Photon statistics is a branch of physics that involves observing the behavior of single or a small number of photons and then aggregating the results through statistical averaging. This process is essential to obtain meaningful and reliable data, especially in quantum optics research. Photon statistics provides valuable information about correlations in the electromagnetic field and characteristics of the type of light being measured. For example, second-order correlation function obtained via Hanbury Brown and Twiss experiment is the fundamental way to differentiate between coherent, chaotic and quantum light. Moreover, extensive investigations into the quantum properties of light resulted in significant progress that allows for precise control of quantum optical systems and sets the stage for genuine quantum engineering. This progress extends to applications in confirming the generation of entangled photons and exploring their properties for various purposes. The non-classical correlation between the entangled photons has resulted in various quantum optical techniques that enable the practical implementation of conceptual experiments that probe the core principles of quantum theory. This enhanced control over quantum phenomena offers exciting opportunities to explore novel information-processing approaches, with the potential to revolutionize technologies rooted in quantum information science. Driven by the significance and pivotal role of photon statistics, our research pursuits were directed toward two specific domains: the characterization of nanolasers and the characterization of time-bin entangled photons. In the first segment, we delve into the realm of metallic coaxial nanolasers, renowned for their intriguing threshold-less lasing behavior. Through comprehensive photon statistics analysis, we seek to unravel the coherence properties inherent in these nanolasers. Our focus also lies on understanding the elusive threshold-less operation, which has remained a subject of debate and intrigue. To evaluate this unique lasing characteristic, we conduct rigorous second-order coherence measurements alongside time-resolved second-order correlation analyses. The second segment of this study ventures into the generation and characterization of high-dimensional time-bin entangled states, a critical resource for quantum technological applications. We simulate a synthetic photonic lattice by employing a coupled fiber-loop system to perform various quantum walk schemes to generate and process high-dimensional time-bin entangled states. Our investigation focuses on the quantum interference phenomena through detailed photon statistics analysis, with an emphasis on their applications across diverse quantum technologies. Through these two interconnected research endeavors, this thesis demonstrates the profound significance of photon statistics as a versatile tool, bridging classical and quantum realms, and paving the way for advancements in diverse applications, ranging from nanolasers to quantum technologies.
Photon statistics is a branch of physics that involves observing the behavior of single or a small number of photons and then aggregating the results through statistical averaging. This process is essential to obtain meaningful and reliable data, especially in quantum optics research. Photon statistics provides valuable information about correlations in the electromagnetic field and characteristics of the type of light being measured. For example, second-order correlation function obtained via Hanbury Brown and Twiss experiment is the fundamental way to differentiate between coherent, chaotic and quantum light. Moreover, extensive investigations into the quantum properties of light resulted in significant progress that allows for precise control of quantum optical systems and sets the stage for genuine quantum engineering. This progress extends to applications in confirming the generation of entangled photons and exploring their properties for various purposes. The non-classical correlation between the entangled photons has resulted in various quantum optical techniques that enable the practical implementation of conceptual experiments that probe the core principles of quantum theory. This enhanced control over quantum phenomena offers exciting opportunities to explore novel information-processing approaches, with the potential to revolutionize technologies rooted in quantum information science. Driven by the significance and pivotal role of photon statistics, our research pursuits were directed toward two specific domains: the characterization of nanolasers and the characterization of time-bin entangled photons. In the first segment, we delve into the realm of metallic coaxial nanolasers, renowned for their intriguing threshold-less lasing behavior. Through comprehensive photon statistics analysis, we seek to unravel the coherence properties inherent in these nanolasers. Our focus also lies on understanding the elusive threshold-less operation, which has remained a subject of debate and intrigue. To evaluate this unique lasing characteristic, we conduct rigorous second-order coherence measurements alongside time-resolved second-order correlation analyses. The second segment of this study ventures into the generation and characterization of high-dimensional time-bin entangled states, a critical resource for quantum technological applications. We simulate a synthetic photonic lattice by employing a coupled fiber-loop system to perform various quantum walk schemes to generate and process high-dimensional time-bin entangled states. Our investigation focuses on the quantum interference phenomena through detailed photon statistics analysis, with an emphasis on their applications across diverse quantum technologies. Through these two interconnected research endeavors, this thesis demonstrates the profound significance of photon statistics as a versatile tool, bridging classical and quantum realms, and paving the way for advancements in diverse applications, ranging from nanolasers to quantum technologies.
