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• W2000082938 abstract "A generalized theoretical description of a light-matter interaction beyond a dipole approximation is developed on the basis of the multipolar Hamiltonian with the aim of understanding the near-field excitation of molecules at the 1 nm scale. The theory is formulated for a system consisting of a molecule and a near field, where a nonuniform electric field plays a crucial role. The nonuniform light-matter interaction is expressed in terms of a spatial integral of the inner product of the total polarization of a molecule and an electric field so that the polarization is treated rigorously without invoking the conventional dipole approximation. A nonuniform electronic excitation of a molecule is demonstrated by solving a time-dependent Kohn-Sham equation in real space and real time with an implementation of the nonuniform light-matter interaction. The computations are performed to a linear chain molecule of dicyanodiacetylene $({text{NC}}_{6}text{N})$. The nonuniform electronic excitation clearly shows inhomogeneous electron dynamics in sharp contrast to the dynamics induced by a uniform electronic excitation under the dipole approximation. Despite the inversion symmetry of ${text{NC}}_{6}text{N}$, the nonuniform excitation generates even harmonics in addition to the odd ones. Higher-order nonlinear optical response and quadrupole excitation are also observed." @default.
• W2000082938 created "2016-06-24" @default.
• W2000082938 creator A5018162583 @default.
• W2000082938 creator A5044762463 @default.
• W2000082938 date "2009-10-13" @default.
• W2000082938 modified "2023-09-23" @default.
• W2000082938 title "Nonuniform light-matter interaction theory for near-field-induced electron dynamics" @default.
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• W2000082938 doi "https://doi.org/10.1103/physreva.80.043409" @default.
• W2000082938 hasPublicationYear "2009" @default.
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