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arXiv:1402.1678 · Physical Review Letters

Decoherence-Assisted Spectroscopy of a Single Mg+ Ion

Govinda Clos, Martin Enderlein, Ulrich Warring, Tobias Schaetz, Dietrich G. Leibfried

Published Mar 17, 2014• 18 citations
arXivHTMLPDF

Abstract

We describe a high-resolution spectroscopy method in which the detection of single excitation events is enhanced by a complete loss of coherence of a superposition of two ground states. Thereby, transitions of a single isolated atom nearly at rest are recorded efficiently with high signal-to-noise ratios. Spectra display symmetric line shapes without stray-light background from spectroscopy probes. We employ this method on a (25)Mg+ ion to measure one-, two-, and three-photon transition frequencies from the 3S ground state to the 3P, 3D, and 4P excited states, respectively. Our results are relevant for astrophysics and searches for drifts of fundamental constants. Furthermore, the method can be extended to other transitions, isotopes, and species. The currently achieved fractional frequency uncertainty of 5 × 10(-9) is not limited by the method.

DOI
10.1103/physrevlett.112.113003

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We describe a high-resolution spectroscopy method in which the detection of single excitation events is enhanced by a complete loss of coherence of a superposition of two ground states. Thereby, transitions of a single isolated atom nearly at rest are recorded efficiently with high signal-to-noise ratios. Spectra display symmetric line shapes without stray-light background from spectroscopy probes. We employ this method on a (25)Mg+ ion to measure one-, two-, and three-photon transition frequencies from the 3S ground state to the 3P, 3D, and 4P excited states, respectively. Our results are relevant for astrophysics and searches for drifts of fundamental constants. Furthermore, the method can be extended to other transitions, isotopes, and species. The currently achieved fractional frequency uncertainty of 5 × 10(-9) is not limited by the method.
We demonstrate a method for precision spectroscopy on trapped ions in the limit of unresolved motional sidebands. By sympathetic cooling of a chain of crystallized ions, we suppress adverse temperature variations induced by the spectroscopy laser that usually lead to a distorted line profile and obtain a Voigt profile with negligible distortions. We applied the method to measure the absolute frequency of the astrophysically relevant D2 transition in single 24Mg+ ions and find 1 072 082 934.33(16) MHz, a nearly 400-fold improvement over previous results. Further, we find the excited state lifetime to be 3.84(10) ns.
Absorption spectroscopy is a fundamental tool for probing molecular structure. However, performing absorption spectroscopy on individual molecules is challenging due to the low signal-to-noise ratio. Here, we report on a nondestructive absorption spectroscopy on a mid-infrared vibrational transition in a single molecular ion that is co-trapped with an atomic ion. The absorption of a single photon is detected via the momentum transfer from the absorbed photon onto the molecule. This recoil signal is amplified using a non-classical state of motion of the two-ion crystal and subsequently read out via the atomic ion. We characterize the recoil detection method and use it to investigate the interaction between femtosecond laser pulses and the O-H stretching vibration in individual CaOH+ molecular ions. Furthermore, we present the single-photon absorption spectrum obtained for the vibrational transition. This method represents a milestone towards quantum non-demolition measurements of complex polyatomic molecules, providing high-fidelity methods for preparation and measurement of the quantum state of a wide range of molecular species.
High-resolution two-photon resonant three-photon spectroscopy was applied to investigate the 3 snf\mathrm{snf}snf Rydberg series of Mg. Hyperfine-induced level shifts were detected for the 1,3F^{1,3}F1,3F states of the odd isotope 25Mg^{25}\mathrm{Mg}25Mg. From these measurements the hyperfine coupling constant a3s{a}_{3s}a3s​ of the 25Mg+^{25}\mathrm{Mg}^{+}25Mg+-ion ground state was derived.
The authors report the precision measurement of 25{}^{25}25Mg+{}^{+}+ ion-doublet transition frequencies using a decoherence-assisted spectroscopy method with the full use of spontaneous emission signals to improve the detection sensitivity. The results indicate that consideration of additional physical effects in theoretical calculations, such as the possible capture of electron correlations, is required.
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.
We have employed the method of shelving to measure Zeeman resonances of a single trapped Ba+ ion. We use optical pumping to place the ion in a selected magnetic sublevel of either the 6S(1/2) ground state or the 5D(3/2) metastable state. The ion is exposed to an rf field, and a probing/shelving mechanism detects whether spin-flip transitions have taken place. We have observed rf transitions with linewidths of 15 Hz, limited by magnetic-field noise. We have also observed the shift in the Zeeman frequency when the ion is illuminated by off-resonant light. A simultaneous measurement of such light shifts in two atomic states of Ba+ will permit a precise determination of the ratio of transition matrix elements.