arXiv subjects

W. C. Stwalley

Publications and source records attributed to W. C. Stwalley.

11 recordsLinked to original sources

arXiv2017

High-Resolution Spectroscopy of {R}ydberg Molecular States of $^{85}${R}b$_2$ Near the $5s+7p$ Asymptote

Rydberg molecules, often exemplified by long-range "trilobite" molecules, are a subject of much recent interest at high principal quantum number $n$. States that use the same bonding mechanism can exist at much lower $n$ and less-extreme internuclear separations that are still quite long range. We use a high-resolution pulsed amplifier to study previously-detected transitions to a low-$n$ Rydberg molecular state near the $5s+7p$ asymptote in $^{85}$Rb$_2$. The observed line structure is modeled using precise ground-state positions and a lower bound of $τ> 1.1 \times 10^{-9}$ s is set on the excited-state autoionization lifetime.

physics.atom-ph↗

arXiv2016

Short-range photoassociation from the inner wall of the lowest triplet potential of $^{85}$Rb$_2$

Ultracold photoassociation is typically performed at large internuclear separations, where the scattering wavefunction amplitude is large and Franck-Condon overlap is maximized. Recently, work by this group and others on alkali-metal diatomics has shown that photoassociation can efficiently form molecules at short internuclear distance in both homonuclear and heteronuclear dimers. We propose that this short-range photoassociation is due to excitation near the wavefunction amplitude maximum at the inner wall of the lowest triplet potential. We show that Franck-Condon factors from the highest-energy bound state can almost precisely reproduce Franck-Condon factors from a low-energy scattering state, and that both calculations match experimental data from the near-zero positive-energy scattering state with reasonable accuracy. We also show that the corresponding photoassociation from the inner wall of the ground-state singlet potential at much shorter internuclear distance is weaker and undetectable under our current experimental conditions. We predict from Franck-Condon factors that the strongest of these weaker short-range photoassociation transitions are one order of magnitude below our current sensitivity.

physics.atom-ph↗

arXiv2013

Excitation of weakly-bound molecules to trilobite-like Rydberg states

We observe "trilobite-like" states of ultracold 85Rb2 molecules, in which a ground-state atom is bound by the electronic wavefunction of its Rydberg-atom partner. We populate these states through the ultraviolet excitation of weakly-bound molecules, and access a regime of trilobite-like states at low principal quantum numbers and with vibrational turning points around 35 Bohr radii. This demonstrates that, unlike previous studies that used free-to-bound transitions, trilobite-like states can also be excited through bound-to-bound transitions. This approach provides high excitation probabilities without requiring high-density samples, and affords the ability to control the excitation radius by selection of the initial-state vibrational level.

physics.atom-ph↗

arXiv2013

Observation and Analysis of Resonant Coupling Between Near-Degenerate Levels of the 2 1Σg+ and 1 1 Πg States of Ultracold 85Rb2

We report on the anomalously high line strength of a single rotational level in the ultracold photoassociation of two 85Rb atoms to form 85Rb2. The v' = 111, J' = 5 level belongs to the Hund's case (c) 2 (0g+) state, which correlates to the Hund's case (a) 2 1 Σg+ state. Its strength is caused by coupling with a very near-resonant long-range state. The long-range component is the energetically degenerate v' = 155, J' = 5 level of the case (c) 2 (1g)$ state, correlating to the case (a) 1 1 Πg state. The line strength is enhanced by an order of magnitude through this coupling, relative to nearby vibrational levels and even to nearby rotational levels of the same vibrational level. This enhancement is in addition to the enhancement seen in all J' = 3 and 5 levels of the 2 (0g+) state due to an l = 4 shape resonance in the a 3 Σu+ state continuum, which alters the distribution of levels formed by photoassociation.

physics.atom-ph↗

arXiv2012

Upper Bound to the Ionization Energy of 85Rb2

We report an upper bound to the ionization energy of 85Rb2 of 31348.0(6) cm-1, which also provides a lower bound to the dissociation energy D0 of 85Rb2+ of 6307.5(6) cm-1. These bounds were measured by the onset of autoionization of excited states of 85Rb2 below the 5s+7p atomic limit. We form 85Rb2 molecules via photoassociation of ultracold 85Rb atoms, and subsequently excite the molecules by single-photon ultraviolet transitions to states above the ionization threshold.

physics.atom-ph↗

arXiv2012

Photoassociation to the 2(1)Sigma(g)(+) state in ultracold 85Rb2 in the presence of a shape resonance

We report the first observation of photoassociation to the 2(1)Sigma(g)(+) state of 85Rb2 . We have observed two vibrational levels (v'=98, 99) below the 5s1/2+5p1/2 atomic limit and eleven vibrational levels (v'=102-112) above it. The photoassociation---and subsequent spontaneous emission---occur predominantly between 15 and 20 Bohr in a region of internuclear distance best described as a transition between Hund's case (a) and Hund's case (c) coupling. The presence of a g-wave shape resonance in the collision of two ground-state atoms affects the photoassociation rate and lineshape of the J'= 3 and 5 rotational levels.

