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Effect of Surface Ligand on Chemical Interface Damping in Nonstoichiometric Cu2–xS Semiconductor Nanocrystals: A Direct Correlation between Ultrafast Carrier Dynamics and Photoconductivity

Cite this: J. Phys. Chem. C 2021, 125, 42, 23250–23258
Publication Date (Web):October 14, 2021
https://doi.org/10.1021/acs.jpcc.1c06085
Copyright © 2021 American Chemical Society
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Abstract

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Understanding and controlling ultrafast relaxation processes of photoexcited infrared active nonstoichiometric semiconducting materials is an important research area where chemical interface damping (CID) plays a significant role in the application of efficient optoelectronic devices. Herein, we have synthesized two different surface ligands (olaylamine and oleic acid) capped near-infrared active plasmonic semiconductor Cu2–xS nanocrystals (NCs), namely, CuOLM and CuOA. Interestingly, steady-state optical spectra of CuOA were found to be broader and red-shifted compared to CuOLM in the near-IR region and can be attributed to a stronger CID effect. The effect of the surface ligand on the relaxation dynamics of the localized surface plasmon resonance (LSPR) band was monitored with the aid of femtosecond broadband (visible-NIR) pump–probe spectroscopy. Broadening of the transient absorption (TA) spectra and faster kinetics have been observed for oleic acid capped NCs due to a strong chemical interface damping effect. We further investigated CID driven photoconductivity measurements and found drastic improvement of photoconductivity in the CuOA system. This work opens up a new direction for near-infrared active devices and its utilization in the field of infrared photosensing, photonics, and phototransistor application, where optical properties of an infrared active nonstoichiometric semiconductor can be manipulated through changing surface ligands.

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The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acs.jpcc.1c06085.

  • Particle size distribution histogram, field emission scanning electron microscopy (FESEM) studies, FESEM images of fabricated thin film devices, Fourier transform infrared spectroscopy (FTIR), transient absorption study at 800 nm pump excitation, temperature-dependent different TA lifetime components, photoconductivity measurements of OLM- and OA-capped NCs under a 400 nm light illumination (PDF)

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Cited By

This article is cited by 1 publications.

  1. Nandan Ghorai, Hirendra N. Ghosh. Chemical Interface Damping in Nonstoichiometric Semiconductor Plasmonic Nanocrystals: An Effect of the Surrounding Environment. Langmuir 2022, 38 (18) , 5339-5350. https://doi.org/10.1021/acs.langmuir.2c00446

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