Isotope-selective trapping of rare calcium ions using high-power incoherent light sources for the second step of photo-ionization

Rare calcium isotope ⁴⁸Ca⁺ (0.187%) has been selectively loaded in a linear Paul trap using two ultraviolet light emitting diodes with the output power of 85 mW for the second excitation in a two-step photo-ionization process. Isotope selectivity has been achieved by utilizing the isotope shifts for the 4s^{2 1} S ₀–4s4p¹ P ₁ transition of neutral calcium atom. Sympathetic cooling of ⁴⁸Ca⁺ ions has been demonstrated using ⁴⁰Ca⁺ ions as refrigerant ions. Purification of rare isotope ⁴²Ca⁺ ions (0.647%) from a mixture of ⁴⁰Ca⁺ (96.9%) and ⁴²Ca⁺ ions has been performed by adjusting the detuning of the cooling laser frequency, which overcomes the imperfect selectivity for some rare isotopes having close resonance frequencies to that of ⁴⁰Ca in the 4s^{2 1} S ₀–4s4p¹ P ₁ transition. The methods can be applied to ⁴³Ca⁺ ion (0.135%) that has been considered as one of the attractive candidates for quantum information processing as well as for an optical frequency standard. PACS 32.80.Fb; 32.80.Pj; 32.80.Rm     

Frequency response measurement of high-speed photodetectors using the spectrum power method in a delay self-heterodyne system

We report on a photoionization scheme for controlled loading of ⁸⁸Sr⁺ ions into a radio-frequency (rf) ion trap. The two-step doubly-resonant process drives the ⁸⁸Sr atom on the 5s^{2 1} S ₀ – 5s5p¹ P ₁ transition at 461 nm using a frequency-doubled diode laser, and then excites the atom to the autoionizing (4d²+5p²) ¹ D ₂ state with 405 nm light from a free-running diode laser. This method of trap loading is quantitatively compared to electron bombardment loading, and shown to reduce the Sr vapour pressure required to load by four orders of magnitude. It also provides more than an order of magnitude reduction in the day-to-day variation of the voltages required to compensate micromotion. We additionally introduce a two-step atomic source consisting of an oven and hotplate, which reduces the number of impurities evaporated towards the trap. This is shown to significantly reduce fluctuations in required micromotion compensation voltages. The demonstrated reduction in flux and increased source purity are expected to improve the reliability of trap operation for precision ion-trap experiments. PACS 32.80.Fb; 32.80.Pj; 39.10.+j     

Simple and efficient photo-ionization loading of ions for precision ion-trapping experiments

We report a simple and efficient method to load a Paul trap with Ca⁺ ions. A beam of neutral atomic calcium is ionized in a two-step photo-ionization process using uv-diode lasers near 423 nm and 390 nm. Photo-ionization of a calcium beam for loading a Paul trap has first been demonstrated by Kjaergaard et al. The advantages of our method are the use of cheap and easily handled diode-laser systems and the large cross section for field ionization when exciting high-lying Rydberg states. Finally, we discuss the advantages of photo-ionization for ion generation compared to loading by electron bombardment. Received: 24 August 2001 / Revised version: 16 October 2001 / Published online: 23 November 2001     

Isotope selective loading of an ion trap using resonance-enhanced two-photon ionization

We have demonstrated that resonance-enhanced two-photon ionization of atomic beams provides an effective tool for isotope selective loading of ions into a linear Paul trap. Using a tunable, narrow-bandwidth, continuous wave (cw) laser system for the ionization process, we have succeeded in producing Mg⁺ and Ca⁺ ions at rates controlled by the atomic beam flux, the laser intensity, and the laser frequency detuning from resonance. We have observed that with a proper choice of control parameters, it is rather easy to load a specific number of ions into a string. This observation has direct applications in quantum optics and quantum computation experiments. Furthermore, resonant photo-ionization loading facilitates the formation of large isotope-pure Coulomb crystals. Received: 21 December 1999 / Published online: 11 May 2000     

Synthesis of two-species ion chains for a new optical frequency standard with an indium ion

Ion chains consisting of different species play an important role in new applications in quantum information processing as well as in optical frequency standards. We demonstrate generation and stabilization of ion chains consisting of Ca⁺ and In⁺. The Ca⁺ chains with In⁺ located at specified positions are synthesized using resonant photo-ionization, real-time imaging and trap field control techniques. A specific configuration of an ion chain is stabilized by destabilizing other configurations via selective excitation of vibrational modes using amplitude modulation on the cooling laser beam. New approaches to an indium ion optical clock are proposed using the ions chains.     

