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Deterministic Preparation of Individual Rubidium-85 Dimers via Photoassociation

R. H. Hobbs

Published Jan 1, 2020• 0 citations
OpenAlex

Abstract

In this thesis, we present experimental methods and results for direct measurements of the photoassociation of two individual ultra-cold rubidium-85 atoms, each prepared in the |F = 2,m_F = −2⟩ ground state. From there two individual rubidium-85 atoms are loaded into separate far-off resonance optical tweezers which are near-deterministically prepared into |F = 2,m_F = −2⟩. The two optical tweezers are then merged and the atoms are exposed to photoassociation light. To ensure the correct frequency of photoassociation light is used a dual cavity locking scheme, capable of generating frequencies with a stability of ±425.7 kHz over a large wavelength range for use in photoassociation spectroscopy, was developed. From there, a light modulation technique is implemented to isolate the photoassociation event from unwanted far-off resonance trap effects, such as the AC Stark shift. By controlling the intensity, frequency, and duration parameters of the photoassociation pulses applied to the rubidium atoms, frequency-dependent, and time-dependent atom loss is observed for a single band of the 0^{+}_{u} series; located at 377.00067±0.00006 THz. The resonance and linewidth data exhibits the same behaviour as photoassociation performed on large atom ensembles within the many-body regime. However, two distinct fast and slow photoassociation rates are observed in contrast to the many-body regime where only a single photoassociation rate constant, K_{PA}, has been reported. This marks a novel physical process which heretofore has not been reported in the field of atomic or molecular physics.

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This thesis presents experimental methods and results for comparative measurements of the photoassociation dynamics of two individual ultracold rubidium-85 atoms when geometry of the trapping potential is changed. An asymmetric trap geometry is hypothesized to change the dynamics of two-atom photoassociation, as the asymmetry increases the probability of the two-atom wavefunction forming as a peaked state. Two atoms in an optical trap, of which the symmetry is controlled via a mechanical iris, are exposed to photoassociation light. The results from the asymmetric trap are compared to the photoassociation dynamics of atoms in a symmetric trap. A paired sample t-test determines a statistically significant difference in the two measurements. This t-test yields a p-value no higher than p = 7 × 10−3 , thus it is likely that the two measurements do not come from the same distribution. This aligns with our hypothesis, and is a new, enlightening piece of research done in the field of few-atom physics.

•Jan 1, 2026•0 citations

Photoassociative Spectroscopy of Ultracold Metastable Argon and Study of Dual Species Trap Loss in a Rubidium-Metastable Argon MOT

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This dissertation presents the findings of two experimental investigations in ultracold atomic and molecular physics: The study of the dual species trap loss in a rubidium - metastable argon magneto-optical trap and the photoassociative spectroscopy of ultracold metastable argon. The interspecies trap loss rate coefficients have been measured for ultracold collisions between 85Rb and 40Ar* in a dual-species magneto-optical trap (MOT) and the two rates have been found to be approximately equal over the range of intensities studied with values of β'Rb–Ar* = 3.0 ± 1.3 × 10-11 cm3/s and β'Ar*–Rb = 1.9 ± 0.9 × 10-11 cm3/s where β' Rb–Ar* is the trap loss coefficient for Rb in the presence of Ar* and β'Ar*–Rb is the reciprocal term. In addition, the trap loss rate coefficient for cold collisions in a metastable argon MOT alone have been measured with an average value of β Ar* = 5.2 ± 1.6 × 10-10 cm3/s. Using a quadrupole mass spectrometer, the production of Ar +, Ar+2, Rb+, and RbAr+ ions in the dual MOT have been observed, clearly identifying heteronuclear Penning and associative ionization as trap loss mechanisms. In the second experiment, the first ever investigation of the photoassociative (PA) spectroscopy of Ar* has been made. The exploratory study focuses on PA spectroscopy near the 4s[3/2]2 + 4p[5/2]3 asymptote of the Ar2* diatomic molecule over a 10 GHz range red detuned of the atomic resonance. With a range of probe laser intensities from ∼ 102–105ISat, 12 resonances have been observed. The spectra have been analyzed using the near-dissociation LeRoy-Bernstein method. Through this analysis, the spectra seem to best correlate with excitations to the 5g state.

