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Physical Review A

Optical and microwave control of resonance fluorescence and squeezing spectra in a polar molecule

M. A. Antón, S. Maede-Razavi, F. Carreño, Ioannis Thanopulos, Emmanuel Paspalakis

Published Dec 8, 2017• 26 citations

Abstract

A two-level quantum emitter with broken inversion symmetry simultaneously driven by an optical field and a microwave field that couples to the permanent dipole's moment is presented. We focus to a situation where the angular frequency of the microwave field is chosen such that it closely matches the Rabi frequency of the optical field, the so-called Rabi resonance condition. Using a series of unitary transformations we obtain an effective Hamiltonian in the double-dressed basis which results in easily solvable Bloch equations which allow us to derive analytical expressions for the spectrum of the scattered photons. We analyze the steady-state population inversion of the system which shows a distinctive behavior at the Rabi resonance with regard to an ordinary two-level nonpolar system. We show that saturation can be produced even in the case that the optical field is far detuned from the transition frequency, and we demonstrate that this behavior can be controlled through the intensity and the angular frequency of the microwave field. The spectral properties of the scattered photons are analyzed and manifest the emergence of a series of Mollow-like triplets which may be spectrally broadened or narrowed for proper values of the amplitude and/or frequency of the low-frequency field. We also analyze the phase-dependent spectrum which reveals that a significant enhancement or suppression of the squeezing at certain sidebands can be produced. These quantum phenomena are illustrated in a recently synthesized molecular complex with high nonlinear optical response although they can also occur in other quantum systems with broken inversion symmetry.

DOI: 10.1103/physreva.96.063812

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A two-level quantum emitter with broken inversion symmetry simultaneously driven by an optical field and a microwave field that couples to the permanent dipole's moment is presented. We focus to a situation where the angular frequency of the microwave field is chosen such that it closely matches the Rabi frequency of the optical field, the so-called Rabi resonance condition. Using a series of unitary transformations we obtain an effective Hamiltonian in the double-dressed basis which results in easily solvable Bloch equations which allow us to derive analytical expressions for the spectrum of the scattered photons. We analyze the steady-state population inversion of the system which shows a distinctive behavior at the Rabi resonance with regard to an ordinary two-level nonpolar system. We show that saturation can be produced even in the case that the optical field is far detuned from the transition frequency, and we demonstrate that this behavior can be controlled through the intensity and the angular frequency of the microwave field. The spectral properties of the scattered photons are analyzed and manifest the emergence of a series of Mollow-like triplets which may be spectrally broadened or narrowed for proper values of the amplitude and/or frequency of the low-frequency field. We also analyze the phase-dependent spectrum which reveals that a significant enhancement or suppression of the squeezing at certain sidebands can be produced. These quantum phenomena are illustrated in a recently synthesized molecular complex with high nonlinear optical response although they can also occur in other quantum systems with broken inversion symmetry.

Coherent, optically dressed media composed of two-level molecular systems without inversion symmetry are considered as all-optically tunable sources of coherent radiation in the microwave domain. A theoretical model and a numerical toolbox are developed to confirm the main finding: the generation of low-frequency radiation, and the buildup and propagation dynamics of such low-frequency signals in a medium of polar molecules in a gas phase. The physical mechanism of the signal generation relies on the permanent dipole moment characterizing systems without inversion symmetry. The molecules are polarized with a DC electric field yielding a permanent electric dipole moment in the laboratory frame; the direction and magnitude of the moment depend on the molecular state. As the system is resonantly driven, the dipole moment oscillates at the Rabi frequency and, hence, generates microwave radiation. We demonstrate the tuning capability of the output signal frequency with the drive amplitude and detuning. We find that even though decoherence mechanisms such as spontaneous emission may damp the output field, a scenario based on pulsed illumination yields a coherent, pulsed output of tunable temporal width. Finally, we discuss experimental scenarios exploiting rotational levels of gaseous ensembles of heteronuclear diatomic molecules.

