Subscribe to the gold package and get unlimited access to Shamra Academy
Register a new userExperimental and Theoretical Investigation of the Crossover from the Ultracold to the Quasiclassical Regime of Photodissociation
97
0
0.0
(
0
)
Ask ChatGPT about the research
No Arabic abstract
At ultralow energies, atoms and molecules undergo collisions and reactions that are best described in terms of quantum mechanical wave functions. In contrast, at higher energies these processes can be understood quasiclassically. Here, we investigate the crossover from the quantum mechanical to the quasiclassical regime both experimentally and theoretically for photodissociation of ultracold diatomic strontium molecules. This basic reaction is carried out with a full control of quantum states for the molecules and their photofragments. The photofragment angular distributions are imaged, and calculated using a quantum mechanical model as well as the WKB and a semiclassical approximation that are explicitly compared across a range of photofragment energies. The reaction process is shown to converge to its high-energy (axial recoil) limit when the energy exceeds the height of any reaction barriers. This phenomenon is quantitatively investigated for two-channel photodissociation using intuitive parameters for the channel amplitude and phase. While the axial recoil limit is generally found to be well described by a commonly used quasiclassical model, we find that when the photofragments are identical particles, their bosonic or fermionic quantum statistics can cause this model to fail, requiring a quantum mechanical treatment even at high energies.
rate research
Read More
Processes that break molecular bonds are typically observed with molecules occupying a mixture of quantum states and successfully described with quasiclassical models, while a few studies have explored the distinctly quantum mechanical low-energy regime. Here we use photodissociation of diatomic strontium molecules to demonstrate the crossover from the ultracold, quantum regime where the photofragment angular distributions strongly depend on the kinetic energy, to the energy-independent quasiclassical regime. Using time-of-flight velocity map imaging for photodissociation channels with millikelvin reaction barriers, we explore photofragment energies in the 0.1-300 mK range experimentally and up to 3 K theoretically, and discuss the energy scale at which the crossover occurs. Furthermore, we find that the effects of quantum statistics can unexpectedly persist to high photodissociation energies.
Photodissociation of a molecule produces a spatial distribution of photofragments determined by the molecular structure and the characteristics of the dissociating light. Performing this basic chemical reaction at ultracold temperatures allows its quantum mechanical features to dominate. In this regime, weak applied fields can be used to control the reaction. Here, we photodissociate ultracold diatomic strontium in magnetic fields below 10 G and observe striking changes in photofragment angular distributions. The observations are in excellent qualitative agreement with a multichannel quantum chemistry model that includes nonadiabatic effects and predicts strong mixing of partial waves in the photofragment energy continuum. The experiment is enabled by precise quantum-state control of the molecules.
The experimental characterization of scattering resonances in low energy collisions has proven to be a stringent test for quantum chemistry calculations. Previous measurements on the NO-H$_2$ system at energies down to $10$ cm$^{-1}$ challenged the most sophisticated calculations of potential energy surfaces available. In this report, we continue these investigations by measuring the scattering behavior of the NO-H$_2$ system in the previously unexplored $0.4 - 10$ cm$^{-1}$ region for the parity changing de-excitation channel of NO. We study state-specific inelastic collisions with both textit{para}- and textit{ortho}-H$_2$ in a crossed molecular beam experiment involving Stark deceleration and velocity map imaging. We are able to resolve resonance features in the measured integral and differential cross sections. Results are compared to predictions from two previously available potential energy surfaces and we are able to clearly discriminate between the two potentials. We furthermore identify the partial wave contributions to these resonances, and investigate the nature of the differences between collisions with textit{para}- and textit{ortho}-H$_2$. Additionally, we tune the energy spreads in the experiment to our advantage to probe scattering behavior at energies beyond our mean experimental limit.
Quantum control of reactive systems has enabled microscopic probes of underlying interaction potentials, the opening of novel reaction pathways, and the alteration of reaction rates using quantum statistics. However, extending such control to the quantum states of reaction outcomes remains challenging. In this work, we realize this goal through the nuclear spin degree of freedom, a result which relies on the conservation of nuclear spins throughout the reaction. Using resonance-enhanced multiphoton ionization spectroscopy to investigate the products formed in bimolecular reactions between ultracold KRb molecules, we find that the system retains a near-perfect memory of the reactants nuclear spins, manifested as a strong parity preference for the rotational states of the products. We leverage this effect to alter the occupation of these product states by changing the coherent superposition of initial nuclear spin states with an external magnetic field. In this way, we are able to control both the inputs and outputs of a bimolecular reaction with quantum state resolution. The techniques demonstrated here open up the possibilities to study quantum interference between reaction pathways, quantum entanglement between reaction products, and ultracold reaction dynamics at the state-to-state level.
We report measurements of the lifetimes of the 3d $^2$D$_{5/2}$ and 3d $^2$D$_{3/2}$ metastable states of a single laser-cooled $^{40}$Ca$^+$ ion in a linear Paul trap. We introduce a new measurement technique based on high-efficiency quantum state detection after coherent excitation to the D$_{5/2}$ state or incoherent shelving in the D$_{3/2}$ state, and subsequent free, unperturbed spontaneous decay. The result for the natural lifetime of the D$_{5/2}$ state of 1168(9) ms agrees excellently with the most precise published value. The lifetime of the D$_{3/2}$ state is measured with a single ion for the first time and yields 1176(11) ms which improves the statistical uncertainty of previous results by a factor of four. We compare these experimental lifetimes to high-precision ab initio all order calculations and find a very good agreement. These calculations represent an excellent test of high-precision atomic theory and will serve as a benchmark for the study of parity nonconservation in Ba$^+$ which has similar atomic structure.
Log in to be able to interact and post comments
comments
Fetching comments
Sign in to be able to follow your search criteria
