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Register a new userPtychographic hyperspectral spectromicroscopy with an extreme ultraviolet high harmonic comb
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We demonstrate a new scheme of spectromicroscopy in the extreme ultraviolet (EUV) spectral range, where the spectral response of the sample at different wavelengths is imaged simultaneously. It is enabled by applying ptychographical information multiplexing (PIM) to a tabletop EUV source based on high harmonic generation, where four spectrally narrow harmonics near 30 nm form a spectral comb structure. Extending PIM from previously demonstrated visible wavelengths to the EUV/X-ray wavelengths promises much higher spatial resolution and more powerful spectral contrast mechanism, making PIM an attractive spectromicroscopy method in both the microscopy and the spectroscopy aspects. Besides the sample, the multicolor EUV beam is also imaged in situ, making our method a powerful beam characterization technique. No hardware is used to separate or narrow down the wavelengths, leading to efficient use of the EUV radiation.
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Laser-driven high-order harmonic generation (HHG) provides tabletop sources of broadband extreme-ultraviolet (XUV) light with excellent spatial and temporal coherence. These sources are typically operated at low repetition rates, $f_{rep}lesssim$100 kHz, where phase-matched frequency conversion into the XUV is readily achieved. However, there are many applications that demand the improved counting statistics or frequency-comb precision afforded by operation at high repetition rates, $f_{rep}$ > 10 MHz. Unfortunately, at such high $f_{rep}$, phase matching is prevented by the accumulated steady-state plasma in the generation volume, setting stringent limitations on the XUV average power. Here, we use gas mixtures at high temperatures as the generation medium to increase the translational velocity of the gas, thereby reducing the steady-state plasma in the laser focus. This allows phase-matched XUV emission inside a femtosecond enhancement cavity at a repetition rate of 77 MHz, enabling a record generated power of $sim$2 mW in a single harmonic order. This power scaling opens up many demanding applications, including XUV frequency-comb spectroscopy of few-electron atoms and ions for precision tests of fundamental physical laws and constants.
We demonstrate a femtosecond enhancement cavity with a crossed-beam geometry for efficient generation and extraction of extreme-ultraviolet (XUV) frequency combs at a 154 MHz repetition rate. We achieve a record-high out-coupled power of 600 {mu}W, directly usable for spectroscopy, at a wavelength of 97 nm. This corresponds to a >60% out-coupling efficiency. The XUV power scaling and generation efficiency are similar to that achieved with a single Gaussian-mode fundamental beam inside a collinear enhancement cavity. The noncollinear geometry also opens the door for the generation of isolated attosecond pulses at >100 MHz repetition rate.
The interaction of strong near-infrared (NIR) laser pulses with wide-bandgap dielectrics produces high harmonics in the extreme ultraviolet (XUV) wavelength range. These observations have opened up the possibility of attosecond metrology in solids, which would benefit from a precise measurement of the emission times of individual harmonics with respect to the NIR laser field. Here we show that, when high-harmonics are detected from the input surface of a magnesium oxide crystal, a bichromatic probing of the XUV emission shows a clear synchronization largely consistent with a semiclassical model of electron-hole recollisions in bulk solids. On the other hand, the bichromatic spectrogram of harmonics originating from the exit surface of the 200 $mu$m-thick crystal is strongly modified, indicating the influence of laser field distortions during propagation. Our tracking of sub-cycle electron and hole re-collisions at XUV energies is relevant to the development of solid-state sources of attosecond pulses.
An effective harmonic potential for photons is achieved in a photonic crystal structure, owing to the balance of the background dispersion and a bichromatic potential. Consequently, ultra-compact resonators with several equi-spaced resonances and high loaded Q factors (0.7 million) are demonstrated. A detailed statistical analysis is carried out by exploiting the complex reflection spectra measured with Optical Coherent Tomography. The log-normal distribution of the intrinsic Q-factors peaks at 3 million. The device is made of $Ga_{0.5}In_{0.5}P$ in order to suppress the two photon absorption in the Telecom spectral range considered here. This is crucial to turn the strong localization of light into ultra-efficient parametric interactions.
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.
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