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Generation of vacuum ultraviolet radiation by intracavity high-harmonic generation toward state detection of single trapped ions

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 Added by Kentaro Wakui
 Publication date 2014
  fields Physics
and research's language is English




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VUV radiation around 159 nm is obtained toward direct excitation of a single trapped $^{115}$In$^{+}$ ion. An efficient fluoride-based VUV output-coupler is employed for intracavity high-harmonic generation of a Ti:S oscillator. Using this coupler, where we measured its reflectance to be about 90%, an average power reaching $6.4,mu$W is coupled out from a modest fundamental power of 650 mW. When a single comb component out of $1.9times10^{5}$ teeth is resonant to the atomic transition, hundreds of fluorescence photons per second will be detectable under a realistic condition.

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The development of alternative platforms for computing has been a longstanding goal for physics, and represents a particularly pressing concern as conventional transistors approach the limit of miniaturization. A potential alternatice paradigm is that of reservoir computing, which leverages unknown, but highly non-linear transformations of input-data to perform computations. This has the advantage that many physical systems exhibit precisely the type of non-linear input-output relationships necessary for them to function as reservoirs. Consequently, the quantum effects which obstruct the further development of silicon electronics become an advantage for a reservoir computer. Here we demonstrate that even the most basic constituents of matter - atoms - can act as a reservoir for optical computers, thanks to the phenomenon of High Harmonic Generation (HHG). A prototype single-atom computer for classification problems is proposed, where parameters of the classification model are mapped to optical elements. We numerically demonstrate that this `all-optical computer can successfully classify data with an accuracy that is strongly dependent on dynamical non-linearities. This may pave the way for the development of petahertz information processing platforms.
We show that high-order harmonics generated from molecules by intense laser pulses can be expressed as the product of a returning electron wave packet and the photo-recombination cross section (PRCS) where the electron wave packet can be obtained from simple strong-field approximation (SFA) or from a companion atomic target. Using these wave packets but replacing the PRCS obtained from SFA or from the atomic target by the accurate PRCS from molecules, the resulting HHG spectra are shown to agree well with the benchmark results from direct numerical solution of the time-dependent Schrodinger equation, for the case of H$_2^+$ in laser fields. The result illustrates that these powerful theoretical tools can be used for obtaining high-order harmonic spectra from molecules. More importantly, the results imply that the PRCS extracted from laser-induced HHG spectra can be used for time-resolved dynamic chemical imaging of transient molecules with temporal resolutions down to a few femtoseconds.
The remarkable progress in the field of laser spectroscopy induced by the invention of the frequency-comb laser has enabled many new high-precision tests of fundamental theory and searches for new physics. Extending frequency-comb based spectroscopy techniques to the vacuum (VUV) and extreme ultraviolet (XUV) spectral range would enable measurements in e.g. heavier hydrogen-like systems and open up new possibilities for tests of quantum electrodynamics and measurements of fundamental constants. The main approaches rely on high-harmonic generation (HHG), which is known to induce spurious phase shifts from plasma formation. After our initial report (Physical Review Letters 123, 143001 (2019)), we give a detailed account of how the Ramsey-comb technique is used to probe the plasma dynamics with high precision, and enables accurate spectroscopy in the VUV. A series of Ramsey fringes is recorded to track the phase evolution of a superposition state in xenon atoms, excited by two up-converted frequency-comb pulses. Phase shifts of up to 1 rad induced by HHG were observed at ns timescales and with mrad-level accuracy at $110$ nm. Such phase shifts could be reduced to a negligible level, enabling us to measure the $5p^6 rightarrow 5p^5 8s~^2[3/2]_1$ transition frequency in $^{132}Xe$ at 110 nm (seventh harmonic) with sub-MHz accuracy. The obtained value is $10^4$ times more precise than the previous determination and the fractional accuracy of $2.3 times 10^{-10}$ is $3.6$ times better than the previous best spectroscopic measurement using HHG. The isotope shifts between $^{132}Xe$ and two other isotopes were determined with an accuracy of $420$ kHz. The method can be readily extended to achieve kHz-level accuracy, e.g. to measure the $1S-2S$ transition in $He^+$. Therefore, the Ramsey-comb method shows great promise for high-precision spectroscopy of targets requiring VUV and XUV wavelengths.
We investigate the electron quantum path interference effects during high harmonic generation in atomic gas medium driven by ultrashort chirped laser pulses. To achieve that, we identify and vary the different experimentally relevant control parameters of such a driving laser pulse influencing the high harmonic spectra. Specifically, the impact of the pulse duration, peak intensity and instantaneous frequency is studied in a self-consistent manner based on Lewenstein formalism. Simulations involving macroscopic propagation effects are also considered. The study aims to reveal the microscopic background behind a variety of interference patterns capturing important information both about the fundamental laser field and the generation process itself. The results provide guidance towards experiments with chirp control as a tool to unravel, explain and utilize the rich and complex interplay between quantum path interferences including the tuning of the periodicity of the intensity dependent oscillation of the harmonic signal, and the curvature of spectrally resolved Maker fringes.
We study the effect of gas pressure on the generation of high-order harmonics where harmonics due to individual atoms are calculated using the recently developed quantitative rescattering theory, and the propagation of the laser and harmonics in the medium is calculated by solving the Maxwells wave equation. We illustrate that the simulated spectra are very sensitive to the laser focusing conditions at high laser intensity and high pressure since the fundamental laser field is severely reshaped during the propagation. By comparing the simulated results with several experiments we show that the pressure dependence can be qualitatively explained. The lack of quantitative agreement is tentatively attributed to the failure of the complete knowledge of the experimental conditions.
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