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RETURN TO ISSUEPREVC: Physical Processe...C: Physical Processes in Nanomaterials and NanostructuresNEXT

Ultrafast Nonlinear Plasmon Decay Processes in Silver Nanoclusters

Cite this: J. Phys. Chem. C 2020, 124, 37, 20477–20487
Publication Date (Web):August 17, 2020
https://doi.org/10.1021/acs.jpcc.0c03160
Copyright © 2020 American Chemical Society

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    Abstract

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    Tunable plasmonic properties of metallic nanostructures play a significant role in enhancing various photo-optical phenomena including solar energy conversion, nonlinear optics, photoluminescence and photocatalysis. Understanding the fast plasmon decay mechanisms is essential for developing practical applications utilizing these light-matter interaction processes, but has been a challenge both experimentally and computationally. Among theoretical simulation methods, real-time density functional theory (RT-TDDFT) is a valuable tool to monitor the electron dynamics of molecules subjected to an electric field. Herein, we use the RT-TDDFT method to identify the possible plasmon decay mechanisms of the bare tetrahedral Ag8 nanocluster. We excite the strong linear plasmonic states and examine dipole response and the electron dynamics in the system. Variation of density matrix elements related to occupied and virtual orbital pairs reveals that the one-photon allowed transitions, which have been excited due to the incident electric field, experience ultrafast decay into high energy transitions, specifically to two-photon allowed transitions. The tetrahedral symmetry representations of these transitions confirm that some of these high energy transitions are only allowed via two-photon absorption whereas others can be activated via both one- and two- photon absorption. Moreover, this work suggests that the collective excitations present in the system play an important role in accumulating an enormous amount of energy to enhance nonlinear processes. Overall, this work provides insights into a possible plasmon decay mechanism of nanoclusters which is activation of nonlinear processes such as two-photon absorption.

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    The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acs.jpcc.0c03160.

    • Coordinates of Ag8 cluster, applied continuous wave field and the dipole moment of the Ag8 cluster in both time and energy domains, transitions responsible for the lowest energy peaks of the Ag8 cluster at 3.05 and 3.96 eV, absorption spectra comparison for LR and RT-TDDFT methods, analysis of spectral properties from the molecular orbital occupation number variation and off-diagonal elements of the density matrix during time propagation, decay and growth of off-diagonal density matrix elements when external continuous wave electric fields oscillating with frequencies of 3.96 and 3.05 eV are applied, variation of the occupation numbers for selected molecular orbitals (3.96 eV excitation), comparison of the dipole response and the POV values when the applied field strengths are 0.001 au and 0.0001 au, variation of applied field, dipole moment along z axis, and Fourier transformed dipole moment when continuous wave electric fields oscillating with frequencies of 1.525 and 1.98 eV are applied (PDF)

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    Cited By

    This article is cited by 11 publications.

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    2. Yuchen Wang, Christine M. Aikens. Effects of Field Strength and Silver Nanowire Size on Plasmon-Enhanced N2 Dissociation. The Journal of Physical Chemistry A 2023, 127 (27) , 5609-5619. https://doi.org/10.1021/acs.jpca.3c00120
    3. Gowri U. Kuda-Singappulige, Christine M. Aikens. Excited-State Absorption in Silver Nanoclusters. The Journal of Physical Chemistry C 2021, 125 (45) , 24996-25006. https://doi.org/10.1021/acs.jpcc.1c05054
    4. Gowri U. Kuda-Singappulige, Christine M. Aikens. Theoretical Insights into Excitation-Induced Oxygen Activation on a Tetrahedral Ag8 Cluster. The Journal of Physical Chemistry A 2021, 125 (43) , 9450-9458. https://doi.org/10.1021/acs.jpca.1c05129
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