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Chemical reactions typically proceed via stochastic encounters between reactants. Going beyond this paradigm, we combined exactly two atoms in a single, controlled reaction. The experimental apparatus traps two individual laser-cooled atoms [one sodium (Na) and one cesium (Cs)] in separate optical tweezers and then merges them into one optical dipole trap. Subsequently, photoassociation forms an excited-state NaCs molecule. The discovery of previously unseen resonances near the molecular dissociation threshold and measurement of collision rates are enabled by the tightly trapped ultracold sample of atoms. As laser-cooling and trapping capabilities are extended to more elements, the technique will enable the study of more diverse, and eventually more complex, molecules in an isolated environment, as well as synthesis of designer molecules for qubits.

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A Rydberg tweezer platform with potassium atoms

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Quantum simulation offers the possibility to study quantum mechanical problems which are untraceable on classical computers. This thesis introduces a novel platform for quantum simulation and presents the first experimental realisation of single potassium atoms trapped in optical tweezers. Interactions between individual atoms are induced by strong energy shifts of atoms excited to states with large principal quantum number, so-called Rydberg states. Either direct excitation to Rydberg states or off-resonant dressing can be used to induce these interactions. We argue that potassium is well-suited for the implementation of Rydberg dressing, enabling simultaneous dressing of both ground states to engineer complex interactions. Using techniques to cool and trap cold atoms, single potassium atoms are prepared in arrays of optical tweezers. Raman sideband cooling reduces vibrational excitations and prepares the atoms close to the motional ground state. This cooling technique mitigates severe limitations for Rydberg dressing, arising from thermal broadening and inhomogeneous light shifts in the array of atoms. To directly excite atoms to Rydberg states, a high power laser setup with two cavity-enhanced frequency doubling stages is constructed, generating up to one Watt of ulta-violet light at 286 nm. By exciting atoms to Rydberg states we observe Rabi oscillations with Rabi frequencies of up to 1 MHz, demonstrating coherent control of Rydberg atoms. Finally, we combine these techniques to observe interactions in two ways: First, we create a so-called superatom of up to four individual atoms using direct excitation and Rydberg-blockade and observe coherent oscillations to this collective state. We measure the expected square root scaling of the effective Rabi frequency with the number of individual atoms, confirming the creation of a many-body entangled state. Secondly, we off-resonantly dress the atoms prepared in a one-dimensional chain and measure correlated interaction shifts over multiple sites. In summary, we have developed a platform for quantum simulation with single atoms in optical tweezers. The presented results show coherent control of single atoms and interactions induced by Rydberg states. We have thus demonstrated that the system is well-suited for quantum simulation of many-body systems.