Exploration of large amplitude motions in the Ca+Ar2 complex

ABSTRACT

We present a theoretical study of the ground electronic state potential of the Ca⁺Ar₂ complex and of its photoabsorption spectra, simulated at temperatures ranging between 20 and 220?K. These calculations exploit a Monte-Carlo (MC) method, based on a one-electron pseudo-potential approach. A pairwise additive potential fitted to coupled cluster ab initio points, is used to model the Ca⁺Ar₂ complex. Our study shows that the most stable form of Ca⁺Ar₂ is a bent C_2v structure, whereas the linear isomer is located at around 90?±?10?cm^?1 above in energy. The analysis of the photoabsorption spectra establishes that a structural transition from bent Ca⁺Ar₂ to linear ArCa⁺Ar occurs at T～100?K. Trends in binding energies of both isomers, bond lengths and bond angles are also discussed. Molecular orbital overlaps provide an explanation for the order of stability between the bent and linear structures.     

In situ 1H NMR Study of Nanoreactor Interaction NH3–H2O in Zeolite Nanopores

The interaction between ammonium NH₃ and H₂O molecules in zeolitic nanopores is studied by in situ ¹H nuclear magnetic resonance (NMR) method. The powder and single crystal samples of natural zeolites, heulandites Ca₄[Al₈Si₂₈O₇₂]·24H₂O and clinoptilolite (Na, K,Ca_1/2)₆[Al₆Si₃₀O₇₂], were used as the model system. It is shown that penetration of NH₃ into the zeolitic nanopores is accompanied by disordering of the hydrogen sublattice of zeolitic water and by the fast proton exchange NH₃ + H₂O ? [NH₄]⁺ + [OH]^? characterized by correlation frequency v _c = ~40 kHz. Another nanoreactor interactions are represented by interaction of [NH₄]⁺ ions with exchangeable Na⁺ and Ca²⁺ ions of the zeolitic structure. The slow ionic exchange [NH₄]⁺ → [Na,Ca_1/2]⁺ and binding of [NH₄]⁺ in cationic sites of the framework were visualized by NMR spectroscopy along with stepwise release of (Na,Ca_1/2)OH from zeolitic pores to the external surface of zeolite grains.     

Theoretical study of ground and excited state potential energy surfaces for the Ca+-H2 complex

The potential energy surfaces of the Ca⁺-H₂ complex are calculated using the internally contracted multireference CI method (ICMR CI) and complete active space SCF (CAS SCF) reference wave functions. The calculations involve both the ground and the excited states correlating to (3d)²D and (4p)²P Ca⁺ terms and are carried out for C_∞v and C_2v configurations. Anisotropy of the potential surfaces has also been analysed by computing the interaction energy for some representative points as a function of the angle between the H₂ molecular axis and the Ca⁺—centre of mass of H₂ bond axis. The calculations have revealed the existence of a conical intersection of the lowest excited (3d)²B₂ potential surface with the ground state one. The obtained global energy minimum of the (3d)²B₂ potential surface lying 0.683 eV below the asymptote indicates a possible stabilization of the Ca⁺-H₂ complex towards formation of an exciplex in the (3d)Ca⁺-H₂(v = 0) collision process. The dependence of the vibrational energy levels of H₂ on the distance from Ca⁺ in the C_2v configuration has also been studied.     

Hyperpolarizabilities of alkaline-earth metal ions Be+, Mg+, and Ca+

The knowledge of the hyperpolarizabilities of atoms and ions is helpful for the analysis of the high order effects of the frequency shifts in precision spectroscopy experiments. Liu et al. [Phys. Rev. Lett. 114, 223001(2015)] proposed to establish all-optical trapped ion clocks using laser at the magic wavelength for clock transition. To evaluate the high-order frequency shifts in this new scheme of optical clocks, hyperpolarizabilities are needed, but absent. Using the finite field method based on the B-spline basis set and model potentials, we calculated the electric-field-dependent energy shifts of the ground and low-lying excited states in Be+, Mg+, and Ca+ in the field strength range of 0.0-6×10.5 a.u.. The scalar and tensor polarizabilities(α0, α2) and hyperpolarizabilities(γ0, γ2, γ4) were deduced. The results of the hyperpolarizabilities for Be+ showed good agreement with the values in literature, implying that the present method can be applied for the effective estimation of the atomic hyperpolarizabilities,which are rarely reported but needed in experiments. The feasibility of optical trapping of Ca+ is discussed, and the contributions of hyperpolarizabilities to the transition frequency shift for Ca+ in the optical dipole trap are estimated using quasi-electrostatic approximation.     

