Time- and frequency-gated two-photon counting is given by a four-time correlation function of the electric field. This reduces to two times with purely time gating. We calculate this function for entangled photon pulses generated by parametric down-conversion. At low intensity, the pulses consist of well-separated photon pairs, and crossover to squeezed light as the intensity is increased. This is illustrated by the two-photon absorption signal of a three-level model, which scales linearly for a weak pump intensity where both photons come from the same pair, and gradually becomes nonlinear as the intensity is increased. We find that the strong frequency correlations of entangled photon pairs persist even for higher photon numbers. This could help facilitate the application of these pulses to nonlinear spectroscopy, where these correlations can be used to manipulate congested signals.
Time- and frequency-gated two-photon counting is given by a four-time correlation function of the electric field. This reduces to two times with purely time gating. We calculate this function for entangled photon pulses generated by parametric down-conversion. At low intensity, the pulses consist of well-separated photon pairs, and crossover to squeezed light as the intensity is increased. This is illustrated by the two-photon absorption signal of a three-level model, which scales linearly for a weak pump intensity where both photons come from the same pair, and gradually becomes nonlinear as the intensity is increased. We find that the strong frequency correlations of entangled photon pairs persist even for higher photon numbers. This could help facilitate the application of these pulses to nonlinear spectroscopy, where these correlations can be used to manipulate congested signals.
We use a nonperturbative theoretical approach to the parametric down-conversion (PDC) process, which generates an entangled-photon field for an arbitrarily strong pump-pulse. This approach can be used to evaluate multipoint field correlation functions to compute nonlinear spectroscopic signals induced by a strong pump. The entangled-photon statistics is studied using Glauber’s g (2) function, which helps understand the significance of the photon entanglement-time and the pump-pulse intensity on spectroscopic signals. Under the nonperturbative treatment of the entangled field, the two-photon absorption (TPA) signal shows linear to strongly nonlinear growth with the pump intensity, rather than the linear to quadratic scaling reported previously. An increase in the range of pump intensity for the linear scaling is observed as the pump bandwidth is increased. We propose an experimental scheme that can select contributions to the TPA signal that arise solely from interactions with the entangled photons, and filter out unentangled-photon contributions, which are dominant at higher pump intensities, paving a way to explore the entanglement effects at higher intensities.
The application of quantum states of light such as entangled photons, for example, created by parametric down conversion, has experienced tremendous progress in the almost 40 years since their first experimental realization. Initially, they were employed in the investigation of the foundations of quantum physics, such as the violation of Bell's inequalities and studies of quantum entanglement. They later emerged as basic platforms for quantum communication protocols and, in the recent experiments on single-photon interactions, in photonic quantum computation. These applications aim at the controlled manipulation of the photonic degrees of freedom, and therefore rely on simple models of matter, where the analysis is simpler. Furthermore, quantum imaging with entangled light can achieve enhanced resolution, and quantum metrology can overcome the shot noise limit for classical light. This Account focuses on an entirely different emerging class of applications using quantum light as a powerful spectroscopic tool to reveal novel information about complex molecules. These applications utilize two appealing properties of quantum light: its distinct intensity fluctuations and its nonclassical bandwidth properties. These give rise to new and surprising behavior of nonlinear optical signals. Nonclassical intensity fluctuations can enhance nonlinear optical signals relative to linear absorption. For instance, the two-photon absorption of entangled photon pairs scales linearly (rather than quadratically) in the photon flux, just like a single photon absorption. This enables nonlinear quantum spectroscopy of photosensitive, for example, biological, samples at low light intensities. We will discuss how the two-photon absorption cross section becomes a function of the photonic quantum state, which can be manipulated by properties of the entangled photon pairs. In addition, the quantum correlations in entangled photon states further influence the nonlinear signals in a variety of ways. Apart from affecting the signal's scaling with intensity, they also constitute an entirely new approach to shaping and controlling excitation pathways in molecular aggregates in a way that cannot be achieved with shaped classical pulses. This is because between the two absorption events in entangled two-photon absorption, the light and material system are entangled. Classical constraints for the simultaneous time and frequency resolution can thus be circumvented, since the two are not Fourier conjugates. Here we review the simplest manifestation of quantum light spectroscopy, two-photon absorption spectroscopy with entangled photons. This will allow us to discuss exemplarily the impact of quantum properties of light on a nonlinear optical signal and explore the opportunities for future applications.
