Controllable generation of photon pairs is essential for the utilization of quantum pair states for quantum applications such as quantum communication, quantum cryptography, teleportation, and linear optics quantum computing. Raman scattering is one of the most fundamental light-matter interactions and can be used to generate photon pairs. Using the spontaneous Stokes Raman interaction, a photon from a strong pump laser pulse is annihilated, and a Stokes photon and Raman-mediated collective excitation are created. This excitation can then be read out deterministically as an anti-Stokes photon with the application of a second laser pulse within the excitation lifetime, creating a photon pair. The heralding capability of the Stokes photon and lifetime of the excitation makes this source quasi-deterministic, where the anti-Stokes photon can be created at a later time than the Stokes. This gives additional advantages and uses over traditional photon-pair sources using nonlinear interactions of light in a transparent medium, which generate the pair of photons simultaneously. In this thesis, we study the correlations of photon pairs generated via spontaneous Raman interactions and demonstrate how these interactions can be used for quantum applications. First, we develop a model to study the spectral correlations between the Raman generated Stokes and anti-Stokes photons. This model is used to calculate the spectral single-photon purity of the photons in a generic material system ignoring the effects of material dispersion. We calculate how various parameters effect the purity including pump spectral bandwidth, excitation linewidth, and time delay between pump pulses. We then introduced an experimental realization of a Raman-mediated photon-pair source in an integrated quantum photonic circuit platform. Interstitial N2 molecules inherently trapped in silicon nitride thin films during the deposition process possess a sharp Raman mission corresponding to the vibrational mode of the molecules, which can be used as a Raman-mediated photon-pair source. We present evidence of N2 defects in silicon nitride thin films and estimate the defect density and excitation lifetime. By patterning the films into waveguide structures, the photon-matter interaction is enhanced. We perform finite-element simulation of light propagation in our fabricated waveguides and use the results to examine effects from the waveguide on ultrafast optical pulses and phase-matching requirements for efficient photon-pair generation. We then present experimental progress towards detecting Stokes and anti-Stokes photon-pair generation from N2 defects in silicon nitride waveguides. We show results from degenerate and non-degenerate wavelength optical pump pulses. We discuss limitations of the experimental methods and study in detail the sources of noise arising from the silicon nitride waveguide, and conclude by discussing future extensions on the results presented here.
Controllable generation of photon pairs is essential for the utilization of quantum pair states for quantum applications such as quantum communication, quantum cryptography, teleportation, and linear optics quantum computing. Raman scattering is one of the most fundamental light-matter interactions and can be used to generate photon pairs. Using the spontaneous Stokes Raman interaction, a photon from a strong pump laser pulse is annihilated, and a Stokes photon and Raman-mediated collective excitation are created. This excitation can then be read out deterministically as an anti-Stokes photon with the application of a second laser pulse within the excitation lifetime, creating a photon pair. The heralding capability of the Stokes photon and lifetime of the excitation makes this source quasi-deterministic, where the anti-Stokes photon can be created at a later time than the Stokes. This gives additional advantages and uses over traditional photon-pair sources using nonlinear interactions of light in a transparent medium, which generate the pair of photons simultaneously. In this thesis, we study the correlations of photon pairs generated via spontaneous Raman interactions and demonstrate how these interactions can be used for quantum applications. First, we develop a model to study the spectral correlations between the Raman generated Stokes and anti-Stokes photons. This model is used to calculate the spectral single-photon purity of the photons in a generic material system ignoring the effects of material dispersion. We calculate how various parameters effect the purity including pump spectral bandwidth, excitation linewidth, and time delay between pump pulses. We then introduced an experimental realization of a Raman-mediated photon-pair source in an integrated quantum photonic circuit platform. Interstitial N2 molecules inherently trapped in silicon nitride thin films during the deposition process possess a sharp Raman mission corresponding to the vibrational mode of the molecules, which can be used as a Raman-mediated photon-pair source. We present evidence of N2 defects in silicon nitride thin films and estimate the defect density and excitation lifetime. By patterning the films into waveguide structures, the photon-matter interaction is enhanced. We perform finite-element simulation of light propagation in our fabricated waveguides and use the results to examine effects from the waveguide on ultrafast optical pulses and phase-matching requirements for efficient photon-pair generation. We then present experimental progress towards detecting Stokes and anti-Stokes photon-pair generation from N2 defects in silicon nitride waveguides. We show results from degenerate and non-degenerate wavelength optical pump pulses. We discuss limitations of the experimental methods and study in detail the sources of noise arising from the silicon nitride waveguide, and conclude by discussing future extensions on the results presented here.
