Optical Properties and Ultrafast Near-Infrared Localized Surface Plasmon Dynamics in Naturally p-Type Digenite Films

Andrea Villa, Madina Telkhozhayeva, Fabio Marangi, Eti Teblum, Aaron M. Ross, Mirko Prato, Luca Andena, Roberto Frassine, Francesco Scotognella, Gilbert Daniel Nessim

Research output: Contribution to journalArticlepeer-review

3 Scopus citations

Abstract

Copper chalcogenides are materials characterized by intrinsic doping properties, allowing them to display high carrier concentrations due to their defect-heavy structures, independent of the preparation method. Such high doping enables these materials to display plasmonic resonances, tunable by varying their stoichiometry. Here, plasmonic dynamics is studied in drop-cast Cu9S5 (digenite) nanocrystals (NCs) film using ultrafast pump–probe spectroscopy. The NCs are synthesized by thermal annealing of copper foil using chemical vapor deposition (CVD), followed by sonication and drop-casting of the isolated few-layered flakes on different substrates. The samples display a broad localized surface plasmon resonance (LSPR) in the near-infrared (NIR), peaking at 2100 nm. The free carrier response is further confirmed by fitting the linear absorption with a Drude–Lorentz effective medium approximation model. The high temporal resolution allows to measure the relaxation dynamics of the photo-excited holes, which are dominated by a fast decay (τ1 = 360 ± 20 fs) and correspond to hole–phonon scattering processes, followed by a long-lived (τ2 > 1 ns) signal associated with phonon–phonon scattering relaxation. These results confirm the possibility of fabricating Cu9S5 films retaining the plasmonic properties of individual NCs, anticipating integrating these films into heterojunctions with suitable hole acceptor materials to build hot-hole-transfer-based optoelectronic devices.

Original languageEnglish
Article number2201488
JournalAdvanced Optical Materials
Volume11
Issue number2
DOIs
StatePublished - 18 Jan 2023

Bibliographical note

Publisher Copyright:
© 2022 The Authors. Advanced Optical Materials published by Wiley-VCH GmbH.

Funding

A.V., M.T., and F.M. contributed equally to this work. This work was supported and funded by the European Research Council (ERC) under the European Union's Horizon 2020 research and innovation program (Grant Agreement No. 816313).

FundersFunder number
Horizon 2020 Framework Programme
European Research Council
Horizon 2020816313

    Keywords

    • copper chalcogenides
    • digenite nanocrystals film
    • localized surface plasmon resonance
    • ultrafast spectroscopy

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