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Physical Review A

Spectrum of second-harmonic generation for multimode fields

Y. B. Band, Donald F. Heller, Jay R. Ackerhalt, Jerzy S. Krasiński

Published Aug 1, 1990• 10 citations
Publisher

Abstract

We calculate the spectrum of second-harmonic generation (SHG) for multimode input fields. We show that SHG cannot be described as the degenerate limit of sum-frequency generation (SFG) for multimode fields, because the dynamical equations describing SFG do not properly account for this degeneracy. We consider SHG for amplitude-modulated as well as frequency-modulated fundamental fields. The bandwidth of the second harmonic generated from an amplitude-modulated fundamental field depends on the fundamental input intensity and the conversion strength of the nonlinear medium. Additional frequencies that are not contained in the set of frequencies ${\mathrm{\ensuremath{\omega}}}_{1\mathit{i}}$+${\mathrm{\ensuremath{\omega}}}_{1\mathit{j}}$ will be created at intermediate conversion strengths. However, the growth of the spectral bandwidth is much less pronounced than in SFG. For very high conversion, the spectrum of the second harmonic narrows with increased conversion strength. For frequency-modulated input fields, the second-harmonic spectrum is independent of both the fundamental input intensity and the conversion strength.

DOI
10.1103/physreva.42.1515

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We calculate the spectrum of second-harmonic generation (SHG) for multimode input fields. We show that SHG cannot be described as the degenerate limit of sum-frequency generation (SFG) for multimode fields, because the dynamical equations describing SFG do not properly account for this degeneracy. We consider SHG for amplitude-modulated as well as frequency-modulated fundamental fields. The bandwidth of the second harmonic generated from an amplitude-modulated fundamental field depends on the fundamental input intensity and the conversion strength of the nonlinear medium. Additional frequencies that are not contained in the set of frequencies \ensuremathω1i{\mathrm{\ensuremath{\omega}}}_{1\mathit{i}}\ensuremathω1i​+\ensuremathω1j{\mathrm{\ensuremath{\omega}}}_{1\mathit{j}}\ensuremathω1j​ will be created at intermediate conversion strengths. However, the growth of the spectral bandwidth is much less pronounced than in SFG. For very high conversion, the spectrum of the second harmonic narrows with increased conversion strength. For frequency-modulated input fields, the second-harmonic spectrum is independent of both the fundamental input intensity and the conversion strength.
The theory of three wave mixing was formulated in a classic paper by Armstrong, Bloembergen, Ducuing, and Pershan over 25 years ago.1 A theoretical description of three wave mixing for multimode time-dependent input fields (as opposed to cw single frequency time independent input fields) has recently been presented.2 Analytic solutions were developed for die time-dependent intensities of the output fields. These solutions differ dramatically from those for single-mode fields. New frequencies in the sum-frequency output spectrum and in the input-field output spectrum are created and grow in magnitude as the input intensities are increased. The output spectrum broadens under conditions of strong nonlinear coupling, ultimately reaching the phasematched bandwidth limit. Here, we review the results presented in Ref. 2 for sum frequency generation (SFG) and explicidy compare these results with those for second harmonic generation (SHG). We show that SHG cannot be described as a limit of the SFG formalism for multimode fields. The SFG formulation for the interaction of photons close to frequency ω1 with photons close to frequency ω2 producing photons close to frequency ω 3= ω 1+ ω 2 does not allow ω1(ω2) photons to interact with each other to produce photons close to frequency 2ω1(2ω2). This self interaction is crucial for SHG and must be incorporated. Therefore, a separate formulation is used to describe SHG with multimode input fields.
We analyze the dynamics of sum-frequency generation (SFG) and difference-frequency generation (DFG) for broadband input fields. We demonstrate that amplitude modulation of the input fields significantly affects conversion efficiency of SFG and DFG, but frequency modulation does not affect conversion efficiency. Analytic results for SFG and DFG output-field intensities are thereby available for arbitrary fields. Self- and cross-phase modulation can affect the dynamics in the limit of very high field strengths, but these effects are of higher nonlinearity and therefore usually negligible. The quantum efficiency of DFG is shown to be generally higher than SFG, but the energy efficiency is much lower if the difference frequency is significantly less than the