Martina Knoop

The problem for molecular identification knows many solutions which include mass spectrometers whose mass sensitivity depends on the performance of the detector involved. The purpose of this article is to show by means of molecular dynamics simulations, how a laser-cooled ion cloud, confined in a linear radio-frequency trap, can reach the ultimate sensitivity providing the detection of individual charged heavy molecular ions. In our simulations, we model the laser-cooled Ca + ions as two-level atoms, confined thanks to a set of constant and time oscillating electrical fields. A singly-charged molecular ion with a mass of 10 6 amu is propelled through the ion cloud. The induced change in the fluorescence rate of the lather is used as the detection signal. We show that this signal is due to a significant temperature variation triggered by the Coulombian repulsion and amplified by the radio-frequency heating induced by the trap itself. We identify the optimum initial energy for the molecular ion to be detected and furthermore, we characterize the performance of the detector for a large range of confinement voltages.

Radio-frequency linear multipole traps have been shown to be very sensitive to mis-positioning of their electrodes, which results in a symmetry breaking and leads to extra local minima in the trapping potential \cite{pedregosa17} disturbing the operation of the trap. In this work, we analytically describe the RF-potential of a realistic octupole trap by including lower order terms to the well-established equation for a perfectly symmetric octupole trap. We describe the geometry by a combination of identified defects, characterised by simple analytical expressions. A complete equation is proposed for a trap with any electrode deviation relying on a combination of the simple cases where the defects are taken individually. Our approach is validated by comparison between analytical and numerical results for defect sizes up to 4\% of the trap radius. As described in \cite{pedregosa18}, an independent fine-tuning of the amplitude of the RF voltage applied on each electrode can be used to mitigate the geometrical defects of a realistic trap. In a different way than in \cite{pedregosa18}, the knowledge of an analytical equation for the potential allows to design the set of RF-voltages required for this compensation, based on the experimental measurement of the ion position in the trap, without information concerning the exact position of each electrode, and with a small number of iterations. The requirements, performances and limitations of this protocol are discussed via comparison of numerical simulations and analytical results.

Stringent conditions on the phase relation of multiple photons are a prerequisite for novel protocols of high-resolution coherent spectroscopy. In a recent experiment we have implemented an interrogation process of a Ca$^+$-ion cloud based on three-photon coherent population trapping, with the potential to serve as a frequency reference in the THz-range. This high-resolution interrogation has been made possible by phase-locking both laser sources for cooling and repumping of the trapped ions to a clock laser at 729~nm by means of an optical frequency comb. The clock laser, a titanium-sapphire laser built in our lab locked onto two high-finesse cavities reaches a linewidth of a few Hertz and a frequency stability below 10$^{-14}$ at one second, performances which can be copied onto the two other sources. In this paper we discuss the performances of the phase-transfer between the three involved lasers via the optical frequency comb.

Radiofrequency multipole traps have been used for some decades in cold collision experiments, and are gaining interest for precision spectroscopy due to their low mi-cromotion contribution, and the predicted unusual cold-ion structures. However, the experimental realisation is not yet fully controlled, and open questions in the operation of these devices remain. We present experimental observations of symmetry breaking of the trapping potential in a macroscopic octupole trap with laser-cooled ions. Numerical simulations have been performed in order to explain the appearance of additional local potential minima, and be able to control them in a next step. We characterize these additional potential minima, in particular with respect to their position, their potential depth and their probability of population as a function of the radial and angular displacement of the trapping rods.

Very long, one-dimensional (1D) ion chains are the basis for many applications, in particular in quantum information processing and reliable diagnostics are needed to quantify them. To that purpose, we have experimentally validated Dubin's model for very long ion chains [Phys. Rev. Lett. 71, 2753 (1993)]. This diagnostic allows to precisely determine the number of trapped ion with an accuracy of almost 1\% without counting them, by measuring the ion-ion distance of the innermost particles, as well as the trapping potential along the ion chain direction. In our experiment, based on a 155 ion chain, the central 30 ions are measured to be equidistant to better than 2\%, and we can determine the total number of trapped ions with a 4.5\% uncertainty, completely dominated by a conservative estimation of the experimental characterisation of the trap.

