Superpositions of coherent light states are vital for quantum technologies. However, restrictions in existing state preparation and characterization schemes, in combination with decoherence effects, prevent their intensity enhancement and implementation in nonlinear optics. Here, by developing a decoherence-free approach, we generate intense femtosecond-duration infrared coherent state superpositions (CSSs) with a mean photon number orders of magnitude higher than the existing CSS sources. We utilize them in nonlinear optics to drive the second harmonic generation process in an optical crystal. We experimentally and theoretically show that the nonclassical nature of the intense infrared CSS is imprinted in the second-order autocorrelation traces. Additionally, theoretical analysis shows that the quantum features of the infrared CSS are also present in the generated second harmonic. The findings introduce the optical CSS into the realm of nonlinear quantum optics, opening up new paths in quantum information science and quantum light engineering by creating nonclassical light states in various spectral regions via nonlinear up-conversion processes.
Superpositions of coherent light states are vital for quantum technologies. However, restrictions in existing state preparation and characterization schemes, in combination with decoherence effects, prevent their intensity enhancement and implementation in nonlinear optics. Here, by developing a decoherence-free approach, we generate intense femtosecond-duration infrared coherent state superpositions (CSSs) with a mean photon number orders of magnitude higher than the existing CSS sources. We utilize them in nonlinear optics to drive the second harmonic generation process in an optical crystal. We experimentally and theoretically show that the nonclassical nature of the intense infrared CSS is imprinted in the second-order autocorrelation traces. Additionally, theoretical analysis shows that the quantum features of the infrared CSS are also present in the generated second harmonic. The findings introduce the optical CSS into the realm of nonlinear quantum optics, opening up new paths in quantum information science and quantum light engineering by creating nonclassical light states in various spectral regions via nonlinear up-conversion processes.
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
The effect of the quantum properties of light on nonlinear processes has been well studied theoretically. It has been shown that the efficiency of n-photon nonlinear processes in many cases scales as the normalized n-th order correlation function. For light with high intensity correlation function, the efficiency of the n-th harmonic generation will be considerably higher than for coherent light. The experimental observation of this effect remained difficult until recently, because of the absence of bright sources with strong and fast intensity fluctuations. For the experimental demonstration of statistical effects in optical harmonic generation we use as a pump the radiation of high-gain parametric down conversion. Such light shows quantum properties (e.g. quadrature or two-mode squeezing) and has large number of photons in one mode. The normalized n-th order correlation function for this light is (2n - 1)!!, which makes it more attractive for nonlinear processes than both coherent and thermal light. For the generation of optical harmonics we used broadband parametric down conversion around frequency-degeneracy (1600 nm) produced in 1cm BBO crystal from Ti:Sapphire laser (800 nm, 1.6ps, 5kHz, 3W mean intensity). Due to spectral filtering and post-selection technique we could vary the statistics of light from coherent to super-bunched, which allowed us to demonstrate the efficiency enhancement for second-, third-, and fourth-harmonic generation. The obtained experimental results show a good agreement with the theory.
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.
We present a theoretical demonstration on the generation of entangled coherent states and of coherent state superpositions, with photon numbers and frequencies orders of magnitude higher than those provided by the current technology. This is achieved by utilizing a quantum mechanical multimode description of the single- and two-color intense laser field driven process of high harmonic generation in atoms. It is found that all field modes involved in the high harmonic generation process are entangled, and upon performing a quantum operation, lead to the generation of high photon number optical cat states spanning from the far infrared to the extreme ultraviolet spectral region. This provides direct insights into the quantum mechanical properties of the optical field in the intense laser matter interaction. Finally, these states can be considered as a new resource for fundamental tests of quantum theory, quantum information processing, or sensing with nonclassical states of light.
Nonlinear dynamics provide an indispensable resource for creating quantum states of light, as well as other bosonic systems. Seminal work using second- and third-order nonlinear optical crystals, cavity quantum electrodynamics, and superconducting circuits, have enabled generating squeezed states, as well as various non-Gaussian quantum states (e.g., single photons, cat states) at both infrared and microwave frequencies. Nevertheless, it remains challenging to generate quantum states of light in broad portions of the electromagnetic spectrum: for example, at terahertz frequencies and at ultraviolet and X-ray frequencies. In this Perspective, I discuss a variety of emerging material platforms, as well as emerging theoretical and experimental tools, which enable overcoming these challenges. The main argument of this Perspective is that advances in driving nonlinear dynamics of material excitations, will enable generating quantum states of these material excitations as well as quantum states of light at new frequency ranges. I will further argue that in order to realize much of the promise of this nascent field, there is a need for innovation in the laser systems used to drive these nonlinear dynamics: specifically, innovations in realizing high-power laser sources that have very low noise, having quantum statistics similar to coherent states of light which describe lower intensity laser systems. I will highlight some experimental and theoretical work, in understanding quantum noise dynamics in complex laser systems, that can address these challenges.
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.