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Physical Review A

Formation of ultrashort pulses from quasimonochromatic XUV radiation via infrared-field-controlled forward scattering

T. R. Akhmedzhanov, V. A. Antonov, Olga A. Kocharovskaya

Published Aug 10, 2016• 4 citations
Publisher

Abstract

We suggest a highly efficient method of ultrashort pulse formation from resonant XUV radiation due to sub-laser-cycle modulation of the excited state of non-hydrogen-like atoms by a nonionizing IR laser field. This modulation results in formation of the Raman-Stokes and anti-Stokes sidebands in coherently forward-scattered radiation, which, in turn, leads to formation of short pulses, when the phases of the sidebands are matched. This method is a generalization of a recently suggested technique [V. A. Antonov et al., Phys. Rev. A 88, 053849 (2013)] for a non-hydrogen-like medium. The possibility to form 2-fs XUV pulses in the gas of helium atoms and 990-as XUV pulses in the plasma of Li+ ions with efficiencies over 80% is shown.

DOI
10.1103/physreva.94.023821

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We suggest a highly efficient method of ultrashort pulse formation from resonant XUV radiation due to sub-laser-cycle modulation of the excited state of non-hydrogen-like atoms by a nonionizing IR laser field. This modulation results in formation of the Raman-Stokes and anti-Stokes sidebands in coherently forward-scattered radiation, which, in turn, leads to formation of short pulses, when the phases of the sidebands are matched. This method is a generalization of a recently suggested technique [V. A. Antonov et al., Phys. Rev. A 88, 053849 (2013)] for a non-hydrogen-like medium. The possibility to form 2-fs XUV pulses in the gas of helium atoms and 990-as XUV pulses in the plasma of Li+ ions with efficiencies over 80% is shown.
This work aims at development of new dynamical methods to control a resonant light-matter interaction as well as at their application for producing new sources of coherent intense sub-fs radiation in x-ray range. The dynamical control is based on modulation in time and in space of the parameters of the atomic transition (coupled to the resonant high-frequency field) by means of sufficiently strong off-resonant low-frequency control field. In particular, it may result in efficient transfer of quasi-monochromatic VUV or XUV radiation into ultrashort pulses via its resonant interaction with atomic hydrogen gas or plasma of hydrogen-like ions respectively by means of two different techniques: time and space dependent linear Stark effect or interruption of resonant interaction by the tunneling ionization, as shown in previous works of our group. \n\nIn this thesis, I further develop these ideas and demonstrate their important potential applications. First of all, both techniques are extended to arbitrary (non-hydrogen-like) atomic medium. Furthermore, advanced analytical and numerical solutions describing a process of pulses formation are found and shown to be in excellent agreement with each other. A deep physical analogy between the processes of coherent forward scattering of γ-ray radiation in the vibrated quasi-resonant nuclear absorber and the XUV field propagation in the quasi-resonant atomic medium in the presence of the moderately strong IR field is established. \n\nFinally, the application of the developed techniques for production of intense coherent attosecond sources of soft X-ray radiation, including so-called “water window” range (2.2-4.3nm) (especially promising for dynamical imaging of the proteins in a living cell) is proposed. Two different paths towards production of intense coherent attosecond pulses in a soft X-ray range are suggested: (i) via efficient transformation of the picosecond radiation of the high energy pulses of the existing x-ray plasma lasers into the trains of attosecond pulses in the resonant passive plasma, and (ii) via amplification of the low energy pulses of the existing high harmonic sources in the resonant active plasma of x-ray lasers.
We derive an analytical solution uncovering the origin of few-cycle attosecond pulse formation from vacuum-ultraviolet (VUV) radiation in an atomic gas simultaneously irradiated by a moderately strong infrared (IR) laser field, which does not perturb atoms in the ground state, but induces rapid quasistatic ionization from the excited states [Polovinkin et al., Opt. Lett. 36, 2296 (2011)]. The derived solution shows that the pulses are produced due to periodic switching of the resonant interaction between the incident VUV radiation and the atoms: turning it off near the crests of the IR-field strength and switching it back on near the IR-field zero crossings. We extend the method originally proposed by Polovinkin et al. [Opt. Lett. 36, 2296 (2011)] to non-hydrogen-like media and show that the pulses can be produced from resonant VUV radiation in a variety of atomic gases. The pulses are nearly bandwidth limited without external adjustment of phases of the generated sidebands. Proximity of the carrier frequency of the produced pulses to intra-atomic resonances may allow their efficient utilization for nondestructive steering of ultrafast dynamics of the bound electrons. The experimental possibilities for attosecond pulse formation from 58.4 nm VUV radiation in helium and from 73.6 nm VUV radiation in neon dressed by the 3.9 \ensuremath{\mu}m laser field, as well as from 122 nm VUV radiation in atomic hydrogen dressed by CO2\mathrm{C}{\mathrm{O}}_{2}CO2​-laser field are discussed.
