arXiv subjects

Edvardas Narevicius

Publications and source records attributed to Edvardas Narevicius.

At least 19 recordsLinked to original sources

arXiv2024

Feshbach Resonances in Cold Collisions: Benchmarking State of the Art ab initio Potential Energy Surfaces

High-quality potential energy surfaces (PES) are a prerequisite for quantitative atomistic simulations, with both quantum and classical dynamics approaches. The ultimate test for the validity of a PES are comparisons with judiciously chosen experimental observables. Here we ask whether cold collision measurements are sufficiently informative to validate and distinguish between high-level, state-of-the art PESs for the strongly interacting Ne-H$_2^+$ system. We show that measurement of the final state distributions for a process that involves only several metastable intermediate states is sufficient to identify the PES that captures the long-range interactions properly. Furthermore, we show that a modest increase in the experimental energy resolution will allow for resolving individual Feshbach resonances and enable a quantitative probe of the interactions at short and intermediate range.

physics.chem-ph↗

arXiv2023

Tomography of Feshbach Resonance States

Feshbach resonances are fundamental to interparticle interactions and become particularly important in cold collisions with atoms, ions, and molecules. Here we present the detection of Feshbach resonances in a benchmark system for strongly interacting and highly anisotropic collisions -- molecular hydrogen ions colliding with noble gas atoms. The collisions are launched by cold Penning ionization exclusively populating Feshbach resonances that span both short- and long-range parts of the interaction potential. We resolved all final molecular channels in a tomographic manner using ion-electron coincidence detection. We demonstrate the non-statistical nature of the final state distribution. By performing quantum scattering calculations on ab initio potential energy surfaces, we show that the isolation of the Feshbach resonance pathways reveals their distinctive fingerprints in the collision outcome.

physics.atom-ph↗

arXiv2022

Observation of the P-wave Shape Resonance

Partial wave resonances are quasi-bound states that are formed by tunneling through the centrifugal barrier. Such states are important to collisions that deviate from the Langevin limit where direct collision path is suppressed due to quantum symmetry or a potential barrier. In such a case, quantum resonances play a major role in the dynamics at low temperatures where scattering process can be described mainly by the resonance contribution. Here we present the first observation of the lowest-lying partial wave resonance in the Penning ionization collisions between metastable neon and rovibrationally ground state HD molecules. We observe the resonance at an energy of $k_B\times$22mK taking advantage of the phase space correlation similar to atomic delta kick cooling. We show that the $p$-wave resonance position is particularly sensitive to the leading term of the van der Waals interaction. We also measure shape resonance at a higher angular momentum state, $l=6$, allowing us to disentangle and probe the short and the long parts of the intermolecular interaction.

physics.atom-ph↗

arXiv2021

Fano interference in quantum resonances from angle-resolved elastic scattering

Asymmetric spectral line shapes are a hallmark of interference of a quasi-bound state with a continuum of states. Such line shapes are well known for multichannel systems, for example, in photoionization or Feshbach resonances in molecular scattering. On the other hand, in resonant single channel scattering, the signature of such interference may disappear due to the orthogonality of partial waves. Here, we show that probing the angular dependence of the cross section allows us to unveil asymmetric Fano profiles also in a single channel shape resonance. We observe a shift in the peak of the resonance profile in the elastic collisions between metastable helium and deuterium molecules with detection angle, in excellent agreement with theoretical predictions from full quantum scattering calculations. Using a model description for the partial wave interference, we can disentangle the resonant and background contributions and extract the relative phase responsible for the characteristic Fano-like profiles from our experimental measurements.

quant-ph↗

arXiv2021

Vortex beams of atoms and molecules

Angular momentum plays a central role in a multitude of phenomena in quantum mechanics, recurring in every length scale from the microscopic interactions of light and matter to the macroscopic behavior of superfluids. Vortex beams, carrying intrinsic orbital angular momentum (OAM), are now regularly generated with elementary particles such as photons and electrons, and harnessed for numerous applications including microscopy and communication. Untapped possibilities remain hidden in vortices of non-elementary particles, as their composite structure can lead to coupling of OAM with internal degrees of freedom. However, thus far, the creation of a vortex beam of a non-elementary particle has never been demonstrated experimentally. We present the first vortex beams of atoms and molecules, formed by diffracting supersonic beams of helium atoms and dimers, respectively, off binary masks made from transmission gratings. By achieving large particle coherence lengths and nanometric grating features, we observe a series of vortex rings corresponding to different OAM states in the accumulated images of particles impacting a detector. This method is general and can be applied to most atomic and molecular gases. Our results may open new frontiers in atomic physics, utilizing the additional degree of freedom of OAM to probe collisions and alter fundamental interactions.

