In recent years, the process of absorbing two photons using a non-classical light sources has been studied thoroughly. In particular, it has been experimentally demonstrated that the absorption cross section of two entangled photons is much greater than the absorption cross section of two uncorrelated photons. In this dissertation a source of entangled photons produced through spontaneous parametric down conversion or SPDC was constructed and characterized. It was found that for a pump laser of 411.32 nm and a BBO crystal of 1 mm the produced photons followed the same optical path as the laser, it was also found that the joint spectrum is symmetric at the degenerate wavelength of 822 ± 0.5 nm. This work conclude by showing a first approximation to execute a measurement of the Hong-Ou-Mandel effect. The objective of the measurements of joint spectrum and the Hong-Ou-Mandel effect are to understand the correlation properties of the photon source, with this information a virtual state spectroscopy technique can be implemented on the experiment constructed
In recent years, the process of absorbing two photons using a non-classical light sources has been studied thoroughly. In particular, it has been experimentally demonstrated that the absorption cross section of two entangled photons is much greater than the absorption cross section of two uncorrelated photons. In this dissertation a source of entangled photons produced through spontaneous parametric down conversion or SPDC was constructed and characterized. It was found that for a pump laser of 411.32 nm and a BBO crystal of 1 mm the produced photons followed the same optical path as the laser, it was also found that the joint spectrum is symmetric at the degenerate wavelength of 822 ± 0.5 nm. This work conclude by showing a first approximation to execute a measurement of the Hong-Ou-Mandel effect. The objective of the measurements of joint spectrum and the Hong-Ou-Mandel effect are to understand the correlation properties of the photon source, with this information a virtual state spectroscopy technique can be implemented on the experiment constructed
The ability to determine the joint spectral properties of photon pairs produced by the processes of spontaneous parametric downconversion (SPDC) and spontaneous four-wave mixing (SFWM) is crucial for guaranteeing the usability of heralded single photons and polarization-entangled pairs for multi-photon protocols. In this paper, we compare six different techniques that yield either a characterization of the joint spectral intensity or of the closely related purity of heralded single photons. These six techniques include: (i) scanning monochromator measurements, (ii) a variant of Fourier transform spectroscopy designed to extract the desired information exploiting a resource-optimized technique, (iii) dispersive fibre spectroscopy, (iv) stimulated-emission-based measurement, (v) measurement of the second-order correlation function g(2) for one of the two photons, and (vi) two-source Hong–Ou–Mandel interferometry. We discuss the relative performance of these techniques for the specific cases of a SPDC source designed to be factorable and SFWM sources of varying purity, and compare the techniques’ relative advantages and disadvantages.
Recently, different experimental methods to investigate the entangled two-photon absorption (ETPA) process in a variety of materials have been reported. The present work reports on a different approach on which the ETPA process is detected based on the changes induced on the Hong-Ou-Mandel (HOM) interferogram of two photons produced by a spontaneous parametric down conversion (SPDC) Type-II process. Using an organic solution of the laser dye Rhodamine B as a model, it is demonstrated that ETPA at 800nm can be monitored by the changes in the temporal-width and visibility of the HOM interferogram produced by the photons at a beam splitter after interacting with the sample. Additionally, we present a detail model in which the sample is modeled as a filtering function which fullfills the energy conservation conditions required by ETPA, allowing to explain the experimental observations with excellent agreement. We believe that this work represents a new perspective to study the ETPA process, by using an ultra-sensitive quantum interference technique and a detailed mathematical model of the process.
In recent years, the use of entangled photons in quantum spectroscopy has gained attention, offering new possibilities for studying materials. In this work, we present an entangled photon source developed for future applications in ultrafast quantum spec- troscopy, particularly in biological research. Entangled photons at visible wavelengths are generated using pulsed type-I spontaneous parametric down-conversion (SPDC) in a Beta-Barium Borate (BBO) crystal, pumped by a 1030 nm laser after third and fourth harmonic generation. Photon detection was performed with an intensified sCMOS cam- era, enabling observation and study of spatial and, after integration of a custom-built spectrograph, spatio-energetic correlations between photon pairs. We optimized detec- tion, imaging, and data processing methods. We believe that our results, combined with the improvements we propose, form a solid foundation for integrating entangled photon pairs into time-resolved optical spectroscopy.
