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The text below was written during two visits that Daniel Segal made at Universit{\'e} Paris 13. Danny stayed at Laboratoire de Physique des Lasers the summers of 2008 and 2009 to participate in the exploration of a novel lead in the field of ultra-high resolution spectroscopy. Our idea was to probe trapped molecular ions using Quantum Logic Spectroscopy (QLS) in order to advance our understanding of a variety of fundamental processes in nature. At that time, QLS, a ground-breaking spectroscopic technique, had only been demonstrated with atomic ions. Our ultimategoals were new approaches to the observation of parity violation in chiral molecules and tests of time variations of the fundamental constants. This text is the original research proposal written eight years ago. We have added a series of notes to revisit it in the light of what has been since realized in the field., Comment: 16 pages, 1 figure. Published in a special issue of Journal of Modern Optics in memory of Prof Danny Segal

We report the laser cooling of a single $^{40}\text{Ca}^+$ ion in a Penning trap to the motional ground state in one dimension. Cooling is performed in the strong binding limit on the 729-nm electric quadrupole $S_{1/2}\leftrightarrow D_{5/2}$ transition, broadened by a quench laser coupling the $D_{5/2}$ and $P_{3/2}$ levels. We find the final ground state occupation to be $98\pm1\%$. We measure the heating rate of the trap to be very low with $\dot{\bar{n}}\approx 0.3\pm0.2\textrm{s}^{-1}$ for trap frequencies from $150-400\textrm{kHz}$, consistent with the large ion-electrode distance., Comment: 4 pages, 6 figures. Accepted: Phys. Rev. Lett. (2016) http://journals.aps.org/prl/accepted/b6074YefH1115b5881f77975417a6ae0bc9f652a7

We study qubit-mediated energy transfer between two electron reservoirs by adopting a numerically-exact influence functional path-integral method. This non-perturbative technique allows us to study the system's dynamics beyond the weak coupling limit. Our simulations for the energy current indicate that perturbative-Markovian Master equation predictions significantly deviate from exact numerical results already at intermediate coupling, $\pi \rho \alpha_{j,j'}\gtrsim 0.4$, where $\rho$ is the metal (Fermi sea) density of states, taken as a constant, and $\alpha_{j,j'}$ is the scattering potential energy of electrons, between the $j$ and $j'$ states. Markovian Master equation techniques should be therefore used with caution beyond the strictly weak subsystem-bath coupling limit, especially when a quantitative knowledge of transport characteristics is desired.

We have performed laser cooling of Mg ions confined in a Penning trap. The externally produced ions were captured in flight, stored and laser cooled. Laser-induced fluorescence was observed perpendicular to the cooling laser axis. Optical detection down to the single ion level together with electronic detection of the ion oscillations inside the Penning trap have been used to acquire information on the ion storage time, ion number and ion temperature. Evidence for formation of ion crystals has been observed. These investigations are an important prerequisite for sympathetic cooling of simultaneously stored highly-charged ions and precision laser spectroscopy of forbidden transitions in these., Comment: 10 pages, 11 figures, 2 tables

We study current-induced vibrational cooling, heating, and instability in a donor-acceptor rectifying molecular junction using a full counting statistics approach. In our model, electron-hole pair excitations are coupled to a given molecular vibrational mode which is either harmonic or highly anharmonic. This mode may be further coupled to a dissipative thermal environment. Adopting a master equation approach, we confirm the charge and heat exchange fluctuation theorem in the steady-state limit, for both harmonic and anharmonic models. Using simple analytical expressions, we calculate the charge current and several measures for the mode effective temperature. At low bias, we observe the effect of bias-induced cooling of the vibrational mode. At higher bias, the mode effective temperature is higher than the environmental temperature, yet the junction is stable. Beyond that, once the vibrational mode (bias-induced) excitation rate overcomes its relaxation rate, instability occurs. We identify regimes of instability as a function of voltage bias and coupling to an additional phononic thermal bath. Interestingly, we observe a reentrant behavior where an unstable junction can properly behave at a high enough bias. The mechanism for this behavior is discussed.

