Two-photon resonance four-wave mixing spectroscopy in polar media

Hadjichristov, Georgi B.; Stamova, M.; Kircheva, P. P.

doi:10.1088/0953-4075/28/15/029

Cited by 11 publications

(4 citation statements)

References 22 publications

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“…Finally, it should be noted that Eqns (1)È(3) neither account for the absorption and population changes nor consider the corresponding change in the phase-matching conditions and, more important, the possible change in the permanent dipoles and *k upon photoexcitation.31 A more reÐned simulation of the resonance CARS spectra in dipolar media should include the real populations of the excited states which are disregarded in the densitymatrix calculation of s(3) in our case. 22 The experimentally obtained CEP is similar to the calculated one presented in Fig. 2(b), but we should point out that the value of m which can be deduced from this dependence should be a rough estimate because of the simpliÐcation of the three-state system related to the poly-4BCMU under consideration.…”

Section: Resultssupporting

confidence: 80%

Two-photon-resonance four-wave mixing for the study of permanent molecular dipoles

Hadjichristov

Киров

Materny

et al. 1998

J. Raman Spectrosc.

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Two‐photon‐resonance four‐wave mixing (TPR‐FWM) spectroscopy was examined for the study of the permanent electric dipole moments of molecular states. A TPR‐FWM process of the type ω4=ω1‐ω2+ω3 in a three‐state dipolar system was considered. The extraction of data for the difference in permanent dipole moments (Δμ) of states involved in TPR was analysed in the case of resonance TPR‐FWM. Resonance TPR‐FWM measurements were performed in a solution of the polydiacetylene poly‐4BCMU. © 1998 John Wiley & Sons, Ltd.

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Section: Resultssupporting

confidence: 80%

Two-photon-resonance four-wave mixing for the study of permanent molecular dipoles

Hadjichristov

Киров

Materny

et al. 1998

J. Raman Spectrosc.

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“…The usual prescriptions of perturbation theory require us to sum such states over the complete set of eigenstates for the unperturbed system, one of which must necessarily generate a diagonal matrix element corresponding to a permanent moment. In this sense, permanent electric dipole moments are particular cases of the transition moments, and they play a significant role (often unacknowledged, though see, for example, recent papers [1][2][3][4]) in the structure of any nonlinear susceptibility. The role of such permanent moments in non-parametric laser-molecule interactions is relatively well attested-see for example [5][6][7][8] and citations therein.…”

Section: Introductionmentioning

confidence: 99%

An algorithm for the nonlinear optical susceptibilities of dipolar molecules, and an application to third harmonic generation

Andrews

Romero

Meath

1999

J. Phys. B: At. Mol. Opt. Phys.

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Abstract. It is well known that a simple transformation of the electric dipole interaction provides a convenient means for ascertaining the effects of permanent dipoles on the optical behaviour of systems with a response dominated by two energy levels. By establishing the general validity of the procedure for parametric processes such as harmonic generation, it is shown how the detailed structure of the optical susceptibilities associated with arbitrary forms of optical nonlinearity can be ascertained by an algorithmic method, based on a novel interpretation of the relevant quantum electrodynamical Feynman diagrams. Application of the algorithm to second and third harmonic generation illustrates its usefulness and simplicity, whilst also providing new results and revealing features, related to the role of permanent dipoles, which have not hitherto been apparent.

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“…In the perturbative sum over such states, at least one route must generate a diagonal matrix element corresponding to a permanent moment. In this sense, permanent electric dipole moments are particular instances of the transition moments, and it is now recognized that these are significantly involved in the structure of any nonlinear susceptibility [21][22][23] . In the semiclassical formulation, the role of permanent moments emerges through calculations based on a transformed electric dipole interaction, by employment of a fluctuation dipole operator 22 given by;…”

Section: Fluctuation Dipoles In Nonlinear Opticsmentioning

confidence: 99%

Resonance damping and optical susceptibilities (Critical Review Lecture)

Andrews¹,

Romero

2003

SPIE Proceedings

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In the formal development of optical response theory in terms of susceptibilities, proper representation of the optical frequency dependence necessitates modeling both the discrete linewidth and the finite signal enhancement associated with the onset of resonance. Such dispersion behavior is generally accommodated by damping factors, featured in both resonant and non-resonant susceptibility terms. For the resonant terms, the sign of such damping corrections is unequivocal; however the correct choice of sign for non-resonant terms has become a matter of debate, heightened by the discovery that entirely opposite conventions are applied in mainstream literature on Raman scattering and nonlinear optics. Where the two conventions are applied to electro-optical processes in fluids there are significant and potentially verifiable differences between the associated results . Through a full thorough quantum electrodynamical treatment the universal correctness of one convention can be ascertained and flaws in the counter-convention identified. Resolution of the central issue requires consideration of a number of fundamental questions concerning the nature of dissipation in quantum mechanical systems. It is concluded that optical susceptibilities formulated with correct signing of the damping corrections must fulfill several fundamental tests: satisfaction of a new sum rule; invariance of the associated quantum amplitudes under time -reversal symmetry, and a resilience to canonical transformation.

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Two-photon resonance four-wave mixing spectroscopy in polar media

Cited by 11 publications

References 22 publications

Two-photon-resonance four-wave mixing for the study of permanent molecular dipoles

Two-photon-resonance four-wave mixing for the study of permanent molecular dipoles

An algorithm for the nonlinear optical susceptibilities of dipolar molecules, and an application to third harmonic generation

Resonance damping and optical susceptibilities (Critical Review Lecture)

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