arXiv subjects

W. Ubachs

Publications and source records attributed to W. Ubachs.

At least 19 recordsLinked to original sources

arXiv2026

Statistics and systematics of electron EDM searches with BaF

The NL-$e$EDM experiment searches for a non-zero electric dipole moment of the electron $d_e$ ($e$EDM) in the ground state of barium monofluoride (BaF). A beam of BaF from a supersonic expansion source is probed with the spin precession method presented in \cite{Boeschoten2024}. This method permits the extraction of an $e$EDM value as well as values for parameters causing a possible systematic bias leading to a false $e$EDM. The currently achievable sensitivity is limited by statistics collected in a period of 34 hours and yields an $d_e$ of $2(3) \times 10^{-25}$ $e\,$cm. Furthermore, from the same dataset sufficiently strong limits on parameters which can induce a false $e$EDM are extracted. These are mainly the electric field \textbf{E} and the intensity of the lasers fields in the fiducial volume of the experiment. We summarize the steps required to upgrade of the experiment to reach a competitive level on $d_e$, e.g. an intense laser-cooled beam from a cryogenic buffer gas source and the light collection efficiency of fluorescence.

physics.atom-ph↗

arXiv2025

A sub-ppm upper limit on the cosmological variations of the fine structure constant alpha

Absorption spectroscopy toward high-redshift quasars provides strong constraints on the putative variation of fundamental constants of physics on cosmological time scales. The submillimeter ground-state transitions of methylidyne (CH) and water (H2O), both molecules widespread and coeval in the interstellar medium, provide a sensitive test for variations of alpha, the fine structure constant, and mu, the proton-to-electron mass ratio, taking advantage of the unmatched spectral resolution and frequency reliability of radio techniques. We used ALMA simultaneous observations of the two species to constrain any velocity offset between their absorption profiles toward the radio-bright lensed quasars PKS1830-211 (z_abs=0.88582) and B0218+357 (z_abs=0.68466). Our observational setup minimizes instrumental errors and known sources of systematics, such as time variability of the absorption profile and frequency-dependent morphology of the background quasar. The excellent correlation between CH and H2O opacities, the large number of individual narrow velocity components, and the number of independent spectra obtained due to the intrinsic time variability of the absorption profiles ensure that even the chemical segregation bias is minimized. We obtained bulk velocity shifts delta_v = -0.048 pm 0.028 km/s and -0.13 pm 0.14 km/s (1 sigma confidence level) between CH and H2O in the direction of PKS1830-211(NE) and B0218+357(SW), respectively. These values convert into the 3sigma upper limits |Delta_alpha/alpha| < 0.55 ppm and 1.5 ppm, respectively, taking into account the independent upper limits on |Delta_mu/mu| previously obtained for these systems. These constraints on |Delta_alpha/alpha|, at look-back times of about half the present age of the Universe, are two to four times deeper than previous constraints on any other single high-z system.

astro-ph.CO↗

arXiv2025

Precision spectroscopy of the $A^2\Pi$ $\leftarrow$ $X^2\Sigma^+$ transition in BaF

High-resolution spectroscopy on the $A^2\Pi$ - $X^2\Sigma^+$ electronic system of $^{138}$Ba$^{19}$F is performed using a cold molecular beam produced by a buffer gas source. The hyperfine structure in both $X^2\Sigma^+$ ground and $A^2\Pi$ excited states is fully resolved and absolute transition frequencies of individual components are measured at the sub-MHz level making use of frequency-comb laser calibration. Sets of molecular constants for the $X^2\Sigma^+$($v=0,1$) and $A^2\Pi$($v=0,1$) levels are determined, with improved accuracy for the $T_{v',v''}$ band origins and spin-orbit interaction constants for the $A^2\Pi$ excited states, that represent the presently measured highly accurate transitions for low-$J$ states as well as previously determined transition frequencies in Fourier-transform emission studies for rotational levels as high as $J \geq 100$. The extracted molecular constants reproduce the measured transition frequencies at the experimental absolute accuracy of 1 MHz. The work is of relevance for future laser cooling schemes, and is performed in the context of a measurement of the electron dipole moment for which BaF is a target system.

physics.atom-ph↗

arXiv2025

Precision measurement of the last bound states in H$_2$ and determination of the H + H scattering length