The manipulation of trapped charged particles by electric fields is an accurate, robust and reliable technique for many applications or experiments in high-precision spectroscopy. The transfer of the ion sample between multiple traps allows the use of a tailored environment in quantum information, cold chemistry, or frequency metrology experiments. In this article, we experimentally study the transport of ion clouds of up to 50 000 ions. The design of the trap makes ions very sensitive to any mismatch between the assumed electric potential and the actual local one. Nevertheless, we show that being fast (100 $μ$s to transfer over more than 20 mm) increases the transport efficiency to values higher than 90 %, even with a large number of ions. For clouds of less than 2000 ions, a 100 % transfer efficiency is observed.

Efficient transport of cold atoms or ions is a subject of increasing concern in many experimental applications reaching from quantum information processing to frequency metrology. For the scalable quantum computer architectures based on the shuttling of individual ions, different transport schemes have been developed, which allow to move single atoms minimizing their energy gain. In this article we discuss the experimental implementation of the transport of a three-dimensional ion cloud in a macroscopic linear radiofrequency (RF) trap. The present work is based on numerical simulations done by molecular dynamics taking into account a realistic experimental environment. The deformation of the trapping potential and the spatial extension of the cloud during transport appears to be the major source of the ion energy gain. The efficiency of transport in terms of transfer probability and ion number is also discussed.

Various techniques are used to detect the presence of charged particles stored in electromagnetic traps, their energy, their mass, or their internal states. Detection methods can rely on the variation of the number of trapped particles (destructive methods) or the use of the ion's interaction with electromagnetic radiation as a non-destructive tool to probe the trapped particles. This review gives an introduction into various methods, discussing the basic mode of operation completed by the description of recent realizations.

Ion traps, which were first introduced in the late 1950s and early 1960s, have established themselves as indispensable tools in many areas of physics, chemistry and technology. This chapter gives a brief survey of the operating principles and development of ion traps, together with a short description of how ions are loaded and detected. This is followed by a brief account of some of the current applications of ion traps.

While the linear radiofrequency trap finds various applications in high-precision spectroscopy and quantum information, its higher-order cousin, the linear multipole trap, is almost exclusively employed in physical chemistry. Recently, first experiments have shown interesting features by laser-cooling multipole-trapped ion clouds. Multipole traps show a flatter potential in their centre and therefore a modified density distribution compared to quadrupole traps. Micromotion is an important issue and will certainly influence the dynamics of crystallized ion structures. Our experiment tends to investigate possible crystallization processes in the multipole. In a more general way, we are interested in the study of the dynamics and thermodynamics of large ion clouds in traps of different geometry.

A small number of laser-cooled ions trapped in a linear radiofrequency multipole trap forms a hollow tube structure. We have studied, by means of molecular dynamics simulations, the structural transition from a double ring to a single ring of ions. We show that the single-ring configuration has the advantage to inhibit the thermal transfer from the rf-excited radial components of the motion to the axial component, allowing to reach the Doppler limit temperature along the direction of the trap axis. Once cooled in this particular configuration, the ions experience an angular dependency of the confinement if the local adiabaticity parameter exceeds the empirical limit. Bunching of the ion structures can then be observed and an analytic expression is proposed to take into account for this behaviour.

Additional radio-frequency (rf) potentials applied to linear multipole traps create extra field nodes in the radial plane which allow one to confine single ions, or strings of ions, in totally rf field-free regions. The number of nodes depends on the order of the applied multipole potentials and their relative distance can be easily tuned by the amplitude variation of the applied voltages. Simulations using molecular dynamics show that strings of ions can be laser cooled down to the Doppler limit in all directions of space. Once cooled, organized systems can be moved with very limited heating, even if the cooling process is turned off.