Modulating macroscopic parameters of materials in time offers innovative avenues for manipulating electromagnetic waves. Due to such enticing prospects, the general research subject of time-varying systems is expanding today in different branches of electromagnetism and optics. However, compared with the research efforts and progresses that have taken place in the realm of classical electrodynamics, the quantum aspects of this emerging subject have been less explored. Here, through the lens of quantum optics, we study the scattering of electromagnetic fields from an isotropic and nondispersive material with a suddenly changing refractive index, creating a time interface. We revisit the transformation of the bosonic mode operators and corresponding quantum states due to this interface, governed by the two-mode squeeze operator. Building on this foundation, at the core of the investigation, our analysis focuses on the quantum state engineering and photon statistics of the scattered light. Notably, such an analysis reveals and connects various quantum optical phenomena and opportunities arising from the time interface, including photon-pair production and destruction, photon bunching and antibunching, vacuum generation, quantum state discrimination, and quantum state freezing. To bridge theory and experiment, we propose a possible circuit quantum electrodynamics approach for validating our theoretical predictions. We hope that our work inspires experimental investigations of such quantum state engineering and photon statistics phenomena, as well as further quantum optical explorations of electromagnetic field interaction with photonic time crystals or with dispersive time-varying materials.
Non-classical light is both easily encoded with quantum information and robust against decoherence, making it a key resource that enables many quantum information applications including quantum computing, quantum communication, and quantum metrology. We present a wide range of experimental and theoretical research toward the generation, detection, characterization, and storage of non-classical states of light with an eye toward quantum information applications. To provide a basis for the rest of the work, we begin by discussing theoretically the role of photon number statistics in optical quantum information and the use of second-order optical coherence to characterize non-classical light. Building on that, we present an original tool for the difficult problem of reconstructing the underlying mode distribution of multi-mode optical fields using simple measurements of higher-order optical coherence. We then move on to the problem of generating and storing single photons. We do this in a solid-state medium, a rare-earth ion-doped crystal, with a long-lived spin transition ideal for storing quantum information. We experimentally demonstrate the feasibility of this concept by showing correlations between the optical fields that herald storage and retrieval of collective excitations. This scheme can be used for the two important and distinct applications of generating single photons on-demand and storing quantum information and entanglement. The detection of non-classical light is a task as important as its generation. To this end, we study detectors with near unity detection efficiency and photon number resolution for use in quantum-enabled metrology. We use such a detector to experimentally demonstrate compression of spatial fringes and investigate the possibility of improving measurement resolution with classical and non-classical light. Finally, we report a set of experiments using photon number statistics to characterize classical and non-classical light. We measure suppression of unwanted multi-photon emission in a heralded single photon source based on four-wave mixing in microstructure optical fiber. And we, for the first time, experimentally demonstrate reconstruction of multi-mode classical and non-classical light from measured photon number statistics.