The binding energies of the five bound rotational levels $J=0-4$ in the highest vibrational level $v=14$ in the X$^1\Sigma_g^+$ ground electronic state of H$_2$ were measured in a three-step ultraviolet-laser experiment. Two-photon UV-photolysis of H$_2$S produced population in these high-lying bound states, that were subsequently interrogated at high precision via Doppler-free spectroscopy of the F$^1\Sigma_g^+$ - X$^1\Sigma_g^+$ system. A third UV-laser was used for detection through auto-ionizing resonances. The experimentally determined binding energies were found to be in excellent agreement with calculations based on non-adiabatic perturbation theory, also including relativistic and quantum electrodynamical contributions. The $s$-wave scattering length of the H + H system is derived from the binding energy of the last bound $J=0$ level via a direct semi-empirical approach, yielding a value of $a_s$ = 0.2724(5) $a_0$, in good agreement with a result from a previously followed theoretical approach. The subtle effect of the $m\alpha^4$ relativity contribution to $a_s$ was found to be significant. In a similar manner a value for the $p$-wave scattering volume is determined via the $J=1$ binding energy yielding $a_p$ = -134.0000(6) $a_0^3$. The binding energy of the last bound state in H$_2$, the ($v=14$, $J=4$) level, is determined at 0.023(4) cm$^{-1}$, in good agreement with calculation. The effect of the hyperfine substructure caused by the two hydrogen atoms at large internuclear separation, giving rise to three distinct dissociation limits, is discussed.

physics.atom-ph↗

arXiv2024

Hyperfine structure of the methanol molecule as traced by Class I methanol masers

We present results on simultaneous observations of Class~I methanol masers at 25, 36, and 44 GHz towards 22 Galactic targets carried out with the Effelsberg 100-m telescope. The study investigates relations between the hyperfine (HF) structure of the torsion-rotation transitions in CH3OH and maser activity. By analyzing the radial velocity shifts between different maser lines together with the patterns of the HF structure based on laboratory measurements and quantum-chemical calculations, we find that in any source only one specific HF transition forms the maser emission and that this transition changes from source to source. The physical conditions leading to this selective behavior are still unclear. Using accurate laboratory rest frequencies for the 25 GHz transitions, we have refined the centre frequencies for the HF multiplets at 36, 44, and 95 GHz: f_36 = (36169.2488 +/- 0.0002_stat +/- 0.0004_sys) MHz. f_44 = (44069.4176 +/- 0.0002_stat +/- 0.0004_sys) MHz, and f_95 = (95169.4414 +/- 0.0003_stat +/- 0.0004_sys) MHz. Comparison with previous observations of 44 GHz masers performed 6-10 years ago with a Korean 21-m KVN telescope towards the same targets confirms the kinematic stability of Class~I maser line profiles during this time interval and reveals a systematic radial velocity shift of 0.013 +/- 0.005 km/s between the two telescopes.

astro-ph.GA↗

arXiv2024

Precision Measurement of Vibrational Quanta in Tritium Hydride (HT)

Saturated absorption measurements of transitions in the (2-0) band of radioactive tritium hydride (HT) are performed with the ultra-sensitive NICE-OHMS intracavity absorption technique in the range 1460-1510 nm. The hyperfine structure of rovibrational transitions of HT, in contrast to that of HD, exhibits a single isolated hyperfine component, allowing for the accurate determination of hyperfineless rovibrational transition frequencies, resulting in R(0) = $203\,396\,426\,692$ (22) kHz and R(1) = $205\,380 \,033 \,644$ (21) kHz. This corresponds to an accuracy three orders of magnitude better than previous measurements in tritiated hydrogen molecules. Observation of an isolated component in P(1) with reversed signal amplitude contradicts models for line shapes in HD based on cross-over resonances.

physics.atom-ph↗

arXiv2023

Lamb dip of a Quadrupole Transition in H$_2$

The saturated absorption spectrum of the hyperfine-less S(0) quadrupole line in the (2-0) band of H$_2$ is measured at $\lambda=1189$ nm, using the NICE-OHMS technique under cryogenic conditions (72~K). It is for the first time that a Lamb dip of a molecular quadrupole transition is recorded. At low (150-200 W) saturation powers a single narrow Lamb dip is observed, ruling out an underlying recoil doublet of 140 kHz. Studies of Doppler-detuned resonances show that the red-shifted recoil component can be made visible for low pressures and powers, and prove that the narrow Lamb dip must be interpreted as the blue recoil component. A transition frequency of 252\,016\,361\,164\,(8) kHz is extracted, which is off by -2.6 (1.6) MHz from molecular quantum electrodynamical calculations therewith providing a challenge to theory.

