Entangled photons could translate complex, ultrafast laser-based spectroscopy and imaging to a chip-sized or distributable platform. The inherent temporal and energy correlations between the two entangled photons created in spontaneous parametric down conversion (SPDC) allow a continuous-wave laser diode source to replicate ultrafast, two-pulse experiments that are usually performed in table-top scale setups. Although entangled photons were originally proposed to enhance multiphoton or nonlinear processes, few entangled experiments to date have outperformed classical photon sources from a full systems perspective. The low pump power criteria and periodically poled nonlinear sources, however, do make entangled photon experiments natural candidates for on-chip photonic circuits and spectroscopy. In our talk, we will discuss experiments that prove that the miniaturization of ultrafast experiments is a key area where entangled photons can compete with or prove superior to classical photon experiments. We will first discuss our progress in creating entangled photon sources in the visible to deep ultraviolet (UV) wavelengths as needed for spectroscopy and imaging, the integration of the subsequent photonic circuitry needed to create on-chip spectrometers, and then experimental results proving that on-chip entangled photon sources can replicate ultrafast pump-probe or be used for fluorescence lifetime imaging microscopy (FLIM) experiments. We will also discuss our increasingly null experiments on topics like entangled two-photon absorption (ETPA) which are equally important for the progressing the field.
Entangled photons could translate complex, ultrafast laser-based spectroscopy and imaging to a chip-sized or distributable platform. The inherent temporal and energy correlations between the two entangled photons created in spontaneous parametric down conversion (SPDC) allow a continuous-wave laser diode source to replicate ultrafast, two-pulse experiments that are usually performed in table-top scale setups. Although entangled photons were originally proposed to enhance multiphoton or nonlinear processes, few entangled experiments to date have outperformed classical photon sources from a full systems perspective. The low pump power criteria and periodically poled nonlinear sources, however, do make entangled photon experiments natural candidates for on-chip photonic circuits and spectroscopy. In our talk, we will discuss experiments that prove that the miniaturization of ultrafast experiments is a key area where entangled photons can compete with or prove superior to classical photon experiments. We will first discuss our progress in creating entangled photon sources in the visible to deep ultraviolet (UV) wavelengths as needed for spectroscopy and imaging, the integration of the subsequent photonic circuitry needed to create on-chip spectrometers, and then experimental results proving that on-chip entangled photon sources can replicate ultrafast pump-probe or be used for fluorescence lifetime imaging microscopy (FLIM) experiments. We will also discuss our increasingly null experiments on topics like entangled two-photon absorption (ETPA) which are equally important for the progressing the field.
The harnessing of the nonclassical properties in photon pairs generated by the process of Spontaneous Parametric Down Conversion (SPDC) to enhance two-photon interactions has long intrigued researchers. Their use in light-matter interactions has been proven to improve efficiency either by increasing the rate of generation or by suppressing noise. Namely, the processes of Entangled Sum Frequency Generation (eSFG) and Entangled Two Photon Absorption (eTPA) have been shown to produce more photons when stimulated with entangled photons than the classical versions of the effects. This has only been effective so far at very low intensities, which, alongside the inability to reproduce previous experimental results, has caused debates about the usefulness of the effect. In the presented work, I aim to shed light on the topic by employing a carefully crafted source of entangled photon pairs to improve two-photon effects. I attempt to demonstrate, through a series of experiments, that the quantum enhancement can be observed at an order of magnitude higher than previously thought possible. To solidify the results, a direct comparison of the quantum effect was conducted by investigating the performance of the phenomenon when it is stimulated by classical radiation from a laser. Our results confirm a quantum improvement in a regime previously considered impossible, and they enabled us to examine the ramifications of the effect on imaging. By doing so, we consider real-life microscopy applications, and therefore, we can set limits to the effect.
