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arXiv:2606.17620

Photon anti-bunching in high harmonic generation

Philipp Stammer, Javier Rivera-Dean, Maciej Lewenstein

quant-phphysics.opticsSubmitted Jun 16, 2026• Announced Jun 17, 2026• 0 citations
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Abstract

Photon anti-bunching is the direct evidence for the existence of photons without having a classical counterpart. Unlike bunching of photons, which can have a semi-classical description, the effect of photon anti-bunching can only be understood with quantized electromagnetic fields. However, for the process of high harmonic generation (HHG), where many photons of the driving field are upconverted to a single photon of higher energy, there is yet no clear evidence for the presence of individual photon emission. The key result of this work is the prediction of photon anti-bunching in the process of HHG, marking it the first theoretical discovery of non-classicality in the temporal correlations of HHG photons. While other non-classical signatures in HHG, such as sub-Poissonian statistics or squeezing, have been discussed for an ensemble of photons, the anti-bunching signature reported here is a signature of a single photon. This is achieved by using the recently developed Heisenberg picture approach for quantum optical HHG, revealing clear anti-bunching signatures in the intensity correlation function across the entire harmonic spectrum.

Comments
5 pages, 4 figures

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Photon anti-bunching is the direct evidence for the existence of photons without having a classical counterpart. Unlike bunching of photons, which can have a semi-classical description, the effect of photon anti-bunching can only be understood with quantized electromagnetic fields. However, for the process of high harmonic generation (HHG), where many photons of the driving field are upconverted to a single photon of higher energy, there is yet no clear evidence for the presence of individual photon emission. The key result of this work is the prediction of photon anti-bunching in the process of HHG, marking it the first theoretical discovery of non-classicality in the temporal correlations of HHG photons. While other non-classical signatures in HHG, such as sub-Poissonian statistics or squeezing, have been discussed for an ensemble of photons, the anti-bunching signature reported here is a signature of a single photon. This is achieved by using the recently developed Heisenberg picture approach for quantum optical HHG, revealing clear anti-bunching signatures in the intensity correlation function across the entire harmonic spectrum.
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-harmonic generation (HHG) driven by intense quantum light has recently emerged as a new frontier in strong-field physics. Yet, the mechanism underlying HHG with nonclassical fields such as bright squeezed vacuum (BSV) light—characterized by a vanishing mean electric field—remains elusive. In this work, we develop a fully quantum theory for HHG under arbitrary quantum driving fields. We show that the fluctuation component of the dipole correlation operator plays a central role in HHG with quantum light and is essential for BSV-driven HHG. Furthermore, our framework reveals the photon statistics distribution within individual harmonics and across different harmonics, demonstrating that the statistics inherit the statistical properties of the driving field. This theory overcomes key limitations of existing approaches and uncovers new quantum features of HHG in the presence of nonclassical light.
High-Harmonic Generation (HHG) is a highly non-linear frequency up conversion process, mostly studied from a classical point of view. Recently, independent theoretical investigations about the quantum nature of HHG predicted several, non-classical effects in the high-harmonic radiation. In addition to the fundamental interest in understanding the physics behind HHG, a better understanding of the quantum nature of this process could potentially have a broad impact on the rapidly developing field of quantum technologies. It is in this context that present here our experimental photon statistics investigations showing the quantum nature of the HHG process.
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.
Recently, the intersection of quantum optics and attosecond physics has attracted growing interest. Here, we study the quantum optical signatures of high-harmonic generation (HHG) from solid-state material driven by squeezed coherent states. We find that squeezed coherent states can either enhance or suppress the HHG yields compared to that driven by coherent light, depending on the photon bunching or antibunching characteristics of driving light. The analysis on semiclassical trajectories indicates that the amplitude fluctuation alters the recombination energy, while the phase fluctuation affects the birth and recombination time of electron-hole pairs. By calculating the Husimi Q distributions of HHG, we demonstrate that the squeezing of the two conjugate quadratures of driving light asymmetrically influence the squeezing phase of harmonics. Surprisingly, we find that even under coherent driving, the harmonics still exhibit squeezing due to the highly nonlinear response of solid-state HHG, which was overlooked previously. Numerical calculations of the Mandel parameter are performed to characterize the photon statistics of emitted HHG arising from different microscopic mechanisms. The results indicate that intraband radiation can exhibit a super-Poissonian distribution, while interband emission exhibits sub-Poissonian distribution under coherent driving.
We present a study of photon statistics associated with high-order harmonic generation (HHG) involving one-mode and intermodal correlations of the high harmonic photons. The aim of the paper is to give insight into the nonclassical properties of high-order harmonic modes. To this end, we use a simplified model describing an elementary quantum emitter: the model of a two-level atom. While the material system is extremely simplified in this description, the conclusions and the methods may be generalized for more complex cases. Our primary interest is an effective model of HHG in which the exciting pulse is classical and the harmonics are quantized, although we touch upon the more generalized, fully quantized model as well. Evolution of the Mandel parameter, photon antibunching, squeezing, and cross correlations are calculated. Results imply that with respect to a single quantized emitter, nonclassicality of the harmonics is present: sub-Poissonian photon statistic and squeezing can characterize certain optical modes, while strong anticorrelation can also be present.