A molecular conveyor belt by controlled delivery of single molecules into ultrashort laser pulses

Kahra, Steffen; Leschhorn, Günther; Kowalewski, Markus; Schiffrin, Agustin; Bothschafter, Elisabeth M.; Fuß, Werner; Vivie‐Riedle, Regina de; Ernstorfer, Ralph; Krausz, Ferenc; Kienberger, Reinhard; Schaetz, Tobias

doi:10.1038/nphys2214

Cited by 41 publications

(32 citation statements)

References 31 publications

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“…Over the past decades, several experimental methods have been devised for quantum control of single trapped ions [2][3][4]. Developments are driven by the urge to make more accurate and precise clocks [5,6] as well as to address questions in different fields of research, e.g., properties of highly charged ions [7,8], ion-neutral collisions [9][10][11][12], molecular physics [13][14][15], and tests of fundamental physics [16][17][18][19][20]. High-resolution spectroscopy measurements [21][22][23][24][25] are of particular interest for studying spatial and temporal fine structure variations of the universe [26][27][28].…”

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confidence: 99%

Decoherence-Assisted Spectroscopy of a SingleMg+Ion

Clos

Enderlein²,

Warring³

et al. 2014

Phys. Rev. Lett.

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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.Quantum systems that are well isolated from their environments, e.g., tailored solid-state systems, photons, and trapped atoms, offer a high level of control [1]. Over the past decades, several experimental methods have been devised for quantum control of single trapped ions [2][3][4]. Developments are driven by the urge to make more accurate and precise clocks [5,6] as well as to address questions in different fields of research, e.g., properties of highly charged ions [7,8], ion-neutral collisions [9][10][11][12], molecular physics [13][14][15], and tests of fundamental physics [16][17][18][19][20]. High-resolution spectroscopy measurements [21][22][23][24][25] are of particular interest for studying spatial and temporal fine structure variations of the universe [26][27][28]. In such experiments, complex atomic and molecular structures need to be probed by singleor multi-photon transitions in isotopically pure samples revealing undisturbed transition line shapes. Weak transitions in trapped ions can be measured with various methods [3,6], and techniques based on the detection of momentum kicks altering the occupation of motional states from few absorbed photons have been developed that are applicable to strong electric dipole transitions as well [25,29]. In this Letter, we experimentally study single-and multi-photon transitions in a single, laser cooled 25 Mg + ion that can be near-perfectly isolated from its environment. We detect the decoherence of a superposition of two electronic ground states due to single scattering events and determine transition frequencies which are relevant for astrophysics and searches for variations of fundamental constants [30,31] with a fractional uncertainty of 5 × 10 −9 .For a simplified description of the method, consider an atom with three states. Two of these states, labeled |↑ and |↓ , which are long-lived and allow for coherent control, are used to study transitions to a third, excited state |e . After preparation in |↑ , a π/2 pulse on the |↑ → |↓ transition creates a superposition state |ψ ≡ 1 √ 2 (|↑ + |↓ ). A spectroscopy pulse probes the couplings |↑ → |e and |↓ → |e during a delay period τ . To decouple the superposition state ...

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mentioning

confidence: 99%

Decoherence-Assisted Spectroscopy of a SingleMg+Ion

Clos

Enderlein²,

Warring³

et al. 2014

Phys. Rev. Lett.

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“…Recent experimental demonstrations with trapped heteronuclear diatomic molecular ions include MgH + [9,12], CaH + /CaD + [13], HD + [14], AlH + [15], HfF + [16], SrCl + [17], and BaCl + [18]. Given the difficulty of detecting scattered photons from dilute molecular-ion samples, rotational-state-selective PD has emerged as a critical tool for molecular ion spectroscopy [15,19] and precision measurements [16,20] theory [13,17,18].…”