We study quantum heat exchange in a multi-state impurity coupled to two thermal reservoirs. Allowing for strong system-bath interactions, we show that a steady-state heat exchange fluctuation theorem holds, though the dynamical processes nonlinearly involve the two reservoirs. We accomplish a closed expression for the cumulant generating function, and use it obtain the heat current and its cumulants in a nonlinear thermal junction, the two-bath spin-boson model.

We produce YbF molecules with a density of 10^18 m^-3 using laser ablation inside a cryogenically-cooled cell filled with a helium buffer gas. Using absorption imaging and absorption spectroscopy we study the formation, diffusion, thermalization and optical pumping of the molecules. The absorption images show an initial rapid expansion of molecules away from the ablation target followed by a much slower diffusion to the cell walls. We study how the time constant for diffusion depends on the helium density and temperature, and obtain values for the YbF-He diffusion cross-section at two different temperatures. We measure the translational and rotational temperatures of the molecules as a function of time since formation, obtain the characteristic time constant for the molecules to thermalize with the cell walls, and elucidate the process responsible for limiting this thermalization rate. Finally, we make a detailed study of how the absorption of the probe laser saturates as its intensity increases, showing that the saturation intensity is proportional to the helium density. We use this to estimate collision rates and the density of molecules in the cell., Comment: 20 pages, 11 figures, minor revisions following referee suggestions

We demonstrate Doppler-free saturated absorption spectroscopy of cold molecular radicals formed by laser ablation inside a cryogenic buffer gas cell. By lowering the temperature, congested regions of the spectrum can be simplified, and by using different temperatures for different regions of the spectrum a wide range of rotational states can be studied optimally. We use the technique to study the optical spectrum of YbF radicals with a resolution of 30 MHz, measuring the magnetic hyperfine parameters of the electronic ground state. The method is suitable for high resolution spectroscopy of a great variety of molecules at controlled temperature and pressure, and is particularly well-suited to those that are difficult to produce in the gas phase., Comment: 11 pages, 4 figures

We report on the design and testing of an array of Penning ion traps made from printed circuit board. The system enables fast shuttling of ions from one trapping zone to another, which could be of use in quantum information processing. We describe simulations carried out to determine the optimal potentials to be applied to the trap electrodes for enabling this movement. The results of a preliminary experiment with a cloud of laser cooled calcium ions demonstrate a round-trip shuttling efficiency of up to 75%., Comment: 7 pages, 12 figures

Since Hund's work on the ammonia molecule, the double well potential has formed a key paradigm in physics. Its importance is further underlined by the central role it plays in the Landau theory of phase transitions. Recently, the study of entanglement properties of many-body systems has added a new angle to the study of quantum phase transitions of discrete and continuous degrees of freedom, i.e., spin and harmonic chains. Here we show that control of the radial degree of freedom of trapped ion chains allows for the simulation of linear and non-linear Klein-Gordon fields on a lattice, in which the parameters of the lattice, the non-linearity and mass can be controlled at will. The system may be driven through a phase transition creating a double well potential between different configurations of the ion crystal. The dynamics of the system are controllable, local properties are measurable and tunnelling in the double well potential would be observable., Comment: 6 pages, 5 figures

We report the experimental characterization of axialization - a method of reducing the magnetron motion of a small number of ions stored in a Penning trap. This is an important step in the investigation of the suitability of Penning traps for quantum information processing. The magnetron motion was coupled to the laser-cooled modified cyclotron motion by the application of a near-resonant oscillating quadrupole potential (the "axialization drive"). Measurement of cooling rates of the radial motions of the ions showed an order-of-magnitude increase in the damping rate of the magnetron motion with the axialization drive applied. The experimental results are in good qualitative agreement with a recent theoretical study. In particular, a classical avoided crossing was observed in the motional frequencies as the axialization drive frequency was swept through the optimum value, proving that axialization is indeed a resonant effect., Comment: 8 pages, 9 figures

