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Physical Review A

Two-photon–two-atom excitation by correlated light states

Zhan Zheng, Pablo L. Saldanha, J. R. Rios Leite, Claude Fabre

Published Sep 12, 2013• 23 citations
Publisher

Abstract

We study the efficiency of different two-photon states of light to induce the simultaneous excitation of two atoms of different kinds when the sum of the energies of the two photons matches the sum of the energies of the two atomic transitions, while no photons are resonant with each individual transition. We find that entangled two-photon states produced by an atomic cascade are indeed capable of enhancing by a large factor the simultaneous excitation probability as compared to uncorrelated photons, as predicted some years ago by Muthukrishnan et al., but that several unentangled, separable, correlated states, produced either by an atomic cascade or parametric down-conversion, or even appropriate combinations of coherent states, have comparable efficiencies. We show that the key ingredient for the increase of simultaneous excitation probability is the presence of strong frequency anticorrelation and neither time correlation nor time-frequency entanglement.

DOI
10.1103/physreva.88.033822

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We study the efficiency of different two-photon states of light to induce the simultaneous excitation of two atoms of different kinds when the sum of the energies of the two photons matches the sum of the energies of the two atomic transitions, while no photons are resonant with each individual transition. We find that entangled two-photon states produced by an atomic cascade are indeed capable of enhancing by a large factor the simultaneous excitation probability as compared to uncorrelated photons, as predicted some years ago by Muthukrishnan et al., but that several unentangled, separable, correlated states, produced either by an atomic cascade or parametric down-conversion, or even appropriate combinations of coherent states, have comparable efficiencies. We show that the key ingredient for the increase of simultaneous excitation probability is the presence of strong frequency anticorrelation and neither time correlation nor time-frequency entanglement.
We study in this paper the efficiency of different two-photon states of light to induce the simultaneous excitation of two atoms of different kinds when the sum of the energies of the two photons matches the sum of the energies of the two atomic transitions, while no photons are resonant with each individual transition. We find that entangled two-photon states produced by an atomic cascade are indeed capable of enhancing by a large factor the simultaneous excitation probability as compared to uncorrelated photons, as predicted some years ago by Muthukrishnan et al, but that several non-entangled, separable, correlated states, produced either by an atomic cascade or parametric down conversion, or even appropriate combinations of coher- ent states, have comparable efficiencies. We show that the key ingredient for the increase of simultaneous excitation probability is the presence of strong frequency anti-correlation and not time correlation nor time-frequency entanglement.
We study in this paper the efficiency of different two-photon states of light to induce the simultaneous excitation of two atoms of different kinds when the sum of the energies of the two photons matches the sum of the energies of the two atomic transitions, while no photons are resonant with each individual transition. We find that entangled two-photon states produced by an atomic cascade are indeed capable of enhancing by a large factor the simultaneous excitation probability as compared to uncorrelated photons, as predicted some years ago by Muthukrishnan et al, but that several non-entangled, separable, correlated states, produced either by an atomic cascade or parametric down conversion, or even appropriate combinations of coher- ent states, have comparable efficiencies. We show that the key ingredient for the increase of simultaneous excitation probability is the presence of strong frequency anti-correlation and not time correlation nor time-frequency entanglement.
Two uncoupled two-level atoms cannot be jointly excited by classical light under general circumstances, due to destructive interference of excitation pathways in two-photon absorption. However, with temporally entangled light, two-atom excitation is shown possible. Photons arising from three-level cascade decay are intrinsically ordered in time of emission. This field correlation induces a joint resonance in the two-atom excitation probability via suppression of one of the time-ordered excitation pathways. The relative gain in two-photon absorption increases with the time-frequency entanglement.
Excitation energy transfer is a photophysical process upon which many chemical and biological phenomena are built. From natural small systems to synthetic multichromophoric macromolecules, energy transfer deals with the process of migration of electronic excitation energy from an excited donor to an acceptor. Although this phenomenon has been extensively studied in the past, the rapid evolution of quantum-enabled technologies has led to the question of whether nonclassical sources of light, such as entangled photon pairs, may provide us with better control (or enhancement) of energy transfer at the nanoscale. In this work we provide a comprehensive study of the joint excitation of two noninteracting two-level atoms by time-frequency-correlated photon pairs (whose central frequencies are not resonant with the individual particles) generated by means of spontaneous parametric down-conversion (SPDC). We demonstrate that while strong frequency anticorrelation between photons guarantees a large two-photon excitation (TPE) probability, photons bearing a sine cardinal spectral shape exhibit an approximately 3.8 times larger TPE signal than photons with a Gaussian spectrum. More importantly, we find that suppression of time-ordered excitation pathways does not substantially modify the TPE probability for two-photon states with a Gaussian spectral shape, whereas photons with a sine cardinal spectrum exhibit the strongest TPE signals when two-photon excitation pathways are not suppressed. Our results not only help elucidate the role of time-frequency correlations in resonance energy transfer with SPDC photons, but also provide valuable information regarding the optimal source to be used in the experimental implementation of said process.
Excitation energy transfer is a photophysical process upon which many chemical and biological phenomena are built. From natural small systems to synthetic multichromophoric macromolecules, energy transfer deals with the process of migration of electronic excitation energy from an excited donor to an acceptor. Although this phenomenon has been extensively studied in the past, the rapid evolution of quantum-enabled technologies has motivated the question on whether nonclassical sources of light, such as entangled photon pairs, may provide us with a better control (or enhancement) of energy transfer at the nanoscale. In this work, we provide a comprehensive study of the joint excitation of two non-interacting two-level atoms by time-frequency correlated photon pairs -- whose central frequencies are not resonant with the individual particles -- generated by means of spontaneous parametric down conversion (SPDC). We demonstrate that while strong frequency anti-correlation between photons guarantees a large two-photon excitation (TPE) probability, photons bearing a sine cardinal spectral shape exhibit a $\sim$3.8 times larger TPE signal than photons with a Gaussian spectrum. More importantly, we find that suppression of time-ordered excitation pathways does not substantially modify the TPE probability for two-photon states with a Gaussian spectral shape; whereas photons with a sine cardinal spectrum exhibit the strongest TPE signals when two-photon excitation pathways are not suppressed. Our results not only help elucidating the role of time-frequency correlations in resonance energy transfer with SPDC photons, but also provide valuable information regarding the optimal source to be used in its experimental implementation.
We find that stimulated Raman excitation of an atom by a two-photon pulse can be enhanced by orders of magnitude if the photons are simultaneously frequency correlated and spatially anticorrelated. That is, a correlated photon pair must have an inherent time delay between its constituent photons. This counterintuitive feature is a manifestation of the uncertainty principle, which yields that frequency-correlated photons cannot be time (spatially) correlated. This is opposite to two-photon absorption by a three-level atom, for which the enhancement occurs if photons in the pulse are frequency anticorrelated and spatially correlated, that is, photons in the pair simultaneously interact with the atom. Our findings can be useful for imaging and spectroscopy of biological samples which demand low illumination intensity.