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Progress in Nanophotonics 2 pp 1–32Cite as

Near-Field Excitation Dynamics in Molecules: Nonuniform Light-Matter Interaction Theory Beyond a Dipole Approximation

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Abstract

We have presented near-field excitation dynamics in molecules beyond diffraction limit of the incident visible laser field. A generalized theoretical description of a light-matter interaction taking account of nonuniformity of the light due to its intensity gradient has been developed on the basis of the multipolar Hamiltonian. The computations are demonstrated in high-harmonic generation spectra of a linear chain molecule of dicyanodiacetylene, NC6N and also in optical forces induced by a near-field for a 1 nm-sized metal particle mimicked by a jellium model and for C60.

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Notes

  1. 1.

    These bond lengths remain almost unchanged (i.e., at most 0.0024 Å for C3–C4) even if the geometry optimization was performed by using the B3LYP functional [58, 59].

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Acknowledgements

This research was supported by a Grant-in-Aid (No. 21350018) and by the Next-Generation Supercomputer Project from the Ministry of Education, Culture, Sports, Science and Technology of Japan. The computation was partly performed at the Research Center for Computational Science, Okazaki, Japan.

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  1. Department of Theoretical and Computational Molecular Science, Institute for Molecular Science, 38 Myodaiji-Nishigonaka, Okazaki, Aichi, 444-8585, Japan

    Katsuyuki Nobusada

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Correspondence to Katsuyuki Nobusada .

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  1. , Graduate School of Engineering, The University of Tokyo, Yayoi, Bunkyo-ku 2-11-16, Tokyo, 113-8656, Japan

    Motoichi Ohtsu

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Nobusada, K. (2013). Near-Field Excitation Dynamics in Molecules: Nonuniform Light-Matter Interaction Theory Beyond a Dipole Approximation. In: Ohtsu, M. (eds) Progress in Nanophotonics 2. Nano-Optics and Nanophotonics. Springer, Berlin, Heidelberg. https://doi.org/10.1007/978-3-642-35719-0_1

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