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Photoassociative Spectroscopy of Ultracold Argon and Krypton Confined in a Magneto Optical Trap

Maha Khaled Omar

Published Oct 21, 2019• 0 citations
Publisher

Abstract

Creating ultracold molecules has attracted considerable interest in the last decade. Once created, such molecules can be used for precision spectroscopy or to study chemical reactions at ultracold tem peratures. Several techniques have been developed to produce ultracold molecules; the most common is photoassociation where two ultracold atoms collide in the presence of light that induces a free-bound transition to an excited molecular state. Photoassociation can also be used to perform spectroscopy in order to map out the ro-vibrational levels of a molecular state. In this dissertaiotn, we report on our Photoasociative Spectroscopy (PAS) studies conducted separately in argon and krypton. For each species, we have studied transitions near two different atomic limits ns[3/2]2 —> np[5/2]2 and ns[3/2]2 —» np[5/2]3where n = 4 for argon and n = 5 for krypton. The former atomic transition is called the “quench transition” since it forms a strong coupled channel to the ground state. As a result for this strong coupling the original atomic sample is degraded and quenched. The latter transition is the one used to cool and confine the atoms and is known as the “trapping transition.” Spectroscopy near the trapping transition in argon was studied previously in our group [1] and specific features were observed in the spectrum. At the time, the features were not definitively identified, but more than one explanation was suggested for further testing. One possible explanation was that these features were a result of resonances happening at “doubly-excited” molecular levels. The population of such states could take place as a result of absorbing two photons of the same frequency which causes photoassociation. In this dissertation we report on a series of experiments that were performed to study and conclusively identify the origin of those features. These experiments led to the conclusion that the features in the spectra were an artifact of otherwise undetectable frequency sidebands on our semiconductor diode laser. Once identified as such, a new laser was constructed to repeat the spectroscopy measurements in argon and take new measurements in krypton that would be free from laser artifacts. In those spectra, no specific vibrational features were observed and resolved in either species. Results were consistent with published results obtained by other groups using other noble gases. Finally, we report on our attempts to perform PAS on a quench transition in order to confirm results obtained for krypton by another group [2]. We were not able to observe any photoassociation signal for both argon and krypton on this transition. We were able to observe similar effects to those reported in Ref. [2] but we attribute these to artifacts from an acousto-optic modulator and not as arising from molecular structure.

DOI
10.25777/a743-4154

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Photoassociative spectroscopy of ultracold argon and krypton

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We report photoassociative spectroscopy performed separately on Kr84 and Ar40. The spectra were obtained as a function of laser intensity with the spectroscopy laser tuned around the ns[3/2]2→np[5/2]3 trapping transition, where n=4 for argon and n=5 for krypton. The resulting spectra are the first ever obtained for krypton on this important transition. This transition in argon was previously studied in our group. At that time, discrete features were observed in the spectrum, but their origin was not conclusively identified. We have now identified these features as artifacts from laser sidebands. We discuss the origin of these sidebands, how they imprint their presence on the spectra, and present spectra for argon with the artifacts removed. For both krypton and argon, while we observe photoassociation, we do not observe any resolved vibrational structure. We present a theoretical analysis of the expected vibrational level spacings based on calculated potential curves and show that the absence of resolved structure in the spectra of our experiments (as configured) is not surprising. Finally, we discuss the requirements of future experiments in which resolution of vibrational structure in this system might be obtained.

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Photoassociative spectroscopy of ultracold metastable argon

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We present results of photoassociative spectroscopy performed on ultracold metastable argon atoms in a magneto-optical trap. Ion spectra are obtained with laser detuning up to a few gigahertz below the $4s[3/2]{}_{2}\ensuremath{\rightarrow}4p[5/2]{}_{3}$ trapping transition at 811 nm and with intensities in a range of $~({10}^{2}\ensuremath{-}{10}^{5}){I}_{\mathrm{Sat}}$. We also compute dipole-dipole potentials for both singly and doubly excited diatomic molecules and use a Leroy-Bernstein analysis to determine the approximate vibrational spacings in the ($s+p$) and ($p+p$) manifolds. Based on this theoretical framework, we explain a broad background feature in our data and suggest that double-excitation mechanisms are likely responsible for sharp dips in the ion signal.