•Jan 1, 2021•4 citations
In this thesis, we present experimental methods and results for direct measurements of the photoassociation of two individual ultra-cold rubidium-85 atoms, each prepared in the |F = 2,m_F = −2⟩ ground state. From there two individual rubidium-85 atoms are loaded into separate far-off resonance optical tweezers which are near-deterministically prepared into |F = 2,m_F = −2⟩. The two optical tweezers are then merged and the atoms are exposed to photoassociation light. To ensure the correct frequency of photoassociation light is used a dual cavity locking scheme, capable of generating frequencies with a stability of ±425.7 kHz over a large wavelength range for use in photoassociation spectroscopy, was developed. From there, a light modulation technique is implemented to isolate the photoassociation event from unwanted far-off resonance trap effects, such as the AC Stark shift. By controlling the intensity, frequency, and duration parameters of the photoassociation pulses applied to the rubidium atoms, frequency-dependent, and time-dependent atom loss is observed for a single band of the 0^{+}{u} series; located at 377.00067±0.00006 THz. The resonance and linewidth data exhibits the same behaviour as photoassociation performed on large atom ensembles within the many-body regime. However, two distinct fast and slow photoassociation rates are observed in contrast to the many-body regime where only a single photoassociation rate constant, K{PA}, has been reported. This marks a novel physical process which heretofore has not been reported in the field of atomic or molecular physics.
This thesis presents experimental methods and results for comparative measurements of the photoassociation dynamics of two individual ultracold rubidium-85 atoms when geometry of the trapping potential is changed. An asymmetric trap geometry is hypothesized to change the dynamics of two-atom photoassociation, as the asymmetry increases the probability of the two-atom wavefunction forming as a peaked state. Two atoms in an optical trap, of which the symmetry is controlled via a mechanical iris, are exposed to photoassociation light. The results from the asymmetric trap are compared to the photoassociation dynamics of atoms in a symmetric trap. A paired sample t-test determines a statistically significant difference in the two measurements. This t-test yields a p-value no higher than p = 7 × 10−3 , thus it is likely that the two measurements do not come from the same distribution. This aligns with our hypothesis, and is a new, enlightening piece of research done in the field of few-atom physics.
This dissertation presents the findings of two experimental investigations in ultracold atomic and molecular physics: The study of the dual species trap loss in a rubidium - metastable argon magneto-optical trap and the photoassociative spectroscopy of ultracold metastable argon. The interspecies trap loss rate coefficients have been measured for ultracold collisions between 85Rb and 40Ar* in a dual-species magneto-optical trap (MOT) and the two rates have been found to be approximately equal over the range of intensities studied with values of β'Rb–Ar* = 3.0 ± 1.3 × 10-11 cm3/s and β'Ar*–Rb = 1.9 ± 0.9 × 10-11 cm3/s where β' Rb–Ar* is the trap loss coefficient for Rb in the presence of Ar* and β'Ar*–Rb is the reciprocal term. In addition, the trap loss rate coefficient for cold collisions in a metastable argon MOT alone have been measured with an average value of β Ar* = 5.2 ± 1.6 × 10-10 cm3/s. Using a quadrupole mass spectrometer, the production of Ar +, Ar+2, Rb+, and RbAr+ ions in the dual MOT have been observed, clearly identifying heteronuclear Penning and associative ionization as trap loss mechanisms. In the second experiment, the first ever investigation of the photoassociative (PA) spectroscopy of Ar* has been made. The exploratory study focuses on PA spectroscopy near the 4s[3/2]2 + 4p[5/2]3 asymptote of the Ar2* diatomic molecule over a 10 GHz range red detuned of the atomic resonance. With a range of probe laser intensities from ∼ 102–105ISat, 12 resonances have been observed. The spectra have been analyzed using the near-dissociation LeRoy-Bernstein method. Through this analysis, the spectra seem to best correlate with excitations to the 5g state.
Chemical reactions typically proceed via stochastic encounters between reactants. Going beyond this paradigm, we combined exactly two atoms in a single, controlled reaction. The experimental apparatus traps two individual laser-cooled atoms [one sodium (Na) and one cesium (Cs)] in separate optical tweezers and then merges them into one optical dipole trap. Subsequently, photoassociation forms an excited-state NaCs molecule. The discovery of previously unseen resonances near the molecular dissociation threshold and measurement of collision rates are enabled by the tightly trapped ultracold sample of atoms. As laser-cooling and trapping capabilities are extended to more elements, the technique will enable the study of more diverse, and eventually more complex, molecules in an isolated environment, as well as synthesis of designer molecules for qubits.
