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Accurate spectroscopic measurements of calculable systems provide a powerful method for testing the Standard Model and extracting fundamental constants. Recently, spectroscopic measurements of finite nuclear size effects in normal and muonic hydrogen resulted in unexpectedly large adjustments of the proton charge radius and the Rydberg constant. We measured the $2^3\mathrm{S}\rightarrow2^1\mathrm{S}$ transition frequency in a Fermi gas of $^3$He with an order of magnitude higher accuracy than before. Together with a previous measurement in a $^4$He Bose-Einstein condensate, a squared charge radius difference $r^2_h - r^2_{\alpha} = 1.0757(15)\ \mathrm{fm^2}$ is determined between the helion and alpha particle. This measurement provides a benchmark with unprecedented accuracy for nuclear structure calculations. A deviation of 3.6$\sigma$ is found with a determination (arXiv:2305.11679) based on spectroscopy of muonic helium ions., Comment: Paper and supplementary in total 13 pages and 5 figures

Accepted values of the masses of several subatomic particles have been under debate since recent measurements in Penning traps produced more precise yet incompatible results, implying possible inconsistencies in closely related physical constants like the proton-electron and deuteron-proton mass ratios. These quantities also influence the predicted vibrational spectrum of the deuterated molecular hydrogen ion in its electronic ground state, of which we measured the v=0 - 9 overtone transition frequency with an uncertainty of 2.9 parts-per-trillion through Doppler-free two-photon laser spectroscopy. Leveraging high-precision ab initio calculations we convert our measurement to tight constraints on the proton-electron and deuteron-proton mass ratios, consistent with the most recent Penning-trap determinations of these quantities, and yielding a new value of the proton-electron mass ratio with an unprecedented precision of 21 parts-per-trillion.

The ionization energy of D$_2$ has been determined experimentally from measurements involving two-photon Doppler-free vacuum-ultraviolet pulsed laser excitation and near-infrared continuous-wave laser excitation to yield $E_\mathrm{I}(\mathrm{D}_2)=124\,745.393\,739(26)$ \wn. From this value, the dissociation energy of D$_2$ is deduced to be $D_0$(D$_2$) = 36\,748.362\,282(26) \wn, representing a 25-fold improvement over previous values, and found in good agreement (at $1.6\sigma$) with recent ab initio calculations of the 4-particle nonadiabatic relativistic energy and of quantum-electrodynamic corrections up to order $m\alpha^6$. This result constitutes a test of quantum electrodynamics in the molecular domain, while a perspective is opened to determine nuclear charge radii from molecules., Comment: 9 pages, 6 figures, Phys. Rev. A, accepted

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.

High-harmonic generation (HHG) is widely used for up-conversion of amplified (near) infrared ultrafast laser pulses to short wavelengths. We demonstrate that Ramsey-comb spectroscopy, based on two such pulses derived from a frequency-comb laser, enables us to observe phase effects in this process with a few mrad precision. As a result, we could perform the most accurate spectroscopic measurement based on light from HHG, illustrated with a determination of the $5p^6 \rightarrow 5p^5 8s~^2[3/2]_1$ transition at 110 nm in $^{132}$Xe. We improve its relative accuracy $10^4$ times to a value of $2.3\times10^{-10}$. This is 3.6 times better than shown before involving HHG, and promising to enable $1S-2S$ spectroscopy of He$^+$ for fundamental tests.

High-precision laser spectroscopy of atomic hydrogen has led to an impressive accuracy in tests of bound-state quantum electrodynamics (QED). At the current level of accuracy many systematics have to be studied very carefully and only independent measurements provide the ultimate cross-check. This has been proven recently by measurements in muonic hydrogen, eventually leading to a significant shift of the CODATA recommended values of the proton charge radius and the Rydberg constant. We aim to contribute to tests of fundamental physics by measuring the 1S-2S transition in the He$^+$ ion for the first time. Combined with measurements in muonic helium ions this can probe the value of the Rydberg constant, test higher-order QED terms, or set benchmarks for ab initio nuclear polarizability calculations. We extend the Ramsey-comb spectroscopy method to the XUV using high-harmonic generation in order to excite a single, trapped He$^+$ ion., Comment: 10 pages, 4 figures, FFK2019

