We investigate generation of the third harmonic (TH; λ = 355 nm) signal by two-colour excitation (λ = 1064 nm and its second harmonic, λ = 532 nm) in argon gas, with emphasis on the influence of relative phases and intensities of the two-colour pump on the third-order nonlinear frequency conversion process. Perturbative nonlinear optics predicts that the TH signal will oscillate periodically with the relative phases of the two-colour driving laser fields due to the interference of TH signals from a direct third-harmonic-generation (THG) channel and a four-wave mixing (FWM) channel. For the first time, we show unequivocal experimental evidence of this effect. A modulation level as high as 0.35 is achieved by waveform control of the two-colour laser field. The modulation also offers a promising way to retrieve the relative phase value of the two-colour laser field.
We investigate generation of the third harmonic (TH; λ = 355 nm) signal by two-colour excitation (λ = 1064 nm and its second harmonic, λ = 532 nm) in argon gas, with emphasis on the influence of relative phases and intensities of the two-colour pump on the third-order nonlinear frequency conversion process. Perturbative nonlinear optics predicts that the TH signal will oscillate periodically with the relative phases of the two-colour driving laser fields due to the interference of TH signals from a direct third-harmonic-generation (THG) channel and a four-wave mixing (FWM) channel. For the first time, we show unequivocal experimental evidence of this effect. A modulation level as high as 0.35 is achieved by waveform control of the two-colour laser field. The modulation also offers a promising way to retrieve the relative phase value of the two-colour laser field.
We report here experimental results of perturbative nonlinear optical wave-mixing processes in the extreme ultraviolet region by using two-color and three-color laser fields. Besides the usual odd-harmonic spectrum of high harmonic generation, new spectral components are observed when multiple incommensurate lasers (one driving plus one or two control field) interact with neutral krypton gas. To demonstrate the wave-mixing process underlying such an observation, we first couple the driving field with either the signal or the idler field of an optical parametric amplifier in the gaseous ensemble to generate certain mixing frequencies. The two control fields are then simultaneously combined with the driving field to produce broad and distinguishable mixing peaks that clearly reveal the contribution of each control laser. Finally, the variation of the intensity of the mixing waves with the intensity of each control field, the gas density, and the relative focus position is examined for signatures of phase-matched generation of the mixing fields in this spectral region.
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 examine the excitation dynamics of a model atom excited by a two-colour laser field. Here the two colours or frequencies are the fundamental and its third harmonic. The atomic model consists of two bound states which are near-resonantly coupled by a three-photon excitation by the fundamental and a one-photon excitation by the third harmonic, and a structureless continuum. We investigate how the laser parameters (intensity and frequency) and the relative phase between the two colours affects the degree of phase modulation in the ionization signal. We compare our findings from this simple model atom with those from more realistic atomic models by carrying out numerical integration of the hydrogenic Schrodinger equation in both one and three dimensions.
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
We present the most prominent features in two-colour coherent control of high-order harmonic generation using a strongly driven two-level atom model, which are known to generate high harmonics as well as hyper-Raman lines with a plateau and a cut-off. Furthermore, for one laser field case, we find, when the hyper-Raman lines are located at the position of the high harmonics, that the high harmonics are strongly enhanced due to the interference effect between the high harmonics and the hyper-Raman lines. Within these conditions, by combining the laser field with another much weaker laser field, we show plentiful and strong high harmonics in the light spectrum of the driven atomic system.
We consider effects which occur when four-wave sum frequency generation and multiphoton ionization are induced by lasers tuned near a three-photon resonance and simultaneously near or at a dipole allowed four-photon resonance. In studies with unfocused laser beams, if the phase mismatch of the generated four-wave-mixing field is large and the related two-photon resonance for the absorption of a four-wave-mixing photon and a laser photon results in strong absorption of the four-wave-mixing field, a coherent cancellation occurs between the pumping of the resonance by two- and four-photon processes. This interference effect occurs when the first laser is tuned on either side of the three-photon resonance and \ensuremath{\Vert}\ensuremath{\Delta}krL\ensuremath{\Vert}\ensuremath{\gg}1, where \ensuremath{\Delta}kr is the mismatch and L is the length of the path of the laser beams in the gas. With focused laser beams large differences occur between ionization with unidirectional beams and with counterpropagating laser beams when \ensuremath{\Vert}\ensuremath{\Delta}krb\ensuremath{\Vert}\ensuremath{\gg}1, where b is the confocal parameter of the focused laser beams. Strong absorption of the four-wave-mixing field is shown not to be necessary for strong destructive interference with focused laser beams when the phase mismatch is large. This work also suggests an explanation for earlier experiments where the presence of a four-photon resonance enabled the generation of third-harmonic light in a positively dispersive wavelength region. We argue that this process can occur when the laser used to achieve the four-photon resonance is focused on the small z (z is the coordinate in the direction of propagation) side of the focal point of the laser responsible for the third-harmonic generation. In this way the absorption of the third-harmonic light on one side of the focal point is made much stronger than on the other side. Correspondingly, contributions to the third-harmonic field from the two sides of the focal point are unequal and cannot undergo complete destructive interference as would otherwise occur in a positively dispersive region.