physics.atom-ph↗

arXiv2023

Novel spin-precession method for sensitive EDM searches

We demonstrate a spin-precession method to observe and analyze multi-level coherence between all hyperfine levels in the $X ^2\Sigma^+,N=0$ ground state of barium monofluoride ($^{138}$Ba$^{19}$F). The signal is sensitive to the state-preparation Rabi frequency and external electric and magnetic fields applied in searches for a permanent electric dipole moment (EDM). In the obtained interference spectrum, the electric field and Rabi frequency become observable simultaneously with the EDM. This method reduces systematic biases and the number of auxiliary measurements for such precision measurements.

physics.atom-ph↗

arXiv2023

Spectroscopic study of the F$^1\Sigma_g^+$ outer well state in H$_2$, HD and D$_2$

Two-photon UV-photolysis of hydrogen sulfide molecules is applied to produce hydrogen molecules in highly excited vibrational levels in the \X\ electronic ground state, up to the dissociation energy and into the quasibound region. Photolysis precursors H$_2$S, HDS and D$_2$S are used to produce vibrationally hot H$_2$, HD and D$_2$. The wave function density at large internuclear separation is excited via two-photon transitions in the \F\ - \X\ system to probe ro-vibrational levels in the first excited \F\ outer well state of \emph{gerade} symmetry. Combining with accurate knowledge of the \X($v,J$) levels from advanced ab initio calculations, energies of rovibrational levels in the \F\ state are determined. For the H$_2$ isotopologue a three-laser scheme is employed yielding level energies at accuracies of $4 \times 10^{-3}$ \wn\ for F($v=0,J$) up to $J=21$ and for some low $J$ values of F($v=1$). A two-laser scheme was applied to determine level energies in H$_2$ for F($v=0-4$) levels as well as for various F levels in HD and D$_2$, also up to large rotational quantum numbers. The latter measurements in the two-laser scheme are performed at lower resolution and the accuracy is strongly limited to 0.5 \wn\ by ac-Stark effects. For H$_2$ a new quasibound resonance ($v=6$, $J=23$) is detected through the Q(23) and O(23) transitions in the F0-X6 band. The experimental results on F($v,J$) level energies are compared with previously reported theoretical results from multi-channel quantum-defect calculations as well as with results from newly performed nonadiabatic quantum calculations.

physics.atom-ph↗

arXiv2022

Rotational level spacings in HD from vibrational saturation spectroscopy

The R(1), R(3) and P(3) ro-vibrational transitions in the (2-0) overtone band of the HD molecule are measured in Doppler-free saturation using the technique of NICE-OHMS spectroscopy. For the P(3) line, hitherto not observed in saturation, we report a frequency of $203\,821\,936\,805\,(60)$ kHz. The dispersive line shapes observed in the three spectra show strong correlations, allowing for extraction of accurate information on rotational level spacings. This leads to level spacings of $Δ_{(J=3)-(J=1)}= 13\,283\,245\,098\,(30)$ kHz in the $v=0$ ground state, and $Δ_{(J=4)-(J=2)}= 16\,882\,368\,179\,(20)$ kHz in the $v=2$ excited vibration in HD. These results show that experimental values for the rotational spacings are consistently larger than those obtained with advanced ab initio theoretical calculations at 1.5$σ$, where the uncertainty is determined by theory. The same holds for the vibrational transitions where systematic deviations of 1.7-1.9$σ$ are consistently found for the five lines accurately measured in the (2-0) band.

physics.atom-ph↗

arXiv2022

Fourier-transform spectroscopy of $^{13}$C$^{17}$O and deperturbation analysis of the A$^1Π$ ($ν$ = 0 - 3) levels

