The hydrogen-like muonium atom ($μ^+e^-$) consists of a positive muon ($μ^+$) and an electron ($e^-$). Since it was first observed by Hughes et al. in 1960, a series of precision experiments could be carried out testing bound state Quantum Electrodynamics (QED) and the nature of the muon as a point-like leptonic particle. Precision values for fundamental constants could be obtained, including the fine structure constant $α$ and the muon's magnetic moment $μ_μ$. Since no internal structure could be revealed for leptons down to dimensions of $10^{-18}$m, the accuracy of theoretical calculations of term energies is higher than for the natural hydrogen atom and its isotopes deuterium and tritium as well as exotic hydrogen-like systems which contain hadrons. Internal structure effects of these particles spoil the precision of theoretical results. Of particular interest for precision muonium experiments, which are carried out in order to test standard theory and to extract accurate values for fundamental constants, are the ground state hyperfine structure splitting $Δν_{HFS}$ and the 1s-2s interval $Δν_{1s2s}$. Both cases involve the n=1 ground state in which the atoms can be produced in sufficient quantities.
The electromagnetic interactions of electrons and muons can be described to very high accuracy within the framework of standard theory, in particular within the hydrogen-like muonium atom. Therefore precision measurements allow to test basic interactions in physics and to search for yet unknown forces. Accurate values for fundamental constants can be obtained. Results from experiments on the ground state hyperfine structure and the 1s-2s intervals in muonium are described together with their relations to a new measurement of the muon magnetic anomaly.
We present the status and the prospects of the ongoing efforts to improve the measurements of the 1S-2S transition in positronium and muonium. These purely leptonic systems represent ideal objects to test bound-state QED to high precision and the Standard-Model Extension.
A new measurement of the 1S-2S energy splitting of muonium by Doppler-free two-photon spectroscopy has been performed at the Rutherford Appleton Laboratory in Chilton, Didcot, UK. Increased accuracy is expected compared to a previous experiment. Spectroscopy of this transistion promises an improvement of the muon mass value.
Positronium and Muonium are purely leptonic atoms and hence free of an internal sub-structure. This qualifies them as potentially well suited systems to probe the existence of physics beyond the Standard Model. We hence carry out a comprehensive study of the sensitivity of current Positronium and Muonium precision spectroscopy to several new physics scenarios. By taking properly into account existing experimental and astrophysical probes, we define clear experimental targets to probe new physics via precise spectroscopy. For Positronium we find that, in order for the spectroscopy bounds to rea…
We show that muonium spectroscopy in the coming years can reach a precision high enough to determine the anomalous magnetic moment of the muon below one part per million (ppm). Such an independent determination of muon g-2, which is not limited by hadronic uncertainties, would certainly shed light on the 2ppm difference currently observed between spin-precession measurements and (R-ratio based) Standard Model predictions. The magnetic dipole interaction between electrons and (anti)muons bound in muonium gives rise to a hyperfine splitting (HFS) of the ground state which is sensitive to the muo…
A hydrogen-like atom consisting of a positive muon and an electron is known as muonium. It is a near-ideal two-body system for a precision test of bound-state theory and fundamental symmetries. The MuSEUM collaboration performed a new precision measurement of the muonium ground-state hyperfine structure at J-PARC using a high-intensity pulsed muon beam and a high-rate capable positron counter. The resonance of hyperfine transition was successfully observed at a near-zero magnetic field, and the muonium hyperfine structure interval of $ν_{\text{HFS}}$ = 4.463302(4) GHz was obtained with a relat…
We present a new experiment, Mu-MASS, aiming for a 1000-fold improvement in the determination of the 1S-2S transition frequency of Muonium (M), the positive-muon/electron bound state. This substantial improvement beyond the current state-of-the-art relies on the novel cryogenic M converters and confinement techniques we developed, on the new excitation and detection schemes which we implemented for positronium spectroscopy and the tremendous advances in generation of UV radiation. This experiment is planned to be performed at the Paul Scherrer Institute (PSI). Interesting anomalies in the muon…
As a new method to determine the resonance frequency, Rabi-oscillation spectroscopy has been developed. In contrast to the conventional spectroscopy which draws the resonance curve, Rabi-oscillation spectroscopy fits the time evolution of the Rabi oscillation. By selecting the optimized frequency, it is shown that the precision is twice as good as the conventional spectroscopy with a frequency sweep. Furthermore, the data under different conditions can be treated in a unified manner, allowing more efficient measurements for systems consisting of a limited number of short-lived particles produc…
