Abstract In recent years, electro-optic sampling, which is based on Pockel’s effect between an electromagnetic mode and a copropagating, phase-matched ultrashort probe, has been largely used for the investigation of broadband quantum states of light, especially in the mid-infrared and terahertz frequency range. The use of two mutually delayed femtosecond pulses at near-infrared frequencies allows the measurement of quantum electromagnetic radiation in different space-time points. Their correlation allows therefore direct access to the spectral content of a broadband quantum state at terahertz frequencies after Fourier transformation. In this work, we will prove experimentally and theoretically that when using strongly focused coherent ultrashort probes, the electro-optic sampling technique can be affected by the presence of a third-order nonlinear mixing of the probes’ electric field at near-infrared frequencies. Moreover, we will show that these third-order nonlinear phenomena can also influence correlation measurements of the quantum electromagnetic radiation. We will prove that the four-wave mixing of the coherent probes’ electric field with their own electromagnetic vacuum at near-infrared frequencies results in the generation of a higher-order nonlinear correlation term. The latter will be characterized experimentally, proving its local nature requiring the physical overlap of the two probes. The parameters regime where higher order nonlinear correlation results predominant with respect to electro-optic correlation of terahertz radiation is provided.
Abstract In recent years, electro-optic sampling, which is based on Pockel’s effect between an electromagnetic mode and a copropagating, phase-matched ultrashort probe, has been largely used for the investigation of broadband quantum states of light, especially in the mid-infrared and terahertz frequency range. The use of two mutually delayed femtosecond pulses at near-infrared frequencies allows the measurement of quantum electromagnetic radiation in different space-time points. Their correlation allows therefore direct access to the spectral content of a broadband quantum state at terahertz frequencies after Fourier transformation. In this work, we will prove experimentally and theoretically that when using strongly focused coherent ultrashort probes, the electro-optic sampling technique can be affected by the presence of a third-order nonlinear mixing of the probes’ electric field at near-infrared frequencies. Moreover, we will show that these third-order nonlinear phenomena can also influence correlation measurements of the quantum electromagnetic radiation. We will prove that the four-wave mixing of the coherent probes’ electric field with their own electromagnetic vacuum at near-infrared frequencies results in the generation of a higher-order nonlinear correlation term. The latter will be characterized experimentally, proving its local nature requiring the physical overlap of the two probes. The parameters regime where higher order nonlinear correlation results predominant with respect to electro-optic correlation of terahertz radiation is provided.
In recent years, electro-optic sampling, which is based on Pockel's effect between an electromagnetic mode and a copropagating, phase-matched ultrashort probe, has been largely used for the investigation of broadband quantum states of light, especially in the mid-infrared and terahertz frequency range. The use of two mutually delayed femtosecond pulses at near-infrared frequencies allows the measurement of quantum electromagnetic radiation in different space-time points. Their correlation allows therefore direct access to the spectral content of a broadband quantum state at terahertz frequencies after Fourier transformation. In this work, we will prove experimentally and theoretically that when using strongly focused coherent ultrashort probes, the electro-optic sampling technique can be affected by the presence of a third-order nonlinear mixing of the probes' electric field at near-infrared frequencies. Moreover, we will show that these third-order nonlinear phenomena can also influence correlation measurements of the quantum electromagnetic radiation. We will prove that the four-wave mixing of the coherent probes' electric field with their own electromagnetic vacuum at near-infrared frequencies results in the generation of a higher-order nonlinear correlation term. The latter will be characterized experimentally, proving its local nature requiring the physical overlap of the two probes. The parameters regime where higher order nonlinear correlation results predominant with respect to electro-optic correlation of terahertz radiation is provided.
Direct detection of vacuum fluctuations and analysis of subcycle quantum properties of the electric field are explored by a paraxial quantum theory of ultrafast electro-optic sampling. The feasibility of such experiments is demonstrated by realistic calculations adopting a thin ZnTe electro-optic crystal and stable few-femtosecond laser pulses. We show that nonlinear mixing of a short near-infrared probe pulse with the multiterahertz vacuum field leads to an increase of the signal variance with respect to the shot noise level. The vacuum contribution increases significantly for appropriate length of the nonlinear crystal, short pulse duration, tight focusing, and a sufficiently large number of photons per probe pulse. If the vacuum input is squeezed, the signal variance depends on the probe delay. Temporal positions with a noise level below the pure vacuum may be traced with subcycle resolution.
Electro-optic quantum coherent interfaces map the amplitude and phase of a quantum signal directly to the phase or intensity of a probe beam. At terahertz frequencies, a fundamental challenge is not only to sense such weak signals (due to a weak coupling with a probe in the near-infrared) but also to resolve them in the time domain. Cavity confinement of both light fields can increase the interaction and achieve strong coupling. Using this approach, current realizations are limited to low microwave frequencies. Alternatively, in bulk crystals, electro-optic sampling was shown to reach quantum-level sensitivity of terahertz waves. Yet, the coupling strength was extremely weak. Here, we propose an on-chip architecture that concomitantly provides subcycle temporal resolution and an extreme sensitivity to sense terahertz intracavity fields below 20 V/m. We use guided femtosecond pulses in the near-infrared and a confinement of the terahertz wave to a volume of V T H z ∼ 10 − 9 ( λ T H z / 2 ) 3 in combination with ultraperformant organic molecules ( r 33 = 170 p m / V ) and accomplish a record-high single-photon electro-optic coupling rate of g e o = 2 π × 0.043 G H z , 10,000 times higher than in recent reports of sensing vacuum field fluctuations in bulk media. Via homodyne detection implemented directly on chip, the interaction results into an intensity modulation of the femtosecond pulses. The single-photon cooperativity is C 0 = 1.6 × 10 − 8 , and the multiphoton cooperativity is C = 0.002 at room temperature. We show > 70 d B dynamic range in intensity at 500 ms integration under irradiation with a weak coherent terahertz field. Similar devices could be employed in future measurements of quantum states in the terahertz at the standard quantum limit, or for entanglement of subsystems on subcycle temporal scales, such as terahertz and near-infrared quantum bits.
The influence of measurement back action on electro-optic sampling of electromagnetic quantum fluctuations is investigated. Based on a cascaded treatment of the nonlinear interaction between a near-infrared coherent probe and the mid-infrared vacuum, we account for the generated electric-field contributions that lead to detectable back action. Specifically, we theoretically address two realistic setups, exploiting one or two probe beams for the nonlinear interaction with the quantum vacuum, respectively. The setup parameters at which back action starts to considerably contaminate the measured noise profiles are determined. We find that back action starts to detrimentally affect the signal once the fluctuations due to the coupling to the mid-infrared vacuum become comparable to the base shot noise. Due to the vacuum fluctuations entering at the beam splitter, the shot noise of two incoming probe pulses in different channels is uncorrelated. Therefore, even when the base shot noise dominates the output of the experiment, it does not contribute to the correlation signal itself. However, we find that further contributions due to nonlinear shot-noise enhancement are still present. Ultimately, a regime in which electro-optic sampling of quantum fields can be considered as effectively back-action free is found.
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.