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arXiv:2608.17854 · New Journal of Physics

A quantum optical concept of attosecond pulses: the attoquants

Sándor Varró, Ákos Gombkötő

quant-phSubmitted Aug 18, 2026• Announced Aug 19, 2026• 0 citations
v1 · Aug 18, 2026v2 · Oct 6, 2026
arXivHTMLPDF

Abstract

High-harmonic generation (HHG) is conventionally understood to produce attosecond pulse trains only when the emitted harmonics are mutually phase-locked, in accordance with the classical theory of mode-locking. Such locking is necessary for pulse synthesis when the harmonic field is in a separable multimode quantum state. This requirement, however, can be circumvented entirely for harmonic combs exhibiting intermodal entanglement. We introduce a novel family of multimode quantum states, termed attoquants: states associated with highly structured pulse trains that are inherently insensitive to relative phases. As a concrete example, we analyse the coherent permanent state, constructed as a completely symmetric superposition of products of coherent states over all permutations of a fixed parameter set. It is shown analytically that its electric-field expectation value is a locked Fourier superposition of the driving-field harmonics, yielding an attosecond pulse train without requiring mode-locking. We further calculate the photon statistics, the Wigner function, and the logarithmic negativity of this state, confirming it to be genuinely nonclassical and entangled. Finally, we offer a phenomenological interpretation for the generation of such entangled states during HHG, as a consequence of multi-atom effects. Since the coherence volume of the driving field greatly exceeds that of its harmonics, a collectively-driven cluster of atoms can radiate the individual harmonics as spatially resolved, but fundamentally indistinguishable sources. This can generate the permutation-symmetric entanglement structure of an attoquant.