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confidence: 99%

Reversing hydride-ion formation in quantum-information experiments withBe+

et al. 2015

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We demonstrate photodissociation of BeH + ions within a Coulomb crystal of thousands of 9 Be + ions confined in a Penning trap. Because BeH + ions are created via exothermic reactions between trapped, laser-cooled Be + ( 2 P 3/2 ) and background H2 within the vacuum chamber, they represent a major contaminant species responsible for infidelities in large-scale trapped-ion quantum information experiments. The rotational-state-insensitive dissociation scheme described here makes use of 157 nm photons to produce Be + and H as products, thereby restoring Be + ions without the need for reloading. This technique facilitates longer experiment runtimes at a given background H2 pressure, and may be adapted for removal of MgH + and AlH + impurities.PACS numbers: 52.27. Jt, 33.80.Gj, 34.50.Lf, Crystals of laser-cooled atomic ions form the basis of many experimental realizations of quantum logic gates [1][2][3] and simulations of quantum many-body physics [4][5][6]. In room-temperature vacuum systems, collisions with neutral background gas molecules limit quantum coherences and quantum logic operations [7]. Here we focus on inelastic (i.e. reactive) collisions where exothermic chemical reactions with background gas molecules can generate, in both Penning and rf traps, co-trapped molecular ions over a wide range of trapping conditions and crystal geometries [6][7][8][9]. These contaminants alter ion-crystal eigenfrequencies and can complicate quantum logic interactions [10]. Impurities may be resonantly ejected from both radiofrequency and Penning traps, but this technique is least efficient when the impurities are similar in mass to the qubit ion [11]. The rate of impurity ion formation increases linearly with the number of ion qubits in the register, and the time required for loading new ions and recalibrating the register increases with the size of the system. Therefore, experimental techniques to prevent or reverse qubit-ion chemistry will be a key tool for many-ion quantum information platforms. [18]. Given the difficulty of detecting scattered photons from dilute molecular-ion samples, rotational-state-selective PD has emerged as a critical tool for molecular ion spectroscopy [15,19] and precision measurements [16,20], while rotationally-insensitive dissociation schemes provide valuable tests of molecular * Electronic address: brian.sawyer@boulder.nist.gov ) after 9000 pulses of 157 nm photodissociation light at 1.6 mJ/pulse. We measure an increase in the Be + fraction from 81% to 97% of the constant total ion number in the crystal. Each image is 1.2 mm × 1.2 mm.

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“…In the presented form, LA-MS represents an easy-toimplement detection method in cold ion experiments that can be used complementarily to (and, perhaps, more robustly than) techniques based on analysing fluorescence images [38,[45][46][47][48] or mass spectrometry based on resonant excitation of the secular ion motion [26,49,50]. It is an ideal tool for spectroscopy of molecular ions and significantly outperforms previous implementations [51][52][53][54].…”

Section: Discussionmentioning

confidence: 99%

Laser-Cooling-Assisted Mass Spectrometry

et al. 2014

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Mass spectrometry is used in a wide range of scientific disciplines including proteomics, pharmaceutics, forensics, and fundamental physics and chemistry. Given this ubiquity, there is a worldwide effort to improve the efficiency and resolution of mass spectrometers. However, the performance of all techniques is ultimately limited by the initial phase-space distribution of the molecules being analyzed. Here, we dramatically reduce the width of this initial phase-space distribution by sympathetically cooling the input molecules with laser-cooled, co-trapped atomic ions, improving both the mass resolution and detection efficiency of a time-of-flight mass spectrometer by over an order of magnitude. Detailed molecular dynamics simulations verify the technique and aid with evaluating its effectiveness. Our technique appears to be applicable to other types of mass spectrometers.

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A molecular conveyor belt by controlled delivery of single molecules into ultrashort laser pulses

Cited by 41 publications

References 31 publications

Decoherence-Assisted Spectroscopy of a SingleMg+Ion

Decoherence-Assisted Spectroscopy of a SingleMg+Ion

Reversing hydride-ion formation in quantum-information experiments withBe+

Laser-Cooling-Assisted Mass Spectrometry

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