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Physical Review Letters

Rabi Resonances of a Single Molecule Driven by rf and Laser Fields

Ch. Brunel, Brahim Lounis, Philippe Tamarat, Michel Orrit

Published Sep 28, 1998• 49 citations
Publisher

Abstract

Single molecules in a crystal at low temperature are driven simultaneously by a laser and by the electric field of an rf. At weak rf power, we observe Rabi transitions within doublets of dressed states, the first such observation in condensed matter in the optical domain. At higher rf power, resonances involving several rf photons appear. The interplay between rf and laser dynamics induces shifts and broadenings that are in excellent agreement with calculations from optical Bloch equations. We also directly display the Rabi and multi-rf-photon resonances by recording the fluorescence signal versus the rf frequency.

DOI
10.1103/physrevlett.81.2679

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Single molecules in a crystal at low temperature are driven simultaneously by a laser and by the electric field of an rf. At weak rf power, we observe Rabi transitions within doublets of dressed states, the first such observation in condensed matter in the optical domain. At higher rf power, resonances involving several rf photons appear. The interplay between rf and laser dynamics induces shifts and broadenings that are in excellent agreement with calculations from optical Bloch equations. We also directly display the Rabi and multi-rf-photon resonances by recording the fluorescence signal versus the rf frequency.
We present pump-probe experiments on single molecules in a solid matrix, with strong laser fields and a new host-guest system, dibenzanthanthrene in a naphthalene crystal. Besides strong light-shifts of the lines, we observe the hyper-Raman resonance, for the first time in condensed matter. For strong pump and probe, we also observe subharmonic resonances due to a''kicked pendulum'' motion of the Bloch vector. Since our results agree with Bloch's equations without any adjustable parameter, they provide a stringent test of the optical two-level model as applied to single molecules in solids.
The photon emission from a single molecule driven simultaneously by a laser and a slow electric radio frequency (rf) field is studied. We use a non-Hermitian Hamiltonian approach which accounts for the radiative decay of a two-level system modeling the single-molecule source. We apply the renormalization group method for differential equations to obtain long time solution of the corresponding Schrodinger equation, which allows us to calculate the average waiting time for the first photon emission. Then, we analyze the conditions for suppression and enhancement of photon emission in this dissipative two-level system. In particular we derive a transcendental equation, which yields the nontrivial rf field control parameters, for which enhancement and suppression of photon emission occurs. For finite values of radiative decay rate an abrupt transition to the state when both situations are indistinguishable is found for certain values of the rf field parameters. Our results are shown to be in agreement with the available experiments [Ch. Brunel et al., Phys. Rev. Lett. 81, 2679 (1998)].
We report on the excitation of single molecules via narrow zero-phonon transitions using short laser pulses. By monitoring the Stokes-shifted fluorescence, we studied the excited state population as a function of the delay time, laser intensity, and frequency detuning. A $\ensuremath{\pi}$-pulse excitation was demonstrated with merely 500 photons, and 5 Rabi cycles were achieved at higher excitation powers. Our findings are in good agreement with theoretical calculations and provide a first step toward coherent manipulation of the electronic states of single molecules with few photons.
Calculations based on a full master equation approach have been made of the absorption spectrum for a certain three-level system in which two states mod 2), mod 1) are strongly driven by a near resonant monochromatic laser field whose Rabi frequency is large compared with the natural lifetime width of mod 2). A third state mod 3) is coupled to the nearby state mod 2) by a static electric field. As the static field coupling increases the spectrum in the neighbourhood of the laser frequency changes from the partly emissive, partly absorptive Mollow form to an absorptive spectrum with two strong peaks. Also, the spectrum in the neighbourhood of the upper level transition frequency changes from an Autler-Townes doublet to a spectrum where a new emissive line appears at the Rabi frequency. In terms of the dressed atom model, this transition corresponds to an intradoublet transition previously forbidden in two-level atoms, though predicted to occur in certain two-level molecular systems. The spectrum is interpreted in terms of a dressed atom model. In general terms not only do the dressed atom transition frequencies correlate well with the spectral features, but there is also good agreement between the heights and widths of the spectral features and those obtained from the full master equation approach. The importance of using the full dipole operator in the basic definitions of the spectral quantities is also demonstrated.
The decay characteristics of two-state Rydberg atoms are investigated in a microwave cavity driven simultaneously by two strong rf fields. Tuning one of the driving fields leads to sharp resonances in the decay rate of the upper atomic level. Their width may become smaller than the cavity linewidth and transit time broadening. We present a theoretical model, interpreting the resonances as cavity-induced decay of Floquet states of the composite atom-field system. The observed phenomena arise from the interplay of cavity-modified Bloch-Siegert shifts and dynamic enhancement of spontaneous emission at single-photon and multiphoton resonances.