Light represents one of the most fundamental and also natural ways of information transfer available in both physics and our everyday life.As a result, quantum optics possesses large overlaps with many fields like nonlinear optics, quantum information theory, spectroscopy and the fundamentals of quantum mechanics.Conventionally, the photon statistics of light are studied using techniques like homodyne detection or coincidence measurements.Recently, a quantum extension of classical electro-optic sampling was developed, which enables the measurement of electric field statistics on ultrashort time scales.This measurement relies on a nonlinear interaction between As I am finishing this thesis, I suddenly realize that my time as a PhD student is slowly coming to an end.
Light represents one of the most fundamental and also natural ways of information transfer available in both physics and our everyday life.As a result, quantum optics possesses large overlaps with many fields like nonlinear optics, quantum information theory, spectroscopy and the fundamentals of quantum mechanics.Conventionally, the photon statistics of light are studied using techniques like homodyne detection or coincidence measurements.Recently, a quantum extension of classical electro-optic sampling was developed, which enables the measurement of electric field statistics on ultrashort time scales.This measurement relies on a nonlinear interaction between As I am finishing this thesis, I suddenly realize that my time as a PhD student is slowly coming to an end.
The fascinating nature of light has driven many discoveries in physics, from the theory of special relativity to quantum mechanics. As a carrier of information, light is at the core of high-speed communication over the internet and facilitates the study of numerous physical properties of materials by the interaction of light and matter. Advances in generating and detecting ultrashort light pulses enabled the spectroscopic investigation of matter with unprecedented detail. Meanwhile, the development of more precise and sensitive measurements, leveraging quantum properties of light, has expanded the experimental frontiers of the physical world. Naturally, the question arises: Could the combination of these two breakthroughs push the frontiers even further? A promising candidate to achieve this combination is electro-optic sampling, an electromagnetic-field measurement comprising an up-conversion and a phase-space measurement based on homodyne detection. While it is predominantly used in classical terahertz time-domain spectroscopy, the high sensitivity and spatio-temporal resolution of electro-optic sampling recently enabled the detection of vacuum fluctuations in the ground state of the electromagnetic field by probing an adjustable space-time volume. Yet, the generation and characterization of more intricate quantum pulses on ultrafast timescales is still challenging, especially in the terahertz frequencies. Exploiting the quantum properties of a light pulse over a broad frequency range requires sophisticated knowledge about the prepared quantum pulse as well as the measurement setup at use. However, Heisenberg's uncertainty relation fundamentally prevents the complete determination of an arbitrary quantum state from a single measurement. Instead, the quantum state has to be reconstructed from the statistics of many measurements — a process known as quantum state tomography. In this thesis, we establish the theoretical foundations for a comprehensive tomographic reconstruction of pulsed quantum states of light, encompassing both the statistics and dynamics of the state. Additionally, we introduce tools to simplify the description of the nonlinear interaction underlying electro-optic sampling and in turn the tomography setups presented here. As a first step, we investigate the application of electro-optic sampling to the time-local reconstruction of various pulsed quantum states of light on ultrafast timescales. We identify two types of noise, which impact the quality of the reconstruction: shot noise, arising from the nonlinear interaction in electro-optic sampling, and thermal noise, due to the localization of the (correlated) quantum state within a small space-time volume during the measurement. To improve the reconstruction, we propose to use a strong probe pulse, suppressing the shot noise, and to select an appropriate detection frequency band, reducing thermal noise. Thus, the proposed tomography enables the characterization of quantum states in terahertz frequency range on ultrafast timescales. However, the time-local nature of the measurement imposes a trade-off between the reconstruction of the quantum state in phase space and the time domain. In a second step, we propose a reconstruction method based on two-time field-correlation measurement, which we call correlation tomography, able to overcome the restriction to time-local states. While the tomography of quantum states in an optimal pulse basis has been demonstrated, it requires prior knowledge about the temporal structure of the quantum state. We introduce an algorithm for reconstructing high-dimensional multimode Gaussian quantum states, which are completely characterized by the covariance matrix of the quadratures of fully distinguishable pulses. The reconstruction is achieved by orthogonalizing the overlapping time windows of the correlation measurement in post-processing. We compare a homodyne-based implementation to electro-optic sampling and develop an optimization scheme for the latter, to mitigate the shot noise in the non-perturbative regime of strong nonlinear interactions. Furthermore, we derive the full-counting statistics of the field-correlation measurement and theoretically demonstrate the reconstruction of pulsed Fock states. This opens an avenue to the full tomography of highly multimode non-Gaussian states. In the third and last step, we derive a formalism to simplify the description of the up-conversion required in electro-optic sampling. If a pulsed quantum states is up-converted and localized in a small space-time region, the transformation of the localized modes during the nonlinear interaction corresponds to an open quantum system, rendering the standard tools of quantum optics inapplicable. By introducing the generalized Bloch-Messiah decomposition, we simplify the input-output relation of the nonlinear interaction to a set of effective modes relevant for subsequent processing, such as detection. Using this framework, we derive an analytic phase-space input-output relation for the nonlinear interaction of pulsed quantum states, applicable to open quantum systems. We study the resulting dynamics using two example input states: a Fock state and a two-mode squeezed state. Based on the von Neumann entropy of the output state, we develop an intuitive understanding of the generalized Bloch-Messiah decomposition. The rich structure of pulsed quantum states of light can be a powerful resource, but also challenging to operate with, in theory as well as in experiment. The characterization methods and theoretical tools developed in this thesis, tailored to pulsed quantum light and the nonlinear interaction thereof, can pave the way to the application of this resource to fundamental research as well as quantum technologies.
