Using a laser that is frequency-locked to a Fabry-Perot etalon of high finesse and stability, we probe the 5d10 6s 2S_1/2 (F=0) - 5d9 6s 2D_5/2 (F=2) Delta-m_F = 0 electric-quadrupole transition of a single laser-cooled 199Hg+ ion stored in a cryogenic radio-frequency ion trap. We observe Fourier-transform limited linewidths as narrow as 6.7 Hz at 282 nm (1.06 X 10^15 Hz), yielding a line Q = 1.6 X 10^14. We perform a preliminary measurement of the 5d9 6s2 2D_5/2 electric-quadrupole shift due to interaction with the static fields of the trap, and discuss the implications for future trapped-ion optical frequency standards.
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 …
We report precision measurement of aluminum atoms ${^{2}P_{1/2}}-{^{2}S_{1/2}}$ transition at 394 nm and ${^{2}P_{3/2}}-{^{2}S_{1/2}}$ transition at 396 nm in a hollow-cathode lamp (HCL). Both absorption spectroscopy and saturated absorption spectroscopy (SAS) are performed. From the absorption spectroscopy the Doppler linewidth is estimated to be 2.6 GHz. The SAS spectroscopy is analyzed based on the velocity-changing-effect model. With a frequency comb calibrated wavemeter, the frequencies of ${^{2}P_{1/2}},{F=3}-{^{2}S_{1/2}},{F=2}$ transition and ${^{2}P_{3/2}},{F=4}-{^{2}S_{1/2}},{F=3}$ t…
Bose-Einstein condensation, an effect long known for material particles as cold atomic gases, has in recent years also been observed for photons in microscopic optical cavitites. Here, we report absorption and emission spectroscopic measurements on the lowest electronic transition ($5\text{p}^6 \rightarrow 5\text{p}^5 6\text{s}$) of xenon, motivated by the search for a thermalization medium for photon Bose-Einstein condensation in the vacuum-ultraviolet spectral regime. We have recorded pressure-broadened xenon spectra in the 135 nm to 190 nm wavelength regime at conditions near the critical p…
Bose-Einstein condensation is a phenomenon well known for material particles as cold atomic gases, and this concept has in recent years been extended to photons confined in microscopic optical cavities. Essential for the operation of such a photon condensate is a thermalization mechanism that conserves the average particle number, as in the visible spectral regime can be realized by subsequent absorption re-emission processes in dye molecules. Here we report on the status of an experimental effort aiming at the extension of the concept of Bose-Einstein condensation of photons towards the vacuu…
We experimentally investigate trap-loss spectra of the cesium 6S1/2(F=4)-71P3/2 Rydberg state by combining the cesium atomic magneto-optical trap with the narrow-linewidth, continuously-tunable 318.6 nm ultraviolet laser. That is, the atoms in the magneto-optical trap are excited to the Rydberg state due to the ultraviolet laser single-step Rydberg excitation, which leads to the reduction of atomic fluorescence. Based on the trap-loss spectroscopy technology, the Autler-Townes splitting due to strong cooling laser is observed, and the parameter dependence of the AT splitting interval of trap-l…
The remarkable progress in the field of laser spectroscopy induced by the invention of the frequency-comb laser has enabled many new high-precision tests of fundamental theory and searches for new physics. Extending frequency-comb based spectroscopy techniques to the vacuum (VUV) and extreme ultraviolet (XUV) spectral range would enable measurements in e.g. heavier hydrogen-like systems and open up new possibilities for tests of quantum electrodynamics and measurements of fundamental constants. The main approaches rely on high-harmonic generation (HHG), which is known to induce spurious phase …
We present a novel time- and phase-resolved, background-free scheme to study the extreme ultraviolet dipole emission of a bound electronic wavepacket, without the use of any extreme ultraviolet exciting pulse. Using multiphoton transitions, we populate a superposition of quantum states which coherently emit extreme ultraviolet radiation through free induction decay. This emission is probed and controlled, both in amplitude and phase, by a time-delayed infrared femtosecond pulse. We directly measure the laser-induced dephasing of the emission by using a simple heterodyne detection scheme based …