With the development of quantum optics, photon correlations acquired a prominent role as a tool to test our understanding of physics, and played a key role in verifying the validity of quantum mechanics. The spatial and temporal correlations in a light field also reveal information about its origin, and allow us to probe the nature of the physical systems interacting with it. Additionally, with the advent of quantum technologies, they have acquired technological relevance, as they are expected to play an important role in quantum communication and quantum information processing. This thesis develops techniques that combine spontaneous Raman scattering with Time Correlated Single Photon Counting, and uses them to study the quantum mechanical nature of high frequency vibrations in crystals and molecules. We demonstrate photon bunching in the Stokes and anti-Stokes fields scattered from two ultrafast laser pulses, and use their cross-correlation to measure the 3.9 ps decay time of the optical phonon in diamond. We then employ this method to measure molecular vibrations in CS2, where we are able to excite the respective vibrational modes of the two isotopic species present in the sample in a coherent superposition, and observe quantum beating between the two signals. Stokes scattering, when combined with a projective measurement, leads to a well defined quantum state. We demonstrate this by measuring the second order correlation function of the anti-Stokes field conditional on detecting one or more photons in the Stokes field, which allows us to observe a phonon modeâ s transition form a thermal state into the first excited Fock state, and measure its decay over the characteristic phonon lifetime. Finally, we use this technique to prepare a highly entangled photon-phonon state, which violates a Bell-type inequality. We measure S = 2.360 ± 0.025, violating the CHSH inequality, compatible with the non-locality of the state. The techniques we developed open the door to the study of a broad range of physical systems, where spectroscopic information is obtained with the preparation of specific quantum states. They also hold potential for future technological use, and promote vibrational Raman scattering to a resource in nonlinear quantum optics -- where it used to be considered as a source of noise instead.
Raman scattering as a candidate for photon-pair generation is explored recently both theoretically and experimentally. Here, we systematically analyze the Stokes–anti-Stokes photon-pair generation in Raman scattering, akin signal–idler photon-pair emission in the spontaneous parametric down conversion, to obtain suitable conditions for photon-pair generation. Non-zero mean phonon number and losses in the phonon mode are observed to be relevant parameters in this context in addition to the Raman active material properties and pump power. Specifically, the Raman active materials with stronger anti-Stokes coupling compared to the Stokes coupling constant are suitable for photon-pair generation. Ideal Stokes–anti-Stokes photon-pair generation is possible even for non-zero thermal phonons provided that the phonon losses are negligible. Here, we characterized the performance of photon-pair generation using noise-reduction parameter in detail. We also discuss the effect of phonon losses on the observed non-classical features.
