Challenges
Datasets
Workspaces
Papers
Discussions
Leaderboard
Log inSign up
Challenges
Datasets
Workspaces
Papers
Discussions
Leaderboard
Blog
Job Board
Q3AS

© 2026 Aqora Quantum S.A.S.

TermsPrivacyLegal Notice

arXiv:2304.14617 · Physical Review A

Unconventional gap dependence of high-order harmonic generation in the extremely strong light-matter-coupling regime

Akira Kofuji, Robert Peters

Published Aug 25, 2023• 2 citations
arXivHTMLPDF

Abstract

High-order harmonic generation (HHG) is one of the most commonly studied nonlinear optical phenomena, originating in the ultrafast dynamics of electrons in atomic gases and semiconductors. It has attracted much attention because of its nonperturbative nature and potential for future attosecond laser pulse sources. On the theory side, a semiclassical picture based on tunneling ionization of electrons is successfully used in explaining key characteristics of the HHG. This model assumes that electric fields nonperturbatively excite electrons beyond the ionization potential or the band gap. Thus, intuitively, a larger gap should lead to an exponentially smaller HHG emission. Despite this intuition, the HHG in the Mott insulator ${\mathrm{Ca}}_{2}{\mathrm{RuO}}_{4}$ has shown an unconventional exponential increase with respect to the gap width. This experiment implies effects beyond the semiclassical theory. However, most theoretical works have focused on the dependence of the HHG on external control parameters, and the gap dependence of the HHG is poorly understood even in noninteracting systems. Thus, it is essential to clarify the gap dependence of the HHG in a fully quantum mechanical approach. Here, we analyze numerically exactly the gap dependence of the HHG in two-level systems. We find an increase in the strength of the HHG when the Rabi frequency is large compared to the gap width. Furthermore, the relaxation and scattering of electrons increase the visibility of this gap dependence. Finally, we find that the enhancement rate follows a universal scaling law regardless of the driving frequency. The existence of this gap dependence in two-level systems suggests that this unconventional gap dependence is a universal behavior that can be found not only in Mott insulators but also in atomic gases and semiconductors.

DOI
10.1103/physreva.108.023521

Related papers

Nonclassical light generation and control from laser-driven semiconductor intraband excitations

Ivan Gonoskov, René Sondenheimer, Christian Hünecke +3 more

The generation of higher-order harmonic radiation originating from the interaction of intense laser pulses with matter is typically described semiclassically: While the electronic structure and dynamics of matter is described quantum mechanically, the intense light field is described classically---and accordingly the generated harmonic radiation. However, pioneering experiments on quantum optical properties of high-order harmonic generation (HHG) in atomic gases from the group of P. Tzallas [I. Gonoskov et al., Sci. Rep. 6, 32821 (2016) and N. Tsatrafyllis et al., Nat. Commun. 8, 15170 (2017)], and theoretical investigations from the group of M. Lewenstein [M. Lewenstein et al., Nat. Phys. 17, 1104 (2021) and P. Stammer et al., Phys. Rev. Lett. 128, 123603 (2022)] have impressively demonstrated that light's quantum properties are observable in the strong-field realm. In this paper, we develop a quantum optical description of HHG in a bulk semiconductor originating from the nonlinear Bloch current. This mechanism of HHG, known as the intraband current, constitutes the major contribution to the emission spectrum for harmonic with energies of quanta roughly below the bandgap. Under certain approximations, employing a quantum description of both light and matter, we obtain analytical solutions, which allow us to analyze the classical and quantum optical characteristics of the fundamental mode of light and the harmonic modes. We find intricate but sufficiently mild modifications of the photon statistics of the fundamental mode and coherent displacements depending on the parameters of the driving laser field. Similar to high-harmonic generation in atoms, the fundamental and emitted harmonic field modes are entangled. Moreover, our analytical model predicts parameter ranges where these quantum optical properties will be most pronounced, allowing protocols for quantum information processing with high photon numbers over a large range of frequencies.