An efficient pathway for Li<Superscript>6</Superscript> isotope enrichment

Separation of lithium isotopes has been achieved using two-step laser photoionization in conjunction with an atomic beam and in-house built time of flight (TOF) mass spectrometer. We present an efficient pathway for the enrichment of Li⁶ isotope by tuning the exciter laser to the 3p ² P _{1/2, 3/2} excited state of Li⁶. A concentration of up to 60% is demonstrated from a natural isotopic abundant lithium sample. In addition, the first measurement of the absolute photoionization cross-section of the 3p excited state of Li⁶ and Li⁷ are reported as 26.8±4 Mb and 25.5±3.8 Mb, respectively. PACS 32.10.Bi; 32.80.t; 32.80.Fb     

Doppler cooling a single Ca+ ion with a violet extended-cavity diode laser

We present a scheme for employing a violet extended-cavity diode laser in experiments with single, trapped ions. For this the grating-stabilised laser is spatially and spectrally filtered and referenced to a Fabry–Pérot cavity. We measure an upper limit to the line width by observing a 305-kHz FWHM beat note with the second harmonic of a titanium sapphire laser. The laser is subsequently used to optically cool a single ⁴⁰Ca⁺ ion close to the Doppler limit. PACS 03.67.Lx; 32.80.Pj; 42.55.Px     

High sensitive photoassociation spectroscopy based on modulated ultra-cold Cs atoms

In this paper, a high sensitive photoassociation spectroscopy based on modulated ultra-cold cesium atoms is reported. The cold cesium gas in the magneto-optical trap is illuminated by a photoassociation laser with red detuning 40 cm^-1 below the 6S _1/2+6P _3/2 dissociation limit and photoassociation to the excited state ultra-cold molecules is observed. The rotationally bound levels of 0_g ^- state are well resolved using the lock-in detection. The 0_g ^-, 1_g and 0_u ⁺ long range states which connect to this dissociation limit are measured. The long-range dipole–dipole interaction constants are determined through a fit of the experimental energy levels. PACS 33.15.Mt; 33.20.Vq; 32.80.Pj     

Observation of sympathetically cooled <Superscript>43</Superscript>Ca<Superscript>+</Superscript> ions in a linear ion trap

We report the observation of sympathetically cooled ⁴³Ca⁺ (natural abundance 0.135%) in a linear ion trap utilizing simultaneously trapped isotope ions as coolant. We investigated different possibilities of realizing efficient sympathetic cooling and observed the peaks of the hyperfine transitions of ⁴³Ca⁺ under various experimental conditions.     

Atomic and molecular ions in intense ultra-fast laser fields

The interaction of a 60 fs 790 nm laser pulse with beams of Ar⁺, C⁺, H₂ ⁺, HD⁺ and D₂ ⁺ are discussed. Intensities up to 10¹⁶ Wcm^-2 are employed. An experimental z-scanning technique is used to resolve the intensity dependent processes in the confocal volume.Received: 6 January 2003, Published online: 15 July 2003PACS: 32.80.Fb Photoionization of atoms and ions - 33.80.Rv Multiphoton ionization and excitation to highly excited states (e.g., Rydberg states) - 42.50.Hz Strong-field excitation of optical transitions in quantum systems; multiphoton processes; dynamic Stark shift     

Preliminary frequency measurement of the electric quadrupole transition in a single laser-cooled 40Ca+ ion

The trapping and laser cooling of ⁴⁰Ca⁺ ion on the way toward optical frequency standards have been developed. A single ⁴⁰Ca⁺ ion is trapped in the miniature Paul trap and laser cooled by two frequency-stabilized diode lasers. A commercial Ti:Sapphire laser system at 729 nm is referenced to a high-finesse cavity to meet the requirements of ultra narrow linewidth of the 4s²S_1/2-3d²D_5/2 electric quadrupole transition. Its center frequency is preliminarily measured to be 411 042 129 686.1 (2.6) kHz. The attempt to finally lock the 729-nm laser system to atomic transition is made. Further work to improve the accuracy of measurement and the stabilization of system locking is in consideration and preparation.     

