We present an experimental demonstration of sum-frequency generation toward tunable picosecond, broadband radiation pulses in the extreme-ultraviolet regime, supported by adiabatically prepared atomic coherences. We drive a two-photon transition in a dense medium of xenon atoms with a long (nanosecond) pump laser pulse at the Fourier-transform-limited bandwidth and with a wavelength of 225 nm. The frequency of the pump pulse is slightly detuned from exact two-photon resonance. In this configuration, the medium is adiabatically driven by a process of coherent population return. The adiabatic passage process generates a maximal coherent superposition of two quantum states with large energy spacing. An additional, short (picosecond) probe laser pulse at a wavelength of 540 nm beats with the maximal atomic coherence and generates a short (picosecond) signal radiation pulse at 93 nm. As compared to conventional (diabatic) frequency conversion, the adiabatically driven maximal atomic coherence yields enhanced conversion efficiency and significantly enhanced stability.
We present an experimental demonstration of sum-frequency generation toward tunable picosecond, broadband radiation pulses in the extreme-ultraviolet regime, supported by adiabatically prepared atomic coherences. We drive a two-photon transition in a dense medium of xenon atoms with a long (nanosecond) pump laser pulse at the Fourier-transform-limited bandwidth and with a wavelength of 225 nm. The frequency of the pump pulse is slightly detuned from exact two-photon resonance. In this configuration, the medium is adiabatically driven by a process of coherent population return. The adiabatic passage process generates a maximal coherent superposition of two quantum states with large energy spacing. An additional, short (picosecond) probe laser pulse at a wavelength of 540 nm beats with the maximal atomic coherence and generates a short (picosecond) signal radiation pulse at 93 nm. As compared to conventional (diabatic) frequency conversion, the adiabatically driven maximal atomic coherence yields enhanced conversion efficiency and significantly enhanced stability.
We present experimental data on adiabatically driven frequency conversion with ultrashort (picosecond) laser pulses towards the vacuum-ultraviolet regime, enhanced by coherent population return and preparation of maximal atomic coherences. We generate the sum frequency of an intense pump pulse and a probe pulse via a two-photon resonance in xenon. When we slightly detune the pump laser from two-photon resonance, the atomic populations are adiabatically driven forth and back from the atomic ground state to an excited state. This coherent population return (CPR) prepares the medium in a transient state of maximal atomic coherence, which enhances frequency mixing with a probe laser. We thoroughly study the variation of CPR-enhanced frequency conversion with experimental parameters and compare CPR with conventional, resonantly enhanced frequency conversion. In particular, we investigate the temporal evolution of the atomic coherence and the effect of inevitable ac Stark shifts. We find that ac Stark shifts induce an asymmetry in the spectral characteristics of CPR, which nevertheless permits enhanced frequency conversion. For the case of resonantly enhanced frequency conversion, we show that the atomic coherences are maintained for several tens of picoseconds after the pump pulse, which permits time-delayed frequency conversion. Moreover, we analyze the pressure dependence of the atomic coherence' lifetime and observe a free induction decay at the two-photon coherence with the generation of a second harmonic field. These findings shall push applications of adiabatic light-matter interactions also to the regime of nonlinear optics, driven by intense laser pulses.
In this work, we thoroughly investigated frequency conversion towards ultrashort picosecond (ps) laser pulses in the vacuum ultraviolet (VUV) spectral regime via nonlinear optics in coherently-driven quantum systems at high intensities. We applied approaches of adiabatic quantum dynamics relying on coherent light-matter interactions, which modify the "bare" eigenstates of a quantum system to "dressed" states and exploit slow (i.e., adiabatic) population evolutions via such dressed states. This enables enhancement of typically low-order, low-intensity nonlinear optics (at MW/cm², GW/cm²), where the light field perturbs the atomic level structure only weakly. On the other hand, aiming at nonlinear optics at higher orders, e.g., high-harmonic generation, strong light fields are applied (100 TW/cm², PW/cm²), which modify the Coulomb potential of the atom strongly. In this case, resonances play no role anymore and adiabatic quantum dynamics via atomic resonances will not work. With this work, we demonstrated the implementation of adiabatic quantum dynamics and coherently prepared media for nonlinear optics in an intermediate intensity regime (TW/cm²), i.e., at Keldysh parameters approaching γ≈1. The fundamental question was, whether the high intensities still permit us to drive and exploit coherent-adiabatic dynamics via dressed states for enhancement of frequency conversion processes. We investigated two approaches to enhance the frequency conversion yield applying nonlinear optics in coherently-driven quantum systems (rare gases). In the first approach, we resonantly enhanced harmonic generation via dressed states with large Autler-Townes splittings. With this approach, we demonstrated how to make atomic resonances available for an initially far detuned fixed-frequency pump laser and showed a compensation for inevitable, perturbing Stark shifts. In the second approach, we investigated frequency conversion, enhanced by coherent population return (CPR) and preparation of maximal atomic coherences at high intensities. With this approach, we showed how to maximally benefit from an atomic resonance via adiabatically driven frequency conversion, i.e., by detuning the strong pump laser slightly from the resonance.