The ionization energy of ortho-H$_2$ has been determined to be $E^\mathrm{o}_\mathrm{I}(\mathrm{H}_2)/(hc)=124\,357.238\,062(25)$ cm$^{-1}$ from measurements of the GK(1,1)--X(0,1) interval by Doppler-free two-photon spectroscopy using a narrow band 179-nm laser source and the ionization energy of the GK(1,1) state by continuous-wave near-infrared laser spectroscopy. $E^\mathrm{o}_\mathrm{I}$(H$_2$) was used to derive the dissociation energy of H$_2$, $D^{N=1}_{0}$(H$_2$), at $35\,999.582\,894(25)$ cm$^{-1}$ with a precision that is more than one order of magnitude better than all previous results. The new result challenges calculations of this quantity and represents a benchmark value for future relativistic and QED calculations of molecular energies., Comment: 6 pages, 5 figures

Improvements in both theory and frequency metrology of few-electron systems such as hydrogen and helium have enabled increasingly sensitive tests of quantum electrodynamics (QED), as well as ever more accurate determinations of fundamental constants and the size of the nucleus. At the same time advances in cooling and trapping of neutral atoms have revolutionized the development of increasingly accurate atomic clocks. Here, we combine these fields to reach the highest precision on an optical tranistion in the helium atom to date by employing a Bose-Einstein condensate confined in a magic wavelength optical dipole trap. The measured transition accurately connects the ortho- and parastates of helium and constitutes a stringent test of QED theory. In addition we test polarizability calculations and ultracold scattering properties of the helium atom. Finally, our measurement probes the size of the nucleus at a level exceeding the projected accuracy of muonic helium measurements currently being performed in the context of the proton radius puzzle.

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.

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 figures

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 figures

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 figures

Recently we reported a high precision optical frequency measurement of the (v,L):(0,2)->(8,3) vibrational overtone transition in trapped deuterated molecular hydrogen (HD+) ions at 10 mK temperature. Achieving a resolution of 0.85 parts-per-billion (p.p.b.) we found the experimental value ($\nu_0= 383,407,177.38(41)$ MHz) to be in agreement with the value from molecular theory ($\nu_\text{th}=383,407,177.150(15)$ MHz) within 0.6(1.1) p.p.b. [Biesheuvel et al., Nat. Commun. 7, 10385 (2016)]. This enabled an improved test of molecular theory (including QED), new constraints on the size of possible effects due to 'new physics', and the first determination of the proton-electron mass ratio from a molecule. Here, we provide the details of the experimental procedure, spectral analysis, and the assessment of systematic frequency shifts. Our analysis focuses in particular on deviations of the HD+ velocity distribution from thermal (Gaussian) distributions under the influence of collisions with fast ions produced during (laser-induced) chemical reactions, as such deviations turn out to significantly shift the hyperfine-less vibrational frequency as inferred from the saturated and Doppler-broadened spectrum, which contains partly unresolved hyperfine structure., Comment: 22 pages, 20 figures

Coherent extreme ultraviolet (XUV) radiation produced by table-top high-harmonic generation (HHG) sources provides a wealth of possibilities in research areas ranging from attosecond physics to high resolution coherent imaging. However, it remains challenging to fully exploit the coherence of such sources for interferometry and Fourier transform spectroscopy (FTS). This is due to the need for a measurement system that is stable at the level of a wavelength fraction, yet allowing a controlled scanning of time delays. Here we demonstrate XUV interferometry and FTS in the 17-55 nm wavelength range using an ultrastable common-path interferometer suitable for high-intensity laser pulses that drive the HHG process. This approach enables the generation of fully coherent XUV pulse pairs with sub-attosecond timing variation, tunable time delay and a clean Gaussian spatial mode profile. We demonstrate the capabilities of our XUV interferometer by performing spatially resolved FTS on a thin film composed of titanium and silicon nitride., Comment: 10 pages, 5 figures