input frequencies. Optimal SFG quantum conversion efficiency for such systems approaches that of second-harmonic generation only if the quantum fluence (total number of photons) in the two input beams are equal. Optimal DFG quantum conversion efficiency occurs when the number of photons of frequency ${\mathrm{\ensuremath{\omega}}}_{2}$ is small yet sufficient for significant stimulation. A recently developed method for obtaining efficient SFG for multimode input fields is theoretically analyzed. The method involves using an arrangement with two or more nonlinear mixing crystals with a time-delay line situated between the crystals that delays one of the fundamental fields relative to the other. The efficiency in the second crystal depends on the cross-correlation function of the two fundamental fields upon leaving the first nonlinear crystal. The time-delay method is not effective for multimode DFG.
We calculate the spectrum of third-harmonic generation (THG) for multimode fundamental input fields. We consider input fields from (1) a laser with gain on several cavity modes, (2) pulses with short temporal duration, and (3) frequency-modulated input fields. The effects of phase modulation in the nonlinear medium on the spectrum of the THG field are considered. Using the estimates by Miles and Harris [IEEE J. Quantum Electron. QE-9, 470 (1973)] for the nonlinear susceptibilities ${\mathrm{\ensuremath{\chi}}}^{(3)}$(-3\ensuremath{\omega};\ensuremath{\omega},\ensuremath{\omega},\ensuremath{\omega}) and ${\mathrm{\ensuremath{\chi}}}^{(3)}$(-\ensuremath{\omega};\ensuremath{\omega},-\ensuremath{\omega},\ensuremath{\omega}) in alkali-metal vapors, we find that phase modulation can profoundly affect the efficiency and the spectrum of the THG. Generally, the self-phase modulation of the fundamental will tend to reduce the phase matching of an intense fundamental field and the third harmonic and thereby lower the conversion efficiency. New frequencies not contained in the set of frequencies ${\mathrm{\ensuremath{\omega}}}_{1\mathit{i}}$+${\mathrm{\ensuremath{\omega}}}_{1\mathit{j}}$+${\mathrm{\ensuremath{\omega}}}_{1\mathit{k}}$, where {${\mathrm{\ensuremath{\omega}}}_{1\mathit{i}}$} are frequencies in the fundamental laser spectrum, are created even at relatively low conversion due to phase modulation. Effects of cross phase modulation are also studied.
The second harmonic generation (SHG) process is investigated theoretically using the quantum mechanics method of coherent control. Based on the extremum conditions for the SHG intensity at the center frequency, a Fresnel-inspired binary phase shaping scheme is proposed for tailoring the fundamental pulse. The SHG spectrum can be compressed into a narrowband signal with lower background by modulating the relative phases between the frequency components within the fundamental pulse, inducing constructive interference at the center frequency and destructive interference elsewhere. Multipeak second harmonic signals can also be obtained by properly modulating various interference pathways. These results have potential applications in high resolution nonlinear spectroscopy, microscopy, and information coding.
In this paper we study the quantum-theoretical description of second-harmonic generation (SHG) in optical waveguides. The interaction operator of three waveguide modes, by means of which the equations for spatially slowly varying annihilation and creation operators of the field strength amplitudes can be determined, is obtained by using the mode fields in the waveguides. The equations for spatially slowly varying annihilation and creation operators of the field are derived. We seek approximate solutions of the operator equations, and obtain the conversion efficiency of SHG.
We consider the process of second-harmonic generation (SHG) in a cavity that is resonant for both the fundamental- and second-harmonic modes. It has been previously shown that such a system displays a phase instability leading to self-pulsing and that one gets important intensity squeezing on both the fundamental- and second-harmonic mode for pump intensities close to but below, this instability threshold. Such a squeezing has been recently observed. We have analytically calculated the intensity-noise spectrum of the frequency-doubled field above such an instability threshold, using a semiclassical input-output technique for the treatment of quantum fluctuations.1 Such a method, introduced to deal with fluctuations around a stable solution, has been generalized to the self-pulsing domain. As expected, the instability brings excess noise to the output beams, especially around the zero-frequency, the self-oscillation frequency, and its harmonics. Remarkably, some regions exist in which where the noise increase is small; squeezing still occurs in this frequency range far in the instability domain.