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

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 figure

UV frequency metrology on CO (a3Pi); isotope effects and sensitivity to a variation of the proton-to-electron mass ratio

UV frequency metrology has been performed on the a3Pi - X1Sigma+ (0,0) band of various isotopologues of CO using a frequency-quadrupled injection-seeded narrow-band pulsed Titanium:Sapphire laser referenced to a frequency comb laser. The band origin is determined with an accuracy of 5 MHz (delta \nu / \nu = 3 * 10^-9), while the energy differences between rotational levels in the a3Pi state are determined with an accuracy of 500 kHz. From these measurements, in combination with previously published radiofrequency and microwave data, a new set of molecular constants is obtained that describes the level structure of the a3Pi state of 12C16O and 13C16O with improved accuracy. Transitions in the different isotopologues are well reproduced by scaling the molecular constants of 12C16O via the common mass-scaling rules. Only the value of the band origin could not be scaled, indicative of a breakdown of the Born-Oppenheimer approximation. Our analysis confirms the extreme sensitivity of two-photon microwave transitions between nearly-degenerate rotational levels of different Omega-manifolds for probing a possible variation of the proton-to-electron mass ratio, \mu=m_p/m_e, on a laboratory time scale

Novel techniques in VUV high-resolution spectroscopy

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, Chin

XUV frequency comb metrology on the ground state of helium

The operation of a frequency comb at extreme ultraviolet (XUV) wavelengths based on pair-wise amplification and nonlinear upconversion to the 15th harmonic of pulses from a frequency comb laser in the near-infrared range is reported. Following a first account of the experiment [Kandula et al., Phys. Rev. Lett. 105, 063001 (2010)], an extensive review is given of the demonstration that the resulting spectrum at 51 nm is fully phase coherent and can be applied to precision metrology. The pulses are used in a scheme of direct-frequency-comb excitation of helium atoms from the ground state to the 1s4p and 1s5p 1P_1 states. Laser ionization by auxiliary 1064 nm pulses is used to detect the excited state population, resulting in a cosine-like signal as a function of the repetition rate of the frequency comb with a modulation contrast of up to 55%. Analysis of the visibility of this comb structure yields an estimated timing jitter between the two upconverted comb laser pulses of 50 attoseconds, whch indicates that extension to even shorter wavelengths should be feasible. The helium metrology investigation results in transition frequencies of 5740806993(10) MHz and 5814248672(6) MHz for excitation of the 1s4p and 1s5p 1P_1 states, respectively. This constitutes the first absolute frequency measurement in the XUV, attaining unprecedented accuracy in this windowless part of the electromagnetic spectrum. From the measured transition frequencies an eight-fold improved 4He ionization energy of 5945204212(6) MHz is derived. Also a new value for the 4He ground state Lamb shift is found of 41247(6) MHz. This experimental value is in agreement with recent theoretical calculations up to order m\alpha^6 and m^2/(M\alpha^5), but with a six times higher precision, therewith providing a stringent test of quantum electrodynamics in bound two-electron systems.Comment: 18 pages, 13 figure

Frequency metrology on the 4s 2S1/2 - 4p 2P1/2 transition in the calcium ion for a comparison with quasar data

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

Bounds on fifth forces from precision measurements on molecules

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 tabl

Dissociation energy of the hydrogen molecule at 10−9^{-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.Comment: 6 pages, 5 figure

Ion distribution and ablation depth measurements of a fs-ps laser-irradiated solid tin target

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 figure