quant-ph↗

arXiv2020

Determining the nature of quantum resonances by probing elastic and reactive scattering in cold collisions

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.

physics.chem-ph↗

arXiv2020

Direct Observation of a Feshbach-resonance by Coincidence-detection of Ions and Electrons in Penning Ionization Collisions

Observation of molecular dynamics with quantum state resolution is one of the major challenges in chemical physics. Complete characterization of collision dynamics leads to the microscopic understanding and unraveling of different quantum phenomena such as scattering resonances. We present a new experimental approach for observing molecular dynamics involving neutral particles and ions that is capable in providing state-to-state mapping of the dynamics. We use Penning ionization reaction between argon and metastable helium to generate argon ion and ground state helium atom pairs at separation of several angstroms. The energy of ejected electron carries the information about the initial electronic state of an ion. The coincidence detection of ionic products provides a state resolved description of the post-ionization ion-neutral dynamics. We demonstrate that correlation between the electron and ion energy spectra enables us to directly observe the spin-orbit excited Feshbach resonance state of HeAr$^+$. We measure the lifetime of the quasi-bound HeAr$^+$ A$_2$ state and discuss possible applications of our method.

physics.atom-ph↗

arXiv2020

Low-energy collisions between carbon atoms and oxygen molecules in a magnetic trap

Trapping of atoms and molecules in electrostatic, magnetic and optical traps has enabled studying atomic and molecular interactions on a timescale of many seconds, allowing observations of ultra-cold collisions and reactions. Here we report the first magnetic deceleration and trapping of neutral carbon atoms in a static magnetic trap. When co-trapping the carbon atoms with oxygen molecules in a superconducting trap, the carbon signal decays in a non-exponential manner, consistent with losses resulting from atom-molecule collisions. Our findings pave the way to studying both elastic and inelastic collisions of species that cannot be laser cooled, and specifically may facilitate the observation of reactions at low temperatures, such as C + O2 --> CO + O, which is important in interstellar chemistry.

physics.atom-ph↗

arXiv2019

Roadmap on STIRAP applications

STIRAP (Stimulated Raman Adiabatic Passage) is a powerful laser-based method, usually involving two photons, for efficient and selective transfer of population between quantum states. A particularly interesting feature is the fact that the coupling between the initial and the final quantum states is via an intermediate state even though the lifetime of the latter can be much shorter than the interaction time with the laser radiation. Nevertheless, spontaneous emission from the intermediate state is prevented by quantum interference. Maintaining the coherence between the initial and final state throughout the transfer process is crucial. STIRAP was initially developed with applications in chemical dynamics in mind. That is why the original paper of 1990 was published in The Journal of Chemical Physics. However, as of about the year 2000, the unique capabilities of STIRAP and its robustness with respect to small variations of some experimental parameters stimulated many researchers to apply the scheme in a variety of other fields of physics. The successes of these efforts are documented in this collection of articles.

quant-ph↗

arXiv2019

Phase protection of Fano-Feshbach resonances

Decay of bound states due to coupling with free particle states is a general phenomenon occurring at energy scales from MeV in nuclear physics to peV in ultracold atomic gases. Such a coupling gives rise to Fano-Feshbach resonances (FFR) that have become key to understanding and controlling interactions - in ultracold atomic gases, but also between quasiparticles such as microcavity polaritons. The energy positions of FFR were shown to follow quantum chaotic statistics. In contrast, lifetimes which are the fundamental property of a decaying state, have so far escaped a similarly comprehensive understanding. Here we show that a bound state, despite being resonantly coupled to a scattering state, becomes protected from decay whenever the relative phase is a multiple of $π$. We observe this phenomenon by measuring lifetimes spanning four orders of magnitude for FFR of spin-orbit excited molecular ions with merged beam and electrostatic trap experiments. Our results provide a blueprint for identifying naturally long-lived states in a decaying quantum system.

physics.atom-ph↗

arXiv2019

Collisions between cold molecules in a superconducting magnetic trap

Collisions between cold molecules are essential for studying fundamental aspects of quantum chemistry, and may enable formation of quantum degenerate molecular matter by evaporative cooling. However, collisions between trapped, naturally occurring molecules have so far eluded direct observation due to the low collision rates of dilute samples. We report the first directly observed collisions between cold, trapped molecules, achieved without the need of laser cooling. We magnetically capture molecular oxygen in a 0.8K x kB deep superconducting trap, and set bounds on the ratio between the elastic and inelastic scattering rates, the key parameter determining the feasibility of evaporative cooling. We further co-trap and identify collisions between atoms and molecules, paving the way to studies of cold interspecies collisions in a magnetic trap.

