Non-destructive detection of large molecules without mass limitation.

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 106 amu is propelled through the ion cloud. The induced change in the fluorescence rate of the latter is used as the detection signal. We show that this signal is due to a significant temperature variation triggered by the Coulomb 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.

Correcting symmetry imperfections in linear multipole traps.

Multipole radio-frequency (RF) traps are central to collisional experiments in cryogenic environments. They also offer possibilities to generate new type of ion crystals topologies and in particular the potential to create infinite 1D/2D structures: ion rings and ion tubes. However, multipole traps have also been shown to be very sensitive to geometrical misalignment of the trap rods, leading to additional local trapping minima. The present work proposes a method to correct non-ideal potentials, by modifying the applied RF amplitudes for each trap rod. This approach is discussed for the octupole trap, leading to the restitution of the ideal Mexican-Hat-like pseudo-potential, expected in multipole traps. The goodness of the compensation method is quantified in terms of the choice of the diagnosis area, the residual trapping potential variations, the required adaptation of the applied RF voltage amplitudes, and the impact on the trapped ion structures. Experimental implementation for macroscopic multipole traps is also discussed, in order to propose a diagnostic method with respect to the resolution and stability of the trap drive. Using the proposed compensation technique, we discuss the feasibility of generating a homogeneous ion ring crystal, which is a measure of quality for the obtained potential well.

Coulomb crystallization of highly charged ions.

Control over the motional degrees of freedom of atoms, ions, and molecules in a field-free environment enables unrivalled measurement accuracies but has yet to be applied to highly charged ions (HCIs), which are of particular interest to future atomic clock designs and searches for physics beyond the Standard Model. Here, we report on the Coulomb crystallization of HCIs (specifically (40)Ar(13+)) produced in an electron beam ion trap and retrapped in a cryogenic linear radiofrequency trap by means of sympathetic motional cooling through Coulomb interaction with a directly laser-cooled ensemble of Be(+) ions. We also demonstrate cooling of a single Ar(13+) ion by a single Be(+) ion-the prerequisite for quantum logic spectroscopy with a potential 10(-19) accuracy level. Achieving a seven-orders-of-magnitude decrease in HCI temperature starting at megakelvin down to the millikelvin range removes the major obstacle for HCI investigation with high-precision laser spectroscopy.

Above threshold dissociation of vibrationally cold HD+ molecules.

The experimental study of molecular dissociation of H2+ by intense laser pulses is complicated by the fact that the ions are initially produced in a wide range of vibrational states, each of which responds differently to the laser field. An electrostatic storage device has been used to radiatively cool HD+ ions enabling the observation of above threshold dissociation from the ground vibrational state by 40 fs laser pulses at 800 nm. At the highest intensities used, dissociation through the absorption of at least four photons is found to be the dominant process.

Evidence for rescattering in intense, femtosecond laser interactions with a negative ion.

It is now well established that energetic electron emission, nonsequential ionization, and high harmonic generation, produced during the interaction of intense, femtosecond laser pulses with atoms (and atomic positive ions), can be explained by invoking rescattering of the active electron in the laser field, the so-called rescattering mechanism. In contrast for negative ions, the role of rescattering has not been established experimentally. By irradiating F- ions with ultrashort laser pulses, F+ ion yields as a function of intensity for both linearly and circularly polarized light have been measured. We find that, at intensities well below saturation for F+ production by sequential ionization, there is a small but significant enhancement in the yield for the case of linearly polarized light, providing the first clear experimental evidence for the existence of the rescattering mechanism in negative ions.