The goal of this work is to examine the coherence of classical light fields in order to assess their usefulness for quantum-informational tasks and to draw conclusions about the properties of the light source. To this end, we use and extend several optical homodyne tomography techniques employing four-port, eight-port, and sixteen-port detection schemes. To understand the role of coherence of a light field in solving a quantum informational task such as coherent qubit control, we begin by analyzing the qubit excitation process from a resource-theoretical perspective. By simulating the light-matter interactions, we demonstrate how the quantum coherence of the driving light field emerges as a key ingredient for coherent qubit control. At the same time, we show how the presence of thermal noise or dephasing significantly degrades the achievable quantum coherence of the light field. After studying the coherence properties of conventional lasers, we turn to non-conventional coherent light sources and investigate the emission of a non-resonantly excited exciton-polariton condensate. By employing long-lived polaritons and minimizing interactions with the reservoir, we optimize the condensation process and achieve a pronounced buildup of quantum superpositions in the condensate immediately above the condensation threshold. Finally, we shift our focus entirely to the matter system itself and use the coherence of the emitted light field to investigate its dynamics. For this purpose, we introduce a sixteen-port detection scheme that enables non-stationary and conditional analyses tailored to the requirements of semiconductor spectroscopy. Benchmarking the setup with a thermal light field, then demonstrate how we can resolve the stochastic fluctuations of the thermal state on the femtosecond level. Overall, our results establish connections between quantum optics, quantum information science, and semiconductor physics, providing insights relevant for quantum technologies and future hybrid quantum devices.
The goal of this work is to examine the coherence of classical light fields in order to assess their usefulness for quantum-informational tasks and to draw conclusions about the properties of the light source. To this end, we use and extend several optical homodyne tomography techniques employing four-port, eight-port, and sixteen-port detection schemes. To understand the role of coherence of a light field in solving a quantum informational task such as coherent qubit control, we begin by analyzing the qubit excitation process from a resource-theoretical perspective. By simulating the light-matter interactions, we demonstrate how the quantum coherence of the driving light field emerges as a key ingredient for coherent qubit control. At the same time, we show how the presence of thermal noise or dephasing significantly degrades the achievable quantum coherence of the light field. After studying the coherence properties of conventional lasers, we turn to non-conventional coherent light sources and investigate the emission of a non-resonantly excited exciton-polariton condensate. By employing long-lived polaritons and minimizing interactions with the reservoir, we optimize the condensation process and achieve a pronounced buildup of quantum superpositions in the condensate immediately above the condensation threshold. Finally, we shift our focus entirely to the matter system itself and use the coherence of the emitted light field to investigate its dynamics. For this purpose, we introduce a sixteen-port detection scheme that enables non-stationary and conditional analyses tailored to the requirements of semiconductor spectroscopy. Benchmarking the setup with a thermal light field, then demonstrate how we can resolve the stochastic fluctuations of the thermal state on the femtosecond level. Overall, our results establish connections between quantum optics, quantum information science, and semiconductor physics, providing insights relevant for quantum technologies and future hybrid quantum devices.
This review examines the use of continuous-variable spectroscopy techniques for investigating quantum coherence and light-matter interactions in semiconductor systems with ultrafast dynamics. Special emphasis is placed on multichannel homodyne detection as a powerful tool to measure the quantum coherence and the full density matrix of a polariton system. Observations, such as coherence times that exceed the nanosecond scale obtained by monitoring the temporal decay of quantum coherence in a polariton condensate, are discussed. Proof-of-concept experiments and numerical simulations that demonstrate the enhanced resourcefulness of the produced system states for modern quantum protocols are assessed. The combination of tailored resource quantifiers and ultrafast spectroscopy techniques that have recently been demonstrated paves the way for future applications of quantum information technologies.
Lasers serve as the fundamental workhorses of photonic quantum technologies, with perfectly coherent light fields being essential for many protocols that generate nonclassical light, implement coherent control schemes, and initialize qubits. However, no laser is absolutely ideal and the implications of deviations from perfect coherence in quantum technological tasks remain unclear. In this study, we theoretically and experimentally explore the quantum coherence properties of lasers from a resource theory perspective, establishing a significant connection between photonics, quantum optics, and quantum information science. We demonstrate that the maximum achievable quantum coherence for laser light is constrained by spontaneous emission and the purity of the dephased laser field state. As a critical example application in quantum information protocols, we show that the quantum coherence of a laser field with a given mean photon number directly governs the maximum purity attainable when initializing a qubit in a superposition state through resonant driving. Our findings are highly relevant for bridging applied physics and engineering with integrated photonic quantum technologies and resource theories, paving the way for reliable benchmarking of various coherent light sources for applications in photonics and quantum protocols.
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.
In this review, we discuss the use of continuous variable spectroscopy techniques for investigating quantum coherence and light-matter interactions in semiconductor systems with ultrafast dynamics. We focus on multichannel homodyne detection as a powerful tool to measure the quantum coherence and the full density matrix of a polariton system. By monitoring the temporal decay of quantum coherence in the polariton condensate, we observe coherence times exceeding the nanosecond scale. Our findings, supported by proof-of-concept experiments and numerical simulations, demonstrate the enhanced resourcefulness of the produced system states for modern quantum protocols. The combination of tailored resource quantifiers and ultrafast spectroscopy techniques presented here paves the way for future applications of quantum information technologies.
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.
Quantum state tomography and the reconstruction of the photon number distribution are techniques to extract the properties of a light field from measurements of its mean and fluctuations. These techniques are particularly useful when dealing with macroscopic or mesoscopic systems, where a description limited to the second order autocorrelation soon becomes inadequate. In particular, the emission of nonclassical light is expected from mesoscopic quantum dot systems strongly coupled to a cavity or in systems with large optical nonlinearities. We analyze the emission of a quantum dot-semiconductor optical amplifier system by quantifying the modifications of a femtosecond laser pulse propagating through the device. Using a balanced detection scheme in a self-heterodyning setup, we achieve precise measurements of the quadrature components and their fluctuations at the quantum noise limit1. We resolve the photon number distribution and the thermal-to-coherent evolution in the photon statistics of the emission. The interferometric detection achieves a high sensitivity in the few photon limit. From our data, we can also reconstruct the second order autocorrelation function with higher precision and time resolution compared with classical Hanbury Brown-Twiss experiments.