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High Harmonic Generation by Bright Squeezed Vacuum

Andrei Rasputnyi, Michael Birk, Zhaopin Chen, Oren Cohen, Michael B. Kruger, Ido E. Kaminer, Maria V. Chekhova, Francesco Tani

Published Jan 1, 2024• 0 citations
Publisher

Abstract

We present the first observation of non-perturbative high-harmonic generation driven by nonclassical light, namely bright squeezed vacuum. Compared to classical light, bright squeezed vacuum leads to higher efficiency, different power scaling, and unique photon-number distributions.
DOI
10.1364/cleo_fs.2024.fm4b.3

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Abstract High-harmonic generation has been driving the development of attosecond science and sources. More recently, high-harmonic generation in solids has been adopted by other communities as a method to study material properties. However, so far high-harmonic generation has only been driven by classical light, despite theoretical proposals to do so with quantum states of light. Here we observe non-perturbative high-harmonic generation in solids driven by a macroscopic quantum state of light, a bright squeezed vacuum, which we generate in a single spatiotemporal mode. The process driven by a bright squeezed vacuum is considerably more efficient in the generation of high harmonics than classical light of the same mean intensity. Due to its broad photon-number distribution, covering states from 0 to 2 × 10 13 photons per pulse, and strong subcycle electric field fluctuations, a bright squeezed vacuum gives access to free carrier dynamics within a much broader range of peak intensities than accessible with classical light.
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 nonlinear optical process in which radiation from a strong driving field is up-converted into its high-order harmonics. In atomic systems, this nonlinearity manifests itself through the intensity scaling of the emitted harmonics with the driving field strength. Despite the highly nonlinear nature of HHG, when the driving field is prepared in a classical Gaussian state and atomic depletion remains negligible, the quantum statistical properties of the generated harmonics retains classical Gaussian quantum statistics. Driving HHG with bright squeezed vacuum (BSV) light challenges this paradigm, as its enhanced field fluctuations can modify the statistical properties of the generated harmonics. In this work, we investigate the conditions under which BSV-driven HHG gives rise to non-classical Gaussian states, and identify the regimes where this Gaussian description breaks down. For bichromatic driving by a strong coherent field at frequency ωωω and a perturbative BSV field at 2ω2ω2ω, the even-harmonic response is approximately linear in the BSV quadrature, leading to non-classical multimode Gaussian entanglement in the harmonic field. We show that this state can be described as a distributed collective squeezed mode over the even-harmonic manifold, and characterize its covariance matrix, entanglement structure, and quantum teleportation fidelity as an operational benchmark. Our results highlight the potential of non-classically driven HHG as a platform for engineering Gaussian and non-Gaussian states of light in the extreme ultraviolet regime.
The extreme light-matter interaction has brought unique tools for the subfemtosecond control of electron dynamics [1] and ultra-fast spectroscopy [2]. Until recently, the strong-field regime was accessible only with coherent states of light, which can be well described by classical electric fields when many photons are present (Fig. 1a). With the use of intense states of non-classical light, this situation has changed. New opportunities emerge with bright squeezed vacuum (BSV), which can be generated from optical parametric amplification of quantum vacuum fluctuations. Unlike classical light, BSV is a quantum superposition of coherent states with an amplitudes spanning a range from zero to very high values, up to ~1 TW/cm2[3]. BSV has a zero mean electric field and the variance of the electric field oscillates at the double carrier frequency (Fig. 1a). How such a non-classical electric field can affect the dynamics of photoemitted electrons was theoretically demonstrated recently [4]. Furthermore, the photon-number distribution of BSV has a very long tail in contrast to coherent light. These photon-number distributions can be imprinted onto the photon statistics of optical harmonics [3] and the statistics of electrons [5].
For decades, most research of high harmonic generation (HHG) considered matter as quantum but light as classical. Recently, HHG driven by quantum states of light such as bright squeezed vacuum was predicted to reach beyond the classical HHG cutoff. Moreover, in squeezed coherent illumination, it was shown that the underlying dynamics are significantly modified by the photon statistics effective force. Here we show that HHG driven by quantum light results in quantum high harmonics. We derive a formula for the quantum state of the high harmonics, when driven by arbitrary quantum light states, and then explore specific cases of experimental relevance. Specifically, for a moderately squeezed pump, HHG driven by squeezed coherent light results in squeezed high harmonics. Harmonic squeezing is optimized by syncing ionization times with the pump's squeezing phase. Beyond this regime, as pump squeezing is increased, the harmonics initially acquire squeezed thermal photon statistics, and then occupy an intricate quantum state which strongly depends on the semiclassical nonlinear response function of the interacting system. Our results pave the way for generation of squeezed extreme-ultraviolet ultrashort pulses, and more generally, quantum frequency conversion into previously inaccessible spectral ranges, which may enable ultrasensitive attosecond metrology. Published by the American Physical Society 2024
Multi-photon processes are extremely important in optics. Optical harmonics generation, multi-photon absorption, ionization, polymerization or spectroscopy are widely used in practical applications. The efficiency of these processes depends on many factors, one of them being the statistics of the incident light. Indeed, the rate of an n-photon effect scales as the nth-order autocorrelation function g(n)of the incident light [1]. Therefore light sources with high correlation functions can enhance the efficiency of such effects by several orders in magnitude compared to coherent light with the same wavelength, pulse duration and energy per pulse. Here we demonstrate this enhancement in the generation of optical harmonics from bright squeezed vacuum (BSV), which can have thermal (g(n)=n!) or superbunched (g(n)=(2n-1)!!) statistics depending on the spectral filtering [2].