The high-resolution ro-vibrational spectroscopy of the H2+ molecular ion by resonance-enhanced multiphoton dissociation (REMPD) requires a state-selective source of H2+. In this thesis we present work on a functional state selective H2+ ion source using resonance enhanced multiphoton ionisation (REMPI) with a 303 nm pulsed laser.The second part of the thesis presents numerical simulations of sympathetic cooling in linear RF traps, whose main application is the GBAR project (Gravitational Behaviour of Antihydrogen at Rest) which involves sympathetic cooling of an antimatter H̄+ ion by laser-cooled Be+ ions. We developed a GPU code using a variable timestep technique enabling a fast description of Coulomb interactions. We discuss the influence of RF heating and scaling laws between cooling times, initial energy and ion numbers in the cooling crystal. We show that the H̄ sympathetic cooling step of GBAR could be feasible using a rotationally asymmetric two-component Be+/HD+ crystal which appears more effective than a single-component Be+ crystal. We find that the H̄+ ion’s capture by this crystal could be detected experimentally by Fourier analysis of the fluorescence data.
The high-resolution ro-vibrational spectroscopy of the H2+ molecular ion by resonance-enhanced multiphoton dissociation (REMPD) requires a state-selective source of H2+. In this thesis we present work on a functional state selective H2+ ion source using resonance enhanced multiphoton ionisation (REMPI) with a 303 nm pulsed laser.The second part of the thesis presents numerical simulations of sympathetic cooling in linear RF traps, whose main application is the GBAR project (Gravitational Behaviour of Antihydrogen at Rest) which involves sympathetic cooling of an antimatter H̄+ ion by laser-cooled Be+ ions. We developed a GPU code using a variable timestep technique enabling a fast description of Coulomb interactions. We discuss the influence of RF heating and scaling laws between cooling times, initial energy and ion numbers in the cooling crystal. We show that the H̄ sympathetic cooling step of GBAR could be feasible using a rotationally asymmetric two-component Be+/HD+ crystal which appears more effective than a single-component Be+ crystal. We find that the H̄+ ion’s capture by this crystal could be detected experimentally by Fourier analysis of the fluorescence data.
Production de source sélectives des ions H2+ et simulations numériques de refroidissement sympathique dans les pièges de radio fréquence La spectroscopie ro-vibrationelle de haute résolution de l’ion moleculaire H2+ par REMPD requiert une source sélective en état interne. Dans cette thèse nous présentons notre travail de conception et de réalisation d’une telle source utilisant la photo-ionisation multiphotonique résonante (REMPI) de H2 à l’aide d’un laser pulsé à 303 nm.Dans un deuxième temps nous présentons nos simulations numériques de refroidissement sympathique dans un piège de Paul linéaire, avec pour application principale le projet GBAR qui implique le refroidissement sympathique d’un ion d’antimatière H̄+ par des ions Be+ refroidis par laser. Nous avons dévelopé un code GPU utilisant un pas de temps variable permettant de décrire les interactions coulombiennes de façon efficace. Nous discutons de l’influence du chauffage RF et de lois d’échelles entre le temps de capture, l’énergie initiale et le nombre d’ions dans le cristal. Nous montrons que le refroidissement sympathique de H̄ requis pour GBAR pourrait fonctionner avec un cristal dissymétrique de Be+/HD+ qui semble plus efficace que le Be+ seul. Nous montrons qu’avec un tel cristal la capture du H̄+ pourrait être détectée expérimentalement par analyse de Fourier des données de fluorescence.
The objective of the project is to perform high-resolution Doppler-free two-photon vibrational spectroscopy of the H2+ molecular ion for accurate electron to proton mass ratio determination. Trapping and laser-cooling of the H2+ ions is necessary. Since H2+ molecular ions cannot be directly laser cooled, a solution is the implementation of sympathetic cooling via a laser cooled Be+ ions. In the first part of this thesis the design and implementation of a linear Paul trap is presented. This trap is suitable to confine H2+ and Be+ ions while allowing good optical access for multiple laser sources and the imaging system. The second part describes a low power, diode based laser system to provide narrow linewidth 626nm light, and a high power, fiber laser based laser system. Subsequently, a bow-tie cavity is presented to frequency double the 626nm light to obtain 313nm light for Be+ Doppler-cooling. In the last part the operational readiness of the trap and the fiber laser based 313nm laser source is demonstrated by the observation of Be+ Coulomb crystals. Electron impact ionization of H2 present in the residual gas allows to observe sympathetic cooling and shows that the developed setup can provide the experimental conditions for precision spectroscopy of H2+.