High-order photon correlations of light fields are important for characterizing the quantum nature. Since Hanbury Brown and Twiss conducted the pioneering experiments in the 1950s, the HBT effect has inspired extensive research on high-order photon correlation in quantum optics, quantum information, and quantum imaging. The Single-photon counting module is one of the most widely used single-photon detectors. Due to its high detection efficiency and low dark counts in the visible and near-infrared region, it is reasonably chosen for basic research on quantum mechanics. Many researches have demonstrated that the maximum value of second-order photon correlation g(2)(τ) at zero delay (τ = 0) can be used to distinguish different light fields. Therefore, the HBT scheme containing two single photon detectors have been widely used in many advanced studies, such as space interference, ghost imaging, single photon detection with high efficiency, etc. However, higher-order photon correlations g(n) (n > 2) can reveal more measurable characteristics of light fields, such as information about the non-Gaussian scattering process, the skewness and kurtosis of photon number distribution, etc. When the extended HBT scheme is used to measure higher-order photon correlations, the experimental conditions including quantum efficiency and background noise greatly affect the photon correlation measurement. The influences of the counting rate and resolution time of the detection system on the measurements are also very important and cannot be ignored. Therefore, the comprehensive considering of various influence factors is necessary for accurately measuring the high-order photon correlations and also a challenge. In this paper, we present a method based on double Hanbury Brown-Twiss scheme for the accurate measuring of high-order photon correlations g(n) (n > 2). The system consists of four single photon counting modules and is used to detect and analyze the joint distribution probability of temporal photon correlation. Considering the effects of the background noise and overall efficiency, theoretically, we analyze the correlations of the third- and fourth-order photon with the incident light intensity, squeezing parameter and photon number respectively for thermal state, coherent state, squeezed vacuum state, and Fock state. Meanwhile, experimentally we study the influences of resolution time and counting rate on correlations of the coherent state and thermal state with third- and fourth-order photon. On condition that the resolution time is 210 ns and the counting rate is 80 kc/s, the correlations of third and fourth-order photon with the thermal state at zero time delay are accurately measured, and the relative statistical deviations of the measured vales from the theoretical values are 0.3% and 0.8%, respectively. In addition, the third- and fourth-order photon correlations of the thermal state at different delay times are also observed. It is demonstrated that the high-order photon correlations of light fields are measured accurately by comprehensively analyzing various influencing factors. This technique provides a promising and useful tool to investigate quantum correlated imaging and quantum coherence of light fields.
Conspectus The enhanced interest in quantum-related phenomena has provided new opportunities for chemists to push the limits of detection and analysis of chemical processes. As some have called this the second quantum revolution, a time has come to apply the rules learned from previous research in quantum phenomena toward new methods and technologies important to chemists. While there has been great interest recently in quantum information science (QIS), the quest to understand how nonclassical states of light interact with matter has been ongoing for more than two decades. Our entry into this field started around this time with the use of materials to produce nonclassical states of light. Here, the process of multiphoton absorption led to photon-number squeezed states of light, where the photon statistics are sub-Poissonian. In addition to the great interest in generating squeezed states of light, there was also interest in the formation of entangled states of light. While much of the effort is still in foundational physics, there are numerous new avenues as to how quantum entanglement can be applied to spectroscopy, imaging, and sensing. These opportunities could have a large impact on the chemical community for a broad spectrum of applications. In this Account, we discuss the use of entangled (or quantum) light for spectroscopy as well as applications in microscopy and interferometry. The potential benefits of the use of quantum light are discussed in detail. From the first experiments in porphyrin dendrimer systems by Dr. Dong-Ik Lee in our group to the measurements of the entangled two photon absorption cross sections of biological systems such as flavoproteins, the usefulness of entangled light for spectroscopy has been illustrated. These early measurements led the way to more advanced measurements of the unique characteristics of both entangled light and the entangled photon absorption cross-section, which provides new control knobs for manipulating excited states in molecules. The first reports of fluorescence-induced entangled processes were in organic chromophores where the entangled photon cross-section was measured. These results would later have widespread impact in applications such as entangled two-photon microscopy. From our design, construction and implementation of a quantum entangled photon excited microscope, important imaging capabilities were achieved at an unprecedented low excitation intensity of 10 7 photons/s, which is 6 orders of magnitude lower than the excitation level for the classical two-photon image. New reports have also illustrated an advantage of nonclassical light in Raman imaging as well. From a standpoint of more precise measurements, the use of entangled photons in quantum interferometry may offer new opportunities for chemistry research. Experiments that combine molecular spectroscopy and quantum interferometry, by utilizing the correlations of entangled photons in a Hong–Ou–Mandel (HOM) interferometer, have been carried out. The initial experiment showed that the HOM signal is sensitive to the presence of a resonant organic sample placed in one arm of the interferometer. In addition, parameters such as the dephasing time have been obtained with the opportunity for even more advanced phenomenology in the future.
