Although α‐CsPbI3 is regarded as an attractive optical luminophore, it is readily degraded to the optically inactive δ‐phase under ambient conditions. Here, we present a simple approach to revive degraded (“optically sick”) α‐CsPbI3 through “medication” with thiol‐containing ligands. The effect of different types of thiols is systematically studied through optical spectroscopy. The structural reconstruction of degraded α‐CsPbI3 nanocrystals to cubic crystals in the presence of thiol‐containing ligands is visualized through high‐resolution transmission electron microscopy and supported by X‐ray diffraction analysis. We found that 1‐dodecanethiol (DSH) effectively revives degraded CsPbI3 and results in high immunity towards moisture and oxygen, hitherto unreported. DSH facilitates the passivation of surface defects and etching of degraded Cs4PbI6 phase, thus reverting them back to the cubic CsPbI3 phase, leading to enhanced PL and environmental stability.
The synthesis of air-stable and cubic phases of all-inorganic halide perovskite nanocrystals (HPNCs) by a hot-injection approach is still challenging due to their rapid in situ phase transformations. Therefore, understanding and preventing this phase conversion by doping of cations is the key to improve the structural stability, environmental durability, and photoluminescence quantum yield. Here, the doping of divalent Cu ions at the Pb-site of cesium lead iodide (CsPbI3) is reported to achieve cubic-phase (α-phase) HPNCs with superior quantum yield and enhanced stability compared to undoped CsPbI3. Rietveld refined X-ray diffraction patterns and atomic-resolution transmission electron microscopy analyses reveal structural transformation from a mixed (γ-orthorhombic and α-cubic) phase to a cubic (α-CsPbI3) one with a smaller lattice constant at an optimal (5.6%) Cu concentration. Computational density functional theory (DFT) analysis credits the resultant structural and environmental stability for the Cu-doped sample to the charge accumulation at the dopant site that leads to increased bond strength with consequent minimization of the energy of the system to give rise to the maximum stability of the HPNCs at this dopant ratio. With the increase of Cu-doping, a red shift is observed in the absorbance and photoluminescence spectra up to a critical doping level, making the system optically tuneable. The optimally doped (5.6% Cu) CsPbI3 HPNCs exhibit stronger light emission with higher carrier lifetime and higher quantum yield (>80%), which are absolutely essential requirements in air-stable optoelectronic devices.
Two dimensional (2D) van der Waals heterostructures (vdWHs) have unique potential in facilitating the stacking of layers of different 2D materials for optoelectronic devices with superior characteristics. However, the fabrication of large area all-2D heterostructures is still challenging towards realizing practical devices at a reduced cost. In the present work, we have demonstrated a rapid yet simple, impurity-free and efficient sonication-assisted chemical exfoliation approach to synthesize hybrid vdWHs based on 2D molybdenum disulphide (MoS2) and tungsten disulphide (WS2), with high yield. Microscopic and spectroscopic studies have confirmed the successful exfoliation of layered 2D materials and formation of their hybrid heterostructures. The co-existence of 2D MoS2 and WS2 in the vdWH hybrids is established by optical absorption and Raman shift measurements along with their chemical stiochiometry determined by X-ray photoelectron spectroscopy. The spectral response of the vdWH/Si (2D/3D) heterojunction photodetector fabricated using the as-synthesized material is found to exhibit broadband photoresponse compared to that of the individual 2D MoS2 and WS2 devices. The peak responsivity and detectivity are found to be as high as ~2.15 A/W and 2.05 ✕ 1011 Jones, respectively for an applied bias of -5 V. The ease of fabrication with appreciable performance of the chemically synthesized vdWH-based devices have revealed their potential use for large area optoelectronic applications on Si-compatible CMOS platforms.
Although α-CsPbI 3 is regarded as an attractive optical luminophore, it is readily degraded to the optically inactive δ-phase under ambient conditions. Here, we present a simple approach to revive degraded ("optically sick") α-CsPbI 3 through "medication" with thiol-containing ligands. The effect of different types of thiols is systematically studied through optical spectroscopy. The structural reconstruction of degraded α-CsPbI 3 nanocrystals to cubic crystals in the presence of thiol-containing ligands is visualized through high-resolution transmission electron microscopy and supported by X-ray diffraction analysis. We found that 1-dodecanethiol (DSH) effectively revives degraded CsPbI 3 and results in high immunity towards moisture and oxygen, hitherto unreported. DSH facilitates the passivation of surface defects and etching of degraded Cs 4 PbI 6 phase, thus reverting them back to the cubic CsPbI 3 phase, leading to enhanced PL and environmental stability.
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