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Register a new userPhotodetachment Spectroscopy of Quasibound States of the Negative Ion of Lanthanum
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The negative ion of lanthanum, La$^-$, has one of the richest bound state spectra observed for an atomic negative ion and has been proposed as a promising candidate for laser-cooling applications. In the present experiments, La$^-$ was investigated using tunable infrared photodetachment spectroscopy. The relative signal for neutral atom production was measured with a crossed ion-beam--laser-beam apparatus over the photon energy range 590 - 920 meV (2100 - 1350 nm) to probe the continuum region above the La neutral atom ground state. Eleven prominent peaks were observed in the La$^-$ photodetachment cross section due to resonant excitation of quasibound transient negative ion states in the continuum which subsequently autodetach. In addition, thresholds were observed for photodetachment from several bound states of La$^-$ to both ground and excited states of La. The present results provide information on the excited state structure and dynamics of La$^-$ that depend crucially on multielectron correlation effects.
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We demonstrated the accurate prediction of a quasibound spectrum of a negative ion using a novel high-precision theoretical approach. We used La$^-$ as a test case due to a recent experiment that measured energies of 11 resonances in its photodetachment spectrum attributed to transitions to quasibound states [C. W. Walter et al., PRA, in press (2020); arXiv:2010.01122]. We identified all of the observed resonances, and predicted one more peak just outside the range of the prior experiment. Following the theoretical prediction, the peak was observed at the predicted wavelength, validating the identification. The same approach is applicable to a wide range of negative ions. Moreover, theory advances reported in this work can be used for massive generation of atomic transition properties for neutrals and positive ions needed for a variety of applications.
The interaction between the field emission resonance states and the photodetached electron in an electric field is studied by semiclassical theory. An analytical expression of the photodetachment cross section is derived in the framework. It is found that the Stark shifted image state modulates the photodetachment cross section by adding irregular staircase or smooth oscillation in the spectrum. When the photodetached electron is trapped in Stark shifted image potential well, the detachment spectrum displays an irregular staircase structure which corresponds to the modified Rydberg series. While the photodetached electron is not bound by the surface potential well, the cross secton contains only a smooth oscillation due to the reflection of electronic wave by the field or the surface.
We propose to use the near-threshold electron scattering data for atoms to guide the reliable experimental determination of their electron affinities (EAs), extracted using the Wigner Threshold Law, from laser photodetachment threshold spectroscopy measurements. Data from the near-threshold electron elastic scattering from W, Te, Rh, Sb and Sn atoms calculated using our complex angular momentum method, wherein is embedded the electron-electron correlations and core polarization interaction, are used as illustrations. We conclude with a remark on the relativistic effects on the EA calculation for the heavy At atom.
Characterizing quasibound states from coupled-channel scattering calculations can be a laborious task, involving extensive manual iteration and fitting. We present an automated procedure, based on the phase shift or S-matrix eigenphase sum, that reliably converges on a quasibound state (or scattering resonance) from some distance away. It may be used for both single-channel and multichannel scattering. It produces the energy and width of the state and the phase shift of the background scattering, and hence the lifetime of the state. It also allows extraction of partial widths for decay to individual open channels. We demonstrate the method on a very narrow state in the Van der Waals complex Ar--H$_2$, which decays only by vibrational predissociation, and on near-threshold states of $^{85}$Rb$_2$, whose lifetime varies over 4 orders of magnitude as a function of magnetic field.
Spectroscopy is a powerful tool for studying molecules and is commonly performed on large thermal molecular ensembles that are perturbed by motional shifts and interactions with the environment and one another, resulting in convoluted spectra and limited resolution. Here, we use generally applicable quantum-logic techniques to prepare a trapped molecular ion in a single quantum state, drive terahertz rotational transitions with an optical frequency comb, and read out the final state non-destructively, leaving the molecule ready for further manipulation. We resolve rotational transitions to 11 significant digits and derive the rotational constant of CaH+ to be B_R = 142501777.9(1.7) kHz. Our approach suits a wide range of molecular ions, including polyatomics and species relevant for tests of fundamental physics, chemistry, and astrophysics.
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