We have studied experimentally the intensity characteristic of the fifth-order harmonic radiation produced by two coherent femtosecond laser pulses with a changeable relative phase.The intensities of the harmonic generation are found to increase with the coherent degree.The maximum intensity of harmonics exhibits an asymmetric characteristic with respect to the point where the two components are superposed completely.This fact verifies the influence of deformation of the merged beam on the harmonic generation.Meanwhile,we have carried out some fundamental experiments,based on the theory of stimulated emission.
We have studied experimentally the intensity characteristic of the fifth-order harmonic radiation produced by two coherent femtosecond laser pulses with a changeable relative phase.The intensities of the harmonic generation are found to increase with the coherent degree.The maximum intensity of harmonics exhibits an asymmetric characteristic with respect to the point where the two components are superposed completely.This fact verifies the influence of deformation of the merged beam on the harmonic generation.Meanwhile,we have carried out some fundamental experiments,based on the theory of stimulated emission.
This work examines the use of higher order multiphoton resonances in higher harmonic generation together with judicious exploitation of coherent interaction properties to achieve efficient harmonic generation. A detailed experimental study on third harmonic generation in two photon resonant coherent interaction and a theoretical study on four photon resonant coherent interaction have been conducted. Two photon resonant coheren propagation in lithium vapor (2S-4S and 2S-3D interaction) has been studied in detail as a function of phase and delay of the interacting pulse sequence. Under coherent lossless propagation of 90 phase shifted pulse pair, third harmonic generation is enhanced. A maximum energy conversion efficiency of 1% was measured experimentally. This experiment shows that phase correlated pulse sequence can be used to control multiphoton coherent resonant effects. A larger two photon resonant enhancement does not result in more efficient harmonic generation, in agreement with the theoretical prediction. An accurate (to at least 0.5 A°) measurement of intensity dependent Stark shift has been done with the newly developed "interferometric wavemeter." Stark shifts as big as several pulse bandwidths (of picosecond pulses) result in a poor tuning of multiphoton resonance and become a limiting factor of resonant harmonic generation. A complete theory has been developed for harmonic generation in a four photon resonant coherent interaction. A numerical application of the theory to the Hg atom successfully interprets the experimental observations in terms of the phase dependent stimulated Raman scattering. With the intensity required for four photon resonant transition, the calculation predicts a dramatic Stark shift effect which completely destroys the resonance condition. This model provides a basis for the development of future schemes for efficient higher order coherent upconversion.
The four-wave mixing produced with two ultrashort phase-locked !-3! laser pulses propagating coherently in a two-level system in the infrared spectral region is shown to depend on the pulses relative phase. The Maxwell-Bloch equations are solved beyond the rotating-wave approximation to account for field frequencies which are largely detuned from the atomic resonance. The relative phase dominating the efficiency of the coupling to the 5! anti-Stokes Raman component is determined by sign of the total ac Stark shift induced in the system, in such a way that the phase influence disappears precisely where the ac Stark effect due to both pulses is compensated. This fundamental quantum interference effect can be the basis for nonlinear ultrafast optical spectroscopy techniques. Phenomena arising from the coherent control of nonlinear interactions are of importance in fields as diverse as optoelectronics and materials research, in high harmonic generation, in photoionization or molecular dissociation, and in biological applications such as spectroscopy and imaging, among others [1, 2, 3, 4, 5, 6, 7]. Optical quantum coherent control is based on the fact that the phases of interfering transition amplitudes in light-matter interactions can be controlled through the optical phase of coherent light sources that drive the interaction, in such a way that the transition rates to final states and the dynamics at various stages of the process can be modified [1]. In a recent paper [8], a theoretical investigation on the quantum coherent control of the optical transient four-wave mixing of two intense phase-locked femtosecond laser pulses of central angular frequencies ω and 3ω propagating in a two-level atom (TLA) was reported. It was shown how the nonlinear (χ (3) ) coupling to the antiStokes Raman field at frequency 5ω depends critically on the initial relative phase φ of the propagating pulses. In Ref. [8], the study was centered to intense pulses in the visible and ultraviolet spectral regions, with frequencies at resonance or lower than the atomic transition. The phenomena observed in [8], however, can be scaled to various laser and material parameters. In the infrared spectral range, for instance, experiments on ultrafast molecular dynamics are frequently performed by help of twocolor pump probe nonlinear spectroscopy techniques. In this type of studies, due to the high intensities inherent to ultrashort (subpicosecond) pulses, nonlinear effects such as stimulated Raman processes may become important and are often utilized as a complementary tool to gain information [9]. In this Letter, we address the conditions for quantum coherent control of transient four-wave mixing interactions with two phase-locked ω-3ω femtosecond laser pulses in the mid-IR spectral region. Our purpose is to reveal the basic physics for a strict two-level medium and to this end the Maxwell-Bloch TLA will be considered. We will study pulses with a duration of 300 fs (with a w 5w
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 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.
It is theoretically and experimentally demonstrated that optical second-harmonic generation (SHG) is possible to be observed in atomic media irradiated with an intense laser pulse. The SHG is induced by a static electric field spontaneously generated in the interaction, and any special condition is not required for the SHG. The experiment to observe the SHG has been made using atomic sodium vapor and a mode-locked Nd-doped yttrium aluminum garnet laser system (pulse duration, 28 psec; output energy \ensuremath{\lesssim}50 mJ). The second harmonic (SH) polarization, spatial beam pattern, and dependences of SH signal on the sodium density and on the fundamental intensity have been examined. The experimental results agree well with the theoretical predictions and numerical results.