulombs per air KERMA of milligray per square centimetre (µC mGyair-1 cm-2) are achieved under irradiation with a 100-kilovolt bremsstrahlung source, which are at least one order of magnitude higher than the sensitivities achieved with currently used amorphous selenium or thallium-doped cesium iodide detectors. We demonstrate X-ray imaging in a conventional thin-film transistor substrate by embedding an 830-micrometre-thick perovskite film and an additional two interlayers of polymer/perovskite composites to provide conformal interfaces between perovskite films and electrodes that control dark currents and temporal charge carrier transportation. Such an all-solution-based perovskite detector could enable low-dose X-ray imaging, and could also be used in photoconductive devices for radiation imaging, sensing and energy harvesting.


Assuntos
Compostos de Cálcio/química , Óxidos/química , Impressão , Doses de Radiação , Radiografia/instrumentação , Radiografia/métodos , Titânio/química , Raios X , Césio/química , Eletrodos , Desenho de Equipamento , Iodetos/química , Imagens de Fantasmas , Selênio/química , Tálio/química , Transistores Eletrônicos
2.
J Phys Chem Lett ; 12(34): 8447-8452, 2021 Sep 02.
Artigo em Inglês | MEDLINE | ID: mdl-34437809

RESUMO

The metal halide Cs3Cu2I5 displays anomalous optical properties: an optical absorption onset in the ultraviolet region (∼ 330 nm) with highly efficient luminescence in the blue region (∼ 445 nm). Although self-trapped exciton formation has been proposed as the origin of giant Stokes shift, its connection to the photoluminescence quantum yield exceeding 90% remains unknown. Here, we explore the photochemistry of Cs3Cu2I5 from first-principles and reveal a low energy barrier for exciton self-trapping associated with Cu-Cu dimerization. Kinetic analysis shows that the quantum yield of blue emission in Cs3Cu2I5 is sensitive to the excited carrier density due to the competition between exciton self-trapping and band-to-band radiative recombination.

3.
Nanoscale Horiz ; 6(12): 987-997, 2021 11 22.
Artigo em Inglês | MEDLINE | ID: mdl-34668915

RESUMO

Flexible and transparent artificial synapses with extremely low energy consumption have potential for use in brain-like neuromorphic electronics. However, most of the transparent materials for flexible memristive artificial synapses were reported to show picojoule-scale high energy consumption with kiloohm-scale low resistance, which limits the scalability for parallel operation. Here, we report on a flexible memristive artificial synapse based on Cs3Cu2I5 with energy consumption as low as 10.48 aJ (= 10.48 × 10-18 J) µm-2 and resistance as high as 243 MΩ for writing pulses. Interface-type resistive switching at the Schottky junction between p-type Cu3Cs2I5 and Au is verified, where migration of iodide vacancies and asymmetric carrier transport owing to the effective hole mass is three times heavier than effective electron mass are found to play critical roles in controlling the conductance, leading to high resistance. There was little difference in synaptic weight updates with high linearity and 250 states before and after bending the flexible device. Moreover, the MNIST-based recognition rate of over 90% is maintained upon bending, indicative of a promising candidate for highly efficient flexible artificial synapses.


Assuntos
Eletrônica , Sinapses , Encéfalo , Condutividade Elétrica , Fenômenos Físicos
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