We report on the production of cold, state-selected H2+ molecular ions in a linear rf trap. The ions are produced by (3+1) resonance-enhanced multiphoton ionization (REMPI) of H2, and sympathetically cooled by laser-cooled Be+ ions. After demonstrating and characterizing the REMPI process, we use photodissociation by a deep UV laser at 213 nm to verify the high vibrational purity of the produced H2+ ion samples. Moreover, the large difference between the photodissociation efficiencies of ions created in the v=0 and v=1 levels provides a way to detect a $v=0\ensuremath{\rightarrow}1$ transition. These results pave the way towards high-resolution vibrational spectroscopy of H2+ for fundamental metrology applications.
We report a method of efficiently generating ultracold hydrogen molecular ions HD+ in a segmented linear ion trap. HD+ ions are created by [2+1′] resonance-enhanced multiphoton ionization (REMPI) of an HD supersonic molecular beam, and sympathetically cooled by laser-cooled Be+ ions. The HD+ ions are generated species-selectively using 201 nm and 395 nm pulse lasers with energies of 0.08 mJ (5.1 × 106 W/cm2) and 1.5 mJ (9.5 × 107 W/cm2) respectively. The average loading rate of 4.3(2) HD+ ions per second in the ion trap is determined by comparing the experimental images with the simulated images of Be+-HD+ bi-component Coulomb crystals. This method paves a way to produce the state-selected HD+ ions, which can improve the signal strengths of the selected rovibrational transitions of HD+ ions.
In recent years there has been much progress in the field of cold and ultracold molecular physics and a variety of experimental techniques for producing cold matter now exist. In particular, the generation of trapped molecular ions at mK temperatures has been achieved by sympathetic-cooling with laser-cooled atomic ions. By implementing schemes to selectively prepare and control the internal quantum state of molecular ions, and developing detection techniques, it will be increasingly possible to study cold state-selected chemical collisions in an ion-trap. Most molecular species produced in a selected rovibrational state have a lifetime of a few seconds, before the population is redistributed across numerous rovibrational states by interaction with the ambient blackbody radiation (BBR). Consequently, the investigation of state-selected reaction dynamics at low temperatures in experiments where long time scales (minutes to hours) are required, is hindered. This thesis looks into developing strategies that maintain state selection in molecular ions, allowing one to observe state-selected reactions in cold environments, in particular the state-selected reaction between C2H+2 and ND3. Examining reactive ion molecule collisions under cold conditions provides insight into fundamental reaction dynamics, which are thermally averaged out at higher temperatures. A theoretical model is used to investigate laser-driven, blackbody-mediated, rotational cooling schemes for several 1Σ and 2Π diatomic species. The rotational cooling is particularly effective for DCl+ and HCl+, for which 92% and >99% (respectively) of the population can be driven into the rovibrational ground state. For the other systems a broadband optical pumping source is found to enhance the population that can be accumulated in the rovibrational ground state by up to 29% more than that achieved when exciting a single transition. The influence of the rotational constant, dipole moments and electronic state of the diatomics on the achievable rotational cooling is also studied. This approach is extended to consider the BBR interaction and rotational cooling of a linear polyatomic ion, C2H+2, which has a 2Π electronic ground state. The (1-0) band of the ν5 cis-bending mode is infrared active and strongly overlaps the 300 K blackbody spectrum. Hence the lifetimes of state-selected rotational levels are found to be short compared to the typical timescale of ion trapping experiments. Laser cooling schemes are proposed that could be experimentally viable, which involves simultaneous pumping of a set of closely spaced Q-branch transitions on the 2Δ5/2-2Π3/2 band together with two 2Σ+– 2Π1/2 lines. It is shown that this should lead to >70% of total population in the lowest rotational level at 300 K and over 99% at 77 K. In order to identify states of the acetylene ion that could be trapped sufficiently long enough for state-selected reactions in the ion trap with decelerated ND3, the theoretical work has been complemented by experimental investigations into the production of C2H+2 in selected states, and ion trapping of the same using sinusoidal and digital trapping voltages. Appropriate (2+1) REMPI (Resonance Enhanced Multiphoton Ionization) schemes are used to produce C2H+2 in different quantum states, with (1+1) Resonance Enhanced Multiphoton Dissociation (REMPD) employed to detect the ion thus produced. The concept of digital ion trapping for ejection onto MCPs is introduced. A comprehensive comparison between sinusoidal and digital trapping fields has been performed with respect to trap depth and