dorsal/arxiv
View SchemaQuantum interference in the fluorescence of a molecular system
| Authors | Jin Wang, H. M. Wiseman, Z. Ficek |
|---|---|
| Categories | |
| ArXiv ID | quant-ph/9909059 |
| URL | https://arxiv.org/abs/quant-ph/9909059 |
| DOI | 10.1103/PhysRevA.62.013818 |
Abstract
It has been observed experimentally [H.R. Xia, C.Y. Ye, and S.Y. Zhu, Phys. Rev. Lett. {\bf 77}, 1032 (1996)] that quantum interference between two molecular transitions can lead to a suppression or enhancement of spontaneous emission. This is manifested in the fluorescent intensity as a function of the detuning of the driving field from the two-photon resonance condition. Here we present a theory which explains the observed variation of the number of peaks with the mutual polarization of the molecular transition dipole moments. Using master equation techniques we calculate analytically as well as numerically the steady-state fluorescence, and find that the number of peaks depends on the excitation process. If the molecule is driven to the upper levels by a two-photon process, the fluorescent intensity consists of two peaks regardless of the mutual polarization of the transition dipole moments. If the excitation process is composed of both a two-step one-photon process and a one-step, two-photon process, then there are two peaks on transitions with parallel dipole moments and three peaks on transitions with antiparallel dipole moments. This latter case is in excellent agreement with the experiment.
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"abstract": "It has been observed experimentally [H.R. Xia, C.Y. Ye, and S.Y. Zhu, Phys.\nRev. Lett. {\\bf 77}, 1032 (1996)] that quantum interference between two\nmolecular transitions can lead to a suppression or enhancement of spontaneous\nemission. This is manifested in the fluorescent intensity as a function of the\ndetuning of the driving field from the two-photon resonance condition. Here we\npresent a theory which explains the observed variation of the number of peaks\nwith the mutual polarization of the molecular transition dipole moments. Using\nmaster equation techniques we calculate analytically as well as numerically the\nsteady-state fluorescence, and find that the number of peaks depends on the\nexcitation process. If the molecule is driven to the upper levels by a\ntwo-photon process, the fluorescent intensity consists of two peaks regardless\nof the mutual polarization of the transition dipole moments. If the excitation\nprocess is composed of both a two-step one-photon process and a one-step,\ntwo-photon process, then there are two peaks on transitions with parallel\ndipole moments and three peaks on transitions with antiparallel dipole moments.\nThis latter case is in excellent agreement with the experiment.",
"arxiv_id": "quant-ph/9909059",
"authors": [
"Jin Wang",
"H. M. Wiseman",
"Z. Ficek"
],
"categories": [
"quant-ph"
],
"doi": "10.1103/PhysRevA.62.013818",
"title": "Quantum interference in the fluorescence of a molecular system",
"url": "https://arxiv.org/abs/quant-ph/9909059"
},
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