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arXiv:2303.00650 · Journal of the Optical Society of America B

Transient fluorescence with a single trapped ion

Nicolás A. Nuñez Barreto, Lucas Giardino, Carla Crucianelli, Muriel Bonetto, Martín Drechsler, Christian Tomás Schmiegelow

Published Feb 8, 2023• 1 citation
arXivHTMLPDF

Abstract

In this paper, we present a method to measure transient fluorescent dynamics with single trapped ions in a Paul trap. We use 40 Ca + ions that exhibit a Λ-type three-level system and measure the characteristic optical pumping times between the ground S 1/2 and the meta-stable D 3/2 levels. We prepare one of these states and then pump it to the opposite via the excited P 1/2 state. By measuring the scattered photons of the ion, we retrieve transient curves of the atomic fluorescence. These curves provide fundamental information about the atomic system, such as branching fractions and excited-state lifetimes, as well as experimental parameters like the efficiency of the detection system and the saturation parameter of one of the transitions. Finally, we study the time-dependent fluorescence as a function of optical power and detuning of the lasers and find a very good agreement with simulating the dynamics via a three-level open quantum system through a set of optical Bloch equations. Being able to record time-dependent fluorescence is of particular interest as it contains information about the temperature, cooling, and heating dynamics of the ion.

DOI
10.1364/josab.482639

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In this paper, we present a method to measure transient fluorescent dynamics with single trapped ions in a Paul trap. We use 40 Ca + ions that exhibit a Λ-type three-level system and measure the characteristic optical pumping times between the ground S 1/2 and the meta-stable D 3/2 levels. We prepare one of these states and then pump it to the opposite via the excited P 1/2 state. By measuring the scattered photons of the ion, we retrieve transient curves of the atomic fluorescence. These curves provide fundamental information about the atomic system, such as branching fractions and excited-state lifetimes, as well as experimental parameters like the efficiency of the detection system and the saturation parameter of one of the transitions. Finally, we study the time-dependent fluorescence as a function of optical power and detuning of the lasers and find a very good agreement with simulating the dynamics via a three-level open quantum system through a set of optical Bloch equations. Being able to record time-dependent fluorescence is of particular interest as it contains information about the temperature, cooling, and heating dynamics of the ion.
This thesis describes work on numerical modelling of the 43Ca+ ion in a Paul trap using the optical Bloch equations. This is a challenging system to study, with many states involved in the internal dynamics. A major outcome is the development of a cooling scheme for the 146.09 gauss atomic clock transitions which makes use of a dark resonance. It is much more effective than methods that avoid coherent effects. The scheme is realised in experiment. Complicated fluorescence data is modelled very well, and predictions for the ion's motional temperature show good agreement with measured values. Data and fits for an ion that has been Doppler cooled below the Doppler limit are presented. I describe GLOBES, a set of routines that simulates an arbitrary ion in the presence of an arbitrary system of laser beams using the optical Bloch equations. Techniques used to efficiently calculate the steady state, analyse fluorescence scans and solve time-dependent problems for small and large times are discussed. A new routine SILVER IMPER that leapfrogs over the initial dynamics to model the approach to the steady state is introduced. Doppler cooling in 40Ca+ is analysed and two extensions made to the basic theory. The ‘excursion method’ of calculation takes account of the non-linear variation with velocity of the scattering rate. The ‘dynamic method’ allows for the fact that the ion may not be in equilibrium with the incident radiation during its oscillations, a necessity as the timescale of the external motion is of order the characteristic timescale of the internal motion for standard secular frequencies. This 'dynamic effect' is a general property of trapped ion systems and is also observed in a two-state system. A two-variable fluorescence scan taken from a four-laser, five-level system in 40Ca+ is analysed. Techniques to fit large data sets and automatically resolve resonant features are demonstrated. A general treatment of resonant behaviour in three, four and five level pump/probe systems is used to describe the data. This is verified by a second, tailor-made set of scans.