Studies on the nature of light have often played pivotal roles in the development of physics. The particle nature of light served as benchmark for the foundation of quantum physics and its derived branches, while its referential-independent speed in the vacuum, as seen through wave equations, led to the merge of space and time and culminated in the foundation of general relativity and cosmology. In spite of that, many light-based measurement techniques still rely heavily on a classical description of light, as has been for many years the case for electrooptic sampling. Luckily, this scenario has been changed in the course of the last few years, with both experimental and theoretical works highlighting the advantages and hidden properties that a quantum and/or relativistic description of light can unveil. Speci fically, the electrooptic sampling of a broadband section of the electric- field vacuum opened an entirely new window of possibilities, and the works presented here aim at filling a small portion of the gap opened by this simple, yet remarkable, technological leap. As a starting point, I study the spectral properties of quantum radiation of ultrashort duration. In particular, I introduce a continuous multimode squeezing operator for the description of subcycle pulses of entangled photons generated by a coherent-pulse driving in a thin nonlinear crystal with second-order susceptibility. The spectra of these ultrabroadband squeezed states can be found perturbatively in the strength of the driving electric-fi eld pulse. These can be related, for suitable choices of the driving pulses, to the spectra that one should hypothetically observe in an Unruh-Davies experiment, in which an observer (more precisely a particle detector) moving with constant proper acceleration in the Minkowski vacuum during a finite (life)time detects a thermal distribution of (virtual) particles. On the other hand, when describing the corresponding behavior of the normally ordered electric- field variance in the time domain, a connection to experiments in which such states have been generated and detected can be traced. This variance builds up as the electric fi eld (or correspondingly its state) evolves via propagation through the nonlinear crystal, and it can be shown that the world lines followed by the fi eld modes when propagating are indeed curved, as is usually the case for the Unruh-DeWitt detectors used to study the Unruh-Davies effect. Alongside the study of the states generated in a nonlinear crystal, I also investigate what influence these states have on the electrooptic measurements that rely on the same effective nonlinear interaction. When electrooptically sampling the electric- field vacuum, the evolution of the electric fi eld leads to a change in the initially sampled vacuum state. This change piles up backaction contributions that remain in superposition with the vacuum state after the measurement. When the superposition coefficients of the back-action contributions are small, the electrooptic-signal variance is dominated by the shot noise, with a small vacuum-related contribution on top. As the sampling regime shifts towards stronger probe-pulse intensities, the state superposition undergoes a change, which can be traced back to the signal variance and the clear change in its behavior, with a steep departure from the shot noise. This approach is then further extended to model another setup in which two probes, time-shifted relative to each other, are impinged on the nonlinear crystal to probe the vacuum. This approach allows for the evasion of shot noise and produces a way richer variety of back-action contributions that are then investigated.
For decades, ultrafast light-matter interactions have provided a powerful means to observe electrons in motion across a wide range of physical systems. This dissertation builds new theoretical frameworks to make sense of the emergent phenomena that arise when light drives matter into the strong-field regime, spanning atomic, molecular, and condensed-matter systems. The resulting dynamics leave their fingerprints on a variety of observables, such as photoionization spectra, high-harmonic generation, and nonlinear spectroscopic signals, each of which provides a different window onto the underlying electronic motion. The work is organized into two parts.The first part focuses on the electric-field observables of nonlinear optical signals. Because both the amplitude and phase of the emitted field are experimentally accessible through techniques such as spectral interferometry and electro-optic sampling, the full field itself serves as a rich observable for characterizing nonlinear responses in atomic, molecular, and condensed-matter systems. Leveraging this, the simulations presented here uncover novel and largely unexplored physical phenomena encoded in these field observables. The second part turns to optical spectroscopy with quantum light. Although nonlinear optical processes are conventionally modeled within a semiclassical framework, treating the matter quantum mechanically while the driving ultrafast fields remain classical, the resulting signals can nonetheless exhibit intrinsically non-classical properties. Building on this insight, a framework for interpreting experimental data is introduced and used to show that four-wave mixing driven by ultrafast femtosecond laser pulses generates bright squeezed light. Beyond squeezed light, strong field-matter interactions can also produce attosecond entangled photons, a distinct form of quantum light. Several strategies are proposed to enhance the efficiency of their generation, with the developed theory predicting rates of energy-time entangled biphoton production orders of magnitude beyond those achievable with conventional spontaneous parametric down-conversion (SPDC) sources. The studies presented here are initial steps toward investigating quantum properties of these systems through quantum phynonlinear spectroscopy, which is not achievable with classical light.