Physical review. B./Physical review. B•Mar 7, 2024•23 citations

High-Order Harmonic Generation with Beyond-Semiclassical Emitter Dynamics: A Strong-Field Quantum Optical Heisenberg Picture Approach

Christian Saugbjerg Lange, Ella Elisabeth Lassen, Rasmus Vesterager Gothelf +1 more

Quantum-optical descriptions of strong-field processes have attracted significant attention in recent years. Typically, the theoretical modeling has been conducted in the Schrödinger picture, where results are only obtainable under certain approximations, while, in contrast, the Heisenberg picture has remained relatively unexplored. In this work, we develop an accurately controlled perturbative expansion of the time-evolution operator in the Heisenberg picture and derive beyond-semiclassical corrections to the emitter dynamics due to the coupling to the quantized electromagnetic field, capturing effects of the quantum fluctuations present in the latter. We focus on high-order harmonic generation (HHG), where the approach is accurate in parameter regimes of current interest and it gives closed-form expressions for key observables. This formulation not only simplifies numerical calculations compared to the Schrödinger-picture approach but also provides a clear correspondence between nonclassical features of the emitted light and the underlying induced dynamics of the generating medium including quantum fluctuations. Moreover, the Heisenberg framework naturally yields scaling relations with the number of independent emitters, enabling us to assess whether nonclassical behavior should persist under typical experimental conditions involving large emitter ensembles. Interestingly, we find that the degree of squeezing increases with the number of emitters, whereas the photon statistics approaches a classical Poissonian distribution in the many-emitter limit. We also find that the beyond-semiclassical emitter dynamics significantly enhances the degree of squeezing of the emitted light. Our work advances the theoretical understanding of quantum-optical HHG and introduces an accessible and well-controlled framework to describe realistic experiments.

quant-pharXiv:2512.14174•Physical Review A•Dec 17, 2025•1 citation

High-Order Harmonic Generation and Its Unconventional Scaling Law in the Mott-Insulating Ca2RuO4

Kento Uchida, Giordano Mattoni, Shingo Yonezawa +3 more

Competition and cooperation among orders is at the heart of many-body physics in strongly correlated materials and leads to their rich physical properties. It is crucial to investigate what impact many-body physics has on extreme nonlinear optical phenomena, with the possibility of controlling material properties by light. However, the effect of competing orders and electron-electron correlations on highly nonlinear optical phenomena has not yet been experimentally clarified. Here, we investigated high-order harmonic generation from the Mott-insulating phase of Ca_{2}RuO_{4}. Changing the gap energy in Ca_{2}RuO_{4} as a function of temperature, we observed a strong enhancement of high order harmonic generation at 50 K, increasing up to several hundred times compared to room temperature. We discovered that this enhancement can be well reproduced by an empirical scaling law that depends only on the material gap energy and photon emission energy. Such a scaling law can hardly be explained by the electronic structure change in the single particle model and has not been predicted by previous theoretical studies on HHG in the simple Mott-Hubbard model. Our results suggest that the highly nonlinear optical response of strongly correlated materials is influenced by competition among the multiple degrees of freedom and electron-electron correlations.

arXiv:2106.15478•Physical Review Letters•Mar 23, 2022•67 citations

Nonclassical states of light after high-harmonic generation in semiconductors: A Bloch-based perspective

Javier Rivera-Dean, Philipp Stammer, Andrew Maxwell +6 more

High-harmonic generation (HHG) has emerged as a pivotal process in strong-field physics, yielding extreme ultraviolet radiation and attosecond pulses for a wide range of applications. Furthermore, its emergent connection with the field of quantum optics has revealed its potential for generating nonclassical states of light. Here, we investigate the process of high-harmonic generation in semiconductors under a quantum optical perspective while using a Bloch-based solid-state description. Through the implementation of quantum operations based on the measurement of high-order harmonics, we demonstrate the generation of nonclassical light states similar to those found when driving atomic systems. These states are characterized using diverse quantum optical observables and quantum information measures, showing the influence of electron dynamics on their properties. Additionally, we analyze the dependence of their features on solid characteristics such as the dephasing time and crystal orientation, while also assessing their sensitivity to changes in driving field strength. This paper provides insights into HHG in semiconductors and its potential for generating nonclassical light sources.

arXiv:2309.14435•Physical review. B./Physical review. B•Jan 19, 2024•24 citations

Nonclassical effects in high-order harmonic radiation

Fu Yifei, ZHAO Di, GAO Shaoyan +1 more

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.

