arXiv subjects

W. Ubachs

Publications and source records attributed to W. Ubachs.

At least 37 records · Page 2Linked to original sources

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↗

arXiv2021

Photolysis production and spectroscopic investigation of the highest vibrational states in H$_2$ (X$^1Σ_g^+$ $v=13,14$)

Rovibrational quantum states in the $X^1Σ_g^+$ electronic ground state of H$_2$ are prepared in the $v=13$ vibrational level up to its highest bound rotational level $J=7$, and in the highest bound vibrational level $v=14$ (for $J=1$) by two-photon photolysis of H$_2$S. These states are laser-excited in a subsequent two-photon scheme into $F^1Σ_g^+$ outer well states, where the assignment of the highest ($v,J$) states is derived from a comparison of experimentally known levels in \F, combined with \emph{ab initio} calculations of \X\ levels. The assignments are further verified by excitation of $F^1Σ_g^+$ population into autoionizing continuum resonances which are compared with multi-channel quantum defect calculations. Precision spectroscopic measurements of the $F-X$ intervals form a test for the \emph{ab initio} calculations of ground state levels at high vibrational quantum numbers and large internuclear separations, for which agreement is found.

physics.chem-ph↗

arXiv2020

Characterization of 1- and 2-$μ$m-wavelength laser-produced microdroplet-tin plasma for generating extreme-ultraviolet light

Experimental spectroscopic studies are presented, in a 5.5--25.5nm extreme-ultraviolet (EUV) wavelength range, of the light emitted from plasma produced by the irradiation of tin microdroplets by 5-ns-pulsed, 2-$μ$m-wavelength laser light. Emission spectra are compared to those obtained from plasma driven by 1-$μ$m-wavelength Nd:YAG laser light over a range of laser intensities spanning approximately $0.3-5 \times 10^{11}$Wcm$^{-2}$, under otherwise identical conditions. Over this range of drive laser intensities, we find that similar spectra and underlying plasma charge state distributions are obtained when keeping the ratio of 1-$μ$m to 2-$μ$m laser intensities fixed at a value of 2.1(6), which is in good agreement with RALEF-2D radiation-hydrodynamic simulations. Our experimental findings, supported by the simulations, indicate an approximately inversely proportional scaling $\sim λ^{-1}$ of the relevant plasma electron density, and of the aforementioned required drive laser intensities, with drive laser wavelength $λ$. This scaling also extends to the optical depth that is captured in the observed changes in spectra over a range of droplet diameters spanning 16-51$μ$m at a constant laser intensity that maximizes the emission in a 2\% bandwidth around 13.5nm relative to the total spectral energy, the bandwidth relevant for EUV lithography. The significant improvement of the spectral performance of the 2-$μ$m- vs 1-$μ$m driven plasma provides strong motivation for the development of high-power, high-energy near-infrared lasers to enable the development of more efficient and powerful sources of EUV light.

physics.plasm-ph↗

arXiv2020

Fourier-transform VUV spectroscopy of $^{14,15}$N and $^{12,13}$C

Accurate Fourier-transform spectroscopic absorption measurements of vacuum ultraviolet transitions in atomic nitrogen and carbon were performed at the Soleil synchrotron. For $^{14}$N transitions from the $2s^22p^3\,^4$S$_{3/2}$ ground state and from the $2s^22p^3\,^2$P and $^2$D metastable states were determined in the $95 - 124$ nm range at an accuracy of $0.025\,\mathrm{cm}^{-1}$. Combination of these results with data from previous precision laser experiments in the vacuum ultraviolet range reveal an overall and consistent offset of -0.04 \wn\ from values reported in the NIST database. %The splitting of the $2s^22p^3\,^4$S$_{3/2}$ -- %$2s2p^4\,^4$P$_{5/2,3/2,1/2}$ The splittings of the $2s^22p^3\,^4$S$_{3/2}$ -- $2s2p^4\,^4$P$_{J}$ transitions are well-resolved for $^{14}$N and $^{15}$N and isotope shifts determined. While excitation of a $2p$ valence electron yields very small isotope shifts, excitation of a $2s$ core electron results in large isotope shifts, in agreement with theoretical predictions. For carbon six transitions from the ground $2s^22p^2\,^3$P$_{J}$ and $2s^22p3s\, ^3$P$_{J}$ excited states at $165$ nm are measured for both $^{12}$C and $^{13}$C isotopes.