DOI
10.1088/1367-2630/aeb044
Comments
10 figures

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High-harmonic generation (HHG) is conventionally understood to produce attosecond pulse trains only when the emitted harmonics are mutually phase-locked, in accordance with the classical theory of mode-locking. Such locking is necessary for pulse synthesis when the harmonic field is in a separable multimode quantum state. This requirement, however, can be circumvented entirely for harmonic combs exhibiting intermodal entanglement. We introduce a novel family of multimode quantum states, termed attoquants: states associated with highly structured pulse trains that are inherently insensitive to relative phases. As a concrete example, we analyse the coherent permanent state, constructed as a completely symmetric superposition of products of coherent states over all permutations of a fixed parameter set. It is shown analytically that its electric-field expectation value is a locked Fourier superposition of the driving-field harmonics, yielding an attosecond pulse train without requiring mode-locking. We further calculate the photon statistics, the Wigner function, and the logarithmic negativity of this state, confirming it to be genuinely nonclassical and entangled. Finally, we offer a phenomenological interpretation for the generation of such entangled states during HHG, as a consequence of multi-atom effects. Since the coherence volume of the driving field greatly exceeds that of its harmonics, a collectively-driven cluster of atoms can radiate the individual harmonics as spatially resolved, but fundamentally indistinguishable sources. This can generate the permutation-symmetric entanglement structure of an attoquant.
High harmonic generation (HHG) is an extremely nonlinear effect generating coherent broadband radiation and pulse durations reaching attosecond timescales. Conventional models of HHG that treat the driving and emitted fields classically are usually very successful but inherently cannot capture the quantum-optical nature of the process. Although prior work considered quantum HHG, it remains unknown in what conditions the spectral and statistical properties of the radiation depart considerably from the known phenomenology of HHG. The discovery of such conditions could lead to novel sources of attosecond light having squeezing and entanglement. Here, we present a fully-quantum theory of extreme nonlinear optics, predicting quantum effects that alter both the spectrum and photon statistics of HHG, thus departing from all previous approaches. We predict the emission of shifted frequency combs and identify spectral features arising from the breakdown of the dipole approximation for the emission. Our results show that each frequency component of HHG can be bunched and squeezed and that each emitted photon is a superposition of all frequencies in the spectrum, i.e., each photon is a comb. Our general approach is applicable to a wide range of nonlinear optical processes, paving the way towards novel quantum phenomena in extreme nonlinear optics.
High-order harmonic generation (HHG) provides a broad spectral bandwidth for synthesizing attosecond pulses. However, in the current HHG schemes, only part of the harmonics can be phase-locked, which limits the ability to achieve shorter attosecond pulses. Here, we study attosecond pulse synthesis from HHG of an atom driven by an intense quantum light, i.e., squeezed light. It is interestingly found that the harmonics in the whole spectrum can be phase-locked and, by using these harmonics, the width of the synthesized attosecond pulse is greatly reduced. By developing strong-field approximation theory in squeezed light, the physics of the phase-locked harmonic generation throughout the HHG spectrum is revealed and is found to be independent of the target system. Furthermore, we uncover the dependence of the synthesized attosecond pulse width on the squeezing parameter of the squeezed light. Our findings provide a robust tool for obtaining phase-locked harmonics throughout the HHG spectrum for synthesizing short attosecond pulses.
Preparation of nonclassical light with special quantum properties is essential for quantum technologies. High-harmonic generation (HHG) is a process which not only enables the creation of attosecond pulses but also has the potential to generate light with intricate quantum properties. In a recent experiment [PRX Quantum 5. 040319], nonclassical inter-harmonic correlations have been measured from a HHG source between low-order harmonics. In this work, we theoretically investigate entanglement between different harmonics within an effective, phenomenological quantum optical model. This model implements a significant degree of simplification regarding the processes within the target material, treating the material through susceptibilities, as it is usual in quantum optics. Such an approach yields a general description of HHG in the few-harmonic generation regime, permitting the implications that can be derived within it to hold broadly within the domain of validity. We find that entanglement is produced as a result of the often neglected back-action. We can qualitatively reproduce experimentally measured nonclassicalities, which suggests that intermodal entanglement can, to an extent, be considered a universal phenomenon associated with HHG, rather than a result of using specific material targets.
The optical phase of the driving field in the process of high harmonic generation and the coherence properties of the harmonics are fundamental concepts in attosecond physics. Here, we consider driving the process by incoherent classical and nonclassical light fields exhibiting an undetermined optical phase. With this, we introduce the notion of quantum optical coherence into high harmonic generation and show that high harmonics can be generated from incoherent radiation despite having a vanishing electric field. We explicitly derive the quantum state of the harmonics when driven by carrier-envelope phase unstable fields and show that the generated harmonics are incoherent and exhibit zero electric field amplitudes. We find that the quantum state of each harmonic is diagonal in its photon number basis, but nevertheless has the exact same photon statistics as the widely considered coherent harmonics. From this, we conclude that assuming coherent harmonic radiation can originate from a preferred ensemble fallacy. These findings have profound implications for attosecond experiments and how to infer the harmonic radiation properties. Published by the American Physical Society 2024
High-harmonic generation (HHG) is a prototypical strong-field process in which intense light drives matter to emit radiation at integer multiples of the driving frequency. Extending HHG into the quantum-optical regime offers new opportunities to probe and control strongly nonlinear light-matter interactions using nonclassical states of light. Yet describing this regime requires a fully quantum treatment of the correlated electron-photon dynamics, which becomes computationally challenging for broadband, strongly squeezed fields. Here we solve the quantum-electrodynamical dynamics of a two-level system driven by bright squeezed vacuum in a converged multimode Hilbert space. Both the driving field and emitted harmonics are fully quantized, with the light-matter interaction treated nonperturbatively. This enables direct access to the multimode quantum state and its higher-order correlations beyond semiclassical sampling or perturbative descriptions. We show that squeezed-vacuum driving produces harmonic emission with qualitatively distinct second- and third-order photon correlations compared with coherent excitation. Moreover, back-action from the driven emitter strongly reshapes the incident squeezed field, generating pronounced Wigner-function negativities that evolve on attosecond timescales. Our results establish a fully quantum framework for broadband strong-field dynamics with squeezed light and provide a route to predicting and interpreting quantum-HHG experiments and their extension to more complex emitters.
High-order harmonic generation (HHG) is a significant nonlinear phenomenon triggered by the interaction of intense laser fields with matter. As a high-quality coherent light source, it has found extensive applications in areas such as attosecond pulse generation and ultrafast spectroscopy. Recent studies have revealed the prevalent existence of nonclassical effects in high-harmonic radiation, including nonclassical photon statistics, intermodal correlations, and entanglement. It holds broad development prospects in directions including the generation of nonclassical states with high photon numbers, precise control of entanglement in solid-state systems, and integration with cavity quantum electrodynamics. This review systematically summarizes the research progress concerning the nonclassical effects in HHG. It begins with an overview of the semiclassical model and strong-field quantum theory, clarifying the differences in the quantum properties of harmonic fields when driven by coherent states versus nonclassical states. Subsequently, it focuses on various physical schemes for generating nonclassical optical field states, such as optical cat states and squeezed states, via this process. Research on strong-field HHG not only deepens our understanding of the fundamental nature of intense laser physics but also opens new avenues for the generation and application of quantum light sources in the extreme ultraviolet to X-ray spectral regions.