We demonstrate an efficient high-precision optical spectroscopy technique for single trapped ions with nonclosed transitions. In a double-shelving technique, the absorption of a single photon is first amplified to several phonons of a normal motional mode shared with a cotrapped cooling ion of a different species, before being further amplified to thousands of fluorescence photons emitted by the cooling ion using the standard electron shelving technique. We employ this extension of the photon recoil spectroscopy technique to perform the first high precision absolute frequency measurement of the 2D(3/2)→2P(1/2) transition in calcium, resulting in a transition frequency of f=346 000 234 867(96) kHz. Furthermore, we determine the isotope shift of this transition and the 2S(1/2)→2P(1/2) transition for 42Ca+, 44Ca+, and 48Ca+ ions relative to 40Ca+ with an accuracy below 100 kHz. Improved field and mass shift constants of these transitions as well as changes in mean square nuclear charge radii are extracted from this high resolution data.
We demonstrate an efficient high-precision optical spectroscopy technique for single trapped ions with nonclosed transitions. In a double-shelving technique, the absorption of a single photon is first amplified to several phonons of a normal motional mode shared with a cotrapped cooling ion of a different species, before being further amplified to thousands of fluorescence photons emitted by the cooling ion using the standard electron shelving technique. We employ this extension of the photon recoil spectroscopy technique to perform the first high precision absolute frequency measurement of the 2D(3/2)→2P(1/2) transition in calcium, resulting in a transition frequency of f=346 000 234 867(96) kHz. Furthermore, we determine the isotope shift of this transition and the 2S(1/2)→2P(1/2) transition for 42Ca+, 44Ca+, and 48Ca+ ions relative to 40Ca+ with an accuracy below 100 kHz. Improved field and mass shift constants of these transitions as well as changes in mean square nuclear charge radii are extracted from this high resolution data.
Laser spectroscopy is a versatile tool to investigate the internal structure of atoms, molecules and nuclei.High precision spectroscopy requires laser cooling to reduce Doppler broadening and Doppler shifts.Sympathetic cooling extends these advantages to species which do not have an appropriate transition for laser cooling and allows precision spectroscopy of previously inaccessible species using the quantum logic technique.The original implementation of quantum logic spectroscopy relies on the long lifetime of the excited spectroscopy state to realize a transfer sequence.Precision spectroscopy of transitions with a short-lived excited state is typically performed using laser induced uorescence or laser absorption spectroscopy.Neither of these methods has reached the fundamental quantum projection noise limit and are rather limited by photon shot noise.For these situations, we develop the technique of photon recoil spectroscopy as an extension of quantum logic spectroscopy to broad transitions.The common motion of a sideband-cooled two-ion crystal is excited by photon recoil during photon absorption on the spectroscopically investigated ion.This motional excitation is transferred to an internal state excitation on the co-trapped ion of a dierent species and detected with high eciency.We demonstrate the technique on the 2 S 1/2 ↔ 2 P 1/2 transition of the 40 Ca + ion and resolve the line center to 1/300 of its observed linewidth.The simplicity and versatility of the technique promises applications to other previously inaccessible species.A variation of the technique is proposed for rotational state preparation of molecular ions.A moving optical lattice is employed to exert a state-dependent force on the molecule.This would allow the detection of the rotational state of the molecular ion and therefore enable precision spectroscopy of specic rovibrational transitions in the molecule.