Abstract The fluorescent radiative properties of a two-level quantum polar system with broken spatial inversion symmetry being realized as a model of a single-electron two-level “atom” with permanent atomic electric dipole moment, so that its electric dipole operator diagonal matrix elements are not equal to each other, were examined. In practice, such a system can be realized as an asymmetric quantum dot. A particular case when this system is driven by a trichromatic external field, with two high-frequency bichromatic field components of equal Rabi frequencies and carrier frequencies being placed symmetrically around the atomic transition frequency, and one more low-frequency component being in resonance with the Rabi frequency of the high-frequency components, was analyzed. It was shown that the high-frequency spectral properties of the fluorescent radiation can be altered with equal efficiency either by controlling the intensity of the low-frequency component of the trichromatic driving field or by changing the degree of the quantum dot asymmetry. Possible options to apply this potentially useful effect for practical purposes in the field of optoelectronics are also discussed.

We study spectral properties of fluorescent radiation from a two-level quantum system with broken inversion spatial symmetry, which can be implemented as a model of a one-electron two-level atom whose electric dipole moment operator has permanent unequal diagonal matrix elements. We consider the case of the excitation of this system by a bichromatic laser field consisting of a high-frequency resonance component with the frequency coinciding with the atomic transition frequency and a low-frequency component whose frequency coincides with the Rabi frequency of the high-frequency component. We show that by changing the intensity of the low-frequency component, we can efficiently control spectral properties of the fluorescent radiation of the system in the high-frequency range. We discuss possible methods for the experimental detection and practical use of the effects under study.

Spectral properties of fluorescent radiation from a two-level quantum system with broken inversion spatial symmetry, which can be described by a model of an one-electron two-level atom whose electric dipole moment operator has permanent unequal diagonal matrix elements, were studied. The case of the excitation of this system by a polychromatic laser field, comprised of

N-1

high-frequency components with the frequencies close to or being in resonance with the atomic transition frequency, and a low-frequency component whose frequency coincides with the Rabi frequency of the high-frequency components, was considered. Special attention was given to the resonant bichromatic and nearly resonant trichromatic excitation. In the former case it was shown that by changing the intensity of the low-frequency component, one can efficiently alter spectral properties of the fluorescent radiation of the system in the high-frequency range, while in the latter case it was found that the fluorescent behavior of the system in question reveals a kind of an optoelectronic transistor effect. Options for the experimental detection and practical usage of the effects under study were discussed.

Abstract We studied spectral properties of high-frequency fluorescent radiation from a two-level quantum system with broken inversion spatial symmetry, which can be implemented as a model of a one-electron two-level asymmetric polar semiconductor quantum dot whose electric dipole moment operator has permanent unequal diagonal matrix elements. The case of the excitation of this system by incoherent pumping of some sort supplemented with an additional driving monochromatic field, which frequency is much lower than the optical transition frequency of the quantum dot, was considered. An analytical expression for the fluorescence spectrum as a function of the amplitude and frequency of the monochromatic driving field, as well as of the pumping intensity, was derived. We also discussed feasible practical applications of the effects under study in the field of quantum optics and optoelectronics for the generation of high-frequency radiation, possessing stationary equidistant spectrum, and for the control of the radiative properties of such nanodevices as spasers (dipole nanolasers).

We present the theory of resonance fluorescence from an asymmetric quantum dot driven by a two-component electromagnetic field with two different frequencies, polarizations, and amplitudes (bichromatic field) in the regime of strong light-matter coupling. It follows from the elaborated theory that the broken inversion symmetry of the driven quantum system and the bichromatic structure of the driving field result in unexpected features of the resonance fluorescence, including the infinite set of Mollow triplets, the quench of fluorescence peaks induced by the dressing field, and the oscillating behavior of the fluorescence intensity as a function of the dressing field amplitude. These quantum phenomena are of general physical nature and, therefore, can take place in various double-driven quantum systems with broken inversion symmetry.