Zhongguo kexue. Wulixue Lixue Tianwenxue•Mar 9, 2026•0 citations

Excitonic effects on high-harmonic generation in Mott insulators

Mina Udono, K. Sugimoto, Tatsuya Kaneko +1 more

To study excitonic effects on high-harmonic generation (HHG) in Mott insulators, we investigate pumped nonequilibrium dynamics in the one-dimensional extended Hubbard model. By employing time-dependent calculations based on the exact diagonalization and infinite time-evolving block decimation methods, we find the strong enhancement of the HHG intensity around the exciton energy. The subcycle analysis in the sub-Mott-gap regime shows that the intensity region of the time-resolved spectrum around the exciton energy splits into two levels and oscillates following the driving electric field. This excitonic dynamics is qualitatively different from the dynamics of free doublon and holon but favorably contributes to HHG in the Mott insulator.

arXiv:2205.06390•Physical review. B./Physical review. B•Jun 10, 2022•29 citations
High-order harmonic generation (HHG) is one of the most commonly studied nonlinear optical phenomena, originating in the ultrafast dynamics of electrons in atomic gases and semiconductors. It has attracted much attention because of its nonperturbative nature and potential for future attosecond laser pulse sources. On the theory side, a semiclassical picture based on tunneling ionization of electrons is successfully used in explaining key characteristics of the HHG. This model assumes that electric fields nonperturbatively excite electrons beyond the ionization potential or the band gap. Thus, intuitively, a larger gap should lead to an exponentially smaller HHG emission. Despite this intuition, the HHG in the Mott insulator Ca2RuO4{\mathrm{Ca}}_{2}{\mathrm{RuO}}_{4}Ca2​RuO4​ has shown an unconventional exponential increase with respect to the gap width. This experiment implies effects beyond the semiclassical theory. However, most theoretical works have focused on the dependence of the HHG on external control parameters, and the gap dependence of the HHG is poorly understood even in noninteracting systems. Thus, it is essential to clarify the gap dependence of the HHG in a fully quantum mechanical approach. Here, we analyze numerically exactly the gap dependence of the HHG in two-level systems. We find an increase in the strength of the HHG when the Rabi frequency is large compared to the gap width. Furthermore, the relaxation and scattering of electrons increase the visibility of this gap dependence. Finally, we find that the enhancement rate follows a universal scaling law regardless of the driving frequency. The existence of this gap dependence in two-level systems suggests that this unconventional gap dependence is a universal behavior that can be found not only in Mott insulators but also in atomic gases and semiconductors.
The generation of higher-order harmonic radiation originating from the interaction of intense laser pulses with matter is typically described semiclassically: While the electronic structure and dynamics of matter is described quantum mechanically, the intense light field is described classically---and accordingly the generated harmonic radiation. However, pioneering experiments on quantum optical properties of high-order harmonic generation (HHG) in atomic gases from the group of P. Tzallas [I. Gonoskov et al., Sci. Rep. 6, 32821 (2016) and N. Tsatrafyllis et al., Nat. Commun. 8, 15170 (2017)], and theoretical investigations from the group of M. Lewenstein [M. Lewenstein et al., Nat. Phys. 17, 1104 (2021) and P. Stammer et al., Phys. Rev. Lett. 128, 123603 (2022)] have impressively demonstrated that light's quantum properties are observable in the strong-field realm. In this paper, we develop a quantum optical description of HHG in a bulk semiconductor originating from the nonlinear Bloch current. This mechanism of HHG, known as the intraband current, constitutes the major contribution to the emission spectrum for harmonic with energies of quanta roughly below the bandgap. Under certain approximations, employing a quantum description of both light and matter, we obtain analytical solutions, which allow us to analyze the classical and quantum optical characteristics of the fundamental mode of light and the harmonic modes. We find intricate but sufficiently mild modifications of the photon statistics of the fundamental mode and coherent displacements depending on the parameters of the driving laser field. Similar to high-harmonic generation in atoms, the fundamental and emitted harmonic field modes are entangled. Moreover, our analytical model predicts parameter ranges where these quantum optical properties will be most pronounced, allowing protocols for quantum information processing with high photon numbers over a large range of frequencies.