We report the achievement of spatial confinement of muonium atoms (the bound state of a positive muon and an electron). Muonium emitted into vacuum from mesoporous silica reflects between two SiO$_2$ confining surfaces separated by 1 mm. From the data, one can extract that the reflection probability on the confining surfaces kept at 100 K is about 90% and the reflection process is well described by a cosine law. This technique enables new experiments with this exotic atomic system and is a very important step towards a measurement of the 1S-2S transition frequency using continuous wave laser s…
A low-emittance, high-intensity atomic beam of muonium ($\mathrm{M}=μ^+ + \mathrm{e}^-$) using superfluid helium as muon-to-muonium converter is being developed at the Paul Scherrer Institute (PSI). This beam could advance laser spectroscopy of muonium and allow the first atomic interferometry experiments for the direct observation of the M gravitational interaction. In this paper, we describe the development of compact detection schemes which resulted in the background-suppressed observation of atomic muonium in vacuum, and can be adapted for cryogenic measurements. Using these setups, we com…
We report a new measurement of the $n=2$ Lamb shift in Muonium using microwave spectroscopy. Our result of $1047.2(2.3)_\textrm{stat}(1.1)_\textrm{syst}$ MHz comprises an order of magnitude improvement upon the previous best measurement. This value matches the theoretical calculation within one standard deviation allowing us to set limits on CPT violation in the muonic sector, as well as on new physics coupled to muons and electrons which could provide an explanation of the muon $g-2$ anomaly.
We present a brief overview of precision tests of bound state QED and mainly pay our attention to laser spectroscopy as an appropriate tool for these tests. We particularly consider different precision tests of bound state QED theory based on the laser spectroscopy of optical transitions in hydrogen, muonium and positronium and related experiments.
Hitherto unknown elementary particles can be searched for with atomic spectroscopy. We conduct such a search using a potential that results from the longitudinal polarization of a pseudovector particle. We show that such a potential, inversely proportional to the boson's mass squared, $V \propto 1/M^2$, can stay finite at $M \to 0$ if the theory is renormalizable. We also look for a pseudoscalar boson, which induces a contact spin-dependent potential that does not contribute to new forces searched for in experiments with macroscopic objects, but may be seen in atomic spectroscopy. We extract l…
High resolution spectroscopy of the hydrogen atom takes on particular importance in the new SI, as it allows to accurately determine fundamental constants, such as the Rydberg constant and the proton charge radius. Recently, the second most precisely measured transition frequency in hydrogen, 1S - 3S, was obtained in our group. In the context of the Proton Radius Puzzle, this result calls for further investigation.
We describe the design and realization of a scheme for uv laser spectroscopy of singly-ionized iron (Fe II) with very high resolution. A buffer-gas cooled laser ablation source is used to provide a plasma close to room temperature with a high density of Fe II. We combine this with a scheme for pulsed-laser saturation spectroscopy to yield sub-Doppler resolution. In a demonstration experiment, we have examined an Fe II transition near 260 nm, attaining a linewidth of about 250 MHz. The method is well-suited to measuring transition frequencies and hyperfine structure. It could also be used to me…
We have performed sub-Doppler spectroscopy on the narrow intercombination line of cold calcium atoms using the amplified output of a femtosecond laser frequency comb. Injection locking of a 657-nm diode laser with a femtosecond comb allows for two regimes of amplification, one in which many lines of the comb are amplified, and one where a single line is predominantly amplified. The output of the laser in both regimes was used to perform kilohertz-level spectroscopy. This experiment demonstrates the potential for high-resolution absolute-frequency spectroscopy over the entire spectrum of the fr…
We report on Doppler-free continuous-wave optical UV-spectroscopy resolving the hyperfine structure of the $\mathrm{A}\,^2Σ^+ \leftarrow \mathrm{X}\,^2Π_{3/2}$ transition in nitric oxide for total angular momenta $J_X=1.5-19.5$ on the $\mathrm{oP_{12ee}}$ branch. The resulting line splittings are compared to calculated splittings and fitted determining new values for the molecular constants $b, c, eQq_0$ and $b_F$ for the $\mathrm{A}\,^2Σ^+$ state. The constants are in good agreement with values previously determined by quantum beat spectroscopy.
