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.
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.
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 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.
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.
Two-photon resonant and near-resonant four-wave difference-frequency mixing in gases in the interaction regime when laser pulse durations are comparable to or shorter than the medium polarization relaxation time ${T}_{2}^{\ensuremath{'}}$ is investigated. The results of experimental studies of the process in Ar and Kr using pump pulses from the ArF-excimer laser are presented demonstrating a generation of tunable short pulse radiation in the range 102--124 nm. The results are discussed in terms of a theoretical model based on a self-consistent solution of the Bloch equations for the atomic transitions and the Maxwell equations for the fields. This enables one to interpret specific nonstationary resonant and quasiresonant phenomena involved in the frequency conversion process. It is shown that the femtosecond-pulse four-wave frequency-mixing technique with probe pulses significantly shorter than the pump pulses makes it possible to study the coherent dynamics of an atomic transition exposed to an intense field. Using atomic Kr as the nonlinear medium, coherent Rabi oscillations and the subsequent phase relaxation of excitation were observed under the condition of two-photon interaction of Kr with femtosecond 193-nm laser pulses. The obtained information is important for controlling and optimizing processes of two-photon resonant frequency conversion and for time-resolved studies of Rydberg states in atoms and molecules.
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.
A theory of quantum control of short-wavelength sum-frequency generation, which employs the continuum states, is developed. The proposed scheme employs all-resonant coupling and trade-off optimization of the accompanying constructive and destructive quantum interference effects in the lower-order and higher-order polarizations controlled by the overlap of two autoionizinglike laser-induced continuum structures. The scheme does not rely on adiabatic passage, coherent population trapping or maximum atomic coherence as a means to facilitate maximum output. The opportunities for manipulating transparency of the medium and refractive index for the fundamental and generated radiations, as well as nonlinear polarization in the multiple-resonant medium, are shown. This opens the feasibility of creating frequency-tunable narrowband filters, polarization rotators, and dispersive elements for vacuum ultraviolet radiation. The features specific for quantum interference in Doppler-broadened media are investigated. The feasibility of almost complete conversion of long-wavelength fundamental radiation into generated short-wavelength radiation, and of a dramatic decrease in the intensity of required fundamental radiations, is shown.