The simplest molecules in nature, molecular hydrogen ions in the form of H2+ and HD+, provide an important benchmark system for tests of quantum electrodynamics in complex forms of matter. Here, we report on such a test based on a frequency measurement of a vibrational overtone transition in HD+ by laser spectroscopy. We find that the theoretical and experimental frequencies are equal to within 0.6(1.1) parts per billion, which represents the most stringent test of molecular theory so far. Our measurement not only confirms the validity of high-order quantum electrodynamics in molecules, but also enables the long predicted determination of the proton-to-electron mass ratio from a molecular system, as well as improved constraints on hypothetical fifth forces and compactified higher dimensions at the molecular scale. With the perspective of comparisons between theory and experiment at the 0.01 part-per-billion level, our work demonstrates the potential of molecular hydrogen ions as a probe of fundamental physical constants and laws.

Results of optical frequency transfer over a carrier-grade dense-wavelength-division-multiplexing (DWDM) optical fibre network are presented. The relation between soil temperature changes on a buried optical fibre and frequency changes of an optical carrier through the fibre is modelled. Soil temperatures, measured at various depths by the Royal Netherlands Meteorology Institute (KNMI) are compared with observed frequency variations through this model. A comparison of a nine-day record of optical frequency measurements through the 2 x 298 km fibre link with soil temperature data shows qualitative agreement. A soil temperature model is used to predict the link stability over longer periods (days-months-years). We show that one-way optical frequency dissemination is sufficiently stable to distribute and compare e.g. rubidium frequency standards over standard DWDM optical fibre networks., Comment: 13 pages, 13 figures, submitted

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, China

Highly accurate results from frequency measurements on neutral hydrogen molecules H_2, HD and D_2 as well as the HD^+ ion can be interpreted in terms of constraints on possible fifth-force interactions. Where the hydrogen atom is a probe for yet unknown lepton-hadron interactions, and the helium atom is sensitive for lepton-lepton interactions, molecules open the domain to search for additional long-range hadron-hadron forces. First principles calculations in the framework of quantum electrodynamics have now advanced to the level that hydrogen molecules and hydrogen molecular ions have become calculable systems, making them a search-ground for fifth forces. Following a phenomenological treatment of unknown hadron-hadron interactions written in terms of a Yukawa potential of the form V_5(r)=\beta exp(-r/\lambda)/r current precision measurements on hydrogenic molecules yield a constraint \beta < 1 \times 10^{-7} eV\AA for long-range hadron-hadron interactions at typical force ranges commensurate with separations of a chemical bond, i.e. \lambda ~1 \AA and beyond., Comment: 7 pages, 3 figures, 1 table

We present full phase stabilization of an amplified Yb:fiber femtosecond frequency comb using an intra-cavity electro-optic modulator and an acousto-optic modulator. These transducers provide high servo bandwidths of 580 kHz and 250 kHz for frep and fceo, producing a robust and low phase noise fiber frequency comb. The comb was self-referenced with an f - 2f interferometer and phase locked to an ultra-stable optical reference used for the JILA Sr optical clock at 698 nm, exhibiting 0.21 rad and 0.47 rad of integrated phase errors (over 1 mHz - 1 MHz) respectively. Alternatively, the comb was locked to two optical references at 698 nm and 1064 nm, obtaining 0.43 rad and 0.14 rad of integrated phase errors respectively.

Precision spectroscopy of simple atomic systems has refined our understanding of the fundamental laws of quantum physics. In particular, helium spectroscopy has played a crucial role in describing two-electron interactions, determining the fine-structure constant and extracting the size of the helium nucleus. Here we present a measurement of the doubly-forbidden 1557-nanometer transition connecting the two metastable states of helium (the lowest energy triplet state 2 3S1 and first excited singlet state 2 1S0), for which quantum electrodynamic and nuclear size effects are very strong. This transition is fourteen orders of magnitude weaker than the most predominantly measured transition in helium. Ultracold, sub-microkelvin, fermionic 3He and bosonic 4He atoms are used to obtain a precision of 8.10^{-12}, providing a stringent test of two-electron quantum electrodynamic theory and of nuclear few-body theory., Comment: 14 pages, 6 figures

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 figure

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)