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Register a new userInternal-state thermometry by depletion spectroscopy in a cold guided beam of formaldehyde
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We present measurements of the internal state distribution of electrostatically guided formaldehyde. Upon excitation with continuous tunable ultraviolet laser light the molecules dissociate, leading to a decrease in the molecular flux. The population of individual guided states is measured by addressing transitions originating from them. The measured populations of selected states show good agreement with theoretical calculations for different temperatures of the molecule source. The purity of the guided beam as deduced from the entropy of the guided sample using a source temperature of 150K corresponds to that of a thermal ensemble with a temperature of about 30 K.
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We present a comprehensive characterization of cold molecular beams from a cryogenic buffer-gas cell, providing an insight into the physics of buffer-gas cooling. Cold molecular beams are extracted from a cryogenic cell by electrostatic guiding, which is also used to measure their velocity distribution. Molecules rotational-state distribution is probed via radio-frequency resonant depletion spectroscopy. With the help of complete trajectory simulations, yielding the guiding efficiency for all of the thermally populated states, we are able to determine both the rotational and the translational temperature of the molecules at the output of the buffer-gas cell. This thermometry method is demonstrated for various regimes of buffer-gas cooling and beam formation as well as for molecular species of different sizes, $rm{CH_3F}$ and $rm{CF_3CCH}$. Comparison between the rotational and translational temperatures provides evidence of faster rotational thermalization for the $rm{CH_3F-He}$ system in the limit of low He density. In addition, the relaxation rates for different rotational states appear to be different.
Electrostatic velocity filtering and guiding is an established technique to produce high fluxes of cold polar molecules. In this paper we clarify different aspects of this technique by comparing experiments to detailed calculations. In the experiment, we produce cold guided beams of the three water isotopologs H2O, D2O and HDO. Their different rotational constants and orientations of electric dipole moments lead to remarkably different Stark shift properties, despite the molecules being very similar in a chemical sense. Therefore, the signals of the guided water isotopologs differ on an absolute scale and also exhibit characteristic electrode voltage dependencies. We find excellent agreement between the relative guided fractions and voltage dependencies of the investigated isotopologs and predictions made by our theoretical model of electrostatic velocity filtering.
Motivated by the observation of non-exponential run-time distributions of bacterial swimmers, we propose a minimal phenomenological model for taxis of active particles whose motion is controlled by an internal clock. The ticking of the clock depends on an external concentration field, e.g. a chemical substance. We demonstrate that these particles can detect concentration gradients and respond to them by moving up- or down-gradient depending on the clock design, albeit measurements of these fields are purely local in space and instantaneous in time. Altogether, our results open a new route in the study of directional navigation, by showing that the use of a clock to control motility actions represents a generic and versatile toolbox to engineer behavioral responses to external cues, such as light, chemical, or temperature gradients.
We make use of an inhomogeneous electrostatic dipole field to impart a quantum-state-dependent deflection to a pulsed beam of OCS molecules, and show that those molecules residing in the absolute ground state, $X ^1Sigma^+$, $ket{00^00}$, J=0, can be separated out by selecting the most deflected part of the molecular beam. Past the deflector, we irradiate the molecular beam by a linearly polarized pulsed nonresonant laser beam that impulsively aligns the OCS molecules. Their alignment, monitored via velocity-map imaging, is measured as a function of time, and the time dependence of the alignment is used to determine the quantum state composition of the beam. We find significant enhancements of the alignment (costhetasqtd $= 0.84$) and of state purity ($> 92$%) for a state-selected, deflected beam compared with an undeflected beam.
Chirped-Pulse millimetre-Wave (CPmmW) rotational spectroscopy provides a new class of information about photolysis transition state(s). Measured intensities in rotational spectra determine species-isomer-vibrational populations, provided that rotational populations can be thermalized. The formation and detection of S0 vinylidene is discussed in the limits of low and high initial rotational excitation. CPmmW spectra of 193 nm photolysis of Vinyl Cyanide (Acrylonitrile) contain J=0-1 transitions in more than 20 vibrational levels of HCN, HNC, but no transitions in vinylidene or highly excited local-bender vibrational levels of acetylene. Reasons for the non-observation of the vinylidene co-product of HCN are discussed.
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