physics.atom-ph↗

arXiv2020

Two-photon Doppler-free ultraviolet laser spectroscopy on sulphur atoms

The $3p^{4}$ $^{3}$P$_{J}$ - $3p^{3}4p$ $^{3}$P$_{J}$ transition in the sulphur atom is investigated in a precision two-photon excitation scheme under Doppler-free and collision-free circumstances yielding an absolute accuracy of 0.0009 cm$^{-1}$, using a narrowband pulsed laser. This verifies and improves the level separations between amply studied odd parity levels with even parity levels in S I. An improved value for the $^{3}$P$_{2}$ - $^{3}$P$_{1}$ ground state fine structure splitting is determined at $396.0564$ (7) cm$^{-1}$. A $^{34}$S - $^{32}$S atomic isotope shift was measured from combining time-of-flight mass spectrometry with laser spectroscopy.

physics.atom-ph↗

arXiv2020

Lamb-peak spectrum of the HD (2-0) P(1) line

A saturation spectroscopy measurement of the P(1) line of the ($2-0$) band in HD is performed in a sensitive cavity-enhanced optical setup involving frequency comb calibration. The spectral signature is that of a Lamb-peak, in agreement with a density-matrix model description involving 9 hyperfine components and 16 crossover resonances of $Λ$-type. Comparison of the experimental spectra with the simulations yields a rovibrational transition frequency at 209,784,242,007 (20) kHz. Agreement is found with a first principles calculation in the framework of non-adiabatic quantum electrodynamics within 2$σ$, where the combined uncertainty is fully determined by theory.

physics.atom-ph↗

arXiv2020

Precision measurement of the fundamental vibrational frequencies of tritium-bearing hydrogen molecules: T$_2$, DT, HT

High-resolution coherent Raman spectroscopic measurements of all three tritium-containing molecular hydrogen isotopologues T$_2$, DT and HT were performed to determine the ground electronic state fundamental Q-branch ($v=0 \rightarrow 1, ΔJ = 0$) transition frequencies at accuracies of $0.0005$ cm$^{-1}$. An over hundred-fold improvement in accuracy over previous experiments allows the comparison with the latest ab initio calculations in the framework of Non-Adiabatic Perturbation Theory including nonrelativisitic, relativisitic and QED contributions. Excellent agreement is found between experiment and theory, thus providing a verification of the validity of the NAPT-framework for these tritiated species. While the transition frequencies were corrected for ac-Stark shifts, the contributions of non-resonant background as well as quantum interference effects between resonant features in the nonlinear spectroscopy were quantitatively investigated, also leading to corrections to the transition frequencies. Methods of saturated CARS with the observation of Lamb dips, as well as the use of continuous-wave radiation for the Stokes frequency were explored, that might pave the way for future higher-accuracy CARS measurements.

physics.chem-ph↗

arXiv2019

Lamb-dips and Lamb-peaks in the saturation spectrum of HD

The saturation spectrum of the R(1) transition in the (2-0) band in HD is found to exhibit a composite line shape, involving a Lamb-dip and a Lamb-peak. We propose an explanation for such behavior based on the effects of cross-over resonances in the hyperfine substructure, which is made quantitative in a density-matrix calculation. This resolves an outstanding discrepancy on the rovibrational R(1) transition frequency, which is now determined at 217 105 181 901 (50) kHz and in agreement with current theoretical calculations.

physics.atom-ph↗

arXiv2019

The spin-forbidden vacuum-ultraviolet absorption spectrum of 14N15N

Photoabsorption spectra of ${}^{14}{\rm N}{}^{15}{\rm N}$ were recorded at high resolution with a vacuum-ultraviolet Fourier-Transform spectrometer fed by synchrotron radiation in the range 81 to 100 nm. The combination of high column density ($3\times 10^{17}$ cm$^{-2}$) and low temperature (98 K) allowed for the recording of weak spin-forbidden absorption bands exciting levels of triplet character. The triplet states borrow intensity from ${}^1Π_u$ states of Rydberg and valence character while causing their predissociation. New predissociation linewidths and molecular constants are obtained for the states $C\,{}^3Π_u(v=7,8,14,15,16,21)$, $G\,{}^3Π_u(v=0,1,4)$, and $F\,{}^3Π_u(v=0)$. The positions and widths of these levels are shown to be well-predicted by a coupled-Schroedinger equation model with empirical parameters based on experimental data on ${}^{14}{\rm N}_2$ and ${}^{15}{\rm N}_2$ triplet levels.

