Third harmonic generation (THG) is known being able to be enhanced though real-state absorption. Suppressing absorption through ground-state depletion, the THG intensity can be modulated for the purpose of resolution improvement of THG microscopy.
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.
We explore the possibility of using an active doubly resonant microtoroid resonator to produce high-efficiency third-harmonic generation (THG) by exploiting optical third-order nonlinearity. In a microresonator, the active fundamental mode is coherently driven with a continuous-wave input laser at the telecommunication wavelength (1550 nm), and then, the visible THG signal (517 nm) is monitored via an individual bus waveguide. We thoroughly compare our results with those obtained from the conventional passive (i.e., loss) microtoroid resonator by a systematic analysis and detailed numerical simulations based on the Heisenberg-Langevin equations of motion. It is shown that the achievable THG spectrum features an ultralow critical input power. The THG power transmission can be significantly enhanced by about three orders of magnitude at a low input power of 0.1 μW as compared with the obtained results in the passive microtoroid resonator THG system. Moreover, the THG efficiency can reach up to 100% with optical critical input power as low as a few microwatts. In turn, the analytical expressions of the critical intracavity intensity of the light in the microcavity, the critical input pump power, and the maximum THG efficiency are obtained. The enhanced THG power transmission and high conversion efficiency are attributed to a gain-induced loss compensation in the microtoroid resonator, reducing the effective loss felt by the resonator photons. With state-of-the art technologies in the field of solid-state resonators, including but not limited to microtoroids, the proposed THG scheme is experimentally realizable.