In recent years, quantum entanglement has attracted much; attention, because its unique properties provide potential; applications, which could not be achieved using conventional; techniques, such as quantum computing, quantum imaging and; lithography. To realize these advancements, one has to obtain an; entanglement-generation source, thoroughly master its physical; properties, and fully understand the light-matter interaction.; This dissertation is an attempt to address such issues as stated; above.; Conventionally, paired photons are created from; \textit{spontaneous parametric down-conversion} (SPDC). It is; known that the transverse correlation in biphotons may improve the; visibility and resolution in quantum imaging and lithography. In; this thesis, we described an alternative biphoton source --; Raman-EIT (\textit{electromagnetically induced transparency}); generator, and emphasize on its geometrical and optical; properties. We found that to utilize the transverse effects in; paired Stokes-anti-Stokes, it is necessary to make the product of; the EIT window times the group delay much greater than unity.; To gain further insight into quantum imaging and lithography, we; studied the transverse correlation in triphoton entanglement; theoretically. We found that in the two-image process, the quality; of images is determined by the optical path-lengths, even though; the Gaussian thin lens equations are satisfied. The ghost; interference-diffraction patterns of double slits show one more; fold interference, which is essentially different from the; biphoton case. Klyshko's advanced-wave model is still applicable,; with some modifications. We also generalized the transverse; correlation to the case of multi-photon entangled states.; To implement quantum computing, one key element is quantum memory.; In this thesis, we have theoretically explored the feasibility of; such a memory by using nonclassical SPDC light in an EIT system at; the single-photon level. We found that both the quantum coherence; of SPDC and atomic coherence of EIT can survive after interacting; within a vapor cell. Due to the inherent mismatch of magnitude; between the spectral bandwidth of SPDC and the very narrow; transmission width of EIT, the coincidence counts of the; two-photon interference is reduced to one pair per second, which; is barely doable in the current experimental situation.
We present a new experiment, in which we measure quantum correlations between single photons that are mediated by the exchange of a single phonon. We create and annihilate a single optical phonon in bulk diamond using two ultrashort laser pulses at two different wavelengths, generated by a Ti:Sapph oscillator and a frequency-doubled optical parametric oscillator (APE Berlin). During Stokes Raman scattering, the first pulse creates a photon-phonon pair, while the second pulse convert the same phonon into an anti-Stokes photon. Using spectral filtering and photon counting, we measure the cross-correlations between the Stokes and anti-Stokes photons with a few hundred femtoseconds time resolution. As expected, the non-classical correlation (g(2) much larger than the classical bound) decays within a few picosecond, following to the dynamics of the phonon mode. Our results demonstrate a new source of broadly tunable quantum correlated photons, and can be extended to provide a new way of measuring non-classical dynamics in nanoscale systems — down to individual nanostructures.
The field of quantum optics offers the intriguing possibility of developing new, potentially ground-breaking technologies based on the laws of quantum physics. Single quanta of light, called photons, are at the heart of many such quantum optical technologies. They can serve, for example, as information carriers in quantum cryptography and in quantum-information processing. If such applications are to fulfill their enormous potential, it is essential to have sources available that provide photons in the required quantum states. An established way of generating states of single photons is based on photon-pair sources. In this approach, the detection of one photon of a pair heralds the presence of the partner photon, which can then be further processed. However, to generate heralded photons in pure quantum states, specific conditions have to be met, making the design and implementation of such sources challenging. This thesis presents two new photon-pair sources that allow the heralded generation of single photons with high purity. Both sources are based on optical fiber, which allows high collection efficiencies for the generated states and opens the possibility of easy integration into modern-day fiber networks. Chapter 1 provides an introduction to quantum optical technologies and gives a short overview of current approaches to generate pure single photons. Chapter 2 presents the basic theory on which the experimental work presented in Chapters 3 and 4 is based. It explains the concept of a spectrally broad single photon and how photon purity can be tested using Hong-Ou-Mandel (HOM) interference. Subsequently, the properties of photon-pair states and the heralded generation of single photons from such states are discussed. It is shown that for a heralded photon to be pure, the original photon pair has to be in a factorable state, that is, free of any correlations. The introduced theory is then applied to spontaneous four-wave mixing (SFWM) in optical fibers, a nonlinear process that allows the generation of photon pairs. It is shown how the factorability of the created pairs depends on the fiber's dispersion properties, and the necessary conditions for the generation of factorable states are derived. The chapter concludes with an analysis of the photon statistics of the four-wave mixing process, explaining how statistics and the g(2) correlation function can be used to evaluate the factorability of the SFWM output state. Chapters 3 and 4 contain the main results of this thesis. Chapter 3 presents the first spectrally decorrelated photon-pair source bridging the visible and telecommunication wavelength ranges. The photon pairs are generated by SFWM in a photonic crystal fiber (PCF). The chapter documents the procedure of how the PCF source was designed and fabricated, as well as its characterization based on spectral measurements and photon statistics. One photon of the pair state is generated in the visible at 513.5 nm, where it can be efficiently detected with silicon-based single-photon detectors. It serves as a herald for its broadband partner photon, which is emitted in the telecom wavelength range at 1547 nm. A spectral coincidence measurement shows that the heralded photon exhibits a purity of up to 0.82. At increased pump powers, even the heralded generation of higher photon-number states in the telecom band becomes feasible. In Chapter 4, we use commercial birefringent fiber to herald high-purity photons of picosecond duration at 848 nm. The presented two-source HOM interference experiment shows that the heralded unfiltered state has a purity of at least 0.73. This value is increased to 0.84 with the application of wavelength filters suppressing low-intensity side peaks in the spectrum. The heralded photons are coupled into a single-mode fiber with an efficiency of 85%, the highest reported value to date for factorable sources. It is also shown that a commercial polarization controller can be used to fine-tune the generated wavelengths. This facilitates matching photons from multiple sources, as required for optical quantum computing schemes. Chapter 5 summarizes all results and provides an outlook toward potential future projects.