physics.atom-ph↗

arXiv2011

Formation of ultracold metastable Rb2 molecules in their v"=0 level by blue-detuned photoassociation

We report on the observation of blue-detuned photoassociation in Rb2, in which vibrational levels are energetically above the corresponding excited atomic asymptote. 85Rb atoms in a MOT were photoassociated at short internuclear distances to levels of the (1)3Pi g state at a rate of approximately 5x10^4 molecules/s. We have observed most of the predicted vibrational levels for all four spin-orbit components 0g+, 0g-, 1g, and 2g, including levels of the 0g+ outer well. These molecules decay to the metastable a3Sigma u+ state, some preferentially to the v"=0 level, as we have observed for photoassociation to the v'=8 level of the 1g component.

physics.atom-ph↗

arXiv2009

Resonant Coupling in the Heteronuclear Alkali Dimers for Direct Photoassociative Formation of X(0,0) Ultracold Molecules

Promising pathways for photoassociative formation of ultracold heteronuclear alkali metal dimers in their lowest rovibronic levels (denoted X(0,0)) are examined using high quality ab initio calculations of potential energy curves currently available. A promising pathway for KRb, involving the resonant coupling of the $2 ^1Π$ and $1 ^1Π$ states just below the lowest excited asymptote (K($4s$)+Rb($5p_{1/2}$)), is found to occur also for RbCs and less promisingly for KCs as well. The resonant coupling of the $3 ^1 Σ^+ $ and $1 ^1Π$ states, also just below the lowest excited asymptote, is found to be promising for LiNa, LiK, LiRb, and less promising for LiCs and KCs. Direct photoassociation to the $1 ^1Π$ state near dissociation appears promising in the final dimers, NaK, NaRb, and NaCs, although detuning more than 100 cm$^{-1}$ below the lowest excited asymptote may be required.

physics.atom-ph↗

arXiv2007

Enhancement of the formation of ultracold $^{85}$Rb$_2$ molecules due to resonant coupling

We have studied the effect of resonant electronic state coupling on the formation of ultracold ground-state $^{85}$Rb$_2$. Ultracold Rb$_2$ molecules are formed by photoassociation (PA) to a coupled pair of $0_u^+$ states, $0_u^+(P_{1/2})$ and $0_u^+(P_{3/2})$, in the region below the $5S+5P_{1/2}$ limit. Subsequent radiative decay produces high vibrational levels of the ground state, $X ^1Σ_g^+$. The population distribution of these $X$ state vibrational levels is monitored by resonance-enhanced two-photon ionization through the $2 ^1Σ_u^+$ state. We find that the populations of vibrational levels $v''$=112$-$116 are far larger than can be accounted for by the Franck-Condon factors for $0_u^+(P_{1/2}) \to X ^1Σ_g^+$ transitions with the $0_u^+(P_{1/2})$ state treated as a single channel. Further, the ground-state molecule population exhibits oscillatory behavior as the PA laser is tuned through a succession of $0_u^+$ state vibrational levels. Both of these effects are explained by a new calculation of transition amplitudes that includes the resonant character of the spin-orbit coupling of the two $0_u^+$ states. The resulting enhancement of more deeply bound ground-state molecule formation will be useful for future experiments on ultracold molecules.

physics.atom-ph↗

arXiv2005

State-Selective Detection of Near-Dissociation Ultracold KRb $X^1Σ^+$ and $a^3Σ^+$ Molecules

We report on the state-selective detection of near-dissociation ultracold KRb molecules in the ground $X^1Σ^+$ state and the metastable $a^3Σ^+$ state. The molecules are produced by photoassociation of ultracold atoms followed by radiative decay into high vibrational levels of the $X$ and $a$ states. Detection utilizes resonance-enhanced one-color two-photon ionization, followed by time-of-flight mass spectroscopy. Scanning the detection laser frequency over the range 582-625 nm, we observe transitions from the $v''$=86-92 levels of the $X$ state, which are bound by up to 30 cm$^{-1}$, and the $v''$=17-23 levels of the $a$ state, which are also bound by up to 30 cm$^{-1}$. The measured vibrational spacings are in excellent agreement with those previously measured and those calculated from the relevant potential curves. Relative vibrational populations are also consistent with Franck-Condon factors for decay from the photoassociated levels.

physics.atom-ph↗

arXiv2004

Photoassociative Production and Trapping of Ultracold KRb Molecules

We have produced ultracold heteronuclear KRb molecules by the process of photoassociation in a two-species magneto-optical trap. Following decay of the photoassociated KRb*, the molecules are detected using two-photon ionization and time-of-flight mass spectroscopy of KRb$^+$. A portion of the metastable triplet molecules thus formed are magnetically trapped. Photoassociative spectra down to 91 cm$^{-1}$ below the K(4$s$) + Rb (5$p_{1/2}$) asymptote have been obtained. We have made assignments to all eight of the attractive Hund's case (c) KRb* potential curves in this spectral region.

physics.atom-ph↗