By controlling quantum interactions of molecules and light, new technology in quantum information science promises to outperform classical-based technology in both function and efficiency. In particular, chemists stand to gain much advantage from quantum sensing techniques, allowing them to measure new spectroscopic signals that classical techniques cannot do, control photochemical reactions in new ways, and even measure nonlinear interactions with a simple push of a button. Much of the current work in using entangled photons for spectroscopy has focused on the unique physics of the photons. There is still much to be learned about how the molecule’s structure influences quantum spectroscopic signals and leaves its signature. In this dissertation, the unique ways that organic chromophores interact with entangled photons from spontaneous parametric down-conversion (SPDC) has been analyzed in detail. In Chapter 3, I calculate entangled two-photon absorption (ETPA) cross-sections for a few diatomic molecules to show how the varying dipole properties of the molecules affect the ETPA cross-section oscillation vs the entanglement time, Te. In Chapter 4, new theory shows that the excited state linewidth from ETPA excitation is extremely narrow compared to classical TPA excitation. I show that the reason for the ETPA linewidth being so narrow is due to the large arrival time uncertainty of the entangled photon pair, which makes the first photons’ absorption time in the molecule largely uncertain and effectively narrows the excited state linewidth. In Chapter 5, I used Type-II SPDC to prove, for the first time, that two halogenated anesthetic ethers, sevoflurane and isoflurane, have the ability to target and interact with quantum particles by showing that they interact with 800 nm entangled photons but not 800 nm classical photons. In Chapter 6, I build an ETPA experimental setup that uses CW laser pumping of Type-I SPDC, which is shown to significantly improve the accuracy, signal-to-noise ratio (SNR), and limit of detection of ETPA while also making the experiment more compact and cost-effective. I also show how to quantify the degree of frequency entanglement using the Schmidt decomposition of the joint frequency spectrum and propose how the Schmidt modes can be tuned to control photochemical reactions. Contrary to prior belief in the literature, I show experimentally in Chapter 7 that ETPA with Type-I SPDC increases linearly with increasing Te, allowing one to increase the ETPA cross-section by an order of magnitude by increasing Te from a few fs to ~10 ps. This enhancement is due to the entanglement area, Ae, decreasing as the frequency bandwidth decreases, which is how Te is increased. This spatial-spectral coupling has previously been overlooked in the context of ETPA, causing previous theoretical models to underestimate the ETPA cross-section at ps Te by 3-4 orders of magnitude. Using ps Te Type-I SPDC, ps-scale excited state dynamics can be studied using ETPA, and photochemical reactions with intermediate steps, such as isomerizations or solvent reorganization, can be controlled. The experimental techniques and theoretical work here has provided a much needed improvement to make ETPA a more quantitatively robust analytical technique that is useful and accessible to the researchers who can benefit most from its applications: chemists, biologists, and anyone who studies the quantum principles underlying all aspects of chemistry.
Nowadays, single-photon sources can be generated experimentally through a wide variety of platforms [1]. Semiconductor quantum dots [2] have demonstrated impressive performance in terms of photon purity and indistinguishability, particularly in Hong-Ou-Mandel experiments. Another widely used method involves nonlinear crystals, which can generate entangled photon pairs via nonlinear processes such as spontaneous parametric down-conversion (SPDC) or spontaneous four-wave mixing (SFWM). These are heralded single-photon sources, rather than deterministic ones, yet they remain essential tools in quantum optics [3]. Moreover, among the most commonly used single photon sources, there are NV centres in diamonds [4]. These single-photon sources emit quantum states of light, i.e., those that have no classical counterpart.