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arXiv:0704.2859 · Physical Review A

Theory of two-photon interactions with broadband down-converted light and entangled photons

Barak Dayan

Published Oct 11, 2007• 141 citations
arXivHTMLPDF

Abstract

When two-photon interactions are induced by down-converted light with a bandwidth that exceeds the pump bandwidth, they can obtain a behavior that is pulselike temporally, yet spectrally narrow. At low photon fluxes this behavior reflects the time and energy entanglement between the down-converted photons. However, two-photon interactions such as two-photon absorption (TPA) and sum-frequency generation (SFG) can exhibit such a behavior even at high power levels, as long as the final state (i.e., the atomic level in TPA, or the generated light in SFG) is narrow-band enough. This behavior does not depend on the squeezing properties of the light, is insensitive to linear losses, and has potential applications. In this paper we describe analytically this behavior for traveling-wave down conversion with continuous or pulsed pumping, both for high- and low-power regimes. For this we derive a quantum-mechanical expression for the down-converted amplitude generated by an arbitrary pump, and formulate operators that represent various two-photon interactions induced by broadband light. This model is in excellent agreement with experimental results of TPA and SFG with high-power down-converted light and with entangled photons [Dayan et al., Phys. Rev. Lett. 93, 023005 (2004); 94, 043602 (2005); Pe'er et al., ibid. 94, 073601 (2005)].