Ions stored in Penning traps may have useful applications in the field of quantum information processing. There are, however, difficulties associated with the laser cooling of one of the radial motions of ions in these traps, namely the magnetron motion. The application of a small radio-frequency quadrupolar electric potential resonant with the sum of the two radial motional frequencies has been shown to couple these motions and to lead to more efficient laser cooling. We present an analytical model that enables us to determine laser cooling rates in the presence of such an 'axializing' field. It is found that this field leads to an averaging of the laser cooling rates for the two motions and hence improves the overall laser cooling efficiency. The model also predicts shifts in the motional frequencies due to the axializing field that are in qualitative agreement with those measured in recent experiments. It is possible to determine laser cooling rates experimentally by studying the phase response of the cooled ions to a near resonant excitation field. Using the model developed in this paper, we study the expected phase response when an axializing field is present., Comment: 22 pages, 7 figures

An overview is presented of laser spectroscopy experiments with cold, trapped, highly-charged ions, which will be performed at the HITRAP facility at GSI in Darmstadt (Germany). These high-resolution measurements of ground state hyperfine splittings will be three orders of magnitude more precise than previous measurements. Moreover, from a comparison of measurements of the hyperfine splittings in hydrogen- and lithium-like ions of the same isotope, QED effects at high electromagnetic fields can be determined within a few percent. Several candidate ions suited for these laser spectroscopy studies are presented., Comment: 5 pages, 1 figure, 1 table. accepted for Canadian Journal of Physics (2006)

We present a thorough analysis of the electronic detection of charged particles, confined in a Penning trap, via image charges induced in the trap electrodes. Trapping of charged particles in an electrode structure leads to frequency shifts, which are due to image charge and space charge effects. These effects are of importance for Penning trap experiments which involve high charge densities or require high precision in the motional frequencies. Our analysis of image charges shows that only (higher order) odd powers of the particle displacement lead to induced charge differences, giving rise to a signal. This implies that, besides the centre-of-mass frequency of a trapped particle cloud, also higher order individual particle frequencies induce a signal, which can be picked up by an electronic detection circuit attached to the trap electrodes. We also derive analytic expressions for the image charge and space charge induced frequency shifts and perform simulations of space charge effects. In relation to this, we discuss the consequences of the shifted particle frequencies for resistive cooling of the particle motion., Comment: 16 pages, 4 figures

We present a number of alternative designs for Penning ion traps suitable for quantum information processing (QIP) applications with atomic ions. The first trap design is a simple array of long straight wires which allows easy optical access. A prototype of this trap has been built to trap Ca+ and a simple electronic detection scheme has been employed to demonstrate the operation of the trap. Another trap design consists of a conducting plate with a hole in it situated above a continuous conducting plane. The final trap design is based on an array of pad electrodes. Although this trap design lacks the open geometry of the traps described above, the pad design may prove useful in a hybrid scheme in which information processing and qubit storage take place in different types of trap. The behaviour of the pad traps is simulated numerically and techniques for moving ions rapidly between traps are discussed. Future experiments with these various designs are discussed. All of the designs lend themselves to the construction of multiple trap arrays, as required for scalable ion trap QIP., Comment: 11 pages, 10 figures

We propose a novel type of precision laser spectrometer for trapped, highly charged ions nearly at rest. It consists of a cylindrical open-endcap Penning trap in which an externally produced bunch of highly charged ions can be confined and investigated by means of laser spectroscopy. The combination of confinement, cooling and compression of a dense ion cloud will allow the ground state hyperfine splitting in highly charged ions to be measured with an accuracy three orders of magnitude better than in any previous experiment. A systematic study of different charge states and different isotopes of the same element allows for highly sensitive tests of bound-state QED and for a precision determination of nuclear properties. Apart from stable isotopes, also radioactive species with half-lives longer than about one hour can be investigated., Comment: 8 pages, 7 figures

