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1.
J Chem Phys ; 128(5): 054104, 2008 Feb 07.
Artigo em Inglês | MEDLINE | ID: mdl-18266442

RESUMO

We investigate theory of single-photon control from a two-level single-molecule source irradiated by laser pulses of various shapes and pulse durations in terms of quantum trajectories which link stochastic dynamics of the radiating source with quantum measurement theory. Using Monte Carlo wave function simulation, we analyze the detailed dissipative dynamics of the single-molecule source and the photon statistics as revealed by repeated Gedanken photon measurement on the single radiating source. We show that much of the photon statistics from the two-level single-molecule single-photon sources, including few-photon emission probability, waiting time distribution, and two-time correlation function of the fluorescent light, can be understood qualitatively from the simple picture of Rabi nutation and pi pulse in terms of pulse areas.

2.
J Chem Phys ; 122(18): 184303, 2005 May 08.
Artigo em Inglês | MEDLINE | ID: mdl-15918700

RESUMO

We investigate the classical and quantum mechanics of diatomic molecules in noncollinear (tilted) static electric and nonresonant linearly polarized laser fields. The classical diatomic in tilted fields is a nonintegrable system, and we study the phase space structure for physically relevant parameter regimes for the molecule KCl. While exhibiting low-energy (pendular) and high-energy (free-rotor) integrable limits, the rotor in tilted fields shows chaotic dynamics at intermediate energies, and the degree of classical chaos can be tuned by changing the tilt angle. We examine the quantum mechanics of rotors in tilted fields. Energy-level correlation diagrams are computed, and the presence of avoided crossings quantified by the study of nearest-neighbor spacing distributions as a function of energy and tilting angle. Finally, we examine the influence of classical periodic orbits on rotor wave functions. Many wave functions in the tilted field case are found to be highly nonseparable in spherical polar coordinates. Localization of wave functions in the vicinity of classical periodic orbits, both stable and unstable, is observed for many states.


Assuntos
Físico-Química/métodos , Algoritmos , Química/métodos , Modelos Estatísticos , Modelos Teóricos , Oscilometria , Física/métodos , Cloreto de Potássio/química , Teoria Quântica
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