The high-resolution B$^1Σ^+$ - A$^1Π$ (0, 0) and (0, 3) emission bands of the less-abundant $^{13}$C$^{17}$O isotopologue have been investigated by Fourier-transform spectroscopy in the visible region using a Bruker IFS 125HR spectrometer at an accuracy 0.003 cm$^{-1}$. These spectra are combined with high-resolution photoabsorption measurements of the $^{13}$C$^{17}$O B$^1Σ^+$ $\leftarrow$ X$^1Σ^+$ (0, 0), B$^1Σ^+$ $\leftarrow$ X$^1Σ^+$ (1, 0) and C$^1Σ^+$ $\leftarrow$ X$^1Σ^+$ (0, 0) bands recorded with an accuracy of 0.01 cm$^{-1}$ using the vacuum ultraviolet Fourier-transform spectrometer, installed on the DESIRS beamline at the SOLEIL synchrotron. In the studied 17,950 - 22,500 cm$^{-1}$ and 86,800 - 92,100 cm$^{-1}$ regions, 480 transitions have been measured. These new experimental data were combined with data from the C $\to$ A and B $\to$ A systems, previously analyzed in 13C17O. The frequencies of 1003 transitions derived from 12 bands were used to analyze the perturbations between the A$^1Π$ ($ν$ = 0 - 3) levels and rovibrational levels of the d$^3Δ_i$, e$^3Σ^-$, a$'{}^3Σ^+$, I$^1Σ^-$ and D$^1Δ$ states as well as to a preliminary investigation of weak irregularities that appear in the B$^1Σ^+$ ($ν$ = 0) level. Deperturbed molecular constants and term values of the A$^1Π$ state were obtained. The spin-orbit and L-uncoupling interaction parameters as well as isotopologue-independent spin-orbit and rotation-electronic perturbation parameters were derived.

physics.chem-ph↗

arXiv2022

Proton-Electron Mass Ratio from Laser Spectroscopy of HD$^+$ at the Part-Per-Trillion Level

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.

physics.atom-ph↗

arXiv2022

Improved Ionization and Dissociation Energies of the Deuterium Molecule

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 $1.6σ$) with recent ab initio calculations of the 4-particle nonadiabatic relativistic energy and of quantum-electrodynamic corrections up to order $mα^6$. This result constitutes a test of quantum electrodynamics in the molecular domain, while a perspective is opened to determine nuclear charge radii from molecules.

physics.atom-ph↗

arXiv2021

Chirp-compensated pulsed titanium-sapphire laser system for precision spectroscopy

Active frequency-chirp compensation for a narrowband pulsed Titanium-Sapphire laser system is demonstrated using an intra-cavity electro-optic modulator resulting in improved spectral resolution and stability. With referencing to an optical frequency comb and further residual frequency chirp detection from shot-to-shot measurements, the resulting laser pulses are frequency up-converted for high-precision spectroscopy measurements in the VUV regime, where the relative uncertainty contribution due to frequency chirp is pushed to the $5 \times 10^{-11}$ level.

physics.optics↗

arXiv2021

Precision measurement of quasi-bound resonances in H$_2$ and the H + H scattering length

Quasi-bound resonances of H$_2$ are produced via two-photon photolysis of H$_2$S molecules as reactive intermediates or transition states, and detected before decay of the parent molecule into three separate atoms. As was previously reported [K.F. Lai et al., Phys. Rev. Lett. 127, 183001 (2021)] four centrifugally bound quantum resonances with lifetimes of multiple $μ$s, lying energetically above the dissociation limit of the electronic ground state X$^1Σ_g^+$ of H$_2$, were observed as X($v,J$) = (7,21)$^*$, (8,19)$^*$, (9,17)$^*$, and (10,15)$^*$, while also the short-lived ($\sim 1.5$ ns) quasi-bound resonance X(11,13)$^*$ was probed. The present paper gives a detailed account on the identification of the quasi-bound or shape resonances, based on laser detection via F-X two-photon transitions, and their strongly enhanced Franck-Condon factors due to the shifting of the wave function density to large internuclear separation. In addition, the assignment of the rotational quantum number is verified by subsequent multi-step laser excitation into autoionization continuum resonances. Existing frameworks of full-fledged ab initio computations for the bound region in H$_2$, including Born-Oppenheimer, adiabatic, non-adiabatic, relativistic and quantum-electrodynamic contributions, are extended into the energetic range above the dissociation energy. These comprehensive calculations are compared to the accurate measurements of energies of quasi-bound resonances, finding excellent agreement. Etc.