The molecular ion ThF$^+$ is the species to be used in the next generation of search for the electron's Electric Dipole Moment (eEDM) at JILA. The measurement requires creating molecular ions in the eEDM sensitive state, the rovibronic ground state $^3Δ_1$, $v^+=0$, $J^+=1$. Survey spectroscopy of neutral ThF is required to identify an appropriate intermediate state for a Resonance Enhanced Multi-Photon Ionization (REMPI) scheme that will create ions in the required state. We perform broadband survey spectroscopy (from 13000 to 44000~cm$^{-1}$) of ThF using both Laser Induced Fluorescence (LIF…
We demonstrate time-resolved nonlinear extreme-ultraviolet absorption spectroscopy on multiply charged ions, here applied to the doubly charged neon ion, driven by a phase-locked sequence of two intense free-electron laser pulses. Absorption signatures of resonance lines due to 2$p$--3$d$ bound--bound transitions between the spin-orbit multiplets $^3$P$_{0,1,2}$ and $^3$D$_{1,2,3}$ of the transiently produced doubly charged Ne$^{2+}$ ion are revealed, with time-dependent spectral changes over a time-delay range of $(2.4\pm0.3)\,\text{fs}$. Furthermore, we observe 10-meV-scale spectral shifts o…
Laser spectroscopy of the $^{\mathrm{229m}}$Th nuclear clock transition is necessary for the future construction of a nuclear-based optical clock. Precision laser sources with broad spectral coverage in the vacuum ultraviolet are needed for this task. Here, we present a tunable vacuum-ultraviolet frequency comb based on cavity-enhanced seventh-harmonic generation. Its tunable spectrum covers the current uncertainty range of the $^{\mathrm{229m}}$Th nuclear clock transition.
Frequency-modulation (FM) spectroscopy has been extended to the vacuum-ultraviolet (VUV) range of the electromagnetic spectrum. Coherent VUV laser radiation is produced by resonance-enhanced sum-frequency mixing ($ν_{\mathrm{VUV}}=2ν_{\mathrm{UV}}+ν_2$) in Kr and Xe using two near-Fourier-transform-limited laser pulses of frequencies $ν_{\mathrm{UV}}$ and $ν_2$. Sidebands generated in the output of the second laser ($ν_2$) using an electro-optical modulator operating at the frequency $ν_{\mathrm{mod}}$ are directly transfered to the VUV and used to record FM spectra. Demodulation is demonstrat…
The development of schemes for coherent nonlinear time-domain spectroscopy in the extreme-ultraviolet regime (XUV) has so far been impeded by experimental difficulties that arise at these short wavelengths. In this work we present a novel experimental approach, which facilitates the timing control and phase cycling of XUV pulse sequences produced by harmonic generation in rare gases. The method is demonstrated for the generation and high spectral resolution characterization of narrow-bandwidth harmonics ($\approx14\,$eV) in argon and krypton. Our technique simultaneously provides high phase st…
A spectral survey of tungsten emission in the ultraviolet region has been completed in the DIII-D tokamak and the CTH torsatron to assess the potential benefit of UV emission for the diagnosis of gross W erosion. A total of 29 W I spectral lines are observed from the two experiments using survey spectrometers between 200-400 nm with level identifications provided based on a structure calculation for many of the excited states that produce strong emission lines. Of the 29 observed lines, 20 have not previously been reported in fusion relevant plasmas, including an intense line at 265.65 nm whic…
Time- and Angle-resolved photoelectron spectroscopy from surfaces can be used to record the dynamics of electrons and holes in condensed matter on ultrafast time scales. However, ultrafast photoemission experiments using extreme-ultraviolet (XUV) light have previously been limited by either space-charge effects, low photon flux, or limited tuning range. In this article, we describe space-charge-free XUV photoelectron spectroscopy experiments with up to 5 nA of average sample current using a tunable cavity-enhanced high-harmonic source operating at 88 MHz repetition rate. The source delivers $ …
The recent development of ultrafast extreme ultraviolet (XUV) coherent light sources bears great potential for a better understanding of the structure and dynamics of matter. Promising routes are advanced coherent control and nonlinear spectroscopy schemes in the XUV energy range, yielding unprecedented spatial and temporal resolution. However, their implementation has been hampered by the experimental challenge of generating XUV pulse sequences with precisely controlled timing and phase properties. In particular, direct control and manipulation of the phase of individual pulses within a XUV p…
