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The Journal of Chemical Physics

Selective two-photon excitation of a vibronic state by correlated photons

Hisaki Oka

Published Mar 28, 2011• 29 citations
Publisher

Abstract

We theoretically investigate the two-photon excitation of a molecular vibronic state by correlated photons with energy anticorrelation. A Morse oscillator having three sets of vibronic states is used, as an example, to evaluate the selectivity and efficiency of two-photon excitation. We show that a vibrational mode can be selectively excited with high efficiency by the correlated photons, without phase manipulation or pulse-shaping techniques. This can be achieved by controlling the quantum correlation so that the photon pair concurrently has two pulse widths, namely, a temporally narrow width and a spectrally narrow width. Though this concurrence is seemingly contradictory, we can create such a photon pair by tailoring the quantum correlation between two photons.

DOI
10.1063/1.3573565

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We theoretically investigate the two-photon excitation of a molecular vibronic state by correlated photons with energy anticorrelation. A Morse oscillator having three sets of vibronic states is used, as an example, to evaluate the selectivity and efficiency of two-photon excitation. We show that a vibrational mode can be selectively excited with high efficiency by the correlated photons, without phase manipulation or pulse-shaping techniques. This can be achieved by controlling the quantum correlation so that the photon pair concurrently has two pulse widths, namely, a temporally narrow width and a spectrally narrow width. Though this concurrence is seemingly contradictory, we can create such a photon pair by tailoring the quantum correlation between two photons.
We theoretically investigate two-photon excitation by correlated photons with energy anticorrelation. A three-level atomic system is used to evaluate selectivity and efficiency of two-photon excitation. It is shown that tailored squeezing of two-photon probability distribution concurrently enhances excitation efficiency and high-contrast selective excitation, without phase manipulation or pulse-shaping techniques. We also discuss candidates to generate such squeezed photons in real material systems.
We theoretically investigate the two-step excitation of a molecular vibronic state using quantum-correlated photons with time delay in order to control the population of the vibronic excited state. A Morse oscillator having three sets of vibronic states, namely, the ground state, intermediate states, and excited states, is used to evaluate the efficiency of the two-step excitation process. We show that we can efficiently and selectively excite only a target state by using correlated photons and can control the excitation population of the target state by adjusting the delay time of the correlated photons. The potential of controlling a chemical reaction using correlated photons is also discussed.
We theoretically investigate strongly enhanced vibrational-mode-selective two-step excitation by ultrabroadband frequency-entangled photons. A diatomic molecule having three sets of vibronic states is used to evaluate the excitation efficiency of the two-step excitation. We show that the photon entanglement has little influence on the populations of intermediate vibrational modes of intermediate states but selectively increases the population of a single vibrational mode of excited states, resonant with the total energy of the entangled photons. For an ultrashort pulse close to a monocycle with high degree of entanglement, the population of the vibrational mode is enhanced 2500 times more than by uncorrelated photons, and the selectivity nearly reaches unity. Our results indicate that the two-step excitation with ultrabroadband frequency-entangled photons can achieve highly selective and strongly enhanced excitation of a single vibrational mode.
We theoretically investigate a two-photon process via molecular internal conversion, driven by correlated photons with time delay. As an example, a molecular system approximated by Morse oscillators is used in order to evaluate the efficiency of the process, in terms of how the efficiency changes with the nonadiabatic coupling rate of vibronic states. We show that an efficient two-photon process requires two different correlated photon pairs with positive and negative energy correlations, depending on the value of the nonadiabatic coupling rate.
We theoretically investigate the dynamics of two-photon excitation by correlated photons with energy anticorrelation in terms of how the excitation efficiency depends on incident pulse width. A three-level atomic system having an intermediate state is used to evaluate the efficiency of two-photon excitation. It is shown that for shorter pulses closer to a monocycle pulse the excitation efficiency by correlated photons is enhanced to become 100100100 times as large as that by uncorrelated photons.
We theoretically investigate two-photon excitation by spectrally shaped entangled photons with energy anticorrelation in terms of how the real excitation of an intermediate state affects two-photon absorption by entangled photons. Spectral holes are introduced in the entangled photons around the energy levels of an intermediate state so that two-step excitation via the real excitation of the intermediated state can be suppressed. Using a three-level atomic system as an example, we show that the spectral holes well suppress the real excitation of the intermediate state and recover two-photon absorption via a virtual state. Furthermore, for a short pulse close to a monocycle, we show that the excitation efficiency by the spectrally shaped entangled photons can be enhanced a thousand times as large as that by uncorrelated photons.