No Arabic abstract
Supersonic beams are a prevalent source of cold molecules utilized in the study of chemical reactions, atom interferometry, gas-surface interactions, precision spectroscopy, molecular cooling and more. The triumph of this method emanates from the high densities produced in relation to other methods, however beam density remains fundamentally limited by interference with shock waves reflected from collimating surfaces. Here we show experimentally that this shock interaction can be reduced or even eliminated by cryo-cooling the interacting surface. An increase in beam density of nearly an order of magnitude was measured at the lowest surface temperature, with no further fundamental limitation reached. Visualization of the shock waves by plasma discharge and reproduction with direct simulation Monte Carlo calculations both indicate that the suppression of the shock structure is partially caused by lowering the momentum flux of reflected particles, and significantly enhanced by the adsorption of particles to the surface. We observe that the scaling of beam density with source pressure is recovered, paving the way to order of magnitude brighter cold molecular beams.
The interaction of strong laser fields with matter intrinsically provides powerful tools to image transient dynamics with an extremely high spatiotemporal resolution. Here, we study strong-field ionisation of laser-aligned molecules and show a full real-time picture of the photoelectron dynamics in the combined action of the laser field and the molecular interaction. We demonstrate that the molecule has a dramatic impact on the overall strong-field dynamics: it sets the clock for the emission of electrons with a given rescattering kinetic energy. This result represents a benchmark for the seminal statements of molecular-frame strong-field physics and has strong impact on the interpretation of self-diffraction experiments. Furthermore, the resulting encoding of the time-energy relation in molecular-frame photoelectron momentum distributions shows the way of probing the molecular potential in real-time and accessing a deeper understanding of electron transport during strong-field interactions.
We study the dynamics of a supersonic molecular beam in a low-finesse optical cavity and demonstrate that most molecules in the beam can be decelerated to zero central velocity by the intracavity optical field in a process analogous to electrostatic Stark deceleration. We show that the rapid switching of the optical field for slowing the molecules is automatically generated by the cavity-induced dynamics. We further show that $sim1%$ of the molecules can be optically trapped at a few millikelvin in the same cavity.
We investigate the photo-doubleionization of $H_2$ molecules with 400 eV photons. We find that the emitted electrons do not show any sign of two-center interference fringes in their angular emission distributions if considered separately. In contrast, the quasi-particle consisting of both electrons (i.e. the dielectron) does. The work highlights the fact that non-local effects are embedded everywhere in nature where many-particle processes are involved.
We report on the focusing and guiding of the van der Waals complex formed between benzonitrile molecules (C$_6$H$_5$CN) and argon atoms in a cold molecular beam using an ac electric quadrupole guide. The distribution of quantum states in the guided beam is non-thermal, because the transmission efficiency depends on the state-dependent effective dipole moment in the applied electric fields. At a specific ac frequency, however, the excitation spectrum can be described by a thermal distribution at a rotational temperature of 0.8 K. From the observed transmission characteristics and a combination of trajectory and Stark-energy calculations we conclude that the permanent electric dipole moment of benzonitrile remains unchanged upon the attachment of the argon atom to within pm5%. By exploiting the different dipole-moment-to-mass (mu/m) ratios of the complex and the benzonitrile monomer, transmission can be selectively suppressed for or, in the limit of 0 K rotational temperature, restricted to the complex.
A method to calculate the bound states of three-atoms without resorting to an explicit partial wave decomposition is presented. The differential form of the Faddeev equations in the total angular momentum representation is used for this purpose. The method utilizes Cartesian coordinates combined with the tensor-trick preconditioning for large linear systems and Arnoldis algorithm for eigenanalysis. As an example, we consider the He$_3$ system in which the interatomic force has a very strong repulsive core that makes the three-body calculations with standard methods tedious and cumbersome requiring the inclusion of a large number of partial waves. The results obtained compare favorably with other results in the field.