arXiv subjects

Etienne F. Walraven

Publications and source records attributed to Etienne F. Walraven.

6 recordsLinked to original sources

arXiv2026

Deterministic loading of molecular arrays by microwave-assisted collisions

Molecular tweezer arrays offer great prospects for quantum simulation, sensing, and computing, and would benefit from methods that enhance loading efficiency. Whereas light-assisted collisions underpin enhanced loading methods for atomic tweezer arrays, this approach cannot be directly extended to molecular arrays due to collisional loss. We show how this collisional loss can be suppressed by shelving molecules in rotationally or vibrationally excited states, so that a shelved molecule interacts with a newly loaded molecule through a repulsive van der Waals interaction. By introducing microwave assisted collisions, we show how to control the final states and the energy released in a collision between a pair of molecules. Following this controlled collision, one of the two molecules can be ejected, and we explore several strategies for ensuring deterministic ejection. Our schemes rely on currently available techniques for laser-coolable molecules, and we predict achievable filling fractions up to 96%, paving the way for scalable molecular arrays.

physics.atom-ph↗

arXiv2026

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↗

arXiv2025

Hyperfine van der Waals repulsion between open-shell polar molecules

We describe a novel type of interaction between open-shell polar molecules at sub-millikelvin temperatures. This hyperfine van der Waals interaction occurs between two molecules in two rotational states that differ by one quantum. Normally, this induces resonant dipolar interactions that lead to rapid collisional loss. For specific hyperfine states, however, selection rules prevent this. One can effectively turn off the dipolar interaction by merely flipping a nuclear spin. The resulting van der Waals interaction can be repulsive and can suppress collisional loss. We focus on laser-coolable CaF, but show this effect occurs universally for open-shell molecules, including MgF, SrF, BaF and YO. We propose that this effect could be measured by merging molecules in optical tweezers, where flipping a spin in one of the tweezers enables tuning of collision rates by five orders of magnitude.

physics.atom-ph↗

arXiv2024

Rotational-state dependence of interactions between polar molecules

The long-range electrostatic interactions between molecules depend strongly on their relative orientation, which manifests as a rotational state dependence. Interactions between molecules in the same rotational quantum state are well-known attractive rotational van der Waals interactions. Interactions in rotational states that differ by one quantum show resonant dipole-dipole interactions. We show that where molecules are in rotational states that differ by more than one quantum, they exhibit repulsive van der Waals interactions. At temperatures below a millikelvin, this effect can reduce collisional loss by multiple orders of magnitude. These repulsive interactions lead to applications in quantum simulation and impurity physics with ultracold polar molecules.

physics.atom-ph↗

arXiv2024

Scheme for Deterministic Loading of Laser-Cooled Molecules into Optical Tweezers

We propose to repeatedly load laser-cooled molecules into optical tweezers, and transfer them to storage states that are rotationally excited by two additional quanta. Collisional loss of molecules in these storage states is suppressed, and a dipolar blockade prevents the accumulation of more than one molecule. Applying three cycles loads tweezers with single molecules at an 80% success rate, limited by residual collisional loss. This improved loading efficiency reduces the time needed for rearrangement of tweezer arrays, which would otherwise limit the scalability of neutral molecule quantum computers.

physics.atom-ph↗

arXiv2021

Quantifying the interplay between fine structure and geometry of an individual molecule on a surface

The pathway toward the tailored synthesis of materials starts with precise characterization of the conformational properties and dynamics of individual molecules. Electron spin resonance based scanning tunneling microscopy can potentially address molecular structure with unprecedented resolution. Here, we determine the fine structure and geometry of an individual TiH molecule, utilizing a combination of a newly developed mK ESR-STM in a vector magnetic field and ab initio approaches. We demonstrate a strikingly large anisotropy of the g-tensor unusual for a spin doublet ground state, resulting from a non-trivial orbital angular momentum stemming from the molecular ground state. We quantify the relationship between the resultant fine structure, hindered rotational modes, and orbital excitations. Our model system provides new avenues to determine the structure and dynamics of individual molecules.

cond-mat.mes-hall↗