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Register a new userDirect probe of anisotropy in atom-molecule collisions via quantum scattering resonances
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Anisotropy is a fundamental property of particle interactions. It occupies a central role in cold and ultra-cold molecular processes, where long range forces have been found to significantly depend on orientation in ultra-cold polar molecule collisions. Recent experiments have demonstrated the emergence of quantum phenomena such as scattering resonances in the cold collisions regime due to quantization of the intermolecular degrees of freedom. Although these states have been shown to be sensitive to interaction details, the effect of anisotropy on quantum resonances has eluded experimental observation so far. Here, we directly measure the anisotropy in atom-molecule interactions via quantum resonances by changing the quantum state of the internal molecular rotor. We observe that a quantum scattering resonance at a collision energy of $k_B$ x 270 mK appears in the Penning ionization of molecular hydrogen with metastable helium only if the molecule is rotationally excited. We use state of the art ab initio and multichannel quantum molecular dynamics calculations to show that the anisotropy contributes to the effective interaction only for $H_2$ molecules in the first excited rotational state, whereas rotationally ground state $H_2$ interacts purely isotropically with metastable helium. Control over the quantum state of the internal molecular rotation allows us to switch the anisotropy on or off and thus disentangle the isotropic and anisotropic parts of the interaction. These quantum phenomena provide a challenging benchmark for even the most advanced theoretical descriptions, highlighting the advantage of using cold collisions to advance the microscopic understanding of particle interactions.
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We theoretically study slow collisions of NH$_3$ molecules with He atoms, where we focus in particular on the observation of scattering resonances. We calculate state-to-state integral and differential cross sections for collision energies ranging from 10${}^{-4}$ cm$^{-1}$ to 130 cm$^{-1}$, using fully converged quantum close-coupling calculations. To describe the interaction between the NH${}_3$ molecules and the He atoms, we present a four-dimensional potential energy surface, based on an accurate fit of 4180 {it ab initio} points. Prior to collision, we consider the ammonia molecules to be in their antisymmetric umbrella state with angular momentum $j=1$ and projection $k=1$, which is a suitable state for Stark deceleration. We find pronounced shape and Feshbach resonances, especially for inelastic collisions into the symmetric umbrella state with $j=k=1$. We analyze the observed resonant structures in detail by looking at scattering wavefunctions, phase shifts, and lifetimes. Finally, we discuss the prospects for observing the predicted scattering resonances in future crossed molecular beam experiments with a Stark-decelerated NH$_3$ beam.
Conventional information processors freely convert information between different physical carriers to process, store, or transmit information. It seems plausible that quantum information will also be held by different physical carriers in applications such as tests of fundamental physics, quantum-enhanced sensors, and quantum information processing. Quantum-controlled molecules in particular could transduce quantum information across a wide range of quantum-bit (qubit) frequencies, from a few kHz for transitions within the same rotational manifold, a few GHz for hyperfine transitions, up to a few THz for rotational transitions, to hundreds of THz for fundamental and overtone vibrational and electronic transitions, possibly all within the same molecule. Here, we report the first demonstration of entanglement between states of the rotation of a $rm^{40}CaH^+$ molecular ion and internal states of a $rm^{40}Ca^+$ atomic ion. The qubit addressed in the molecule has a frequency of either 13.4 kHz or 855 GHz, highlighting the versatility of molecular qubits. This work demonstrates how molecules can transduce quantum information between qubits with different frequencies to enable hybrid quantum systems. We anticipate that quantum control and measurement of molecules as demonstrated here will create opportunities for quantum information science, quantum sensors, fundamental and applied physics, and controlled quantum chemistry.
Scattering resonances play a central role in collision processes in physics and chemistry. They help building an intuitive understanding of the collision dynamics due to the spatial localization of the scattering wavefunctions. For resonances that are localized in the reaction region, located at short separation behind the centrifugal barrier, sharp peaks in the reaction rates are the characteristic signature, observed recently with state-of-the-art experiments in low energy collisions. If, however, the localization occurs outside of the reaction region, mostly the elastic scattering is modified. This may occur due to above barrier resonances, the quantum analogue of classical orbiting. By probing both elastic and inelastic scattering of metastable helium with deuterium molecules in merged beam experiments, we differentiate between the nature of quantum resonances -- tunneling vs above barrier -- and corroborate our findings by calculating the corresponding scattering wavefunctions.
Using the quantum collapse and revival phenomenon of a Bose--Einstein condensate in three-dimensional optical lattices, the atom number statistics on each lattice site are experimentally investigated. We observe an interaction driven time evolution of on-site number fluctuations in a constant lattice potential with the collapse and revival time ratio as the figure of merit. Through a shortcut loading procedure, we prepare a three-dimensional array of coherent states with Poissonian number fluctuations. The following dynamics clearly show the interaction effect on the evolution of the number fluctuations from Poissonian to sub-Poissonian. Our method can be used to create squeezed states which are important in precision measurement.
In recent years it became possible to align molecules in free space using ultrashort laser pulses. Here we explore two schemes for controlling molecule-surface scattering process, which are based on the laser-induced molecular alignment. In the first scheme, a single ultrashort non-resonant laser pulse is applied to a molecular beam hitting the surface. This pulse modifies the angular distribution of the incident molecules, and causes the scattered molecules to rotate with a preferred sense of rotation (clockwise or counter-clockwise). In the second scheme, two properly delayed laser pulses are applied to a molecular beam composed of two chemically close molecular species (isotopes, or nuclear spin isomers). As the result of the double pulse excitation, these species are selectively scattered to different angles after the collision with the surface. These effects may provide new means for the analysis and separation of molecular mixtures.
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