This thesis reports on the setup of a new ion trap apparatus designed for experiments with single ⁴⁰Ca⁺ ions to perform molecular spectroscopy. The calcium ion is laser cooled, allowing for sympathetic cooling of the nonfluorescing molecular ion. The aim of these experiments is to explore loading and identifying molecular ions in RF-Paul traps, as well as developing new spectroscopic tools to measure transitions of molecular ions via the fluorescence of co-trapped ⁴⁰Ca⁺ ions. Ground state cooling of a mixed ion pair is implemented as a first step towards increasing the sensitivity of our technique to the level necessary to measure transitions with low scattering rates (like those present in molecular ions). Doppler cooling on the S(1/2)->P(1/2) transition of the calcium ion results in the formation of a Coulomb crystal, the behavior of which may be used to infer properties of the molecular ion. Following cooling, sideband spectroscopy on the narrow S(1/2)->D(5/2) quadrupole transition of calcium may be used to identify the mass of single molecular ions. This method is verified via a non-destructive measurement on ⁴⁰CaH⁺ and ⁴⁰Ca¹⁶O⁺. The normal modes of the Coulomb crystal can also be used to extract information from the target ion to the control ion. By driving the blue side of a transition, laser induced heating can be put into the two ion system, which leads to changes in fluorescence of the ⁴⁰Ca⁺ ion, first demonstrated with two Ca⁺ isotopes. Increasing the sensitivity of this technique requires ground state cooling of both the ⁴⁰Ca⁺ ion and the ion of interest, enabling the transfer of the ion's motional state into the ground state with high probability. This thesis demonstrates ground state cooling of the atomic ion and sympathetic cooling of a second ion (⁴⁴Ca⁺). Once in the ground state, heating of the Coulomb crystal by scattering photons off of the spectroscopy ion can be measured by monitoring the resolved motional sidebands of the S(1/2)->D(5/2) transition of ⁴⁰Ca⁺, allowing for spectral lines to be inferred. Future experiments will investigate this technique with molecular ions.
We experimentally demonstrate a method to determine the temperature of trapped ions which is suitable for monitoring fast thermalization processes. We show that observing and analyzing the lineshape of dark resonances in the fluorescence spectrum provides a temperature measurement which is accurate over a large dynamic range, applied to single ions and small ion crystals. Laser induced fluorescence is detected over a time of only , allowing for rapid determination of the ion temperature. In the measurement range of 10 −1 – mK we reach better than accuracy. Tuning the cooling laser to selected resonance features allows us to control the ion temperatures between mK and more than mK. Experimental work is supported by a solution of the eight-level optical Bloch equations when including the ions' classical motion. This technique paves the way for many experiments, including heat transport in ion strings, heat engines, non-equilibrium thermodynamics or thermometry of large ion crystals.
We investigate the temporal dynamics of Doppler cooling of an initially hot single trapped atom in the weak-binding regime using a semiclassical approach. We develop an analytical model for the simplest case of a single vibrational mode for a harmonic trap, and show how this model allows us to estimate the initial energy of the trapped particle by observing the time-dependent fluorescence during the cooling process. The experimental implementation of this temperature measurement provides a way to measure atom heating rates by observing the temperature rise in the absence of cooling. This method is technically relatively simple compared to conventional sideband detection methods, and the two methods are in reasonable agreement. We also discuss the effects of rf micromotion, relevant for a trapped atomic ion, and the effect of coupling between the vibrational modes on the cooling dynamics.
Trapped laser-cooled atomic ions are a new tool for understanding cold molecular ions. The atomic ions not only sympathetically cool the molecular ions to millikelvin temperatures, but the bright atomic ion fluorescence can also serve as a detector of both molecular reactions and molecular spectra. We are working towards the detection of single molecular ion spectra by sympathetic heating spectroscopy. Sympathetic heating spectroscopy uses the coupled motion of two trapped ions to measure the spectra of one ion by observing changes in the fluorescence of the other ion. Sympathetic heating spectroscopy is a generalization of quantum logic spectroscopy, but does not require ions in the motional ground state or coherent control of the ion internal states. We have recently demonstrated this technique using two isotopes of Ca+ [Phys. Rev. A, 81, 043428 (2010)]. Limits of the method and potential applications for molecular spectroscopy are discussed.
Abstract We discuss the statistics of emission of photons by a single atom or ion illuminated by a laser beam at the frequency of quasi-resonance between two energy levels, a situation that corresponds to real experiments. We extend this to the case of two laser beams resonant with the energy differences between two excited levels and the ground state (three level atom in V-configuration). We use a novel approach to this type of problem by considering a Kolmogorov equation for the probability distribution of the atomic state, which takes into account first the deterministic evolution of this state under the effect of the incoming laser beam and second the random emission of photons during the spontaneous decay of the excited state(s) to the ground state. This approach yields solvable equations in the two level atom case. For the three level atom case we set the problem and clearly define its frame. The results obtained are valid in both opposite limits of rare and frequent spontaneous decay, compared to the period of the optical Rabi oscillations due to the interaction between resonant excitation and atomic levels. Our analysis gives access to various statistical properties of the fluorescence light, including one showing that its fluctuations in time are not invariants under time reversal. This result makes evident the fundamentally irreversible character of quantum measurements, represented here by the emission of photons of fluorescence.