Laser spectroscopy studies are being prepared to measure the 1s ground state hyperfine splitting in trapped cold highly charged ions. The purpose of such experiments is to test quantum electrodynamics in the strong electric field regime. These experiments form part of the HITRAP project at GSI. A brief review of the planned experiments is presented., Comment: 4 pages, 4 figures, accepted for publication (NIMB)

We report a study of the axialisation and laser cooling of single ions and small clouds of ions in a Penning trap. A weak radiofrequency signal applied to a segmented ring electrode couples the magnetron motion to the cyclotron motion, which results in improved laser cooling of the magnetron motion. This allows us to approach the trapping conditions of a Paul trap, but without any micromotion. Using an ICCD camera we show that the motion of a single ion can be confined to dimensions of the order of 10 $\mu$m. We have measured increased magnetron cooling rates using an rf-photon correlation technique. For certain laser cooling conditions, the magnetron motion of the centre of mass of the cloud grows and stabilises at a large value. This results in the ions orbiting the centre of the trap together in a small cloud, as confirmed by photon-photon correlation measurements., Comment: 10 pages, 6 figures, proceedings of the TCPFI 2002 conference, to be published in J. Phys. B

Interest in lossless nonlinearities has focussed on the the dispersive properties of $\Lambda $ systems under conditions of electromagnetically induced transparency (EIT). We generalize the lambda system by introducing further degenerate states to realize a `Chain $ \Lambda $' atom where multiple coupling of the probe field significantly enhances the intensity dependent dispersion without compromising the EIT condition., Comment: 6 pages, 7 figures, revtex 4, Two errors corrected (|D_0^{(7)}> and R^{(7)}, Replaced with version accepted in Phys. Rev. A

This paper presents a wide-ranging theoretical and experimental study of non-adiabatic transient phenomena in a $\Lambda $ EIT system when a strong coupling field is rapidly switched on or off. The theoretical treatment uses a Laplace transform approach to solve the time-dependent density matrix equation. The experiments are carried out in a Rb$^{87}$ MOT. The results show transient probe gain in parameter regions not previously studied, and provide insight into the transition dynamics between bare and dressed states., Comment: 19 Pages, 9 Figures, 1 in colour. RevTex 4.0 Submitted to Physical Review A

We have observed clear Rabi oscillations of a weak probe in a strongly driven three-level lambda system in laser-cooled rubidium for the first time. When the coupling field is non-adiabatically switched on using a Pockels cell, transient probe gain without population inversion is obtained in the presence of uncoupled absorptions. Our results are supported by three-state computations., Comment: 4 pages, 4 figures, experimental results

A theoretical description of quantum mechanical steady states is developed. Applications for simple quantum mechanical systems described in terms of coupled level structures yield a formulation equivalent to time independent scattering theory. Applications to steady states of thermally relaxing systems leads to time independent scattering theory in Liouville space that is equivalent to the tetradic Green's function formalism. It provides however a direct route to derive particular forms of the Liouville equation applicable in steady state situations. The theory is applied to study the conduction properties in the super-exchange model of a metal-molecule-metal contact weakly coupled to the thermal environment. The energy resolved temperature dependent transmission probability, as well as its coherent (tunneling) and incoherent (activated) parts, are calculated using the Redfield approximation. These components depend differently on the energy gap (or barrier), on the temperature and on the bridge length. The coherent component is most important at low temperatures, large energy gaps and small chain lengths. The incoherent component dominates in the opposite limits. The integrated transmission provides a generalization of the Landauer conduction formula for small junctions in the presence of thermal relaxation., Comment: 31 pages, 6 figures. Chemical Physics, in press

Observations of a doubly driven V system probed to a fourth level in an N configuration are reported. A dressed state analysis is also presented. The expected three-peak spectrum is explored in a cold rubidium sample in a magneto-optic trap. Good agreement is found between the dressed state theory and the experimental spectra once light shifts and uncoupled absorptions in the rubidium system are taken into account., Comment: 8 pages, 8 figures, Replaced with version scheduled to appear in 1 July 2001 issue of Physical Review A