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arXiv:2310.15030 · Physical Review Letters

Entanglement and Squeezing of the Optical Field Modes in High Harmonic Generation

Philipp Stammer, Javier Rivera-Dean, Andrew Maxwell, Theocharis Lamprou, Javier Argüello-Luengo, P. Tzallas, Marcelo F. Ciappina, Maciej Lewenstein

Published Apr 5, 2024• 60 citations
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Abstract

Squeezed optical fields are a powerful resource for a variety of investigations in basic research and technology. However, the generation of intense squeezed light is challenging. Here, we show that intense squeezed light can be produced using strongly laser driven atoms and the so far unrelated process of high harmonic generation. We demonstrate that when the intensity of the driving field significantly depletes the ground state of the atoms, leading to dipole moment correlations, the quantum state of the driving field and the generated high harmonics are entangled and squeezed. Furthermore, we analyze how the resulting quadrature squeezing of the fundamental laser mode after the interaction can be controlled. The findings open the way for the generation of high intensity squeezed light states for a wide range of applications.

DOI
10.1103/physrevlett.132.143603

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•Oct 3, 2021•2 citations
Squeezed optical fields are a powerful resource for a variety of investigations in basic research and technology. However, the generation of intense squeezed light is challenging. Here, we show that intense squeezed light can be produced using strongly laser driven atoms and the so far unrelated process of high harmonic generation. We demonstrate that when the intensity of the driving field significantly depletes the ground state of the atoms, leading to dipole moment correlations, the quantum state of the driving field and the generated high harmonics are entangled and squeezed. Furthermore, we analyze how the resulting quadrature squeezing of the fundamental laser mode after the interaction can be controlled. The findings open the way for the generation of high intensity squeezed light states for a wide range of applications.
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.
High-harmonic generation (HHG) has recently emerged as a promising method for generating nonclassical states of light with frequencies spanning from the infrared up to the extreme ultraviolet regime. In this work, we theoretically investigate the generation of squeezed states of light through HHG processes in atomic systems that were initially driven to their first excited state. Our study reveals significant single-mode squeezing in both the driving field and low-order harmonic modes. Additionally, we characterize two-mode squeezing features in the generated states, both between fundamental and harmonic modes, and among the harmonic modes themselves. Using these correlations, we demonstrate the generation of optical Schr\"odinger kitten states through heralding measurements, specifically via photon subtraction in one of the modes influenced by two-mode squeezing.
High-harmonic generation is a light up-conversion process occurring in a strong laser field, leading to coherent bursts of extreme ultrashort broadband radiation [1]. As a new perspective, we propose that ultrafast strong-field electronic or photonic processes such as high-harmonic generation can potentially generate non-classical states of light well before the decoherence of the system occurs [2, 3]. This could address fundamental challenges in quantum technology such as scalability, decoherence or the generation of massively entangled states [4]. Here, we report experimental evidence of the non-classical nature of the harmonic emission in several semiconductors excited by a femtosecond infrared laser. By investigating single- and double beam intensity cross-correlation [5], we measure characteristic, non-classical features in the single photon statistics. We observe two-mode squeezing in the generated harmonic radiation, which depends on the laser intensity that governs the transition from Super-Poissonian to Poissonian photon statistics. The measured violation of the Cauchy-Schwarz inequality realizes a direct test of multipartite entanglement in high-harmonic generation [6]. This result is supported by the theory of multimodal detection and the Hamiltonian from which the effective squeezing modes of the harmonics can be derived [7, 8]. With this work, we show experimentally that high-harmonic generation is a new quantum bosonic platform that intrinsically produces non-classical states of light with unique features such as multipartite broadband entanglement or multimode squeezing. The source operates at room temperature using standard semiconductors and a standard commercial fiber laser, opening new routes for the quantum industry, such as optical quantum computing, communication and imaging.
High-harmonic generation is a light up-conversion process occurring in a strong laser field, leading to coherent bursts of extreme ultrashort broadband radiation [Lewenstein , Phys. Rev. A , 2117 (1994)]. As a new perspective, we propose that ultrafast strong-field electronic or photonic processes such as high-harmonic generation can potentially generate nonclassical states of light well before the decoherence of the system occurs [Gorlach , Nat. Commun. , 4598 (2020); Stammer ., Phys. Rev. Lett. , 123603 (2022)]. This could address fundamental challenges in quantum technology such as scalability, decoherence, or the generation of massively entangled states [Lewenstein , Luca Argenti Michael Chini, 27 (2024)]. Here, we report experimental evidence of the nonclassical nature of the harmonic emission in several semiconductors excited by a femtosecond infrared laser. By investigating single- and double-beam intensity cross-correlation [Loudon, Rep. Prog. Phys. , 913 (1980)], we measure characteristic nonclassical features in the single-photon statistics. We observe two-mode squeezing in the generated harmonic radiation, which depends on the laser intensity that governs the transition from super-Poissonian to Poissonian photon statistics. The measured violation of the Cauchy-Schwarz inequality realizes a direct test of multipartite entanglement in high-harmonic generation [Wasak, Phys. Rev. A , 033616 (2014)]. This result is supported by the theory of multimodal detection and the Hamiltonian from which the effective squeezing modes of the harmonics can be derived [Gonoskov , Phys. Rev. B , 125110 (2024); Christ New J. Phys. , 033027 (2011)]. With this work, we show experimentally that high-harmonic generation is a new quantum bosonic platform that intrinsically produces nonclassical states of light with unique features such as multipartite broadband entanglement or multimode squeezing. The source operates at room temperature, using standard semiconductors and a standard commercial fiber laser, opening up new routes for the quantum industry, such as optical quantum computing, communication, and imaging. Published by the American Physical Society 2024
We investigate the generation of higher-order harmonics from a quantum optics perspective via the interaction of a semiconductor with a coherent pump field focusing on the regime where strong-field intraband excitations dominate. The related Schrödinger equation for the system is solved approximately and the classical and quantum characteristics of the fundamental light mode as well as the higher frequency modes are analyzed. We find intricate but sufficiently mild modifications of the fundamental mode and coherent displacements depending on the position quadrature component of the driving laser field for the harmonic modes within our approximations due to the intricate induced nonlinear interactions. Similar to high-harmonic generation in atoms, all radiation field modes are entangled, allowing for potential novel protocols for quantum information processing with high photon numbers over a large range of frequencies.
Recently we have demonstrated the quantum nature of light in strongly laser driven atoms, and we have shown how the process of high harmonic generation can be used for the creation of highly non-classical light states, in particular superpositions of two coherent states, i.e., optical Schr\{o}dinger states [M. Lewenstein et al., Generation of optical Schr\odinger cat states in intense laser-matter interactions, Nat. Phys., 17 1104-1108 (2021)]. Here, we investigate the quantum optical description of the interaction, incorporating many atoms and the back-action of the high harmonic generation or above threshold ionization processes on the coherent state of the driving laser field. We show how the conditioning on high harmonic generation and above threshold ionization can lead to non-classical light states, and we discuss the key parameters that can be used for controlling and characterizing the non-classical states obtained after high harmonic generation. The theoretical results have been experimentally confirmed by demonstrating how the obtained coherent state superposition changes from an optical to kitten state by changing the number of atoms participating in the high harmonic generation process. Additionally, we experimentally verify the applicability of the approach for generating high photon number non-classical light states. This is shown by demonstrating the generation of a 9--photon optical state which, to our knowledge, is the highest photon number optical state experimentally reported. Our findings anticipate the development of new methods that naturally lead to the creation of high photon number controllable coherent state superpositions, advancing investigations in quantum technology.