Spectrally resolved single-shot wavefront sensing of broadband high-harmonic sources

Wavefront sensors are an important tool to characterize coherent beams of extreme ultraviolet radiation. However, conventional Hartmann-type sensors do not allow for independent wavefront characterization of different spectral components that may be present in a beam, which limits their applicability for intrinsically broadband high-harmonic generation (HHG) sources. Here we introduce a wavefront sensor that measures the wavefronts of all the harmonics in a HHG beam in a single camera exposure. By replacing the mask apertures with transmission gratings at different orientations, we simultaneously detect harmonic wavefronts and spectra, and obtain sensitivity to spatiotemporal structure such as pulse front tilt as well. We demonstrate the capabilities of the sensor through a parallel measurement of the wavefronts of 9 harmonics in a wavelength range between 25 and 49 nm, with up to lambda/32 precision.Comment: 12 pages, 6 figure

Novel techniques in VUV high-resolution spectroscopy

Novel VUV sources and techniques for VUV spectroscopy are reviewed. Laser-based VUV sources have been developed via non-linear upconversion of laser pulses in the nanosecond (ns), the picosecond (ps), and femtosecond (fs) domain, and are applied in high-resolution gas phase spectroscopic studies. While the ns and ps pulsed laser sources, at Fourier-transform limited bandwidths, are used in wavelength scanning spectroscopy, the fs laser source is used in a two-pulse time delayed mode. In addition a Fourier-transform spectrometer for high resolution gas-phase spectroscopic studies in the VUV is described, exhibiting the multiplex advantage to measure many resonances simultaneously.Comment: 17 Pages, 8 figures, Conference proceedings of the VUV/X-ray 2013 at Hefei, Chin

Sub-Doppler frequency metrology in HD for test of fundamental physics

Weak transitions in the (2,0) overtone band of the HD molecule at $\lambda = 1.38 \, \mu$m were measured in saturated absorption using the technique of noise-immune cavity-enhanced optical heterodyne molecular spectroscopy. Narrow Doppler-free lines were interrogated with a spectroscopy laser locked to a frequency comb laser referenced to an atomic clock to yield transition frequencies [R(1) = $217\,105\,181\,895\,(20)$ kHz; R(2) = $219\,042\,856\,621\,(28)$ kHz; R(3) = $220\,704\,304\,951\,(28)$ kHz] at three orders of magnitude improved accuracy. These benchmark values provide a test of QED in the smallest neutral molecule, and open up an avenue to resolve the proton radius puzzle, as well as constrain putative fifth forces and extra dimensions.Comment: 5 pages, 4 figure

Direct frequency comb spectroscopy of trapped ions

Direct frequency comb spectroscopy of trapped ions is demonstated for the first time. It is shown that the 4s^2S_(1/2)-4p^2P_(3/2) transition in calcium ions can be excited directly with a frequency comb laser that is upconverted to 393 nm. Detection of the transition is performed using a shelving scheme to suppress background signal from non-resonant comb modes. The measured transition frequency of f=761 905 012.7(0.5) MHz presents an improvement in accuracy of more than two orders of magnitude.Comment: 4 pages, 5 figur

Frequency metrology on the 4s 2S1/2 - 4p 2P1/2 transition in the calcium ion for a comparison with quasar data

High accuracy frequency metrology on the 4s 2S1/2 - 4p 2P1/2 transition in calcium ions is performed using laser cooled and crystallized ions in a linear Paul trap. Calibration is performed with a frequency comb laser, resulting in a transition frequency of f=755222766.2(1.7) MHz. The accuracy presents an improvement of more than one order of magnitude, and will facilitate a comparison with quasar data in a search for a possible change of the fine structure constant on a cosmological time scale.Comment: Corrected typos (including one on the axis of figure 6

Deep-Ultraviolet Frequency Metrology of H2 for Tests of Molecular Quantum Theory

Molecular hydrogen and its isotopic and ionic species are benchmark systems for testing quantum chemical theory. Advances in molecular energy structure calculations enable the experimental verification of quantum electrodynamics and potentially a determination of the proton charge radius from H2 spectroscopy. We measure the ground state energy in ortho-H2 relative to the first electronically excited state by Ramsey-comb laser spectroscopy on the EF1Σg+-X1Σg+(0,0) Q1 transition. The resulting transition frequency of 2 971 234 992 965(73) kHz is 2 orders of magnitude more accurate than previous measurements. This paves the way for a considerably improved determination of the dissociation energy (D0) for fundamental tests with molecular hydrogen

Diffractive shear interferometry for extreme ultraviolet high-resolution lensless imaging

We demonstrate a novel imaging approach and associated reconstruction algorithm for far-field coherent diffractive imaging, based on the measurement of a pair of laterally sheared diffraction patterns. The differential phase profile retrieved from such a measurement leads to improved reconstruction accuracy, increased robustness against noise, and faster convergence compared to traditional coherent diffractive imaging methods. We measure laterally sheared diffraction patterns using Fourier-transform spectroscopy with two phase-locked pulse pairs from a high harmonic source. Using this approach, we demonstrate spectrally resolved imaging at extreme ultraviolet wavelengths between 28 and 35 nm

Ion distribution and ablation depth measurements of a fs-ps laser-irradiated solid tin target

The ablation of solid tin surfaces by an 800-nanometer-wavelength laser is studied for a pulse length range from 500 fs to 4.5 ps and a fluence range spanning 0.9 to 22 J/cm^2. The ablation depth and volume are obtained employing a high-numerical-aperture optical microscope, while the ion yield and energy distributions are obtained from a set of Faraday cups set up under various angles. We found a slight increase of the ion yield for an increasing pulse length, while the ablation depth is slightly decreasing. The ablation volume remained constant as a function of pulse length. The ablation depth follows a two-region logarithmic dependence on the fluence, in agreement with the available literature and theory. In the examined fluence range, the ion yield angular distribution is sharply peaked along the target normal at low fluences but rapidly broadens with increasing fluence. The total ionization fraction increases monotonically with fluence to a 5-6% maximum, which is substantially lower than the typical ionization fractions obtained with nanosecond-pulse ablation. The angular distribution of the ions does not depend on the laser pulse length within the measurement uncertainty. These results are of particular interest for the possible utilization of fs-ps laser systems in plasma sources of extreme ultraviolet light for nanolithography.Comment: 8 pages, 7 figure

Demonstration of Ramsey-Comb Precision Spectroscopy in Xenon at Vacuum Ultraviolet Wavelengths Produced with High-Harmonic Generation

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