arXiv subjects

H. L. Bethlem

Publications and source records attributed to H. L. Bethlem.

15 recordsLinked to original sources

arXiv2026

Spectroscopy of $^4$He at 0.25 ppt Uncertainty and Improved Alpha-Helion Charge-Radius Difference Determination

High-precision spectroscopy of simple atomic systems can be used to advance the theory of atomic energy levels but can also serve as a sensitive probe of nuclear charge radii. For this last purpose, we report an improved measurement of the $2\,^3{S}_1 \to 2\,^1{S}_0$ transition frequency in $^4$He with 48 Hz uncertainty (0.25 ppt), using a Bose-Einstein condensed sample confined in a magic-wavelength optical dipole trap. A systematic Doppler shift from condensate motion is suppressed by time-resolved ion detection, and the transition frequency is calibrated via a White Rabbit link to a remote active hydrogen maser clock. Combined with previous $^3$He measurements and improved theory, we obtain the most precise determination to date of the charge-radius difference between the helion and alpha particle ($r_{h}^2 -r_α^2$) of $1.0676(10)\text{fm}^2$. This is consistent with other recent determinations and confirms that the current discrepancy between QED theory and experimentally observed ionization energies of excited states in helium is not apparent in the isotope shift.

physics.atom-ph↗

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 $A^2Π$ $\leftarrow$ $X^2Σ^+$ transition in BaF

High-resolution spectroscopy on the $A^2Π$ - $X^2Σ^+$ 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 $X^2Σ^+$ ground and $A^2Π$ 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 $X^2Σ^+$($v=0,1$) and $A^2Π$($v=0,1$) levels are determined, with improved accuracy for the $T_{v',v''}$ band origins and spin-orbit interaction constants for the $A^2Π$ 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↗

arXiv2023

The alpha and helion particle charge radius difference from spectroscopy of quantum-degenerate helium

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 $r^2_h - r^2_α = 1.0757(15)\ \mathrm{fm^2}$ 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$σ$ is found with a determination (arXiv:2305.11679) based on spectroscopy of muonic helium ions.

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 $X ^2Σ^+,N=0$ 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↗

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

Deceleration and trapping of SrF molecules

We report on the electrostatic trapping of neutral SrF molecules. The molecules are captured from a cryogenic buffer-gas beam source into the moving traps of a 4.5 m long traveling-wave Stark decelerator. The SrF molecules in $X^2Σ^+(v=0, N=1)$ state are brought to rest as the velocity of the moving traps is gradually reduced from 190 m/s to zero. The molecules are held for up to 50 ms in multiple electric traps of the decelerator. The trapped packets have a volume (FWHM) of 1 mm$^{3}$ and a velocity spread of 5(1) m/s which corresponds to a temperature of $60(20)$ mK. Our result demonstrates a factor 3 increase in the molecular mass that has been Stark-decelerated and trapped. Heavy molecules (mass$>$100 amu) offer a highly increased sensitivity to probe physics beyond the Standard Model. This work significantly extends the species of neutral molecules of which slow beams can be created for collision studies, precision measurement and trapping experiments.

physics.atom-ph↗

arXiv2019

Lifetime Measurements of the $A^2Π_{1/2}$ and $A^2Π_{3/2}$ States in BaF

Time resolved detection of laser induced fluorescence from pulsed excitation of electronic states in barium monofluoride (BaF) molecules has been performed in order to determine the lifetimes of the $A^2Π_{1/2}$ and $A^2Π_{3/2}$ states. The method permits control over experimental parameters such that systematic biases in the interpretation of the data can be controlled to below $10^{-3}$ relative accuracy. The statistically limited values for the lifetimes of the $A^2Π_{1/2}(ν=0)$ and $A^2Π_{3/2}(ν=0)$ states are 57.1(3) ns and 47.9(7)~ns, respectively. The ratio of these values is in good agreement with scaling for the different excitation energies. The investigated molecular states are of relevance for an experimental search for a permanent electric dipole moment (EDM) of the electron in BaF.

physics.atom-ph↗

arXiv2018

Dissociation energy of the hydrogen molecule at 10$^{-9}$ accuracy

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.

physics.chem-ph↗

arXiv2017

Testing the variability of the proton-to-electron mass ratio from observations of methanol in the dark cloud core L1498

