Floquet Theory Of The Interaction Of A Molecule With A Laser Field: Techniques And An Application

Leasure, Steven C.; Wyatt, Róbert E.

doi:10.1117/12.7972468

Cited by 39 publications

(12 citation statements)

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“…The Floquet theory of laser-induced vibrational-rotational excitation of diatomic molecules has been described in detail by Leasure and co-workers [19][20]. Here this theory is briefly summarized and our application of the method is presented.…”

Section: Floquet Theorymentioning

confidence: 98%

“…A statistical mechanical theory has also been formulated [18] and several quantum dynamical calculations have been performed [13,15,[19][20][21][22][23][24][25]. A significant recent development has been the .application of Floquet theory [26], by Leasure and Wyatt [19][20][21][22], to the laser-induced multiphoton excitation of the vibrational-rotational levels of diatomic molecules. This method requires the solution of the time-dependent Schr6dinger equation over the first optical cycle of the laser field, which is represented by the semiclassical electric dipole approximation.…”

Section: Introductionmentioning

confidence: 99%

“…Several classical trajectory calculations have been carried out on the muhiphoton absorption and dissociation process [13][14][15][16][17]. A statistical mechanical theory has also been formulated [18] and several quantum dynamical calculations have been performed [13,15,[19][20][21][22][23][24][25]. A significant recent development has been the .application of Floquet theory [26], by Leasure and Wyatt [19][20][21][22], to the laser-induced multiphoton excitation of the vibrational-rotational levels of diatomic molecules.…”

Section: Introductionmentioning

confidence: 99%

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Quantum dynamical study of molecular overtone transitions induced by intense laser radiation

Clary

1982

Molecular Physics

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Section: Floquet Theorymentioning

confidence: 98%

Section: Introductionmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

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Quantum dynamical study of molecular overtone transitions induced by intense laser radiation

Clary

1982

Molecular Physics

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“…a two-state model may be applied. 15,16,18,20,[22][23][24][25][26][27][28][43][44][45][46][47][48][49][50][51][52] To be clear, the assumption is that the character of the fluorescence emission process, including the effect of the probe radiation, is dominated by two electronic levels; it is not to be presumed that the state from which the fluorescence decay occurs is necessarily the same as the state initially populated by photoexcitation. …”

Section: Two-level Systemsmentioning

confidence: 99%

Laser-Controlled Fluorescence in Two-Level Systems

Leeder

Andrews

2010

J. Phys. Chem. B

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The ability to modify the character of fluorescent emission by a laser-controlled, optically nonlinear process has recently been shown theoretically feasible, and several possible applications have already been identified. In operation, a pulse of off-resonant probe laser beam, of sufficient intensity, is applied to a system exhibiting fluorescence, during the interval of excited state decay following the initial excitation. The result is a rate of decay that can be controllably modified, the associated changes in fluorescence behavior affording new, chemically-specific information. In this paper, a two-level emission model is employed in the further analysis of this all-optical process; the results should prove especially relevant to the analysis and imaging of physical systems employing fluorescent markersthese ranging from quantum dots to green fluorescence protein. Expressions are presented for the lasercontrolled fluorescence anisotropy exhibited by samples in which the fluorophores are randomly oriented. It is also shown that, in systems with suitably configured electronic levels and symmetry properties, fluorescence emission can be produced from energy levels that would normally decay nonradiatively.2

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“…Moreover, the materials that are most effective for the utilization of nonlinear optical effects in frequency conversion (especially in the case of second harmonic generation, forbidden in an isotropic gas) are those whose energy level structures are significantly more complex than atoms. Nonetheless, the two-level model has received wide application in such a context; [6][7][8][9][10][11][12][13][14][15][16][17][18][19][20][21][22] it not only delivers results of a relatively simple form, it also relates well to long-established concepts of chemical structure. In particular, a wealth of synthetic studies [23][24][25][26][27][28][29][30][31][32][33] have been based upon the anticipated and oft-proven connection between 'push-pull' chromophore structures [34][35][36][37][38][39][40] (these facilitating intramolecular electron transfer) and an enhanced second harmonic response.…”

Section: Introductionmentioning

confidence: 99%

Limitations and improvements upon the two-level approximation for molecular nonlinear optics

Andrews¹,

Coles

2011

Nonlinear Frequency Generation and Conversion: Materials, Devices, and Applications X

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When parametric nonlinear processes are employed in the cause of efficient optical frequency conversion, the media involved are generally subjected to substantially off-resonant input radiation. As such, it is usually only electronic ground states of the conversion material that are significantly populated; higher levels are engaged only in the capacity of virtual states, and it is frequently assumed that just one such state dominates in determining the response. Calculating the nonlinear optical susceptibilities of molecules on this basis, excluding all but the ground and one excited state in a sum-over-states formulation, signifies the adoption of a two-level model, a technique that is widely deployed in the calculation and analysis of nonlinear optical properties. The two-level model offers tractable and physically simple representations of molecular response, including wavelength dependence; it is also the origin of the widely applied 'push-pull' approach to designing optically nonlinear chromophores. By contrast, direct ab initio calculations of optical susceptibility are commonly frustrated by a complete failure to determine such dispersion features. However, caution is required; the two-level model can deliver potentially misleading results if it is applied without regard to the criteria for its validity, especially when molecular excited states are significantly populated. On the basis of a precise, quantum electrodynamical basis for the theory, we explore in detail why there are grounds for questioning the general validity of two-level calculations in nonlinear optics; we assess the criteria for high frequency conversion efficiency and provide a new graphical method to assist in determining the applicability of a two-level model for hyperpolarizability calculations. Lastly, this paper also explores the applicability and detailed conditions for the two-level model for electronically excited molecules, identifying problematic results and providing tractable methods for improving the accuracy of calculations on real molecule-photon interactions.

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Floquet Theory Of The Interaction Of A Molecule With A Laser Field: Techniques And An Application

Cited by 39 publications

References 0 publications

Quantum dynamical study of molecular overtone transitions induced by intense laser radiation

Quantum dynamical study of molecular overtone transitions induced by intense laser radiation

Laser-Controlled Fluorescence in Two-Level Systems

Limitations and improvements upon the two-level approximation for molecular nonlinear optics

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