physics.atom-ph↗

arXiv2021

Shape resonances in H$_2$ as photolysis reaction intermediates

Shape resonances in H$_2$, produced as reaction intermediates in the photolysis of H$_2$S precursor molecules, are measured in a half-collision approach. Before desintegrating into two ground state H atoms, the reaction is quenched by two-photon Doppler-free excitation to the F electronically excited state of H$_2$. For $J=13,15,17,19$ and 21, resonances with lifetimes in the range of nano to milliseconds were observed with an accuracy of 30~MHz (1.4~mK). The experimental resonance positions are found to be in excellent agreement with theoretical predictions when nonadiabatic and quantum electrodynamical corrections are included. This is the first time such effects are observed in collisions between neutral atoms. From the potential energy curve of the H$_2$ molecule, now tested at high accuracy over a wide range of internuclear separations, the s-wave scattering length for singlet H(1s)+H(1s) scattering is determined at $a = 0.2735^{39}_{31}~a_0$.

physics.atom-ph↗

arXiv2021

A study of submillimeter methanol absorption toward PKS1830-211: Excitation, invariance of the proton-electron mass ratio, and systematics

Methanol is an important tracer to probe physical and chemical conditions in the interstellar medium of galaxies. Methanol is also the most sensitive target molecule for probing potential space-time variations of the proton-electron mass ratio, mu, a dimensionless constant of nature. We present an extensive ALMA study of the strongest submillimeter absorption lines of methanol [...] in the z=0.89 molecular absorber toward PKS1830-211, the only high-redshift object in which methanol has been detected. Our goals are to constrain the excitation of the methanol lines and to investigate the cosmological invariance of mu based on their relative kinematics. [...] We explore methanol excitation by running the non local thermal equilibrium radiative transfer code RADEX [...] The excitation analysis points to a cool (~10-20 K) and dense (~10^{4-5} cm-3) methanol gas. [...] In addition, we measure an abundance ratio A/E = 1.0 +/- 0.1, an abundance ratio CH3OH/H2 ~ 2 x 10^{-8}, and a 12CH3OH/13CH3OH ratio 62 +/- 3. Our analysis shows that the bulk velocities of the different transitions are primarily correlated with the observing epoch due to morphological changes in the background quasar's emission. There is a weaker correlation between bulk velocities and the lower level energies of the transitions, which could be a signature of temperature-velocity gradients in the absorbing gas. As a result, we do not find evidence for variations of mu, and we estimate Dmu/mu = (-1.8 +/- 1.2) x 10^{-7} at 1sigma from our multivariate linear regression. We set a robust upper limit | \Dmu/mu | < 3.6 x 10^{-7} (3sigma) for the invariance of mu at a look-back time of half the present age of the Universe. Our analysis highlights that systematics need to be carefully taken into account in future radio molecular absorption studies aimed at testing Dmu/mu below the 10^{-7} horizon. (Abridged)

astro-ph.GA↗

arXiv2021

Characterization of angularly resolved EUV emission from 2-$μ$m-wavelength laser-driven Sn plasmas using preformed liquid disk targets

The emission properties of tin plasmas, produced by the irradiation of preformed liquid tin targets by several-ns-long 2-$μ$m-wavelength laser pulses, are studied in the extreme ultraviolet (EUV) regime. In a two-pulse scheme, a pre-pulse laser is first used to deform tin microdroplets into thin, extended disks before the main (2$μ$m) pulse creates the EUV-emitting plasma. Irradiating 30- to 300-$μ$m-diameter targets with 2-$μ$m laser pulses, we find that the efficiency in creating EUV light around 13.5nm follows the fraction of laser light that overlaps with the target. Next, the effects of a change in 2-$μ$m drive laser intensity (0.6-1.8$\times 10^{11}$W/cm$^2$) and pulse duration (3.7-7.4ns) are studied. It is found that the angular dependence of the emission of light within a 2\% bandwidth around 13.5nm and within the backward 2$π$ hemisphere around the incoming laser beam is almost independent of intensity and duration of the 2-$μ$m drive laser. With increasing target diameter, the emission in this 2\% bandwidth becomes increasingly anisotropic, with a greater fraction of light being emitted into the hemisphere of the incoming laser beam. For direct comparison, a similar set of experiments is performed with a 1-$μ$m-wavelength drive laser. Emission spectra, recorded in a 5.5-25.5nm wavelength range, show significant self-absorption of light around 13.5nm in the 1-$μ$m case, while in the 2-$μ$m case only an opacity-related broadening of the spectral feature at 13.5nm is observed. This work demonstrates the enhanced capabilities and performance of 2-$μ$m-driven plasmas produced from disk targets when compared to 1-$μ$m-driven plasmas, providing strong motivation for the use of 2-$μ$m lasers as drive lasers in future high-power sources of EUV light.

physics.plasm-ph↗