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.
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.
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].
The rate of an n-photon effect generally scales as the nth order autocorrelation function of the incident light, which is high for light with strong photon-number fluctuations. Therefore, "noisy" light sources are much more efficient for multiphoton effects than coherent sources with the same mean power, pulse duration, and repetition rate. Here we generate optical harmonics of the order of 2-4 from a bright squeezed vacuum, a state of light consisting of only quantum noise with no coherent component. We observe up to 2 orders of magnitude enhancement in the generation of optical harmonics due to ultrafast photon-number fluctuations. This feature is especially important for the nonlinear optics of fragile structures, where the use of a noisy pump can considerably increase the effect without overcoming the damage threshold.
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
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.