physics.atom-ph↗

arXiv2018

Phase-locking between different partial-waves in atom-ion spin-exchange collisions

We present a joint experimental and theoretical study of spin dynamics of a single $^{88}$Sr$^+$ ion colliding with an ultracold cloud of Rb atoms in various hyperfine states. While spin-exchange between the two species occurs after 9.1(6) Langevin collisions on average, spin-relaxation of the Sr$^+$ ion Zeeman qubit occurs after 48(7) Langevin collisions which is significantly slower than in previously studied systems due to a small second-order spin-orbit coupling. Furthermore, a reduction of the endothermic spin-exchange rate was observed as the magnetic field was increased. Interestingly, we found that, while the phases acquired when colliding on the spin singlet and triplet potentials vary largely between different partial waves, the singlet-triplet phase difference, which determines the spin-exchange cross-section, remains locked to a single value over a wide range of partial-waves which leads to quantum interference effects.

physics.atom-ph↗

arXiv2016

Trapping of molecular Oxygen together with Lithium atoms

We demonstrate simultaneous deceleration and trapping of a cold atomic and molecular mixture. This is the first step towards studies of cold atom-molecule collisions at low temperatures as well as application of sympathetic cooling. Both atoms and molecules are cooled in a supersonic expansion and are loaded into a moving magnetic trap which brings them to rest via the Zeeman interaction from an initial velocity of 375 m/s. We use a beam seeded with molecular Oxygen, and entrain it with Lithium atoms by laser ablation prior to deceleration. The deceleration ends with loading of the mixture into a static quadrupole trap, which is generated by two permanent magnets. We estimate $10^9$ trapped O$_2$ molecules and $10^5$ Li atoms with background pressure limited lifetime on the order of 1 second. With further improvements to Lithium entrainment we expect that sympathetic cooling of molecules is within reach.

physics.atom-ph↗

arXiv2016

Molecular beam brightening by shock-wave suppression

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.

physics.atom-ph↗

arXiv2016

Direct probe of anisotropy in atom-molecule collisions via quantum scattering resonances

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.

physics.chem-ph↗

arXiv2016

Photoassociation spectroscopy in Penning ionization reactions at sub-Kelvin temperatures

Penning ionization reactions in merged beams with precisely controlled collision energies have been shown to accurately probe quantum mechanical effects in reactive collisions. A complete microscopic understanding of the reaction is, however, faced with two major challenges---the highly excited character of the reaction's entrance channel and the limited precision of even the best state-of-the-art ab initio potential energy surfaces. Here, we suggest photoassociation spectroscopy as a tool to identify the character of orbiting resonances in the entrance channel and probe the ionization width as a function of inter-particle separation. We introduce the basic concept and discuss the general conditions under which this type of spectroscopy will be successful.

physics.atom-ph↗

arXiv2013

Magneto-Optical Cooling of Atoms

We propose an alternative method to laser cooling. Our approach utilizes the extreme brightness of a supersonic atomic beam, and the adiabatic atomic coilgun to slow atoms in the beam or to bring them to rest. We show how internal-state optical pumping and stimulated optical transitions, combined with magnetic forces can be used to cool the translational motion of atoms. This approach does not rely on momentum transfer from photons to atoms, as in laser cooling. We predict that our method can surpass laser cooling in terms of flux of ultra-cold atoms and phase-space density, with lower required laser power and reduced complexity.

physics.atom-ph↗

arXiv2012

Observation of Quantum Effects in sub Kelvin Cold Reactions

There has been a long-standing quest to observe chemical reactions at low temperatures where reaction rates and pathways are governed by quantum mechanical effects. So far this field of Quantum Chemistry has been dominated by theory. The difficulty has been to realize in the laboratory low enough collisional velocities between neutral reactants, so that the quantum wave nature could be observed. We report here the first realization of merged neutral supersonic beams, and the observation of clear quantum effects in the resulting reactions. We observe orbiting resonances in the Penning ionization reaction of argon and molecular hydrogen with metastable helium leading to a sharp increase in the absolute reaction rate in the energy range corresponding to a few degrees kelvin down to 10 mK. Our method is widely applicable to many canonical chemical reactions, and will enable a breakthrough in the experimental study of Quantum Chemistry.

physics.chem-ph↗