In this thesis we study: the dynamics leading to a near-deterministic preparation of single atoms in a microscopic optical dipole trap; the non destructive imaging and counting of trapped atoms; and a system for sorting single atoms between optical dipole traps using a high numerical aperture lens and a spatial light modulator. \n \nWe near-deterministically prepare trapped single Rubidium atoms by exposing them to a tailored light field which induces light assisted collisions. By preparing pairs of Rubidium atoms in an optical micro-trap we can study the outcome of light assisted collisions at the single event level. Using this knowledge we tailor the light such that each collision releases only enough energy for one atom of a colliding atom-pair to escape the trap. This thereby yields an 83% single atom loading efficiency. \n \n \nWe demonstrate a method to count small numbers of atoms held in a deep, microscopic optical dipole trap by collecting fluorescence from atoms exposed to a standing wave of light that is blue-detuned from resonance. While scattering photons, the atoms are cooled by a Sisyphus mechanism that results from the spatial variation in light intensity. The use of a small blue detuning limits the losses due to light assisted collisions, thereby making the method suitable for counting several atoms in a microscopic volume. \n \nWe create two overlapping one-dimensional optical lattices using a single laser beam, a spatial light modulator and a high numerical aperture lens. These lattices have the potential to trap single atoms, and using the dynamic capabilities of the spatial light modulator may shift and sort atoms to a minimum atom-atom separation of 1.52 µm. We show how a simple feedback circuit can compensate for the spatial light modulator's intensity modulation.
We investigate the photoassociation dynamics of exactly two laser-cooled ^{85}Rb atoms in an optical tweezer and reveal fundamentally different behavior to photoassociation in many-atom ensembles. We observe nonexponential decay in our two-atom experiment that cannot be described by a single rate coefficient and find its origin in our system's pair correlation. This is in stark contrast to many-atom photoassociation dynamics, which are governed by decay with a single rate coefficient. We also investigate photoassociation in a three-atom system, thereby probing the transition from two-atom dynamics to many-atom dynamics. Our experiments reveal additional reaction dynamics that are only accessible through the control of single atoms and suggest photoassociation could measure pair correlations in few-atom systems. It further showcases our complete control over the quantum state of individual atoms and molecules, which provides information unobtainable from many-atom experiments.
Quantum simulation offers the possibility to study quantum mechanical problems which are untraceable on classical computers. This thesis introduces a novel platform for quantum simulation and presents the first experimental realisation of single potassium atoms trapped in optical tweezers. Interactions between individual atoms are induced by strong energy shifts of atoms excited to states with large principal quantum number, so-called Rydberg states. Either direct excitation to Rydberg states or off-resonant dressing can be used to induce these interactions. We argue that potassium is well-suited for the implementation of Rydberg dressing, enabling simultaneous dressing of both ground states to engineer complex interactions. Using techniques to cool and trap cold atoms, single potassium atoms are prepared in arrays of optical tweezers. Raman sideband cooling reduces vibrational excitations and prepares the atoms close to the motional ground state. This cooling technique mitigates severe limitations for Rydberg dressing, arising from thermal broadening and inhomogeneous light shifts in the array of atoms. To directly excite atoms to Rydberg states, a high power laser setup with two cavity-enhanced frequency doubling stages is constructed, generating up to one Watt of ulta-violet light at 286 nm. By exciting atoms to Rydberg states we observe Rabi oscillations with Rabi frequencies of up to 1 MHz, demonstrating coherent control of Rydberg atoms. Finally, we combine these techniques to observe interactions in two ways: First, we create a so-called superatom of up to four individual atoms using direct excitation and Rydberg-blockade and observe coherent oscillations to this collective state. We measure the expected square root scaling of the effective Rabi frequency with the number of individual atoms, confirming the creation of a many-body entangled state. Secondly, we off-resonantly dress the atoms prepared in a one-dimensional chain and measure correlated interaction shifts over multiple sites. In summary, we have developed a platform for quantum simulation with single atoms in optical tweezers. The presented results show coherent control of single atoms and interactions induced by Rydberg states. We have thus demonstrated that the system is well-suited for quantum simulation of many-body systems.