Jump to main content
Jump to site search
PLANNED MAINTENANCE Close the message box

Scheduled maintenance upgrade on Thursday 4th of May 2017 from 8.00am to 9.00am (BST).

During this time our websites will be offline temporarily. If you have any questions please use the feedback button on this page. We apologise for any inconvenience this might cause and thank you for your patience.



Importance of Double-Resonance Effects in Two-Photon Absorption Properties of Au25 (SR)18-

Abstract

The two-photon absorption (TPA) cross sections of small thiolate-protected gold clusters have been shown to be much larger than typical small organic molecules. In comparison with larger nanoparticles, their TPA cross sections per gold atom are also found to be larger. Theoretical simulations have suggested that the large enhancement of these TPA cross sections comes from a one-photon double resonance mechanism. However, it remains difficult to simulate TPA cross sections of thiolate-protected gold clusters due to their large system size and a high density of states. In this work, we report a time-dependent density functional theory (TDDFT) study of the TPA spectra of Au25 (SR)18- cluster based on a damped response theory formalism. Damped response theory enables a consistent treatment of on- and off-resonance molecular properties even for molecules with a high density of states, and thus is well-suited for studying TPA properties for gold clusters. Our results indicate that the one- and two-photon double resonance effect is much smaller than previously found, and thus unlikely the main cause of the large TPA cross sections found experimentally. The effect of symmetry-breaking of the Au25 (SR)18- cluster due to the ligands on the TPA cross sections has been studied and found to only slightly increase the cross section. Furthermore, by comparing with larger nanoparticles we find that the TPA cross section per gold atom scales linearly with the diameter of the particles, and that the Kerr nonlinear response of the Au25 (SR)18- cluster is on the same order as that of bulk gold films.

Back to tab navigation
Please wait while Download options loads

Supplementary files

Publication details

The article was received on 02 Mar 2017, accepted on 18 Apr 2017 and first published on 19 Apr 2017


Article type: Edge Article
DOI: 10.1039/C7SC00968B
Citation: Chem. Sci., 2017, Accepted Manuscript
  • Open access: Creative Commons BY license
  •   Request permissions

    Importance of Double-Resonance Effects in Two-Photon Absorption Properties of Au25 (SR)18-

    Z. Hu and L. Jensen, Chem. Sci., 2017, Accepted Manuscript , DOI: 10.1039/C7SC00968B

    This article is licensed under a Creative Commons Attribution 3.0 Unported Licence. Material from this article can be used in other publications provided that the correct acknowledgement is given with the reproduced material.

    Reproduced material should be attributed as follows:

    • For reproduction of material from NJC:
      [Original citation] - Published by The Royal Society of Chemistry (RSC) on behalf of the Centre National de la Recherche Scientifique (CNRS) and the RSC.
    • For reproduction of material from PCCP:
      [Original citation] - Published by the PCCP Owner Societies.
    • For reproduction of material from PPS:
      [Original citation] - Published by The Royal Society of Chemistry (RSC) on behalf of the European Society for Photobiology, the European Photochemistry Association, and RSC.
    • For reproduction of material from all other RSC journals:
      [Original citation] - Published by The Royal Society of Chemistry.

    Information about reproducing material from RSC articles with different licences is available on our Permission Requests page.

Search articles by author