Quantum-optical descriptions of strong-field processes have attracted significant attention in recent years. Typically, the theoretical modeling has been conducted in the Schrödinger picture, where results are only obtainable under certain approximations, while, in contrast, the Heisenberg picture has remained relatively unexplored. In this work, we develop an accurately controlled perturbative expansion of the time-evolution operator in the Heisenberg picture and derive beyond-semiclassical corrections to the emitter dynamics due to the coupling to the quantized electromagnetic field, capturing effects of the quantum fluctuations present in the latter. We focus on high-order harmonic generation (HHG), where the approach is accurate in parameter regimes of current interest and it gives closed-form expressions for key observables. This formulation not only simplifies numerical calculations compared to the Schrödinger-picture approach but also provides a clear correspondence between nonclassical features of the emitted light and the underlying induced dynamics of the generating medium including quantum fluctuations. Moreover, the Heisenberg framework naturally yields scaling relations with the number of independent emitters, enabling us to assess whether nonclassical behavior should persist under typical experimental conditions involving large emitter ensembles. Interestingly, we find that the degree of squeezing increases with the number of emitters, whereas the photon statistics approaches a classical Poissonian distribution in the many-emitter limit. We also find that the beyond-semiclassical emitter dynamics significantly enhances the degree of squeezing of the emitted light. Our work advances the theoretical understanding of quantum-optical HHG and introduces an accessible and well-controlled framework to describe realistic experiments.
Competition and cooperation among orders is at the heart of many-body physics in strongly correlated materials and leads to their rich physical properties. It is crucial to investigate what impact many-body physics has on extreme nonlinear optical phenomena, with the possibility of controlling material properties by light. However, the effect of competing orders and electron-electron correlations on highly nonlinear optical phenomena has not yet been experimentally clarified. Here, we investigated high-order harmonic generation from the Mott-insulating phase of Ca_{2}RuO_{4}. Changing the gap energy in Ca_{2}RuO_{4} as a function of temperature, we observed a strong enhancement of high order harmonic generation at 50 K, increasing up to several hundred times compared to room temperature. We discovered that this enhancement can be well reproduced by an empirical scaling law that depends only on the material gap energy and photon emission energy. Such a scaling law can hardly be explained by the electronic structure change in the single particle model and has not been predicted by previous theoretical studies on HHG in the simple Mott-Hubbard model. Our results suggest that the highly nonlinear optical response of strongly correlated materials is influenced by competition among the multiple degrees of freedom and electron-electron correlations.
High-harmonic generation (HHG) has emerged as a pivotal process in strong-field physics, yielding extreme ultraviolet radiation and attosecond pulses for a wide range of applications. Furthermore, its emergent connection with the field of quantum optics has revealed its potential for generating nonclassical states of light. Here, we investigate the process of high-harmonic generation in semiconductors under a quantum optical perspective while using a Bloch-based solid-state description. Through the implementation of quantum operations based on the measurement of high-order harmonics, we demonstrate the generation of nonclassical light states similar to those found when driving atomic systems. These states are characterized using diverse quantum optical observables and quantum information measures, showing the influence of electron dynamics on their properties. Additionally, we analyze the dependence of their features on solid characteristics such as the dephasing time and crystal orientation, while also assessing their sensitivity to changes in driving field strength. This paper provides insights into HHG in semiconductors and its potential for generating nonclassical light sources.
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.
To study excitonic effects on high-harmonic generation (HHG) in Mott insulators, we investigate pumped nonequilibrium dynamics in the one-dimensional extended Hubbard model. By employing time-dependent calculations based on the exact diagonalization and infinite time-evolving block decimation methods, we find the strong enhancement of the HHG intensity around the exciton energy. The subcycle analysis in the sub-Mott-gap regime shows that the intensity region of the time-resolved spectrum around the exciton energy splits into two levels and oscillates following the driving electric field. This excitonic dynamics is qualitatively different from the dynamics of free doublon and holon but favorably contributes to HHG in the Mott insulator.