Barium monohydride (BaH) is an attractive candidate for extending laser cooling and trapping techniques to diatomic hydrides. The apparatus and high-resolution optical spectroscopy presented here demonstrate progress toward this goal. A cryogenic buffer-gas-cooled molecular beam of BaH was constructed and characterized. Pulsed laser ablation into cryogenic helium buffer gas delivers $\sim1\times10^{10}$ molecules/sr/pulse in the X$^2Σ^+$ ($v''=0,N''=1$) state of primary interest. More than $1\times10^7$ of these molecules per pulse enter the downstream science region with forward velocities be…
Attosecond photoelectron spectroscopy is often performed with interferometric experimental setups that require outstanding stability. We demonstrate and characterize in detail an actively stabilized, versatile, high spectral resolution attosecond beamline. The active-stabilization system can remain ultra-stable for several hours with an RMS stability of 13 as and a total pump-probe delay scanning range of \sim 400 fs. A tunable femtosecond laser source to drive high-order harmonic generation allows for precisely addressing atomic and molecular resonances. Furthermore, the interferometer includ…
We demonstrate a diode laser system which is suitable for high-resolution spectroscopy in the 1200 nm and yellow spectral ranges. It is based on a two-facet quantum dot chip in a Littrow-type external cavity configuration. The laser is tunable in the range 1125 -1280 nm, with an output power of more than 200 mW and exhibits a free-running linewidth of 200 kHz. Amplitude and frequency noise were characterized, including the dependence of frequency noise on the cavity length. Frequency stabilization to a high-finesse reference cavity is demonstrated reducing the linewidth to about 20 - 30 kHz. Y…
We present a method for recovery of narrow homogeneous spectral features out of broad inhomogeneous overlapped profile based on second-derivative processing of the absorption spectra of alkali metal atomic vapor nanocells. The method is shown to preserve the frequency positions and amplitudes of spectral transitions, thus being applicable for quantitative spectroscopy. The proposed technique was successfully applied and tested for: measurements of hyperfine splitting and atomic transition probabilities; development of an atomic frequency reference; determination of isotopic abundance; study of…
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 …
We demonstrate the measurement of ultrafast dynamics using ghost spectroscopy and a pump-probe approach with an optical pump and a short-wavelength radiation probe. The ghost spectroscopy approach is used to overcome the challenge of the strong intensity and spectrum fluctuations at free-electron lasers and to provide high -spectral resolution, which enables the measurement of small energy shifts in the absorption spectrum. We exploit the high resolution to explore the dynamics of the charge carrier excitations and relaxations and their impact on the photoinduced structural changes in silicon …
The dynamics of vibrational wave packets in triplet states of rubidium dimers (Rb2) formed on helium nanodroplets are studied using femtosecond pump-probe photoionization spectroscopy. Due to fast desorption of the excited Rb2 molecules off the droplets and due to their low internal temperature, wave packet oscillations can be followed up to very long pump-probe delay times >1.5ns. In the first excited triplet state (1)^3Σ_g^+, full and fractional revivals are observed with high contrast. Fourier analysis provides high-resolution vibrational spectra which are in excellent agreement with ab ini…
We demonstrate cryogenic buffer-gas cooling of gas-phase methyltrioxorhenium (MTO). This molecule is closely related to chiral organometallic molecules where the parity-violating energy differences between enantiomers may be measurable. The molecules are produced with a rotational temperature of approximately 6~K by laser ablation of an MTO pellet inside a cryogenic helium buffer gas cell. Facilitated by the low temperature, we demonstrate absorption spectroscopy of the 10.2~$μ$m antisymmetric Re=O stretching mode of MTO with a resolution of 8~MHz and a frequency accuracy of 30~MHz. We partial…
Long-lived isotopes of plutonium were studied using two complementary techniques, high-resolution resonance ionisation spectroscopy (HR-RIS) and collinear laser spectroscopy (CLS). Isotope shifts have been measured on the $5f^67s^2\ ^7F_0 \rightarrow 5f^56d^27s\ (J=1)$ and $5f^67s^2\ ^7F_1 \rightarrow 5f^67s7p\ (J=2)$ atomic transitions using the HR-RIS method and the hyperfine factors have been extracted for the odd mass nuclei $^{239,241}$Pu. Collinear laser spectroscopy was performed on the $5f^67s\ ^8F_{1/2} \rightarrow J=1/2\; (27523.61\text{cm}^{-1})$ ionic transition with the hyperfine …
The laser spectroscopy with a narrow linewidth and high signal to noise ratio (S/N) is very important in the precise measurement of optical frequencies. Here, we present a novel high-resolution backward resonance Bragg-scattering (RBS) spectroscopy from a population difference grating (PDG). The PDG is formed by a standing-wave (SW) pump field in thermal 87Rb vapor, which periodically modulates the space population distribution of two levels in the 87Rb D1 line. A probe beam, having the identical frequency and the orthogonal polarization with the SW pump field, is Bragg-scattered by the PDG. S…
The conversion electrons from the decay of the 35.5-keV excited state of 125Te following the electron capture decay of 125I have been investigated at high resolution using an electrostatic spectrometer. The penetration parameter lambda = -1.2(6) and mixing ratio |delta| = 0.015(2) were deduced by fitting to literature values and present data. The shake probability of the conversion electrons is estimated to be 0.5, more than two times larger than the predicted value of 0.2.