We analyse the possibility of cooling ions with a single laser beam, due to the coupling between the three components of their motion induced by the Coulomb interaction. For this purpose, we numerically study the dynamics of ion clouds of up to 140 particles, trapped in a linear quadrupole potential and cooled with a laser beam propagating in the radial plane. We use Molecular Dynamics simulations and model the laser cooling by a stochastic process. For each component of the motion, we systematically study the dependence of the temperature with the anisotropy of the trapping potential. Results obtained using the full radio-frequency (rf) potential are compared to those of the corresponding pseudo-potential. In the rf case, the rotation symmetry of the potential has to be broken to keep ions inside the trap. Then, as for the pseudo-potential case, we show that the efficiency of the Coulomb coupling to thermalize the components of motion depends on the geometrical configuration of the cloud. Coulomb coupling appears to be not efficient when the ions organise as a line or a pancake and the three components of motion reach the same temperature only if the cloud extends in three dimensions.

A ring crystal of ions trapped in a linear multipole trap is studied as a basis for an optical frequency standard. The equilibrium conditions and cooling possibilities are discussed through an analytical model and molecular dynamics simulations. A configuration which reduces the frequency sensitivity to the fluctuations of the number of trapped ions is proposed. The systematic shifts for the electric quadrupole transition of calcium ions are evaluated for this ring configuration. This study shows that a ring of 10 or 20 ions allows to reach a short term stability better than for a single ion without introducing limiting long term fluctuations.

The radiofrequency quadrupole linear ion trap is a widely used device in physics and chemistry. When used for trapping of large ion clouds, the presence of anharmonic terms in the radiofrequency potential limits the total number of stored ions. In this paper, we have studied the anharmonic content of the trapping potential for different implementations of a quadrupole trap, searching for the geometry best suited for the trapping of large ion clouds. This is done by calculating the potential of a real trap using SIMION8.0, followed by a fit, which allows us to obtain the evolution of anharmonic terms for a large part of the inner volume of the trap.

The interrogation of an ultra-narrow clock transition of a single trapped ion for optical frequency metrology requires a laser stabilized to a couple of Hz per second with a linewidth of the same order of magnitude. Today, lasers in the visible have reached the Hz-range in frequency stability, if locked onto a high-finesse, ultra-stable reference cavity. Vertical mounting of the reference cavity can reduce its sensitivity to vibrations as described in \cite{notcutt05}. We have designed a comparable vertical cavity with an overall length of 150 mm resulting in a Free Spectral Range of 1GHz. Optimisation of the cavity design has been carried out with a Finite-Elements Method, leading to expected relative length variations below 10$^{-14}$ under the influence of gravity acceleration (1 $g$). The variation of different geometric parameters has been studied. The analysis of the different noise sources shows that, for a regime superior to a tenth of a hertz, the fast linewidth of the laser will not be limited by the cavity characteristics.

A scheme for a THz frequency standard based on three-photon coherent population trapping in stored ions is proposed. Assuming the propagation directions of the three lasers obey the phase matching condition, we show that stability of few 10$^{-14}$ at one second can be reached with a precision limited by power broadening to $10^{-11}$ in the less favorable case. The referenced THz signal can be propagated over long distances, the useful information being carried by the relative frequency of the three optical photons.

A recent evaluation of the frequency uncertainty expected for an optical frequency standard based on a single trapped $^{43}$Ca$^+$ ion was published in Phys. Rev. A {\bf 72} (2005) 043404. The paper contains some interesting information like systematic frequency shifts but fails to depict their uncertainty, leading to confuse accuracy and precision. The conclusions about the major contribution to the frequency shift are not consistent with the presented calculations and omit comparisons with data published previously.

The lifetime of the 3d^2D_5/2-level in singly-ionized calcium has been measured by the electron-shelving technique on different samples of rf trapped ions. The metastable state has been directly populated by exciting the dipole-forbidden 4S_1/2 - 3D_5/2 transition. In ion clouds, the natural lifetime of this metastable level has been measured to be (1095+-27) ms. For the single-ion case, we determined a lifetime of (1152+-20) ms. The 1sigma-error bars at the 2%-level have different origins for the two kinds of experiments: data fitting methods for lifetime measurements in an ion cloud and control of experimental parameters for a single ion. De-shelving effects are extensively discussed. The influence of differing approaches for the processing of the single-ion quantum jump data on the lifetime values is shown. Comparison with recent measurements shows excellent agreement when evaluated from a given method.