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↗

arXiv2019

H$_2$/HD molecular data for analysis of quasar spectra in search of varying constants

Absorption lines of H$_2$ and HD molecules observed at high redshift in the line of sight towards quasars are a test ground to search for variation of the proton-to-electron mass ratio $μ$. For this purpose, results from astronomical observations are compared with a compilation of molecular data of the highest accuracy, obtained in laboratory studies as well as in first-principles calculations. Aims: A comprehensive line list is compiled for H$_2$ and HD absorption lines in the Lyman ($B^1Σ_u^+$ - $X^1Σ_g^+$) and Werner ($C^1Π_u$ - $X^1Σ_g^+$) band systems up to the Lyman cutoff at 912 Angstroms. Molecular parameters listed for each line $i$ are the transition wavelength $λ_i$, the line oscillator strength $f_i$, the radiative damping parameter of the excited state $Γ_i$, and the sensitivity coefficient $K_i$ for a variation of the proton-to-electron mass ratio. Methods: The transition wavelengths $λ_i$ for the H$_2$ and HD molecules are determined by a variety of advanced high-precision spectroscopic experiments involving narrowband vacuum ultraviolet lasers, Fourier-transform spectrometers, and synchrotron radiation sources. Results for the line oscillator strengths $f_i$, damping parameters $Γ_i$, and sensitivity coefficients $K_i$ are obtained in theoretical quantum chemical calculations. Results: A new list of molecular data is compiled for future analyses of cold clouds of hydrogen absorbers, specifically for studies of $μ$-variation from quasar data. The list is applied in a refit of quasar absorption spectra of B0642$-$5038 and J1237$+$0647 yielding constraints on a variation of the proton-to-electron mass ratio $Δμ/μ$ consistent with previous analyses.

astro-ph.CO↗

arXiv2018

Precision spectroscopy and comprehensive analysis of perturbations in the $A\,{}^1Π(v=0$) state of ${}^{\rm 13}$C${}^{\rm 18}$O

We have reinvestigated the A$^1Π$$(v=0)$ level of $^{13}$C$^{18}$O\ using new high-resolution spectra obtained via multi-photon laser excitation as well as with synchrotron-based Fourier-transform absorption spectroscopy of the A$^1Π-\textrm{X}^1Σ^+$$(0, 0)$, e$^3Σ^--\textrm{X}^1Σ^+$$(1, 0)$, d$^3Δ-\textrm{X}^1Σ^+$$(4, 0)$, a$'^3Σ^+-\textrm{X}^1Σ^+$$(9, 0)$, and \atX$(11, 0)$ bands. In addition, Fourier-transform emission spectroscopy in the visible range is performed on the ${\rm B}^1Σ^+-{\rm A}^1Π$$(0, 0)$ band. Spectra of the \BX$(0, 0)$ band are measured in order to tie information from the latter emission data to the level structure of A$^1Π$$(v=0)$. The high pressures in the absorption cell at the synchrotron and the high temperatures in the emission discharge permitted monitoring of high rotational quantum levels in A$^1Π$$(v=0)$ up to $J=43$. All information, in total over 900 spectral lines, was included in an effective-Hamiltonian analysis of the A$^1Π(v=0, J)$ levels that are directly perturbed by the e$\,^3Σ^-$$(v=1)$, d$^3\!Δ$$(v=4)$, a$'^3Σ^+$$(v=9)$, d$^3\!Δ$$(v=0)$, I$\,^1Σ^-$$(v=0, 1)$ close-lying levels and the e$\,^3Σ^-$$(v=0,2)$, d$^3\!Δ$$(v=3,5)$, a$'^3Σ^+$$(v=8,10)$ remote levels, as well being indirectly influenced by the a$^3Π$$(v=10, 11)$ state. The influence of nine further perturber levels and their interactions was investigated and are not significant for reproducing the present experimental data. This analysis leads to a much improved description in terms of molecular constants and interaction parameters, compared to previous studies of the same energy region for other CO isotopologues.

