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Register a new userZeeman-tuned rotational level-crossing spectroscopy in a diatomic free radical
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Rotational levels of molecular free radicals can be tuned to degeneracy using laboratory-scale magnetic fields. Because of their intrinsically narrow width, these level crossings of opposite-parity states have been proposed for use in the study of parity-violating interactions and other applications. We experimentally study a typical manifestation of this system using $^{138}$BaF. Using a Stark-mixing method for detection, we demonstrate level-crossing signals with spectral width as small as 6 kHz. We use our data to verify the predicted lineshapes, transition dipole moments, and Stark shifts, and to precisely determine molecular magnetic g-factors. Our results constitute an initial proof-of-concept for use of this system to study nuclear spin-dependent parity violating effects.
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We present a novel slowing scheme for beams of laser-coolable diatomic molecules reminiscent of Zeeman slowing of atomic beams. The scheme results in efficient compression of the 1-dimensional velocity distribution to velocities trappable by magnetic or magneto-optical traps. 3D Monte Carlo simulations for the prototype molecule $^{88}mathrm{Sr}^{19}mathrm{F}$ and experiments in an atomic testbed demonstrate a performance comparable to traditional atomic Zeeman slowing and an enhancement of flux below v=35 m/s by a factor of $approx 20$ compared to white-light slowing. This is the first experimentally shown continuous and dissipative slowing technique in molecule-like level structures, promising to provide the missing link for the preparation of large ultracold molecular ensembles.
We demonstrate the mixing of rotational states in the ground electronic state using microwave radiation to enhance optical cycling in the molecule yttrium (II) monoxide (YO). This mixing technique is used in conjunction with a frequency modulated and chirped continuous wave laser to slow longitudinally a cryogenic buffer gas beam of YO. We generate a measurable flux of YO below 10~m/s, directly loadable into a three-dimensional magneto-optical trap. This technique opens the door for laser cooling of molecules with more complex structure.
We present models for a heteronuclear diatomic molecular ion in a linear Paul trap in a rigid-rotor approximation, one purely classical, the other where the center-of-mass motion is treated classically while rotational motion is quantized. We study the rotational dynamics and their influence on the motion of the center-of-mass, in the presence of the coupling between the permanent dipole moment of the ion and the trapping electric field. We show that the presence of the permanent dipole moment affects the trajectory of the ion, and that it departs from the Mathieu equation solution found for atomic ions. For the case of quantum rotations, we also evidence the effect of the above-mentioned coupling on the rotational states of the ion.
The rich information content of measurements in the molecular frame rather than the laboratory frame has motivated the development of several methods for aligning gas phase molecules in space. Even so, for asymmetric tops the problem of making molecular frame measurements remains challenging due to its inherently multi-dimensional nature. In this Letter we present a method, based on the analysis of observables measured from rotational wavepackets, that does not require either 3D alignment or coincident momentum measurements to access the molecular frame. As an application we describe the first fully-orientation-resolved measurements of strong-field ionization and dissociation of an asymmetric top (ethylene).
Accurate and comprehensive diatomic molecular spectroscopic data have long been vital in a wide variety of applications for measuring and monitoring astrophysical, industrial and other gaseous environments. These data are also used extensively for benchmarking quantum chemistry and applications from quantum computers, ultracold chemistry and the search for physics beyond the standard model. Useful data can be highly detailed like line lists or summative like molecular constants, and obtained from theory, experiment or a combination. There are plentiful (though not yet sufficient) data available, but these data are often scattered. For example, molecular constants have not been compiled since 1979 despite the existing compilation still being cited more than 200 times annually. Further, the data are interconnected but updates in one type of data are not yet routinely applied to update interconnected data: in particular, new experimental and ab-initio data are not routinely unified with other data on the molecule. This paper provide information and strategies to strengthen the connection between data producers (e.g. ab-initio electronic structure theorists and experimental spectroscopists), data modellers (e.g. line list creators and others who connect data on one aspect of the molecule to the full energetic and spectroscopic description) and data users (astronomers, chemical physicists etc). All major data types are described including their source, use, compilation and interconnectivity. Explicit advice is provided for theoretical and experimental data producers, data modellers and data users to facilitate optimal use of new data with appropriate attribution.
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