Physical Review A•May 24, 2011•7 citations
Creating ultracold molecules has attracted considerable interest in the last decade. Once created, such molecules can be used for precision spectroscopy or to study chemical reactions at ultracold tem peratures. Several techniques have been developed to produce ultracold molecules; the most common is photoassociation where two ultracold atoms collide in the presence of light that induces a free-bound transition to an excited molecular state. Photoassociation can also be used to perform spectroscopy in order to map out the ro-vibrational levels of a molecular state. In this dissertaiotn, we report on our Photoasociative Spectroscopy (PAS) studies conducted separately in argon and krypton. For each species, we have studied transitions near two different atomic limits ns[3/2]2 —> np[5/2]2 and ns[3/2]2 —» np[5/2]3where n = 4 for argon and n = 5 for krypton. The former atomic transition is called the “quench transition” since it forms a strong coupled channel to the ground state. As a result for this strong coupling the original atomic sample is degraded and quenched. The latter transition is the one used to cool and confine the atoms and is known as the “trapping transition.” Spectroscopy near the trapping transition in argon was studied previously in our group [1] and specific features were observed in the spectrum. At the time, the features were not definitively identified, but more than one explanation was suggested for further testing. One possible explanation was that these features were a result of resonances happening at “doubly-excited” molecular levels. The population of such states could take place as a result of absorbing two photons of the same frequency which causes photoassociation. In this dissertation we report on a series of experiments that were performed to study and conclusively identify the origin of those features. These experiments led to the conclusion that the features in the spectra were an artifact of otherwise undetectable frequency sidebands on our semiconductor diode laser. Once identified as such, a new laser was constructed to repeat the spectroscopy measurements in argon and take new measurements in krypton that would be free from laser artifacts. In those spectra, no specific vibrational features were observed and resolved in either species. Results were consistent with published results obtained by other groups using other noble gases. Finally, we report on our attempts to perform PAS on a quench transition in order to confirm results obtained for krypton by another group [2]. We were not able to observe any photoassociation signal for both argon and krypton on this transition. We were able to observe similar effects to those reported in Ref. [2] but we attribute these to artifacts from an acousto-optic modulator and not as arising from molecular structure.
We report photoassociative spectroscopy performed separately on Kr84 and Ar40. The spectra were obtained as a function of laser intensity with the spectroscopy laser tuned around the ns[3/2]2→np[5/2]3 trapping transition, where n=4 for argon and n=5 for krypton. The resulting spectra are the first ever obtained for krypton on this important transition. This transition in argon was previously studied in our group. At that time, discrete features were observed in the spectrum, but their origin was not conclusively identified. We have now identified these features as artifacts from laser sidebands. We discuss the origin of these sidebands, how they imprint their presence on the spectra, and present spectra for argon with the artifacts removed. For both krypton and argon, while we observe photoassociation, we do not observe any resolved vibrational structure. We present a theoretical analysis of the expected vibrational level spacings based on calculated potential curves and show that the absence of resolved structure in the spectra of our experiments (as configured) is not surprising. Finally, we discuss the requirements of future experiments in which resolution of vibrational structure in this system might be obtained.
We report photoassociative spectroscopy performed separately on Kr84 and Ar40. The spectra were obtained as a function of laser intensity with the spectroscopy laser tuned around the ns[3/2]2→np[5/2]3 trapping transition, where n=4 for argon and n=5 for krypton. The resulting spectra are the first ever obtained for krypton on this important transition. This transition in argon was previously studied in our group. At that time, discrete features were observed in the spectrum, but their origin was not conclusively identified. We have now identified these features as artifacts from laser sidebands. We discuss the origin of these sidebands, how they imprint their presence on the spectra, and present spectra for argon with the artifacts removed. For both krypton and argon, while we observe photoassociation, we do not observe any resolved vibrational structure. We present a theoretical analysis of the expected vibrational level spacings based on calculated potential curves and show that the absence of resolved structure in the spectra of our experiments (as configured) is not surprising. Finally, we discuss the requirements of future experiments in which resolution of vibrational structure in this system might be obtained.