physics.atom-ph↗

arXiv2018

Energy Level Structure of Sn$^{3+}$ Ions

Laser-produced Sn plasma sources are used to generate extreme ultraviolet (EUV) light in state-of-the-art nanolithography. An ultraviolet and optical spectrum is measured from a droplet-based laser-produced Sn plasma, with a spectrograph covering the range 200 - 800 nm. This spectrum contains hundreds of spectral lines from lowly charged tin ions Sn$^{1+}$ - Sn$^{4+}$ of which a major fraction was hitherto unidentified. We present and identify a selected class of lines belonging to the quasi-one-electron, Ag-like ([Kr]$4d^{10} nl$ electronic configuration), Sn$^{3+}$ ion, linking the optical lines to a specific charge state by means of a masking technique. These line identifications are made with iterative guidance from COWAN code calculations. Of the 53 lines attributed to Sn$^{3+}$, some 20 were identified from previously known energy levels, and 33 lines are used to determine previously unknown level energies of 13 electronic configurations, i.e., $ 7p $, $ (7,8)d $, $ (5,6)f $, $ (6-8)g $, $ (6-8)h $, $ (7,8)i $. The consistency of the level energy determination is verified by the quantum-defect scaling procedure. The ionization limit of Sn$^{3+}$ is confirmed and refined to 328908.4 cm$^{-1}$ with an uncertainty of 2.1 cm$^{-1}$. The relativistic Fock space coupled cluster (FSCC) calculation of the measured level energies are generally in good agreement with experiment, but fail to reproduce the anomalous behavior of the $5d$ $^2$D and $nf$ $^2$F terms. By combining the strengths of FSCC, COWAN code calculations, and configuration interaction many-body perturbation theory (CI+MBPT), this behavior is shown to arise from interactions with doubly-excited configurations.

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↗

arXiv2018

Relativistic and QED effects in the fundamental vibration of T$_2$

The hydrogen molecule has become a test ground for quantum electrodynamical calculations in molecules. Expanding beyond studies on stable hydrogenic species to the heavier radioactive tritium-bearing molecules, we report on a measurement of the fundamental T$_2$ vibrational splitting $(v= 0 \rightarrow 1)$ for $J=0-5$ rotational levels. Precision frequency metrology is performed with high-resolution coherent anti-Stokes Raman spectroscopy at an experimental uncertainty of $10-12$~MHz, where sub-Doppler saturation features are exploited for the strongest transition. The achieved accuracy corresponds to a fifty-fold improvement over a previous measurement, and allows for the extraction of relativistic and QED contributions to T$_2$ transition energies.

physics.chem-ph↗

arXiv2018

Short-wavelength out-of-band EUV emission from Sn laser-produced plasma

We present the results of spectroscopic measurements in the extreme ultraviolet (EUV) regime (7-17 nm) of molten tin microdroplets illuminated by a high-intensity 3-J, 60-ns Nd:YAG laser pulse. The strong 13.5 nm emission from this laser-produced plasma is of relevance for next-generation nanolithography machines. Here, we focus on the shorter wavelength features between 7 and 12 nm which have so far remained poorly investigated despite their diagnostic relevance. Using flexible atomic code calculations and local thermodynamic equilibrium arguments, we show that the line features in this region of the spectrum can be explained by transitions from high-lying configurations within the Sn$^{8+}$-Sn$^{15+}$ ions. The dominant transitions for all ions but Sn$^{8+}$ are found to be electric-dipole transitions towards the $n$=4 ground state from the core-excited configuration in which a 4$p$ electron is promoted to the 5$s$ sub-shell. Our results resolve some long-standing spectroscopic issues and provide reliable charge state identification for Sn laser-produced plasma, which could be employed as a useful tool for diagnostic purposes.

physics.atom-ph↗

arXiv2017

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

Weak transitions in the (2,0) overtone band of the HD molecule at $λ= 1.38 \, μ$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.

physics.atom-ph↗

arXiv2017

Rayleigh-Brillouin light scattering spectroscopy of nitrous oxide (N$_2$O)

High signal-to-noise and high-resolution light scattering spectra are measured for nitrous oxide (N$_2$O) gas at an incident wavelength of 403.00 nm, at 90$^\circ$ scattering, at room temperature and at gas pressures in the range $0.5-4$ bar. The resulting Rayleigh-Brillouin light scattering spectra are compared to a number of models describing in an approximate manner the collisional dynamics and energy transfer in this gaseous medium of this polyatomic molecular species. The Tenti-S6 model, based on macroscopic gas transport coefficients, reproduces the scattering profiles in the entire pressure range at less than 2\% deviation at a similar level as does the alternative kinetic Grad's 6-moment model, which is based on the internal collisional relaxation as a decisive parameter. A hydrodynamic model fails to reproduce experimental spectra for the low pressures of 0.5-1 bar, but yields very good agreement ($< 1$\%) in the pressure range $2-4$ bar. While these three models have a different physical basis the internal molecular relaxation derived can for all three be described in terms of a bulk viscosity of $η_b \sim (6 \pm 2) \times 10^{-5}$ Pa$\cdot$s. A 'rough-sphere' model, previously shown to be effective to describe light scattering in SF$_6$ gas, is not found to be suitable, likely in view of the non-sphericity and asymmetry of the N-N-O structured linear polyatomic molecule.

physics.flu-dyn↗