DOI
10.1103/physreva.76.043813

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When two-photon interactions are induced by down-converted light with a bandwidth that exceeds the pump bandwidth, they can obtain a behavior that is pulselike temporally, yet spectrally narrow. At low photon fluxes this behavior reflects the time and energy entanglement between the down-converted photons. However, two-photon interactions such as two-photon absorption (TPA) and sum-frequency generation (SFG) can exhibit such a behavior even at high power levels, as long as the final state (i.e., the atomic level in TPA, or the generated light in SFG) is narrow-band enough. This behavior does not depend on the squeezing properties of the light, is insensitive to linear losses, and has potential applications. In this paper we describe analytically this behavior for traveling-wave down conversion with continuous or pulsed pumping, both for high- and low-power regimes. For this we derive a quantum-mechanical expression for the down-converted amplitude generated by an arbitrary pump, and formulate operators that represent various two-photon interactions induced by broadband light. This model is in excellent agreement with experimental results of TPA and SFG with high-power down-converted light and with entangled photons [Dayan et al., Phys. Rev. Lett. 93, 023005 (2004); 94, 043602 (2005); Pe'er et al., ibid. 94, 073601 (2005)].
We address theoretically the question of classical stochastic fields mimicking quantum states of light in the context of nonlinear spectroscopy and nonlinear optics, in particular two-photon absorption (TPA) and sum-frequency generation (SFG) driven by weak or bright broadband squeezed vacuum with time-frequency entanglement between photons. Upon using a well-defined but ad hoc subtraction of vacuum-energy terms (renormalization), we find that the classical stochastic model yields exactly the same predictions as the full quantum-field theory for all of the phenomena considered here, in both the low-gain and high-gain regimes of squeezed vacuum. Such predictions include the linear-flux scaling of TPA and SFG rates at low incident photon flux, as well as the dependence of TPA and SHG rates on the relative linewidths of the squeezed light and the ground-to-final-state transition in the material system, and the spectrum of SFG generated by bright squeezed vacuum.
We experimentally demonstrate two-photon absorption with broadband down-converted light (squeezed vacuum). Although incoherent and exhibiting the statistics of a thermal noise, broadband down-converted light can induce two-photon absorption with the same sharp temporal behavior as femtosecond pulses, while exhibiting the high spectral resolution of the narrow band pump laser. Using pulse-shaping methods, we coherently control two-photon absorption in rubidium, demonstrating spectral and temporal resolutions that are 3-5 orders of magnitude below the actual bandwidth and temporal duration of the light itself. Such properties can be exploited in various applications such as spread-spectrum optical communications, tomography, and nonlinear microscopy.
The coherence properties of broadband down converted light are investigated theoretically and experimentally in both the classical and quantum mechanical frameworks. Although broadband down converted light is one-photon incoherent noise, it possesses unique two-photon coherence. Thus, for performing two-photon processes, down-converted light is equivalent to coherent ultrashort pulses in some aspects and to coherent CW laser radiation in others. This equivalence is theoretically established and experimentally demonstrated in the classical, high-power regime. Two applications that take advantage of multi-photon coherence are then described in detail; one for optical spread spectrum communication and the other for sub-diffraction limit optical lithography. A key part of this research is the design and implementation of an efficient source that generates high-power broadband down conversion in a cavity. A broadband oscillation in the cavity is ensured by a mechanism very similar to passive mode-locking of ultrashort pulse laser sources, which we term as pair-wise mode locking, thus extending the equivalence to ultrashort pulses to the light generating sources also. Finally, the quantum mechanical properties of broadband down-conversion are explored experimentally, by performing a two-photon process (sum frequency generation) at the low power level of entangled photon pairs. The non-classical nature of the light is expressed by a linear intensity dependence of the non-linear process. Temporal shaping with femtosecond resolution of the entangled photon pairs is demonstrated using this non-linear interaction.
Nonlinear optics has had extensive application into a vast array of scientific fields. One such nonlinear process, two-photon absorption (TPA), has had a wildly successful \nadoption into the field of biological imaging and microscopy. As far and as fast as this field is progressing, limitations stemming from the use of ultrafast lasers are starting to appear. \nIn this work, an alternative nonclassical light source will be motivated for the application \nof low photon-flux two-photon microscopy. The origin and properties of the chosen \nnonclassical source, spontaneous parametric downconversion (SPDC), will be discussed along with the spatial and spectral properties modelled. Nonlinear processes such as TPA and sum frequency generation (SFG) will be viewed as "ultrafast coincidence measurements" of two photons arriving at a molecule within the time window of excitation. These ultrafast coincidence measurements will be viewed in an alternative manner: in terms of the second-order coherence from a light source. This degree of second-order coherence can be subdivided into two categories arising from different combinations of correlations within and between entangled photon pairs. Of interest, the energy-time correlations within the photon pair allow for enhancements in ultrafast coincidence rates over coherent light sources. The makings of an experimental setup to demonstrate enhanced rates from ultrafast two-photon coincidences taking place in SFG in a nonlinear crystal will be discussed.
While two-photon absorption (TPA) and other forms of nonlinear interactions of molecules with isolated time-frequency-entangled photon pairs (EPP) have been predicted to display a variety of fascinating effects, their potential use in practical quantum-enhanced molecular spectroscopy requires close examination. This paper presents a detailed theoretical study of quantum-enhanced TPA by both photon-number correlations and spectral correlations, including an account of the deleterious effects of dispersion. While such correlations in EPP created by spontaneous parametric down conversion can increase the TPA rate significantly in the regime of extremely low optical flux, we find that for typical molecules in solution this regime corresponds to such low TPA event rates as to be unobservable in practice. Our results support the usefulness of EPP spectroscopy in atomic or other narrow-linewidth systems, while questioning the efficacy of such approaches for broadband systems including molecules in solution.
We closely replicated and extended a recent experiment ("Spatial properties of entangled two-photon absorption," Phys. Rev. Lett. 129, 183601, 2022) that reportedly observed enhancement of two-photon absorption rates in molecular samples by using time-frequency-entangled photon pairs, and we found that in the low-flux regime, where such enhancement is theoretically predicted in-principle, the two-photon fluorescence signal is below detection threshold using current state-of-the-art methods. The results are important in the context of efforts to enable quantum-enhanced molecular spectroscopy and imaging at ultra-low optical flux. Using an optical parametric down-conversion photon-pair source that can be varied from the low-gain spontaneous regime to the high-gain squeezing regime, we observed two-photon-induced fluorescence in the high-gain regime but in the low-gain regime any fluorescence was below detection threshold. We supplemented the molecular fluorescence experiments with a study of nonlinear-optical sum-frequency generation, for which we are able to observe the low-to-high-gain crossover, thereby verifying our theoretical models and experimental techniques. The observed rates (or lack thereof) in both experiments are consistent with theoretical predictions and with our previous experiments, and indicate that time-frequency photon entanglement does not provide a practical means to enhance in-solution molecular two-photon fluorescence spectroscopy or imaging with current techniques.