Measurement of photon-number statistics of fields composed of photon pairs generated in spontaneous parametric down-conversion pumped by strong ultrashort pulses is described. Finite detection quantum efficiencies, noises as well as possible loss of one or both photons from a pair are taken into account. Measured data provided by an intensified CCD camera are analyzed along the developed model. The joint signal-idler photon-number distribution is obtained using the expectation maximization algorithm. Covariance of the signal and idler photon-numbers exceeds 98%. Entanglement area of the correlated photon pairs is determined.
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.
Efficient Generation of Entangled Photon-Pairs The first experiments with correlated photons have been performed in the context of EPR-Bell experiments on the realistic and local properties of quantum mechanics. The source used there produced pairs of polarization entangled photons from a 2-photon decay of Calcium atoms. The technical requirements of these experiments were high (vacuum systems, stronge dye-lasers, etc.) whereas the efficiency of the source was quite low. An important step forward was the introduction of spontaneous parametric down conversion (SPDC), which has become the most common source in quantum optics for generating correlated or entangled photon pairs. In this process photons of an intense pump laser convert to photon pairs in an optical nonlinear crystal. Conservation of energy and momentum leads to strong correlations between the generated photons. With this kind of two-photon source it was possible to realize or improve many experiments on the foundations of quantum mechanics addressing the EPR-Paradoxon and in the new field of quantum information. But again, more advanced experiments and applications suffer from the limited ef- ficiency of the fluorescence process. Many photon pairs are lost by spatial and spectral filtering, which is necessary to achieve polarization entanglement and long coherence times. Different techniques have been implemented to increase the number of photon pairs using two-crystal arrangements, focusing techniques or periodically poled crystals. Most of these methods have the disadvantage that no entangled photons have been observed. It is the aim of this work to increase the yield and to improve the mode definition of entangled photon pairs generated by resonant enhancement of the pump mode and the fluorescence modes. As a first step a linear cavity for the pump mode was realized. Since the conversion probability is proportional to the pump power it was possible to increase the photon pair count rate by factor of 7 over the previous source. Besides the possibility of further improvement on already established pair correlation experiments, such an enhancement allows to build a compact source for photon pairs, in which an expensive argon-ion laser is replaced by a cheap diode laser. Among other applications such sources are of strong interest for quantum cryptography. 3 In many quantum information experiments optical fibers are use to carry the photons over long distance. Therefore, light from the parametric down-conversion source has to be efficiently coupled into fibers. In the second part we report on a new method to optimize collection efficiency by matching the angular distribution of the parametric fluorescence to the spatial mode of an optical fiber. By using this technique, we detected 366500 polarization-entangled photon pairs per second in the near-infrared region in single-mode optical fibers for 465 mW pump power (at 351.1 nm) with a 2 mm BBOcrystal. The entanglement of the photon pairs was verified by measuring polarization correlations of more than 96% in a HV-basis and in a ±45◦-basis. To our knowledge, such enormous count rates of highly entangled photon pairs have not been reached yet with any other technique. In the third part of this thesis we investigated the process of parametric downconversion in a cavity which is resonant to certain longitudinal down-conversion modes only. The idea of placing the parametric down-conversion source inside a cavity is not new. Such a device is usually referred to as a single or double resonant optical parametric oscillator (OPO) and is mainly used to generate squeezed quantum states. In that kind of application the system is operating close to but still under the threshold of oscillation. In our application the situation is quite different. The system is operating far below threshold so that mainly spontaneous emission occurs. In that mode correlations between single photons can still be observed. But bouncing the light back and forth inside the cavity increases the interaction length and hence enhances the signal levels of the down-conversion fields. Further, by resonating two certain modes only, the bandwidth is reduced by orders of magnitude and the coherence time is found to be inverse proportional to the bandwidth. A similar experiment has already been realized with a type-I parametric down-converter in the resonator. We have tried to realize a compact double resonant OPO far below threshold with a type-II parametric down-converter in a high-finesse cavity to realize a bright source of entangled photon pairs with extremely narrow bandwidth.
Entangled two-photon absorption (ETPA) could form the basis of nonlinear quantum spectroscopy at very low photon fluxes, since, at sufficiently low photon fluxes, ETPA scales linearly with the photon flux. When different pairs start to overlap temporally, accidental coincidences are thought to give rise to a "classical" quadratic scaling that dominates the signal at large photon fluxes and, thus, recovers a supposedly classical regime, where any quantum advantage is thought to be lost. Here, we scrutinize this assumption and demonstrate that quantum-enhanced absorption cross sections can persist even for very large photon numbers. To this end, we use a minimal model for quantum light, which can interpolate continuously between the entangled pair and a high-photon-flux limit, to analytically derive ETPA cross sections and the intensity crossover regime. We investigate the interplay between spectral and spatial degrees of freedom and how linewidth broadening of the sample impacts the experimentally achievable enhancement.