Fundamental interactions and symmetries define the structure and properties of all matter, in particular of its small and diverse visible constituents—the atoms. The study of their distinctive spectra through precision spectroscopy is therefore a vital tool to advance our understanding of nature. Highly charged ions (HCIs) constitute the largest fraction of all atoms since every atom has as many charge states as electrons it can bind. Although most of the matter on Earth is neutral, HCIs are ubiquitous in the universe and their systematic study is essential not only for atomic physics but eminently for astrophysics, nuclear physics, and fusion research, among others. Recently, HCIs have been identified as ideal candidates for sensitive tests of physics beyond the Standard Model of particle physics and for use in future high-accuracy optical atomic clocks. However, the realization of such proposals has been hindered by the hitherto constrained laboratory control and limited spectroscopic accuracy of about parts-per-million fractional uncertainty levels. This thesis reports the first coherent laser spectroscopy of HCIs, boosting the achievable spectroscopic precision by eight orders of magnitude compared to traditional spectroscopy methods. The 2P1/2–2P3/2 fine-structure ground-state transition in highly charged 40Ar13+ at an optical wavelength of 441 nm was chosen as a proof-of-principle case. A single ion of this species was isolated from a megakelvin-hot plasma cloud and co-trapped together with a laser-cooled singly charged 9Be+ ion in a two-ion crystal, confined in the harmonic potential of a cryogenic linear Paul trap. This coupled quantum-mechanical system was then cooled to its ground state of axial motion, corresponding to the lowest temperature of a HCI ever achieved. The spectroscopy was realized by implementing quantum logic techniques which allow preparation of the quantum state of the HCI and to map its electronic state after spectroscopy onto the 9Be+ logic ion in order to detect it there with high efficiency through electron shelving. In addition to the increase of spectroscopic precision, the excited-state lifetime and g-factor were measured—the latter one to unprecedented accuracy, resolving effects from special relativity, interelectronic interactions, and quantum electrodynamics. Moreover, it settled a discrepancy between theoretical predictions. The demonstrated techniques are not limited to the specific 40Ar13+ species but universally applicable to other HCIs. Thereby, this work unlocks the potential of HCIs for unrivaled tests of fundamental physics, the search for new physics—such as a 5th force, variations of fundamental constants and dark matter candidates—as well as the use of HCIs in novel optical atomic clocks.
This dissertation reports on precision measurements of the atomic structure of calcium ions (40Ca+), application of trapped 40Ca+ ions as a probe for a violation of fundamental symmetry and prospects of performing quantum simulations with trapped ion.We demonstrate a novel technique to perform spectroscopy on the dipole transition of 40Ca+ that circumvents usual difficulties from dark resonances and Doppler heating. The center of the atomic transition can be detected to a precision of 200 kHz or less with an integration time of 10 minutes. We apply this method to directly measure the influence of micromotion on the fluorescence spectra and confirm the dependence of the modulation index on the radial trap frequency. We measure the branching fraction of the excited 2P1/2 state of 40Ca+ to be 0.93565(7) using a simple experimental scheme readily applicable to many other ion species. Our result for 40Ca+ distinguishes well among various theoretically calculated values, which is important in guiding further developments of the theoretical work.We apply the Ramsey spectroscopy technique based on a pair of correlated ions to probe the effect of the violation of local Lorentz invariance (LLI). The energy difference between the two components of the Bell state |PsiB> = |mJ=5/2,mJ=-5/2>+|mJ=1/2,mJ=-1/2> in the D5/2 manifold of 40Ca+ is monitored for 12 hours. We found that the energy component related to the violation of LLI varies less than 17±22 mHz. Assuming a hydrogen-like model of 40Ca+, the measurement result provides us the bound of the LLI parameter C(2)0 to be 1.7±2.2x10-17.Based on numerical simulations, we show that the Aubry transition in the Frenkel-Kontorova model with trapped ion can be observed for practical experimental parameters such as the strength and wavelength of the optical lattice, which serves as an external perturbing periodic potential. Moreover, we also show that the normal mode structure of ion chain can change significantly as we vary the strength of the optical lattice.
