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Applied Sciences

Second Harmonic Revisited: An Analytic Quantum Approach

Giovanni Chesi, Matteo M. Wauters, Nadir Fasola, Alessia Allevi, Maria Bondani

Published Apr 24, 2019• 10 citations
Publisher

Abstract

We address the second-harmonic generation process in a quantum frame. Starting with a perturbative approach, we show that it is possible to achieve a number of analytic results, ranging from the up-conversion probability to the statistical properties of the generated light. In particular, the moments and the correlations of the photon-number distribution of the second-harmonic light generated by any initial state are retrieved. When possible, a comparison with the results achieved with the classical regime is successfully provided. The nonclassicality of some benchmark states is investigated by inspecting the corresponding autocorrelation function.

DOI
10.3390/app9081690

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We address the second-harmonic generation process in a quantum frame. Starting with a perturbative approach, we show that it is possible to achieve a number of analytic results, ranging from the up-conversion probability to the statistical properties of the generated light. In particular, the moments and the correlations of the photon-number distribution of the second-harmonic light generated by any initial state are retrieved. When possible, a comparison with the results achieved with the classical regime is successfully provided. The nonclassicality of some benchmark states is investigated by inspecting the corresponding autocorrelation function.
In this review, we compare different descriptions of photon-number statistics in harmonic generation processes within quantum, classical and semiclassical approaches. First, we study the exact quantum evolution of the harmonic generation by applying numerical methods including those of Hamiltonian diagonalization and global characteristics. We show explicitly that the harmonic generations can indeed serve as a source of nonclassical light. Then, we demonstrate that the quasi-stationary sub-Poissonian light can be generated in these quantum processes under conditions corresponding to the so-called no-energy-transfer regime known in classical nonlinear optics. By applying method of classical trajectories, we demonstrate that the analytical predictions of the Fano factors are in good agreement with the quantum results. On comparing second and higher harmonic generations in the no-energy-transfer regime, we show that the highest noise reduction is achieved in third-harmonic generation with the Fano-factor of the third harmonic equal to 13/16.
Photon number and phase fluctuations and correlations in the second harmonic generation are discussed. The new Pegg-Barnett Hermitian phase formalism is used to deal with the phase properties of the field. The method of numerical diagonalization of the interaction Hamiltonian is applied to find the state evolution and, consequently, the number and phase quantum fluctuations. It is shown that the joint phase probability distribution evolves into a multi-peak structure indicating clearly the transition from the second harmonic to the down-conversion regime, and back. The evolution of all relevant quantities is illustrated graphically, and their dependence on the mean number of photons of the initial field is shown explicitly. The number-phase uncertainty product for the fundamental mode is plotted making evident the abrupt transition from the low to the high level of quantum fluctuations.
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 quantum statistical equations for the field produced in the process of second-harmonic generation (SHG) are expressed, based on a method proposed for four-wave mixing.1 We start from the following assumptions: 1) the field absorption in the nonlinear medium may be neglected; 2) the amplitude of the fundamental field is much greater than that of the SH field; 3) the Wigner function associated with the density operator of the field depends significantly only on the variables of the SH field. The coefficients of the Fokker–Planck equation thus obtained depend on the Laplace transforms of the correlation functions of the atomic polarization operator. The moments of the Wigner function2 are related to the moments of the SH field photon number; consequently, we impose the condition for sub-Poissonian photon-statistics and derive the corresponding relationships satisfied by the atomic correlation functions. A numerical interpretation is given.
Nonlinear optical effects where quantum mechanical predictions are at variance with the results of classical calculations are studied. Certain initial conditions, those of unstable equilibrium or those that lead to unstable equilibrium, classically, give rise to an aperiodicity in the intensity of the emitted radiation. One example of such a system is second-harmonic generation, which is studied in detail because of the potential amenability of the aperiodicity to experimental observation. Numerical and analytic predictions for the evolution of the intensity and photon statistics of the second harmonic light are presented. The photon statistics of the second harmonic light are predicted to undergo a sharp transition following the first maximum of the intensity.