A systematic study of a new hybrid organicinorganic material where the cation has been replaced with imidazolium is presented. Imidazolium lead iodide (ImPI) shares the same stoichiometry of ABX 3 as a perovskite, however, it has a hexagonal structure. This material shows a vastly improved thermal stability as compared to the more popular hybrid perovskite, methyl ammonium lead iodide (MAPI). ImPI also exhibits a dramatic phase stability as compared to MAPI as demonstrated by the variable temperature XRD data (both low temperature and high temperature). In addition to the enhanced thermal robustness, ImPI shows three times better stability than MAPI under ambient conditions. The stability can be attributed to better packing efficiency of the ImPI lattice which in turn depends on the symmetrical and bulkier organic cation, imidazolium. Optoelectronic measurements were also performed and specifically, unlike for MAPI, photoluminescence measurements of ImPI showcased a broad emission over a range of 500 nm to 900 nm which could be attributed to the presence of selftrapped excitons and as such this broad emission holds promise for light emitting device applications.[a] C.
Organic–inorganic
hybrid crystals with lead halides as the
inorganic moiety are remarkable, in that they show low-dimensional
behavior despite their three-dimensional structures. Here, we report
on a unique structure, imidazolium lead iodide C3N2H5PbI3 (ImPI), and show that its electronic
ground state represents a one-dimensional (1D) solid with carrier
motion confined along nanometer-thin corrugated chains formed by face-sharing
PbI6
4– octahedrons. ImPI has a very broad
photoluminescence (PL) spectrum peaking around 688 nm (1.8 eV) with
a width of 173 nm at high temperatures. This PL emission shows a significant
red shift of 1.3 eV relative to the excitonic band gap of ImPI at
400 nm (3.1 eV) estimated from PL excitation spectroscopy. These results
are compared with measurements on PbI2. Calculations based
on the effective-mass theory show that the increased band gap of ImPI
originates from quantum confinement, with the PbI6
4– chains acting as 1D quantum wires. Time-resolved
and pump intensity-dependent PL studies provide evidence that PL emission
arises from self-trapped exciton recombination, a characteristic of
1D systems with easily deformable lattice. This study establishes
ImPI as a 1D hybrid semiconductor with a broad emission spectrum with
promise for opto-electronic device applications.
CH3NH3PbI3 has been deposited on three different substrates: FTO and two types of TiO2 electron transport layers. It has been evaluated for degradation under UV and visible light, and the phase has also been regenerated by a simple chemical treatment.
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