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Stach E. J. Kuijpers

Publications and source records attributed to Stach E. J. Kuijpers.

4 recordsLinked to original sources

Evolution of dipole-dipole dynamics in cold ammonia collisions

Cold polar molecules offer fascinating prospects for ultracold chemistry and quantum physics, including new platforms for quantum simulation or computation. However, their inherent collision properties remain largely unknown. It has proven extremely hard to experimentally probe collisions between two dipolar molecules at sufficiently low energies and high precision, as it appears fundamentally impossible to merge two beams of molecules with significant dipole moments. Here we report measurements of state-to-state cross sections for collisions between ammonia isotopologues at energies between 0.3 and 100 cm$^{-1}$ using a novel beam merger. We experimentally observed a local maximum in the cross sections that indicates the effective dipole moments can switch off at low collision energies. Scattering calculations reproduced this maximum in good agreement and explained the observed scaling with the parity splitting energies in the molecular energy level structures. Measurements of the correlated energy transfer in both collision partners yielded direct evidence of the suppression of the dipole-dipole interaction at low energies. Our results demonstrate how collisions between an important class of polar molecules evolve from the high temperature limit towards the ultracold regime in a counterintuitive way, have major consequences for the feasibility of future experiments and the interpretation of previous work, and offer distinctive opportunities to control cold molecular collisions with external fields.

physics.atom-ph↗

Imaging scattering resonances in low-energy inelastic ND$_3$-H$_2$ collisions

A scattering resonance is one of the most striking quantum effects in low-temperature molecular collisions. Predicted decades ago theoretically, they have only been resolved experimentally for systems involving at most four atoms. Extension to more complex systems is essential to probe the true quantum nature of chemically more relevant processes, but is thus far hampered by major obstacles. Here, we present a joint experimental and theoretical study of scattering resonances in state-to-state inelastic collisions for the six-atom ND$_3$-H$_2$/HD systems across the collision energy range 0.5-25 cm$^{-1}$, bringing this type of experiment into the realm of polyatomic symmetric top molecules. Strong resonances are resolved in the integral cross sections, whereas differential cross sections are measured with high resolution using a laser ionization scheme involving VUV light. The experimental data could only be reproduced using theoretical predictions based on a potential energy surface at the CCSD(T) level of theory with corrections at the CCSDT(Q) level.

physics.atom-ph↗

Sensitive Low-Recoil VUV 1+1$'$ REMPI Detection of ND$_3$

In molecular beam scattering experiments, an important technique for measuring product energy and angular distributions is velocity map imaging following photoionization. For studies with cold molecular beams, the resolution is often limited by the product detection process. When state-selective ionization detection is used, excess photon energy can transfer to kinetic energy in the molecular ion-electron pair, resulting in measurable cation recoil. With advanced molecular beam technology, velocity spreads as small as a few m/s are possible. Thus, a suitable product detection scheme must be not only sensitive, state-selective, and background-free, it must also produce less cation recoil than the velocity spread of the molecular beams. To date this has only been possible with the NO molecule. Our goal here is to extend this low-recoil capability to fully deuterated ammonia, ND$_3$. We present a resonance-enhanced multi-photon ionization (REMPI) detection scheme for ND$_3$, that imparts sufficiently low ion recoil, allowing, for the first time, high-resolution imaging of ND$_3$ products in a cold ND$_3$-HD scattering experiment. The first step of the 1+1$'$ REMPI scheme requires vacuum ultra-violet (VUV) photons of ~160 nm, which are generated through four-wave-mixing in Xe. We varied the wavelength of the second, ionization step between 434 and 458 nm, exciting ND$_3$ to a wide range of autoionizing neutral states. By velocity mapping the resulting photoelectrons, it was possible to fully chart the ion recoil across this range with vibrational resolution for the final ionic states. Additionally, rotational resolution in the photoionization dynamics was achieved for selected excitation energies near one of the vibrational thresholds. Many of the peaks in the spectrum of autoionizing Rydberg states are assigned to specific Rydberg series using a simple Rydberg formula model.

physics.atom-ph↗

Merging Two Molecular Beams of ND$_3$ up to the Liouville Limit

In low-energy collisions between two dipolar molecules, the long-range dipole-dipole interaction plays an important role in the scattering dynamics. Merged beam configurations offer the lowest collision energies achievable, but they generally can not be applied to most dipole-dipole systems as the electrodes used to merge one beam would deflect the other. This paper covers the design and implementation of a merged electrostatic guide whose geometry was numerically optimized for ND$_3$-ND$_3$ and ND$_3$-NH$_3$ collisions. This device guides both beams simultaneously and makes them converge up to an effective collision angle of 2$\mathrm{^\circ}$, yielding the optimal compromise between spatial overlap and the lowest possible collision energy. We present preliminary data for inelastic ND$_3$-ND$_3$ collisions.

physics.atom-ph↗