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2010


Molecular QED of coherent and incoherent sum-frequency and second-harmonic generation in chiral liquids in the presence of a static electric field
Molecular QED of coherent and incoherent sum-frequency and second-harmonic generation in chiral liquids in the presence of a static electric field

Fischer, P., Salam, A.

MOLECULAR PHYSICS, 108(14):1857-1868, 2010 (article)

Abstract
Coherent second-order nonlinear optical processes are symmetry forbidden in centrosymmetric environments in the electric-dipole approximation. In liquids that contain chiral molecules, however, and which therefore lack mirror image symmetry, coherent sum-frequency generation is possible, whereas second-harmonic generation remains forbidden. Here we apply the theory of molecular quantum electrodynamics to the calculation of the matrix element, transition rate, and integrated signal intensity for sum-frequency and second-harmonic generation taking place in a chiral liquid in the presence and absence of a static electric field, to examine which coherent and incoherent processes exist in the electric-dipole approximation in liquids. Third- and fourth-order time-dependent perturbation theory is employed in combination with single-sided Feynman diagrams to evaluate two contributions arising from static field-free and field-induced processes. It is found that, in addition to the coherent term, an incoherent process exists for sum-frequency generation in liquids. Surprisingly, in the case of dc-field-induced second-harmonic generation, the incoherent contribution is found to always vanish for isotropic chiral liquids even though hyper-Rayleigh second-harmonic generation and electric-field-induced second-harmonic generation are both independently symmetry allowed in any liquid.

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DOI [BibTex]

2008


Voltage-Controllable Magnetic Composite Based on Multifunctional Polyethylene Microparticles
Voltage-Controllable Magnetic Composite Based on Multifunctional Polyethylene Microparticles

Ghosh, A., Sheridon, N. K., Fischer, P.

SMALL, 4(11):1956-1958, 2008 (article)

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DOI [BibTex]

2008



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Frequency analysis with coupled nonlinear oscillators

Buchli, J., Righetti, L., Ijspeert, A.

Physica D: Nonlinear Phenomena, 237(13):1705-1718, August 2008 (article)

Abstract
We present a method to obtain the frequency spectrum of a signal with a nonlinear dynamical system. The dynamical system is composed of a pool of adaptive frequency oscillators with negative mean-field coupling. For the frequency analysis, the synchronization and adaptation properties of the component oscillators are exploited. The frequency spectrum of the signal is reflected in the statistics of the intrinsic frequencies of the oscillators. The frequency analysis is completely embedded in the dynamics of the system. Thus, no pre-processing or additional parameters, such as time windows, are needed. Representative results of the numerical integration of the system are presented. It is shown, that the oscillators tune to the correct frequencies for both discrete and continuous spectra. Due to its dynamic nature the system is also capable to track non-stationary spectra. Further, we show that the system can be modeled in a probabilistic manner by means of a nonlinear Fokker–Planck equation. The probabilistic treatment is in good agreement with the numerical results, and provides a useful tool to understand the underlying mechanisms leading to convergence.

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link (url) DOI [BibTex]

link (url) DOI [BibTex]

2001


Isotropic second-order nonlinear optical susceptibilities
Isotropic second-order nonlinear optical susceptibilities

Fischer, P., Buckingham, A., Albrecht, A.

PHYSICAL REVIEW A, 64(5), 2001 (article)

Abstract
The second-order nonlinear optical susceptibility, in the electric dipole approximation, is only nonvanishing for materials that are noncentrosymmetric. Should the medium be isotropic, then only a chiral system. such as an optically active liquid, satisfies this symmetry requirement. We derive the quantum-mechanical form of the isotropic component of the sum- and difference-frequency susceptibility and discuss its unusual spectral properties. We show that any coherent second-order nonlinear optical process in a system of randomly oriented molecules requires the medium to be chiral. and the incident frequencies to be different and nonzero. Furthermore, a minimum of two nondegenerate excited molecular states are needed for the isotropic part of the susceptibility to be nonvanishing. The rotationally invariant susceptibility is zero in the static field limit and shows exceptionally sensitive resonance and dephasing effects that are particular to chiral centers.

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DOI [BibTex]

2001


DOI [BibTex]


Reply to ``Comment on `Phenomenological damping in optical response tensors'{''}
Reply to “Comment on ‘Phenomenological damping in optical response tensors’”

Buckingham, A., Fischer, P.

PHYSICAL REVIEW A, 63(4), 2001 (article)

Abstract
We show that damping factors must not be incorporated in the perturbation of the ground state by a static electric field. If they are included, as in the theory of Stedman et al. {[}preceding Comment. Phys. Rev. A 63, 047801 (2001)], then there would be an electric dipole in the y direction induced in a hydrogen atom in the M-s = + 1/2 state by a static electric field in the x direction. Such a dipole is excluded by symmetry.

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DOI [BibTex]