This thesis reports on the setup of a new ion trap apparatus designed for experiments with single ⁴⁰Ca⁺ ions to perform molecular spectroscopy. The calcium ion is laser cooled, allowing for sympathetic cooling of the nonfluorescing molecular ion. The aim of these experiments is to explore loading and identifying molecular ions in RF-Paul traps, as well as developing new spectroscopic tools to measure transitions of molecular ions via the fluorescence of co-trapped ⁴⁰Ca⁺ ions. Ground state cooling of a mixed ion pair is implemented as a first step towards increasing the sensitivity of our technique to the level necessary to measure transitions with low scattering rates (like those present in molecular ions). Doppler cooling on the S(1/2)->P(1/2) transition of the calcium ion results in the formation of a Coulomb crystal, the behavior of which may be used to infer properties of the molecular ion. Following cooling, sideband spectroscopy on the narrow S(1/2)->D(5/2) quadrupole transition of calcium may be used to identify the mass of single molecular ions. This method is verified via a non-destructive measurement on ⁴⁰CaH⁺ and ⁴⁰Ca¹⁶O⁺. The normal modes of the Coulomb crystal can also be used to extract information from the target ion to the control ion. By driving the blue side of a transition, laser induced heating can be put into the two ion system, which leads to changes in fluorescence of the ⁴⁰Ca⁺ ion, first demonstrated with two Ca⁺ isotopes. Increasing the sensitivity of this technique requires ground state cooling of both the ⁴⁰Ca⁺ ion and the ion of interest, enabling the transfer of the ion's motional state into the ground state with high probability. This thesis demonstrates ground state cooling of the atomic ion and sympathetic cooling of a second ion (⁴⁴Ca⁺). Once in the ground state, heating of the Coulomb crystal by scattering photons off of the spectroscopy ion can be measured by monitoring the resolved motional sidebands of the S(1/2)->D(5/2) transition of ⁴⁰Ca⁺, allowing for spectral lines to be inferred. Future experiments will investigate this technique with molecular ions.
The 435 mum171Yb+transition is a good candidate for an atomic clock based on an optical transition. We have stored single171Yb ions for several months in RF traps. The ions are cooled, repumped and the clock transition is interrogated by (frequency-doubled) diode lasers. The interrogation laser linewidth was 30 Hz determining the resolvable linewidth of the Yb+transition interrogated. The absolute frequency of this transition was measured using an optical comb generator, self referenced by broadening the spectrum to above one octave, with respect to a Cs fountain clock. Of all systematic frequency shifts to which this transition is subject an estimate indicates that the electric quadruple shift appears is the largest. To obtain a magnitude of the quadruple shift (and the quadruple moment) the clock frequencies of two independently stored and cooled171Yb ions were compared while varying the static electric field in one trap. The measured frequency shift amounting to ~1 Hz/V. This result would seem to permit clocks with much higher accuracy than the clocks based on microwave transition, particularly if the technique of aligning the ions with respect to the electric field were applicable. Anticipating even more precise clocks, we are presently investigating a blue nuclear transition in229Th. Such a nuclear transition should be even better shielded from environmental influences than transitions in the electron shell. This nuclear transition has not yet been directly optically observed. We are presently investigating the luminescence after incoherent broad band optical excitation. The triply ionized223Th is then a suitable system for trapped single ion spectroscopy. The cooling transition lies conveniently in the near infrared and the nuclear clock transition can be read out by nuclear/electron shell double resonance
With the advent of optical clocks featuring fractional frequency uncertainties on the order of 10−17 and below, new applications such as chronometric leveling with few-centimeter height resolution emerge. We are developing a transportable optical clock based on a single trapped aluminum ion, which is interrogated via quantum logic spectroscopy. We employ singly charged calcium as the logic ion for sympathetic cooling, state preparation, and readout. Here, we present a simple and compact physics and laser package for manipulation of 40Ca+. Important features are a segmented multilayer trap with separate loading and probing zones, a compact titanium vacuum chamber, a near-diffraction-limited imaging system with high numerical aperture based on a single biaspheric lens, and an all-in-fiber 40Ca+ repump laser system. We present preliminary estimates of the trap-induced frequency shifts on 27Al+, derived from measurements with a single calcium ion. The micromotion-induced second-order Doppler shift for 27Al+ has been determined to be δνEMMν=−0.4−0.3+0.4×10−18 and the black-body radiation shift is δνBBR/ν = (−4.0 ± 0.4) × 10−18. Moreover, heating rates of 30 (7) quanta per second at trap frequencies of ωrad,Ca+ ≈ 2π × 2.5 MHz (ωax,Ca+ ≈ 2π × 1.5 MHz) in radial (axial) direction have been measured, enabling interrogation times of a few hundreds of milliseconds.