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The Journal of Chemical Physics

Control of vibronic excitation using quantum-correlated photons

Hisaki Oka

Published Oct 25, 2011• 19 citations
Publisher

Abstract

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.

DOI
10.1063/1.3654136

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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 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 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 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.
In this paper, we theoretically investigate the control of the non-resonant two-photon absorption induced by two time-delayed laser pulses, and an analytical solution for the dependence of the two-photon transition probability on the time delay and relative carrier-envelope phase of the two laser pulses is achieved. We show that the two-photon absorption can be significantly enhanced or completely suppressed by varying the time delay between the two laser pulses or their relative carrier-envelope phase. We also show that the two-photon absorption can be selectively excited when two excited states are simultaneously excited. Furthermore, we discuss the two-photon absorption control in the molecular system and analyze the effect of the absorption bandwidth on the control efficiency of the two-photon absorption.
Using second-order perturbation theory in the light-matter interaction, we derive an analytical approximation for the vibronic populations of a diatomic system excited by ultrabroadband frequency-entangled photons and evaluate the population dynamics for different degrees of entanglement between photon pairs. Our analytical approach makes the same predictions as previously derived via numerical solutions of the complete Schrödinger equation [H. Oka, ], with the added advantage of providing clear physical insights into the vibronic selectivity as a function of the degree of photon correlations while requiring significantly reduced computational effort. Specifically, our analytical expression for the probability of vibronic excitation includes a factor which predicts the enhancement of vibrational selectivity as a function of the degree correlation between the entangled photon pairs, the targeted vibrational energy level, and the vibrational molecular structure encoded in the Franck-Condon factors. Our results illustrate the importance of going beyond the usual approximations in second-order perturbation theory to capture the relevance of the vibrational structure of the molecular system of interest in order to gain a deeper understanding of the possible quantum-enhancement provided by the interaction between quantum light and matter.
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.