Chemical origin of C–O blue shift and nature of Cu+…C bonding in non-classical copper carbonyl Cu+(CO)n (n = 1–8) complexes

Natural bond orbital (NBO) method and atoms-in-molecules (AIM) theory are used to study the chemical origin in the direction and ordering of C–O frequency shift, as well as Cu^+…C bond nature in copper carbonyl cations Cu⁺(CO)_n (n = 1–8). This study emphasises the role of π-back donation in explaining the ordering of C–O blue shift. NBO analyses show that the interplay of two competing factors, including π-back donation and rehybridization, is responsible for both the direction and the ordering of C–O stretching frequency shift in Cu⁺(CO)_n (n = 1–8) complexes. In addition, the Cu^+…C interaction is interesting because Cu⁺(CO)_n (n = 1–4) structure has one-sphere CO ligands but Cu⁺(CO)_n (n = 5–8) has two-sphere CO ligands. Topological analyses of electron density are applied to characterise the Cu^+…C interactions of first- and second-sphere CO with Cu⁺ and to explore the Cu^+…C interactions in the nature.     

Loading rate of Yb<Superscript>+</Superscript> loaded through photoionization in radiofrequency ion trap

We investigate the loading rate of Yb⁺ ions loaded through photoionization in a radiofrequency trap. The absolute or relative number of the loaded trapped ions is measured by use of an electric resonance of the secular motion. This method is applicable even in the presence of anharmonicity. In two-color photoionization, where the first-excitation laser drives the ¹S₀–¹P₁ transition in the Yb atom and the second one ionizes the atom from the ¹P₁ state, the loading rate is at its highest by the excitation of the ionization potential. A similar loading rate is observed at the second-laser wavelength around 369.5 nm, which is the wavelength for the cooling transition of Yb⁺. We estimate the loading cross section to be 40(15) Mb for the two-color excitation of the ionization potential. The excitation of the Yb atoms in the Rydberg states is detected by the enhancement of the loading rate. By irradiation with only the first-excitation laser, Yb⁺ is produced at a rate three orders of magnitude smaller than that when the non-resonant two-photon absorption from the ¹P₁ state is the dominant process. We also measure the charge-exchange rate between Yb⁺ and Yb, and discuss its effect on isotope-selective photoionization loading.     

Laser cooling and isotope-shift measurement of Zn<Superscript>+</Superscript> with 202-nm ultraviolet coherent light

We have laser-cooled all even isotopes of Zn⁺ ions confined in a linear radio-frequency ion trap, and measuredoptical isotope shifts in the 4s ² S _1/2-4p ² P _3/2 transition. Tunable continuous-wave coherent light near 202 nm was generated for this experiment by means of frequency conversion of light from diode and solid-state lasers. The measured isotope shifts are as follows: ⁶⁶Zn⁺-⁶⁴Zn⁺, 0.676(6) GHz; ⁶⁸Zn⁺-⁶⁶Zn⁺, 0.670(4) GHz; and ⁷⁰Zn⁺-⁶⁸Zn⁺, 0.568(10) GHz. In all cases, the transition line of the heavier isotope was observed at the higher frequency. The mass and the field shifts were estimated using a King plot. This is the first isotope-shift measurement in the transition involving the ground (4s ² S _1/2) state of Zn⁺ ions. Received: 18 July 2002 / Revised version: 20 October 2002 / Published online: 5 February 2003 RID="*" ID="*"Corresponding author. Fax: +81-42/327-6694, E-mail: matubara@crl.go.jp Present address: Communications Research Laboratory, 4-2-1 Nukui-Kitamachi, Koganei, Tokyo 184-8795, Japan     

Preliminary frequency measurement of the electric quadrupole transition in a single laser-cooled 40Ca+ ion

The trapping and laser cooling of ⁴⁰Ca⁺ ion on the way toward optical frequency standards have been developed. A single ⁴⁰Ca⁺ ion is trapped in the miniature Paul trap and laser cooled by two frequency-stabilized diode lasers. A commercial Ti:Sapphire laser system at 729 nm is referenced to a high-finesse cavity to meet the requirements of ultra narrow linewidth of the 4s²S_1/2-3d²D_5/2 electric quadrupole transition. Its center frequency is preliminarily measured to be 411 042 129 686.1 (2.6) kHz. The attempt to finally lock the 729-nm laser system to atomic transition is made. Further work to improve the accuracy of measurement and the stabilization of system locking is in consideration and preparation.