Vibrational Energy Transport through a Capping Layer of Appropriately Designed Peptide Helices over Gold Nanoparticles

Physikalisch-Chemisches Institut, Universität Zürich, CH-8057 Zürich, Switzerland.
Nano Letters (Impact Factor: 13.59). 08/2010; 10(8):3057-61. DOI: 10.1021/nl101580w
Source: PubMed


We design and characterize spherical gold nanoparticles, which are covalently linked to and completely covered by
3(10)-helical peptides. These helices provide a scaffold to place C-13=O isotope labels at defined distances from the gold surface, which we employ as local thermometers. Probing
these reporter groups with transient infrared spectroscopy, we monitor the vibrational energy flow across the peptide capping layer following excitation of the nanoparticle plasmon resonance.

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    • "Nevertheless, as shown by Leitner and coworkers, localized highfrequency modes preferably couple to other localized modes that overlap in space, while the anharmonic coupling between a localized and a delocalized mode is typically very small [39]. Therefore, one can assume that the local C=O thermometer in our experiments [19] [20] [21] [22] tentatively overestimates the contribution of other localized parking modes and does not sufficiently account for the energy in the delocalized transporting modes. In such a scenario, the measured apparent heat diffusivity is dominated by localized modes that receive vibrational energy delayed through intra-site "
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    ABSTRACT: In a previous paper [M. Schade, P. Hamm, Vibrational energy transport in the presence of intrasite vibrational energy redistribution, J. Chem. Phys. 131 (2009) 044511], it has been shown that on ultrashort length and time scales, the speed of vibrational energy transport along a molecular chain is limited by intrasite vibrational relaxation rather than the actual intersite propagation. However, since intrasite vibrational relaxation is length independent, the intersite propagation rate is expected to become rate-limiting at some length scale, where propagation approaches the bulk limit. In the present paper, we investigate the transition between both regimes. The response of different types of modes may be very different at early times, depending on how much they contribute directly to energy transport. Surprisingly though, when averaging the energy content over all vibrational modes of the various chain sites, the complexity of the intrasite vibrational relaxation process is completely hidden so that energy transport on the nanoscale can be described by an effective propagation rate, that equals the bulk value, even at short times.
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    ABSTRACT: The stabilizing action of C(α)-tetrasubstituted α-amino acids inserted into a sequence of short peptides allowed for the first time the preparation of water-soluble nanoparticles of different materials coated with a helix-structured undecapeptide. This peptide coating strongly favors nanoparticle uptake by human immune system cells.
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