There is a growing belief that we are currently in the midst of a Second Quantum Revolution. More and more quantum technologies, such as communication, computing, and imaging, are moving from academic exploration to practical industrial applications. These technologies often depend on entangled photons, and their increasing use requires the development of novel quantum light sources that are compact, versatile, and integrable into modern photonic systems. Additionally, the trend toward miniaturization and nano-optics is accelerating, driven by rapid advances in nanofabrication. Therefore, there is an urgent need to create new classes of miniaturized and tunable two-photon sources. This thesis is dedicated to the theoretical investigation and experimental demonstration of miniaturized sources of entangled photons based on spontaneous parametric down-conversion in thin nonlinear films. It focuses not only on traditional crystalline materials but also on the emerging platform of liquid crystals, marking the first-ever demonstration of photon-pair generation in a liquid crystal within this thesis. A significant achievement is the ability to relax phase-matching constraints in ultra-thin nonlinear layers, allowing the full utilization of the nonlinear tensor and enhancing the variety of possible entangled two-photon states. Several aspects of two-photon state engineering with relaxed phase-matching are discussed in the thesis. First, this relaxation facilitates the switching between different polarization two-photon states, with a varying degree of polarization entanglement and the ability to generate non-maximally entangled states. In terms of spectral properties, miniaturized two-photon sources generate exceptionally broad two-photon frequency spectra, leading to a high degree of frequency entanglement and an unprecedented number of frequency modes, which also leads to ultra-narrow time correlations. By considering the effects of Fabry-Perot resonances, it becomes possible to engineer the two-photon spectra and even achieve backward emission of photon pairs. Remarkably, the Fabry-Perot effect can be accurately described by a simple modification of the rigorous quantum theory, providing a powerful predictive tool for photon pair generation in advanced nanostructures, metasurfaces, and nonlinear nano-antennas when properly applied. Another central contribution of this work is the introduction of liquid crystals as tunable nonlinear media for photon pair generation. Controlling the molecular orientation through a static twist or applying an external electric field makes it possible to tune the generated two-photon states dynamically. A theoretical model of this process, verified through direct experimental measurements, predicts quasi-phase-matching-like behavior and enhanced conversion efficiency, which can be utilized to develop exceptionally tunable and integrable sources of photon pairs and squeezed light. Finally, a fundamental challenge addressed in this thesis is mitigating a parasitic photoluminescent background. This study demonstrates a two-order-of-magnitude reduction in photoluminescence-induced contamination of photon pairs generated from thin nonlinear films by switching from the commonly used continuous-wave regime to the pulsed regime and performing time-resolved distillation. It also shows a developed theory that relates measured experimental parameters to the intrinsic purity of the two-photon state. Overall, this thesis advances the quantum micro- and nano-photonics field by providing a deeper understanding and enhanced control over photon pair generation in thin nonlinear films. It bridges theoretical insights with experimental realizations and paves the way toward practical, tunable, and highly integrated quantum light sources.