We perform an ab initio study of the ultimate capabilities and limits of applicability of the method for few-cycle pulse formation via the resonant interaction of extreme ultraviolet (XUV) radiation with atoms dressed by a moderately strong infrared (IR) laser field proposed in two earlier works [Y. V. Radeonychev et al., Phys. Rev. Lett. 105, 183902 (2010) and V. A. Polovinkin et al., Opt. Lett. 36, 2296 (2011)]. Taking into account all the multiphoton processes in the systems under consideration on the basis of numerical solution of the three-dimensional time-dependent Schr\"odinger equation (TDSE) in the single-active-electron approximation, we show the possibilities to produce 1.1-fs pulses from 124.6-nm XUV radiation via the linear Stark effect in atomic hydrogen, as well as 500-as pulses from 58.4-nm XUV radiation via excited-state ionization in helium. We derive a generalized analytical solution, which takes into account the interplay between sub-laser-cycle Stark effect and excited-state ionization and allows us to analyze the results of TDSE calculations. We found that the ultimate intensity of the IR field suitable for few-cycle pulse formation via the linear Stark effect or excited-state ionization is limited by the threshold for atomic ionization from the resonant excited state or the ground state, respectively. We show that the pulses with shorter duration can be produced in the medium of ions with higher values of the ionization potential.
We find that intense short pulses of XUV radiation can be produced by cooperative spontaneous emission from visible or IR laser pulses driving atoms or ions. The process depends on the generation and utilization of atomic coherence as is the case in lasing without inversion. However, the radiation process is not stimulated emission, but is rather cooperative spontaneous emission in the sense of Dicke. More precisely, the many atom mathematics of superradiance has much in common with coherent anti-Stokes Raman scattering. The generation of Raman coherence is considered from the perspectives of multi-photon excitation and breaking of adiabaticity. In particular, we find that the advent of an ultrashort (e.g. single cycle) pulse rewards rethinking of conventional (nanosecond) nonlinear optics with new insights.
We have demonstrated that coherent molecular modulation can result in the collinear generation of mutually-coherent spectral sidebands that extend in frequency from the infrared to the far ultraviolet. Our technique is based on adiabatic preparation of a highly coherent molecular superposition-state, which is achieved by using narrow-linewidth lasers slightly detuned from a Raman resonance. The phases of the resultant Stokes and anti-Stokes sidebands are adjusted in order to synthesize desired single-cycle pulse trains at the target. In this article we review recent improvements and developments in this area, including: techniques for increasing the number of generated sidebands; synchronization of the pulse trains with the molecular motion in the given molecular system; laser self-focusing and spatial soliton formation due to the coherent interaction of light with oscillating molecules. In the future, this Raman source may produce sub-cycle optical pulses, and allow synthesis of waveforms where the electric field is a predetermined function of time, not limited to a quasi-sinusoidal oscillation.
Extreme ultraviolet (XUV) light is a valuable frequency range for ultrafast optics experiments. The short wavelength is a requirement for ultrashort pulses, which are widely used to characterize fast dynamics. Additionally, the high photon energy enables quantum control of high frequency transitions in atoms. These transitions are of interest for ultrafast quantum control as the bandwidth of the control pulses needs to be less than the transition frequency. Presently, however, no good modulators exist for these frequencies, which significantly reduces the possible ultrafast optics experiments or applications in the XUV regime. This thesis addresses this problem and focuses on the control of XUV light in time and space. To enable control of XUV light a method is described which modulates the phase of XUV light emitted from a gas of noble atoms. The atoms are resonantly excited with a coherent XUV pulse generated through high order harmonic generation. After the excitation pulse has passed through the gas, the atoms will emit light in the absence of an external field, known as free induction. The phase of the emitted light is changed by shifting the resonance frequencies through the AC Stark shift with a non-resonant infrared control pulse. This phase-control of the emitting atoms also translates into a control of the phase of the emitted XUV field.With the method described in the previous paragraph, the direction of XUV light emitted from noble gases was controlled, and the temporal dynamics of the emission was studied. The redirection of the XUV emission, through the use of a spatially offset IR pulse, was found to change both with intensity of the control pulse and by changing the spatial offset between the pulses. By varying the delay between the excitation and the control pulse the time of redirection was controlled, which enabled high signal to noise study of the temporal dynamics of the emission. Furthermore, with two control pulses the emission was redirected twice, resulting in an XUV pulse shape with controlled duration emitted with a certain angle. Hopefully the presented work will result in more research into the development of this technique, to fully realize the possibility to shape the amplitude and phase of XUV pulses. Such a development would open the door for ultrafast XUV quantum control.