A facile interfacial charge transfer (CT) with a reduced inter-layer energy band regulates the charge transport mechanism in any optoelectronic device. The enhancement in semiconductor-based device performance often demands improved CT dynamics and collection of free carriers with reduced charge recombination. In this work, we present a detailed inspection of the photo-induced CT between inorganic lead halide perovskite nanocrystals (PNCs) with varied compositions and their consequence on the charge transport process. The superior CT rate in mixed halide CsPbBr2Cl PNCs with naphthoquinone (NPQ) is revealed when compared with the parent CsPbBr3 PNCs and its anion-exchanged counterpart CsPbCl3. The glimpses of hole transfer contribution along with electron transfer are detected for CsPbBr2Cl with superior CT efficiency. The enhanced conduction current after the insertion of NPQ into the PNCs with a reduced hysteresis suggests an improved charge transport in the fabricated device compared to the pristine PNCs. These findings can contribute to a better understanding of multiple ways of engineering optoelectronic devices to boost performance and efficiencies and the concurrent role of the CT process in the conduction mechanism.
Perovskites (PVKs) have emerged as an exciting class of semiconducting materials owing to their magnificent photophysical properties and been used in solar cells, lightemitting diodes, photodetectors, etc. The growth of multidimensional nanostructures has revealed many exciting alterations in their optoelectronic properties compared to those of their bulk counterparts. In this work, we have spotlighted the influence of quantum confinement in CsPbBr 3 PVKs like the quantum dot (PQD), nanoplatelet (PNPL), and nanorod (PNR) on their charge transfer (CT) dynamics with 1,4-naphthoquinone (NPQ). The energy band alignment facilitates the transfer of both electrons and holes in the PNPL to NPQ, enhancing its CT rate, while only electron transfer in the PQD and PNR diminishes CT. The tunneling current across a metal−nanostructure−metal junction for the PNPL is observed to be higher than others. The higher exciton binding energy in the PNPL results in efficient charge transport by enhancing the mobility of the excited-state carrier and its lifetime compared to those of the PNR and PQD.
Optimization of perovskite-based optoelectronic performance demands prudent engineering in the device architecture with facile transport of generated charge carriers. Herein, we explore the charge transfer (CT) kinetics in perovskite nanocrystals (PNCs), CsPbBr 3 , with two redox-active quinones, menadione (MD) and anthraquinone (AQ), and its alteration in halide exchanged CsPbCl 3 . With a series of spectroscopic and microscopic measurements, we infer that both electron and hole transfer (ET−HT) prevail in CsPbCl 3 with quinones, resulting in a faster CT, while ET predominates for CsPbBr 3 . Furthermore, current-sensing atomic force microscopy measurements demonstrate that the conductance across a metal−PNC−metal nanojunction is improved in the presence of quinones. The contributions of ET and HT to current conduction across PNCs are well supported and validated by theoretical calculations of the density of states. These outcomes convey a new perspective on the relevance of ET and HT in the optimal current conduction and optoelectronic device engineering of perovskites.
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