n this presentation, we discuss results from two separate bodies of work. In the first, we investigate all-optical excitation methods to produce metastable-state krypton. The high energies required to excite rare gases out of their ground state present a unique challenge in the context of laser experiments. Laser physics work with rare gases often relies on excitation within an RF discharge. All-optical excitation is a promising replacement for RF discharges, avoids problems caused by ion production and may eventually allow for higher efficiencies. We examine three separate methods of all-optical metastable-state production: using an ArF excimer laser, using the third harmonic of the Jefferson Lab free-electron laser (FEL), and using a commercially available UV lamp. In the second body of work, we perform photoassociation spectroscopy in an ultracold, heteronuclear Rb + Ar* system. Photoassociation is a method that may be used to both 1) produce ultracold molecules, and 2) perform high-resolution spectroscopy on excited molecular states. Most work within the field has been performed within all alkali-metal systems. We examine a unique noble gas–alkali system within a dual species magneto-optical trap. We have performed a comprehensive search for evidence of excitation to molecular levels of RbAr. We illuminate atom pairs with a photoassociation laser in a spectral region detuned a few GHz below an atomic asymptote of argon, analogous to previous work in the homo-nuclear argon or krypton systems. We discuss our methodology and findings. We conclude with a discussion of how our results may be applied to future spectroscopic searches
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.
Photoassociation is the process in which two colliding atoms absorb a photon to form an excited molecule. The development of laser-cooling techniques for producing gases at ultracold (<1mK)(<1\phantom{\rule{0.3em}{0ex}}\mathrm{mK})(<1mK) temperatures allows photoassociation spectroscopy to be performed with very high spectral resolution. Of particular interest is the investigation of molecular states whose properties can be related, with high precision, to the properties of their constituent atoms with the ``complications'' of chemical binding accounted for by a few parameters. These include bound long-range or purely long-range vibrational states in which two atoms spend most or all of their time at large internuclear separations. Low-energy atomic scattering states also share this characteristic. Photoassociation techniques have made important contributions to the study of all of these. This review describes what is special about photoassociation spectroscopy at ultracold temperatures, how it is performed, and a sampling of results including the determination of scattering lengths, their control via optical Feshbach resonances, precision determinations of atomic lifetimes from molecular spectra, limits on photoassociation rates in a Bose-Einstein condensate, and briefly, production of cold molecules. Discussions are illustrated with examples on alkali-metal atoms as well as other species. Progress in the field is already past the point where this review can be exhaustive, but an introduction is provided on the capabilities of photoassociation spectroscopy and the techniques presently in use.
We present results of photoassociative spectroscopy performed on ultracold metastable argon atoms in a magneto-optical trap. Ion spectra are obtained with laser detuning up to a few gigahertz below the $4s[3/2]{}_{2}\ensuremath{\rightarrow}4p[5/2]{}_{3}$ trapping transition at 811 nm and with intensities in a range of $~({10}^{2}\ensuremath{-}{10}^{5}){I}_{\mathrm{Sat}}$. We also compute dipole-dipole potentials for both singly and doubly excited diatomic molecules and use a Leroy-Bernstein analysis to determine the approximate vibrational spacings in the (s+ps+ps+p) and (p+pp+pp+p) manifolds. Based on this theoretical framework, we explain a broad background feature in our data and suggest that double-excitation mechanisms are likely responsible for sharp dips in the ion signal.