The quantization of light is the basis for quantum optics and has led to the observation of a multitude of genuine quantum effects which cannot be explained by classical physics. Yet, there exist different views when we refer to the distinct quantum character of light as opposed to classical fields. A major impact on how we describe photonic states is caused by the detection method we use for the quantum state characterization. In the theoretical modelling measuring light always means the recording of photon statistics of some kind, though the way we interpret the results is quite different and depends mainly on the intensity of actual detected light. If we use conventional photodiodes and monitor bright light, we attribute the detected statistics to quadrature measurements in a phase space representation, or—in other words—we identify the quantum state by studying its uncertainties of its field amplitude and phase properties which correspond to conjugate quantum observables. For multi-photon states with very low intensity we have to employ avalanche photodiodes (APDs) to be able to see any signal, but photon number resolution seems difficult in this regime. Recent developments allow one to ascertain information about the photon statistics from APD measurements opening up new routes for characterizing photonic states. In this article we review the different methods for modern quantum state metrology where we include theoretical aspects as well as the description of the state-of-the-art technology for measuring photon statistics.
As this century unfolds we will witness the rise of the quantum computer. A quantum computer is a device that utilizes the laws of one of the most fundamental theories of physics— quantum mechanics. By utilizing properties of quantum mechanics a quantum computer is able to perform certain information processing tasks much more effciently than an ordinary classical computer. The last century of modern society was revolutionized by some of the simplest ideas in quantum mechanics like energy quantization and quantum tunnelling, which led to technologies like the laser and the transistor. We can expect to see additional technological revolutions occur in this century since we are beginning to build technologies with some of the more complex properties of quantum mechanics such as quantum entanglement and quantum superposition. These quantum effects make more radical technologies like the quantum computer possible. This thesis is based upon the work I have done during my PhD candidature at Macquarie University. In this work we develop quantum technologies that are directed towards realising a quantum computer. Specifically, we have made many theoretical advancements in a type of quantum information processing protocol called Boson Sampling. This device effciently simulates the interaction of quantum particles called bosons, which no classical computer can effciently simulate. In this thesis we explore quantum random walks, which are the basis of how the bosons in Boson Sampling interfere with each other. We explore implementing BosonSampling using the most readily available photon source technology. We invented a completely new architecture which can implement Boson Sampling in time rather than space and has since been used to make the worlds largest Boson Sampling experiment ever performed. We look at variations to the traditional Boson Sampling architecture by considering other quantum states of light. We show a worlds first application inspired by Boson Sampling in quantum metrology where measurements may be made more accurately than with any classical method. Lastly, dealing with Boson Sampling, we look at reformulating the formalism of Boson Sampling using a quantum optics approach. In addition, but not related to BosonSampling, we show a protocol for effciently generating large-photon Fock states, which are a type of quantum state of light, that are useful for quantum computation. Also, we show a method for generating a specific quantum state of light that is useful for quantum error correction — an essential component of realising a quantum computer — by coupling together light and atoms.
Generation and measurement of quantum states of the electromagnetic field represent a hot and widely discussed topic in the Physics community, since optical states are useful not only in fundamental experiments but also in several applications in the fields of Quantum Optics and Quantum Information (Bouwmeester et al., 2000). In fact, optical radiation is endowed with relevant characteristics as it travels at maximum possible speed, it is almost unaffected by the interaction with the environment, which in many cases represents an unavoidable decoherence source, and it can be integrated in optoelectronic circuits to implement quantum computing protocols (Sansoni et al., 2010). The possibility of using optical fields in applicative protocols depends on the capability of generating and manipulating optical states that are robust with respect to losses (i.e. that contain a sizeable number of photons) and that can be produced and measured at high rate. For all these reasons, mesoscopic pulsed optical states containing few tens of photons per pulse seem to be the ideal candidates for applications to quantum communication protocols in which each pulse must be addressed individually. Moreover, the problem of generating suitable pulsed states must be considered together with the question of their measurement and characterization. In fact, nowadays we have many types of pulsed-light sources at our disposal, each of them characterized by different pulse durations (from few fs up to few ns), different pulse-repetition rates (from few Hz to 100 MHz) and a wide range of energies per pulse (from few nJ to several J). However, not all these pulsed light can be easily measured. In the mesoscopic intensity regime, for example, detectors endowed with photon-number resolution are required so as to determine shot-by-shot photon numbers or, at least, to characterize some features of the optical states. In fact, full characterization of the optical state, obtained e.g. by evaluating its Wigner function, can be achieved with optical homodyne tomography (OHT) (Raymer, 1997), a technique that over the years has proved its effectiveness in reconstructing both classical and quantum states, even if further optimizations are needed in the case of pulsed fields (Zavatta et al., 2006). Direct detection schemes are an alternative to OHT in all the cases in which knowing the statistics of detected photons is sufficient to characterize the signal state, as demonstrated in the pioneering work of Arecchi (Arecchi, 1965). Obviously, the implementation of a direct detection scheme requires a proper choice of the detector, the development of a calibration 11