Characterization of photon statistics of a light source is one of the most basic tools in quantum optics. Existing methods rely on an implicit and unverifiable assumption that the source never emits too many photons to stay within the measuring range of the detectors. As a result, they fail to fulfill the demand arising from emerging applications of quantum information such as quantum cryptography. Here, we propose a characterization method using a conventional Hanbury-Brown-Twiss setup to produce rigorous bounds on emission probabilities of low photon numbers from an unknown source. As an application, we show that our characterization method can be used for a practical light source in a quantum key distribution protocol to forsake the commonly used a priori assumption without significant change in efficiency. Our versatile and flexible formula for rigorous bounds will make an essential contribution to the optics toolbox in the era of quantum information.
The researches on higher-order coherence and quantum statistics of light field are the important researching issues in quantum optics. In 1956, Hanbury-Brown and Twiss (HBT) (Hanbury-Brown R, Twiss R Q 1956 Nature 177 27) revolutionized optical coherence and demonstrated a new form of photon correlation. The landmark experiment has far-reaching influenced and even inspired the quantum theory of optical coherence that Glauber developed to account for the conclusive observation by HBT. Ever since then, the HBT effect has motivated extensive studies of higher-order coherence and quantum statistics in quantum optics, as well as in quantum information science and cryptography. Based on the HBT scheme, the degree of coherence and photon number distribution of light field can be derived from correlation measurement and photon counting technique. With the rapid development of the photoelectric detection technology, single-photon detection, which is the most sensitive and very widespread method of optical measurement, is used to characterize the natures of light sources and indicate their differences. More recently, HBT scheme combined with single-photon detection was used to study spatial interference, ghost imaging, azimuthal interference effect, deterministic manipulation and detection of single-photon source, etc. Due to broadband RF spectrum, noiselike feature, hypersensitivity to the initial conditions and long-term unpredictability, chaotic laser meets the essential requirements for information security and cryptography, and has been developed in many applications such as chaos-based secure communications and physical random number generation, as well as public-channel secure key distribution. But the research mainly focused on macroscopic dynamics of the chaotic laser. Moreover, the precision of measurement has reached a quantum level at present. Quantum statistcs of light field can also uncover profoundly the physical nature of the light. Thus, it is important to exploit the higher-order degree of coherence and photon statistics of chaotic field, which contribute to characterizing the field and distinguishing it from others. In this paper, photon number distribution and second-order degree of coherence of a chaotic laser are analyzed and measured based on HBT scheme. The chaotic laser is composed of a distributed feedback laser diode with optical feedback in fiber external cavity configuration. The bandwidth of the chaotic laser that we obtain experimentally is 6.7 GHz. The photon number distribution of chaotic laser is fitted by Gaussian random distribution, Possionian distribution and Bose-Einstein distribution. With the increase of the mean photon number, the photon number distribution changes from Bose-Einstein distribution into Poissonian distribution and always accords with Gaussian random distribution well. The second-order coherence g(2)(0) drops gradually from 2 to 1. By changing the bias current (I = 1.0Ith-2.0Ith) and feedback strength (010%), we compare and illustrate different chaotic dynamics and g(2)(0). From low frequency fluctuation to coherence collapse, the chaotic laser shows bunching effect and fully chaotic field can be obtained at the broadest bandwidth. Furthermore, the physical explanation for sub-chaotic or weakening of bunching effect is provided. It is concluded that this method can well reveal photon statistics of chaotic laser and will open up an avenue to the research of chaos with quantum optics, which merges two important fields of modern physics and is extremely helpful for the high-speed remote chaotic communication.