We present a high-resolution laser spectroscopic study of the $\tilde{A}\,^2B_2- \tilde{X}\,^2A_1$ and $\tilde{B}\,^2B_1- \tilde{X}\,^2A_1$ transitions of calcium (I) phenoxide, CaOPh (CaOC$_6$H$_5$). The rotationally resolved band systems are analyzed using an effective Hamiltonian model and are accurately modeled as independent perpendicular ($b$- or $c$-type) transitions. The structure of calcium monophenoxide is compared to previously observed Ca-containing radicals and implications for direct laser cooling are discussed. This work demonstrates that functionalization of aromatic molecules …
We reported a detailed experimental study of the cold collision of Barium monofluoride (BaF) with buffer gas and the high-resolution spectroscopy relevant with direct laser cooling. BaF molecules are efficiently produced with laser ablation and buffer-gas cooled in a cryogenic apparatus. The laser cooling relevant transition $|X^2Σ, v=0, N=1\rangle$ to $|A^2Π, v'=0, J'=1/2\rangle$ is identified. The collision cross section with buffer gas is measured to be $1.4(7)\times10^{-14} cm^{-2}$, which is very suitable for buffer gas cooling. Both rotational and vibrational temperatures are effectively…
We present precision spectroscopy on electrically trapped formaldehyde (H$_2$CO), demonstrating key attributes which will enable molecular spectroscopy with unprecedented precision. Our method makes use of a microstructured electric trap with homogeneous fields in the trap center and rotational transitions with minimal Stark broadening at a 'magic' offset electric field. Using molecules cooled to the low millikelvin temperature regime via optoelectrical Sisyphus cooling, we reduce Stark broadening on the $J=5\leftarrow4$ ($K=3$) transition at 364 GHz to well below 1 kHz, observe Doppler-limite…
We report a study of high-resolution microwave spectroscopy of nitrogen-vacancy centers in diamond crystals at and around zero magnetic field. We observe characteristic splitting and transition imbalance of the hyperfine transitions, which originate from level anti-crossings in the presence of a transverse effective field. We use pulsed electron spin resonance spectroscopy to measure the zero-field spectral features of single nitrogen-vacancy centers for clearly resolving such level anti-crossings. To quantitatively analyze the magnetic resonance behavior of the hyperfine spin transitions in t…
Parity violation (PV) effects in chiral molecules have so far never been experimentally observed. To take this challenge up, a consortium of physicists, chemists, theoreticians and spectroscopists has been established and aims at measuring PV energy differences between two enantiomers by using high-resolution laser spectroscopy. In this article, we present our common strategy to reach this goal, the progress accomplished in the diverse areas, and point out directions for future PV observations. The work of André Collet on bromochlorofluoromethane enantiomers, their synthesis and their chiral r…
Rapid progress in cooling and trapping of molecules has enabled first experiments on high resolution spectroscopy of trapped diatomic molecules, promising unprecedented precision. Extending this work to polyatomic molecules provides unique opportunities due to more complex geometries and additional internal degrees of freedom. Here, this is achieved by combining a homogeneous-field microstructured electric trap, rotational transitions with minimal Stark broadening at a 'magic' offset electric field, and optoelectrical Sisyphus cooling of molecules to the low millikelvin temperature regime. We …
We demonstrate buffer-gas cooling, high-resolution spectroscopy and cycling fluorescence of cold barium monofluoride (BaF) molecules. Our source produces an intense and internally cold molecular beam containing the different BaF isotopologues with a mean forward velocity of 190 m/s. For a well-collimated beam of 138BaF we observe a flux of more than 1e10 molecules/sr/pulse in the X2Sigma, N=1 state in our downstream detection region. Studying the absorption line strength of the intermediate A'Delta state we infer a lifetime of 790+\-346 ns, significantly longer than previously estimated. Final…
