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arXiv:0906.0213 · Journal of the Physical Society of Japan

Full Quantum Analysis of Two-Photon Absorption Using Two-Photon Wave Function: Comparison of Two-Photon Absorption with One-Photon Absorption

Toshihiro Nakanishi, Hirokazu Kobayashi, Kazuhiko Sugiyama, Masao Kitano

Published Sep 25, 2009• 9 citations
arXivHTMLPDF

Abstract

For dissipation-free photon-photon interaction at the single photon level, we analyze one-photon transition and two-photon transition induced by photon pairs in three-level atoms using two-photon wavefunctions. We show that the two-photon absorption can be substantially enhanced by adjusting the time correlation of photon pairs. We study two typical cases: Gaussian wavefunction and rectangular wavefunction. In the latter, we find that under special conditions one-photon transition is completely suppressed while the high probability of two-photon transition is maintained.

DOI
10.1143/jpsj.78.104401

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For dissipation-free photon-photon interaction at the single photon level, we analyze one-photon transition and two-photon transition induced by photon pairs in three-level atoms using two-photon wavefunctions. We show that the two-photon absorption can be substantially enhanced by adjusting the time correlation of photon pairs. We study two typical cases: Gaussian wavefunction and rectangular wavefunction. In the latter, we find that under special conditions one-photon transition is completely suppressed while the high probability of two-photon transition is maintained.
We present a theoretical analysis of two-photon absorption of classical and squeezed light valid when one-photon absorption to an intermediate state is either resonant or far-detuned from resonance, and in both the low and high intensity regimes. In this paper we concentrate on continuous-wave excitation, although the approach we develop is more general. We calculate the energy removed from an incident field for typical experimental parameters and consider the limiting cases when the photon pairs are narrowband or broadband compared to the molecular linewidths. We find an enhancement of the two-photon absorption due to resonant contributions from the large squeezed light bandwidth and due to photon bunching in the low intensity regime. However, in both cases, for the parameters we choose, the one-photon absorption is the dominant process in the region of parameter space where a large enhancement of the two-photon absorption is possible.
We show that it is possible to use a single sideband to induce two-photon transparency in a three-level cascade medium. The medium simultaneously absorbs two photons as a one-step process when the middle level is far off one-photon resonance. A resonant sideband coupling on the upper transition and the two-photon one-step process drive the medium into a trapped state, and the dominant component is the ground state. Thus almost all population is trapped in the ground state and the two-photon absorption is dramatically suppressed. We present a numerical calculation for arbitrary values of the atomic and field parameters and also provide an analytic description for the required conditions.
Two-photon transitions have provided the basis for numerous useful nonlinear interactions with radiation. In this paper we calculate the absorption and coupling coefficients for one-, two-, and three-wave mixing in two-photon homogeneously broadened media. The resulting field equations form the basis for understanding saturation spectroscopy, phase conjugation,1 and single-mode instabilities2 in lasers and optical bistability in two-photon media. We assume that the wave frequencies are not resonant with any intermediate state j and that the probe and conjugate waves cannot saturate the two-photon transition. This allows us to use the two-photon two-level model and to transfer much of our knowledge of the one-photon two-level systems to the two-photon case. Two major differences occur between the two models. First, dynamic Stark shifts of the active levels play an important role in generating asymmetric spectra and nonzero dispersion (≃ω s T1) at line center. Second, high pump intensities do not bleach the absorption coefficient at the Rabi sidebands.
The process of two-photon absorption from two beams of light is treated theoretically. Expressions are derived for the time dependences of the joint photon probability distribution of the beams, their photon-number factorial moments and the photon-number correlation between the beams. These expressions are illustrated by numerical results for special cases and their significance is discussed in physical terms. Simpler approximate expressions are also derived for the case where one beam is much more intense than the other.
The interaction of single photons with single atoms is a fundamental process in quantum optics which manifests the quantum mechanical nature of light and matter. As an experimentally controlled process it enables the implementation of quantum technological applications, such as quantum information processing and quantum metrology. In the last decades, substantial progress has been attained to experimentally control and manipulate single atoms. For example, single or multiple ions can be stored in an ion trap and their quantum states can be controlled with great precision. At the same time, experimental techniques to generate and control single photons and entangled photon pairs have been widely developed. However, only modest progress has been attained in controlling the interaction of single atoms with sin~le photons. The aim of this thesis project was to experimentally study he absorption of single photons and entangled photons pairs by single trapped DCa· ions. To this end, a source of polarization-entangled photon pairs based on the process of spontaneous parametric down-conversion (SPDC) was designed and constructed . Generating photon pairs whose interaction with an atom can be controlled imposed stringent requirements on the bandwidth, tunability, stability and brightness of the source, making its setup much more complex than usual SPDC sources. In a parallel project, a set of two separate ion traps were built, capable of storing a single or a set of a few 4DCa· ions. he first part of the thesis documents the design, construction , operation and characterization of the entangled photon pair source. The characterization proves all the necessary requirements for the photons to interact with either of two transitions, D312 P312 and D5i2 P312 at 850 and 854 nm respectively, in 4DCa· One of the crucial requirements was to make the source bandwidth match the bandwidth of these transitions (22MHz). This was not straightforward since the typical emission bandwidths of the SPDC process is several orders of magnitude higher (1 05MHz). The ion trap setup is also briefly described. One of its crucial features is the inclusion of two high numerical-aperture objectives very close to the ion trap, allowing to enhance the interaction efficiency of the SPDC photons with the ion, and to efficiently collect the fluorescence light they emit. In a second part of the thesis, a concise description of the schemes and techniques used to detect the absorption of single photons by a single trapped ion is given, including a heoretical treatment of the methods used to analyze the data. he core part of the thesis describes the methods used to couple the entangled photon source to one of the ion traps, and explains the results obtained with the combined setup. First it shows how the source is configured to produce heralded single photons. It then presents experiments in which the absorption by a single ion of photons produced by the source is detected, and how these absorption events are time-correlated with the detection of the heralding photon. These experiments are performed under several conditions, with a growing level of control over the interaction process. Finally, two proof-of-principle experiments are presented. In the first one, the ion is pumped to polarization-sensitive Zeeman substates and the polarization dependence of the correlated absorption rate is observed. This is a first step toward more advanced experiments in which the polarization entanglemen of the photon pairs is transferred to the entanglement of one photon with one atom or to two distant atoms. A second experiment performs heralded single photon spectroscopy on a single ion, showing the expected frequency dependence of the absorption process. Finally, methods to extend these experiments to implement entanglement transfer from photons to atoms are outlined. In particular, it is shown how the efficiency of the source can be improved to make these experiments feasible.
Two-photon absorption is theoretically analyzed within the semiclassical formalism of radiation-matter interaction. We consider an ensemble of inhomogeneously broadened three-level atoms subjected to the action of two counterpropagating fields of the same frequency. By concentrating in the limit of large detuning in one-photon transitions, we solve perturbatively the Bloch equations in a non-usual way. In this way we derive an analytical expression for the width of the two-photon resonance that makes evident sub-Doppler two--photon spectroscopy. We also derive an analytical expression for the Stark shift of the two-photon resonance.