This thesis deals with the production of entangled photons using spontaneous parametric down-conversion (SPDC). We start with a short overview of some important theoretical concepts. First we provide a brief reminder of the theory of entanglement. We then discuss how the state of quantum systems can be determined using quantum state tomography. We also explain SPDC, the physical process which we use to produce entangled photons. Finally, we give an overview of the methods which have been used to produce entangled photons in the past, both for two- and three-photon entanglement. \n \nThe first experiment is the design of an efficient source of entangled photon pairs based on a polarizing Sagnac interferometer configuration. With this configuration, we can use quasi-phasematched materials which allow for higher efficiencies than standard bulk nonlinear materials. The source is pumped by a low-power continuous-wave laser diode, and produces degenerate photon pairs at 809nm. It has a spectral brightness of 87,500 pairs/(s mW nm), and the fidelity of the produced quantum states with a Bell state is 98.9%. The source is used for experiments in quantum key distribution, cluster state quantum computing, remote state preparation, state discrimination, and entanglement-enhanced classical communication. \n \nThe second experiment discussed in this thesis is the generation of photon triplets using cascaded SPDC. In this experiment, a primary SPDC source is pumped with a low-power, continuous-wave laser diode, producing photon pairs. Single photons from these pairs serve as the pump for a second down-conversion, resulting in photon triplets. This is the first demonstration of the direct production of photon triplets, and the first observation of SPDC at the single photon level. This method could potentially be used to produce entangled photon triplets without post-selection, and as a source of triggered Bell pairs.
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.
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.
Quantum states of photons such as entangled and single photons are indispensable components for applications in optical quantum information processing. Being able to generate and manipulate quantum states of photons on a chip is a crucial step towards realizing real-world quantum information processing systems such as an optical quantum computer. In this thesis, theoretical and experimental research was carried out for on-chip generation of quantum states of photons via the nonlinear process of spontaneous parametric down-conversion (SPDC), including polarization entangled photons, hyperentangled photons and heralded pure single photons. A majority of the study was based on III-V semiconductor AlGaAs, which could lead to monolithic integration of pump lasers and enable electrically pump sources operating at room temperature. The generation of cross-polarized entangled photons via a type-II SPDC in an AlGaAs Bragg reflection waveguide (BRW) was first investigated. The lack of material birefringence enables the direct generation of wavelength-multiplexed polarization entangled photons with a concurrence of at least 0.77 in a bandwidth of 95 nm. Second, a technique using concurrent type-0 and type-I processes on an AlGaAs chip to generate polarization entangled photon was developed. This technique allows the generation of both co-polarized and cross-polarized entangled photons on the same chip without the need of off-chip compensation, interferometer and bandpass filter. Third, a technique of generating hyperentangled photons on an AlGaAs chip was developed by utilizing spatial modes of different guiding mechanisms. High quality entanglement could be achieved with bandpass filtering of a few nanometers without off-chip phase compensation. Four, a generic technique using nonlinear photonic nanowires to engineer two-photon quantum states was proposed. Via dispersion engineering which controls the group velocity of each mode, maximally entangled polarization entangled photons and pure heralded single photons can be generated on-chip. Design examples were applied to III-V semiconductor and ferroelectric materials. Last, a strategy to enhance the bandwidths of wavelength conversion and SPDC spectrum was developed by tapering the waveguides. Combined with further integration of pump lasers, photonic circuits and detectors, the techniques developed in this thesis provides a viable route to achieve fully integrated generation and manipulations of photonic quantum qubits.
Fluorescence microscopy has become integral to biological studies for the technique’s ability to elucidate structures of biomolecules for in-situ studies with high selectivity and specificity. Imaging of intrinsic indicators, such as fluorescent amino acids in proteins, provides important information, but can be challenging to accomplish. Current microscopy techniques that measure native fluorescence without the use of exogenous labels involve either direct UV excitation which is commonly non-localized and can be detrimental to the system, or multiphoton absorption which must be conducted at high intensities, therefore posing high risks of photodamage. As such, we seek to investigate an efficient way to gently excite native fluorescence in biological systems in a way that overcomes these limitations. Quantum entangled photon pairs generated via spontaneous parametric downconversion (SPDC), may be an alternative to conducting two-photon absorption (TPA) to excite fluorescence in amino acids without the high fluences currently used. These photon pairs are highly correlated in time. Thus, the arrival of one photon is simultaneously followed by the arrival of its sister photon. As a result, a molecule interacting with the photon pair should simultaneously absorb both photons, leading to a linear two-photon absorption rate, and the linearity of the two-photon process should dramatically reduce the light intensity necessary for TPA. Therefore, quantum entangled photon pairs offer the possibility of performing low intensity UV excitation using photons in the visible wavelength range. With this work, we generated and characterized entangled photons generated via SPDC, and investigated whether fluorescent amino acids can be excited, and the subsequent fluorescence induced with entangled two-photon absorption. Results show that much higher entangled two-photon rates than what are currently available are needed to measure significant signals with entangled two-photon excitation.