The dependence of the proton-to-electron mass ratio, mu, on the local matter density was investigated using methanol emission in the dense dark cloud core L1498. Towards two different positions in L1498, five methanol transitions were detected and an extra line was tentatively detected at a lower confidence level in one of the positions. The observed centroid frequencies were then compared with their rest frame frequencies derived from least-squares fitting to a large data set. Systematic effects, as the underlying methanol hyperfine structure and the Doppler tracking of the telescope, were investigated and their effects were included in the total error budget. The comparison between the observations and the rest frame frequencies constrains potential mu variation at the level of Dmu/mu < 6 x 10^(-8), at a 3 sigma confidence level. For the dark cloud we determine a total CH3OH (A+E) beam averaged column density of 3-4 x 10^(12) cm(-2) (within roughly a factor of two), an E- to A-type methanol column density ratio of N(A-CH3OH)/N(E-CH3OH) = 1.00 +/- 0.15, a density of n(H2) = 3 x 10^5 cm^(-3) (again within a factor of two), and a kinetic temperature of Tkin = 6 +/- 1 K. In a kinetic model including the line intensities observed for the methanol lines, the n(H2) density is higher and the temperature is lower than that derived in previous studies based on different molecular species; the intensity of the 1_0 --> 1_-1 E line strength is not well reproduced.

astro-ph.CO↗

arXiv2014

Constraints on changes in the proton-electron mass ratio using methanol lines

We report Karl G. Jansky Very Large Array (VLA) absorption spectroscopy in four methanol (CH$_3$OH) lines in the $z = 0.88582$ gravitational lens towards PKS1830-211. Three of the four lines have very different sensitivity coefficients $K_μ$ to changes in the proton-electron mass ratio $μ$; a comparison between the line redshifts thus allows us to test for temporal evolution in $μ$. We obtain a stringent statistical constraint on changes in $μ$ by comparing the redshifted 12.179 GHz and 60.531 GHz lines, $[Δmu/μ] \leq 1.1 \times 10^{-7}$ ($2σ$) over $0 < z \leq 0.88582$, a factor of $\approx 2.5$ more sensitive than the best earlier results. However, the higher signal-to-noise ratio (by a factor of $\approx 2$) of the VLA spectrum in the 12.179 GHz transition also indicates that this line has a different shape from that of the other three CH$_3$OH lines (at $> 4σ$ significance). The sensitivity of the above result, and that of all earlier CH$_3$OH studies, is thus likely to be limited by unknown systematic errors, probably arising due to the frequency-dependent structure of PKS1830-211. A robust result is obtained by combining the three lines at similar frequencies, 48.372, 48.377 and 60.531 GHz, whose line profiles are found to be in good agreement. This yields the $2σ$ constraint $[Δμ/μ] \lesssim 4 \times 10^{-7}$, the most stringent current constraint on changes in $μ$. We thus find no evidence for changes in the proton-electron mass ratio over a lookback time of $\approx 7.5$ Gyrs.

astro-ph.CO↗

arXiv2014

Ramsey-type microwave spectroscopy on CO ($a^3Π$)

Using a Ramsey-type setup, the lambda-doublet transition in the $J=1,\, Ω=1$ level of the $a^3Π$ state of CO was measured to be 394 064 870(10) Hz. In our molecular beam apparatus, a beam of metastable CO is prepared in a single quantum level by expanding CO into vacuum and exciting the molecules using a narrow-band UV laser system. After passing two microwave zones that are separated by 50 cm, the molecules are state-selectively deflected and detected 1 meter downstream on a position sensitive detector. In order to keep the molecules in a single $m_J^B$ level, a magnetic bias field is applied. We find the field-free transition frequency by taking the average of the $m_J^B = +1 \rightarrow m_J^B = +1$ and $m_J^B = -1 \rightarrow m_J^B = -1$ transitions, which have an almost equal but opposite Zeeman shift. The accuracy of this proof-of-principle experiment is a factor of 100 more accurate than the previous best value obtained for this transition.

physics.chem-ph↗

arXiv2014

Traveling-wave deceleration of SrF molecules

We report on the production, deceleration and detection of a SrF molecular beam. The molecules are captured from a supersonic expansion and are decelerated in the X$^2Σ^+ (v=0, N=1)$ state. We demonstrate the removal of up to 40% of the kinetic energy with a 2 meter long modular traveling-wave decelerator. Our results demonstrate a crucial step towards the preparation of ultracold gases of heavy diatomic molecules for precision spectroscopy.

physics.atom-ph↗

arXiv2003

Slowing heavy, ground-state molecules using an alternating gradient decelerator

Cold supersonic beams of molecules can be slowed down using a switched sequence of electrostatic field gradients. The energy to be removed is proportional to the mass of the molecules. Here we report deceleration of YbF, which is 7 times heavier than any molecule previously decelerated. We use an alternating gradient structure to decelerate and focus the molecules in their ground state. We show that the decelerator exhibits the axial and transverse stability required to bring these molecules to rest. Our work significantly extends the range of molecules amenable to this powerful method of cooling and trapping.

physics.atom-ph↗