stability regions. Programs have been developed to calculate the stability regions for different ions under varying experimental conditions. The trap depth has been derived for both digital and sinusoidal trapping fields. It is observed that as τ increases, the trap depth of a digital trap increases. For τ = 0.293, the trap depth and stability diagram for both sinusoidal and digital trapping fields would be equivalent. The trap depth at which the sinusoidal trap operates experimentally in our research group is ˜1.36 eV. In contrast, the experimental parameters at which the digital trap operates generates a trap depth of 1.21 eV. Ca+ Coulomb crystals have been formed, stably trapped and stored for extended periods of time in both sinusoidally and digitally time-varying trapping fields. The sympathetic cooling of a diverse range of ions into Ca+ Coulomb crystals is demonstrated, again using both sinusoidal and digital trapping fields. Mass spectrometric detection of ionic reaction products using a novel ejection scheme has been developed, where ejection is achieved by switching off the trapping voltage and converting the quadrupole trap into an extractor-repeller pair by providing the ion trap electrodes with appropriate ejection pulses. This technique is developed using a digital trapping voltage rather than the sinusoidal trapping voltage, as ejection with sinusoidal trapping voltages is not clean (resonance circuitry used in the electronics induces ringing after switching off the trapping voltage). Coulomb crystals, both pure Ca+ and multi-component crystals, are ejected from the ion trap and the TOF trace obtained is recorded on an oscilloscope. When the integrated, base-line subtracted TOF peak is plotted against the number of ions in a Ca+ crystal and sympathetically-cooled Ca+ – CaF+ crystal, a linear relationship is obtained. This technique is found to be well mass-resolved, with the signal arising from CaOH+ (57 amu) and CaOD+ (58 amu) resolvable on the TOF trace. This technique would enable one to monitor a reaction in a Coulomb crystal where the reactant and product species are both either lighter or heavier than calcium, such as the reaction between C2H+2 and ND3, something which has not been previously possible. It is, also, potentially a very important technique for reactions with many product channels.
The GBAR (Gravitational Behaviour of Antihydrogen at Rest) experiment at CERN, situated on the antiproton decelerator ring (AD), is aimed at investigating the free fall of antihydrogen atoms prepared at rest, as suggested by J. Walz and Th. Hänsch [1]. This experiment employs two trapped ions: one is a Be+ ion cooled via laser, while the other, an Hbar+ ion, undergoes cooling through interactions with the Be+ ion (sympathetic cooling). We are developing a test-bed experiment designed to explore sympathetic cooling of a light ion using a cloud of laser-cooled heavy ions, mimicking the conditions anticipated in the GBAR project [2]. The experimental setup involves the pairing of 88Sr+ (laser-cooled ion) and 9Be+ (sympathetically cooled ion). The choice of these ions offers two advantages: the ability to optically address the 9Be+ ion for thermometry measurements and their mass ratio (88/9 ≈ 9.8) closely resembling that in the GBAR project (9/1). Preliminary experimental results [3] demonstrate sympathetic cooling of 9Be+ ions by laser-cooled 88Sr+ ions, forming a Coulomb crystal. Detection of sympathetically cooled ions relies on analyzing Coulomb crystal images, revealing dark areas where non-laser-cooled Be+ ions reside. Molecular dynamics simulations showed strong spatial segregation for both species, due to their high mass ratios [4]. However, the initial experiment did not include laser addressing of the 9Be+ ions for measuring cooling dynamics and control over the initial energy of Be+ ions. The next stage of the project therefore involves adding the 313nm laser for addressing Be+ ions and utilizing a 2-zone trap to control the initial energy of a single Be+ ion. This will enable us to measure for the first time the capture dynamics of a light ion by a Coulomb crystal and to follow its cooling over several decades (typically from 10000K to mK). We will compare these measurements with numerical simulations [4]. Initially, only Sr+ ions were employed to validate trapping and cooling conditions, characterize photon collection optics, and test ion transport protocols between trapping zones. A method utilizing Doppler recooling was developed to characterize the initial energy of Sr+ ions upon arrival in the target trap. Subsequently, using the Be+ ion cooling laser at 313 nm, it will be possible to cool a single Be+ ion and transport it with controlled kinetic energy to the second trapping zone, already loaded with a Sr+ Coulomb crystal. The kinetic energy loss of the Be+ ion is quantified by measuring laser-induced fluorescence rate at resonance, which produces no laser cooling or heating. Thermalization of the light ion via coulomb interactions will then be studied for different heavy-ion crystal temperatures, shapes and ion numbers.