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Phase-space theory for pulsed quantum light in the context of ultrafast field measurements

Emanuel Hubenschmid

Published May 22, 2026• 0 citations
OpenAlex

Abstract

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.

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Following recent progress in the experimental application of electro-optic sampling to the detection of the quantum fluctuations of the electromagnetic-field ground state and ultrabroadband squeezed states on a subcycle scale, we propose an approach to elevate broadband electro-optic sampling from a spectroscopic method to a full quantum tomography scheme, able to reconstruct a free-space quantum state directly in the time domain. By combining two recently developed methods to theoretically describe quantum electro-optic sampling, we analytically relate the photon-count probability distribution of the electro-optic signal to a transformed phase-space quasiprobability distribution of the sampled quantum state as a function of the time delay between the sampled midinfrared pulsed state and an ultrabroadband near-infrared probe pulse. We catalog and analyze sources of noise and show that in quantum electro-optic sampling with an ultrabroadband probe pulse one can expect to observe thermalization due to entanglement breaking. Mitigation of the thermalization noise enables a tomographic reconstruction of broadband quantum states while granting access to its dynamics on a subcycle scale. Published by the American Physical Society 2024

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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.

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•Apr 29, 2026•0 citations
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.
Following recent progress in the experimental application of electro-optic sampling to the detection of the quantum fluctuations of the electromagnetic-field ground state and ultrabroadband squeezed states on a subcycle scale, we propose an approach to elevate broadband electro-optic sampling from a spectroscopic method to a full quantum tomography scheme, able to reconstruct a free-space quantum state directly in the time domain. By combining two recently developed methods to theoretically describe quantum electro-optic sampling, we analytically relate the photon-count probability distribution of the electro-optic signal to a transformed phase-space quasiprobability distribution of the sampled quantum state as a function of the time delay between the sampled midinfrared pulsed state and an ultrabroadband near-infrared probe pulse. We catalog and analyze sources of noise and show that in quantum electro-optic sampling with an ultrabroadband probe pulse one can expect to observe thermalization due to entanglement breaking. Mitigation of the thermalization noise enables a tomographic reconstruction of broadband quantum states while granting access to its dynamics on a subcycle scale. Published by the American Physical Society 2024
Abstract Quantum light pulses (QLPs) can be described by spatio-temporal modes, each of which is associated with a quantum state. In the mid-infrared spectral range, electro-optic sampling (EOS) provides a means to characterize quantum fluctuations in the electric field of such light pulses. Here, we present a protocol based on the two-port EOS technique that enables the complete characterization of multimode Gaussian quantum light, demonstrating robustness to both the shot noise and cascading effects. We validate this approach theoretically by reconstructing a multimode squeezed state of light generated in a thin nonlinear crystal driven by a single-cycle pulse. Our findings establish the two-port EOS technique as a versatile tool for characterizing ultrafast multimode quantum light, thereby broadening the reach of quantum state tomography. Potential applications include the characterization of complex quantum structures, such as correlations and entanglement in light and matter. Further, extensions to study multimode non-Gaussian QLPs can be envisaged.
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.
Quantum light is considered to be one of the key resources of the coming second quantum revolution expected to give rise to groundbreaking technologies and applications. If the spatio-temporal and polarization structure of modes is known, the properties of quantum light are well understood. This information provides the basis for contemporary quantum optics and its applications in quantum communication and metrology. However, thinking about quantum light at the most fundamental timescale, namely the oscillation cycle of a mode or the inverse frequency of an involved photon, we realize that the corresponding picture has been missing until now. For instance, how to comprehend and characterize a single photon at this timescale? To fill this gap, we demonstrate theoretically how local quantum measurements allow to reconstruct and visualize a quantum field under study at subcycle scales, even when its temporal mode structure is a priori unknown. In particular, generation and tomography of ultrabroadband squeezed states as well as photon-subtracted states derived from them are described, incorporating also single-photon states. Our results set a cornerstone in the emerging chapter of quantum physics termed time-domain quantum optics. We expect this development to elicit new spectroscopic concepts for approaching e.g. fundamental correlations and entanglement in the dynamics of quantum matter, overcoming the temporal limitation set by the oscillation cycles of both light and elementary excitations.
Quantum physics holds promise to revolutionise a number of technologies by enabling performance beyond what is feasible with classical resources, such as secure communications, precision measurement and high-speed simulation and computation. To realise this, quantum information must be encoded into one of the physical degrees of freedom of light. The time-frequency (TF) domain provides a infinite-dimensional space which is naturally compatible with integrated optical platforms. Additionally, future quantum networks will require coherent coupling of quantum systems that do not necessarily exhibit TF mode overlap. The ability to generate, coherently control and measure a variety of TF states of quantum light is therefore a necessary step towards implementing optical quantum technologies. Developing the building blocks for future optical quantum applications calls for an assortment of methods for measuring the properties of TF states of quantum light. Whilst much progress has been made towards this goal recently, deficiencies with existing methods remain. Efficient spectrally-resolved detection away from the telecoms wavelength range and a robust approach to single-photon state characterisation that is sensitive to the spectral phase have so far proven challenging. Additionally, accessing quantum advantages requires measurements that are sensitive to the nonclassical correlations that can exist between separate subsystems. However, until now a flexible approach to determining the full quantum state of systems of multiple time/frequency entangled photons has been lacking. Here we develop a toolbox of techniques for the measurement of TF quantum states of light for few-photon systems, and apply these to the task of precision measurement. Firstly, we propose, construct and demonstrate efficient single-photon spectrometers based on dispersive time-to-frequency mapping, using chirped fibre Bragg gratings to apply the necessary group delay dispersion. We use two such devices operating in coincidence to realise a full phase-sensitive reconstruction of the TF state of a single photon, by spectrally resolving the output of a nonclassical interference process with an external reference. We also demonstrate a complementary, optical reference-free method. This characterisation tool, an implementation of electro-optic spectral shearing interferometry with coincident spectrally-resolved single-photon detection, melds techniques from ultrafast metrology and quantum optics. We proceed to demonstrate the flexibility of this device by reconstructing a wide range of test pulses generated with a pulse shaper. By implementing this technique in conjunction with spectrally-resolved detection of a second photon, we realise complete characterisation of the TF wave function of a spectrally-entangled broadband photon pair. This method is robust to a wide range of inputs and is generalisable to spectrally mixed states and across a wide range of wavelengths, including to spectrally non-degenerate photon pairs. To demonstrate, we generate an entangled photon pair with controllable TF entanglement and perform a full reconstruction. Lastly, we present a new technique for using TF entangled photon pairs to realise quantum-enhanced measurement of a time delay in a quantum channel in the presence of environmental noise. This scheme is based on entanglement-enhanced rejection of background light. A simple experiment demonstrating the feasibility of such a measurement is presented.
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.