We present experimental data on the coherent control of frequency conversion toward the vacuum-ultraviolet regime in xenon atoms, applying intense ultrashort picoseconds (ps) radiation pulses. We report on quantum interference between two resonantly enhanced frequency conversion processes (i.e., fifth harmonic generation and four-wave mixing). The conversion processes are driven by a fundamental (ps) laser pulse at 530 nm and the phase-locked second harmonic at 265 nm. Both fifth harmonic generation and four-wave mixing yield vacuum-ultraviolet radiation at 106 nm. The two frequency conversion pathways interfere with each other---either constructively or destructively, depending on the relative phase of the driving laser pulses. Thus, by variation of the relative phase, we substantially enhance or reduce the conversion efficiency (i.e., the yield of generated vacuum-ultraviolet radiation).
We present experimental data on quantum interferences in resonantly enhanced frequency up-conversion towards the vacuum-ultraviolet spectral regime. The process is driven in xenon atoms by ultrashort (picosecond) laser pulses. We use two simultaneous frequency conversion pathways via an excited intermediate state, i.e., fifth harmonic generation of the fundamental wavelength and four-wave mixing of the fundamental and two photons of its second harmonic wavelength. Both conversion pathways yield radiation at 102 nm. The two pathways interfere, depending on the relative phase of the fundamental and second harmonic. By appropriate choice of the phase we get constructive interference (resulting in increased conversion efficiency) or destructive interference (resulting in reduced conversion efficiency). The total conversion yield shows very pronounced constructive and destructive quantum interference with a visibility of roughly 90%. A stable and highly accurate phase control setup enables such strong quantum interferences for more than 260 oscillation cycles. In an extension of the experiment, simultaneously to frequency conversion we also monitor laser-induced fluorescence as a measure for the excitation probability to the excited intermediate state. Also, in the excitation probability we observe strong quantum interferences. As an interesting feature, a small phase lag occurs between the quantum interference patterns of frequency conversion and population transfer. This is due to an additional atomic phase acquired during frequency conversion.
A cascaded sum frequency generation (SFG) conversion scheme based on the stimulated Raman adiabatic passage (STIRAP) technique is proposed for generating an ultraviolet laser radiation at 228 nm. The conversion involves two simultaneous SFG processes, in which the signal laser radiation is converted to ultraviolet laser radiation through a negligible intermediate laser radiation. Dark state expressions and adiabatic conditions are given. Numerical simulations demonstrate the efficient conversion processes in a nonlinear LaBGeO 5 (LBGO) crystal, and the effects of the coupling modulation function, pump laser intensity, and temperature on the quantum conversion efficiency are investigated. Tunable output of ultraviolet laser radiation in the 210–250 nm range is achieved by varying the signal or pump laser radiation wavelength while maintaining other input parameters. The large amount of optical data obtained in this work will contribute to the generation of deep ultraviolet laser sources based on nonlinear cascaded frequency conversion.
We carry out the theoretical study for the generation of vacuum-ultraviolet pulses with a Doppler-broadened gas utilizing high atomic coherence. It is essentially a difference-frequency generation scheme induced by the two-photon near-resonant pump and probe pulses, where the key point is to generate high atomic coherence between the ground and two-photon near-resonant states through a variant of stimulated Raman adiabatic passage with a time-dependent detuning. The advantage of our scheme is that the degree of coherence is sensitive to neither the exact amount and even sign of the detuning, nor the exact timing between the pump, auxiliary, and probe pulses. Hence our scheme is practically insensitive to Doppler broadening. As a specific example, we consider the generation of picosecond Lyman-α pulses with a Kr gas, and quantitatively study the influence of Doppler broadening as well as the intensity and incident timing of the picosecond probe pulse with respect to the pump pulse. The numerical results indicate that our scheme has a certain advantage over the conventional scheme which utilizes two-photon resonant excitation.