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 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.
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
Modern quantum optics primarily operates in the quasistationary regime, isolated from the intrinsic timescales of ultrafast optical fields. Pushing these boundaries into the femtosecond and attosecond domains is a critical frontier. Here, we generate, shape, and interrogate the quantum state of an ultrafast squeezed light field. Our optical metrology reveals a highly dynamic, time dependent squeezing distribution across individual half cycles of the electric field. Incorporating this intracycle squeezing into strong field simulations demonstrates that the temporal redistribution of quantum uncertainty fundamentally reshapes the quantum strong field physics of high harmonic emission. Furthermore, we achieve attosecond scale control of the squeezed state, visualized through inferred effective Wigner representations. Finally, we show that ultrafast squeezed light encodes its quantum properties into a photoinduced tunneling current within a petahertz phototransistor with subfemtosecond resolution, demonstrating a direct optical electronic quantum coupling. This work lays the foundation for the emerging field of ultrafast quantum optics and unlocks new avenues for high speed quantum communication and photonics.
The technologies utilizing quantum states of light have been in the spotlight for the last two decades. In this regard, quantum metrology, quantum imaging, quantum-optical communication are some of the important applications that exploit fascinating quantum properties like quantum superposition, quantum correlations, and nonclassical photon statistics. However, the state-of-art technologies operating at the single-photon level are not robust enough to truly realize a reliable quantum-photonic technology. In Chapter 1, I present a historical account of photon-based technologies. Furthermore, I discuss recent efforts and encouraging developments in the field of quantum-photonic technologies, and major challenges for the experimental realization of reliable quantum technologies utilizing photons, setting up a stage for unveiling our smart methodologies to cope with them. Similarly, in Chapter 2, I review the fundamental concepts such as states of light, spatial modes of light, and machine learning. In Chapter 3 of this dissertation, I present a theoretical work on a nonlinear quantum metrology scheme, showing a sub-shot-noise limited phase estimation using the displaced-squeezed light and on/off detection. Furthermore, I discuss a camera-based squeezed-light detection technique that can be a smart and time-efficient alternative to conventional balanced-homodyne detection. In Chapter 4, I discuss our efforts to incorporate artificial intelligence in a quest to improve the efficiency of discriminating thermal light sources from coherent light sources. The conventional identification technique requires a large number of measurements. We utilize artificial neural networks to dramatically reduce the number of measurements required to distinguish thermal light and coherent light. In Chapter 5, I present a communication protocol that utilizes the spatial modes of light. Despite being valuable resources for a wide variety of quantum technologies, spatial modes of light are extremely vulnerable to random phase fluctuations. The conventional techniques to cope with these challenges are relatively inefficient. We utilize convolutional neural networks to perform the spatial mode correction of single photons, resulting in a near-unity fidelity of correction. I wrap up my dissertation in Chapter 6 by summarizing the historical context of quantum technologies, challenging problems facing state-of-art quantum technologies, and the importance of our efforts to introduce artificial intelligence in photonic 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.
In quantum optics, quantization of the electromagnetic field typically occurs in a finite volume - a cavity - which results in discrete frequency modes where photons are created, annihilated and exchanged between such modes. As a result, evolution of quantum optical states is periodic in the carrier wave of the field, measurement protocols return cycle-averaged information, and any sub-cycle evolution that is foundational to many light-matter interactions, especially at high field strengths, remains hidden. Adapting an attosecond technique, here we capture the electric-field evolution of a quantum optical state, femtosecond bright squeezed vacuum, with sub-cycle precision. We find that it consists of many stochastic, time-localized bursts within each pump pulse whose phase randomly switches between two values. We exploit the random phase flips to generate quantum random bit sequences with a generation rate that can reach petahertz frequencies. In addition, the sub-cycle resolution allows us to measure coherence functions of the waveforms between any two times, which we explain with a superposition of time-limited modes. These results bridge attosecond metrology and quantum optics and pave the way to measuring quantum light-matter interactions as they evolve on a few-femtosecond time scale, and integrate quantum randomness in petahertz electronics.
A time-domain approach to quantum electrodynamics is presented, covering the entire mid-infrared and terahertz frequency ranges. Ultrabroadband electro-optic sampling with few-femtosecond laser pulses allows direct detection of the vacuum fluctuations of the electric field in free space [1,2]. Besides the Planck and electric field fundamental constants, the variance of the ground state is determined solely by the inverse of the four-dimensional space-time volume over which a measurement or physical process integrates. Therefore, we can vary the contribution of multi-terahertz vacuum fluctuations and discriminate against the trivial shot noise due to the constant flux of near-infrared probe photons. Subcycle temporal resolution based on a nonlinear phase shift provides signals from purely virtual photons for accessing the ground-state wave function without amplification to finite intensity. Recently, we have succeeded in generation and analysis of mid-infrared squeezed transients with quantum noise patterns that are time-locked to the intensity envelope of the probe pulses. We find subcycle temporal positions with a noise level distinctly below the bare vacuum which serves as a direct reference. Delay times with increased differential noise indicate generation of highly correlated quantum fields by spontaneous parametric fluorescence. Our time-domain approach offers a generalized understanding of spontaneous emission processes as a consequence of local anomalies in the co-propagating reference frame modulating the quantum vacuum, in combination with the boundary conditions set by Heisenberg’s uncertainty principle. [1] C. Riek et al., Science 350, 420 (2015) [2] A. S. Moskalenko et al., Phys. Rev. Lett. 115, 263601 (2015)