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Optics Letters

Third-harmonic generation modulation achieved through ground-state depletion

Szu-Yu Chen, Hao-Hao Wu

Published Jan 8, 2019• 1 citation
Publisher

Abstract

Without real-state transition, third-harmonic generation (THG) cannot be modulated simply by fluorescence-based methods. However, utilizing the absorption-enhancement property of THG, the modulation of THG intensity has been demonstrated through ground-state depletion (GSD) in this Letter. By suppressing the absorption of materials with GSD, the THG intensity can be reduced due to a decreasing of absorption enhancement. The ability to modulate THG intensity can benefit from applying super-resolution techniques to THG microscopy.

DOI
10.1364/ol.44.000315

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Without real-state transition, third-harmonic generation (THG) cannot be modulated simply by fluorescence-based methods. However, utilizing the absorption-enhancement property of THG, the modulation of THG intensity has been demonstrated through ground-state depletion (GSD) in this Letter. By suppressing the absorption of materials with GSD, the THG intensity can be reduced due to a decreasing of absorption enhancement. The ability to modulate THG intensity can benefit from applying super-resolution techniques to THG microscopy.
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.
In Part I [1], we presented a quantum theory of third-harmonic generation (THG) under two-photon absorption in a two-level atomic medium. We studied the time evolution of the third-harmonic field and its coherence properties by neglecting the depletion of the pump power. In this paper we extend the theory by taking the depletion of pump power into account. The density matrix for the third-harmonic field is derived. The study of the growth rate of the density matrix in time shows the quantum mechanical effects more clearly. The effects of detuning in the two-photon interactions and atomic motion are pointed out. The results are compared with the earlier results and differences are brought out.
A numerical investigation is made of third harmonic generation (THG) under conditions of two-photon resonance between the fundamental frequency and a selected transition in the atoms of a medium. It is shown that under conditions of coherent interaction between the pump pulse and the medium, a THG efficiency of ∼20% or higher may be achieved. In this case, THG in the form of high-power ultrashort pulses may be obtained. It is shown that experimental observation of similar effects in specific media should not present particular difficulties.