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arXiv:2012.07576 · Physical Review A

Electric-field-induced wave-packet dynamics and geometrical rearrangement of trilobite Rydberg molecules

Frederic Hummel, Kevin Keiler, Peter Schmelcher

Published Feb 19, 2021• 15 citations
arXivHTMLPDF

Abstract

We investigate the quantum dynamics of ultra-long-range trilobite molecules exposed to homogeneous electric fields. A trilobite molecule consists of a Rydberg atom and a ground-state atom, which is trapped at large internuclear distances in an oscillatory potential due to scattering of the Rydberg electron off the ground-state atom. Within the Born-Oppenheimer approximation, we derive an analytic expression for the two-dimensional adiabatic electronic potential energy surface in weak electric fields valid up to 500 V/m. This is used to unravel the molecular quantum dynamics employing the multiconfigurational time-dependent Hartree method. Quenches of the electric field are performed to trigger the wave-packet dynamics including the case of field inversion. Depending on the initial wave packet, we observe radial intrawell and interwell oscillations as well as angular oscillations and rotations of the respective one-body probability densities. Opportunities to control the molecular configuration are identified, a specific example being the possibility to superimpose different molecular bond lengths by a series of periodic quenches of the electric field.

DOI
10.1103/physreva.103.022827

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We investigate the quantum dynamics of ultra-long-range trilobite molecules exposed to homogeneous electric fields. A trilobite molecule consists of a Rydberg atom and a ground-state atom, which is trapped at large internuclear distances in an oscillatory potential due to scattering of the Rydberg electron off the ground-state atom. Within the Born-Oppenheimer approximation, we derive an analytic expression for the two-dimensional adiabatic electronic potential energy surface in weak electric fields valid up to 500 V/m. This is used to unravel the molecular quantum dynamics employing the multiconfigurational time-dependent Hartree method. Quenches of the electric field are performed to trigger the wave-packet dynamics including the case of field inversion. Depending on the initial wave packet, we observe radial intrawell and interwell oscillations as well as angular oscillations and rotations of the respective one-body probability densities. Opportunities to control the molecular configuration are identified, a specific example being the possibility to superimpose different molecular bond lengths by a series of periodic quenches of the electric field.
We investigate the impact of an electric field on the structure of ultra-long-range polar diatomic rubidium Rydberg molecules. Both the sss-wave and ppp-wave interactions of the Rydberg electron and the neutral ground-state atom are taken into account. In the presence of the electric field the angular degree of freedom between the electric field and the internuclear axis acquires vibrational character and we encounter two-dimensional oscillatory adiabatic potential energy surfaces with an antiparallel equilibrium configuration. The electric field allows shifting of the corresponding potential wells in such a manner that the importance of the ppp-wave interaction can be controlled and the individual wells are energetically lowered at different rates. As a consequence the equilibrium configuration and corresponding energetically lowest well move to larger internuclear distances for increasing field strength. For strong fields the admixture of nonpolar molecular Rydberg states leads to the possibility of exciting the large angular momentum polar states via two-photon processes from the ground state of the atom. The resulting properties of the electric dipole moment and the vibrational spectra are analyzed with varying field strength.
Trilobite molecules are ultralong-range Rydberg molecules formed when a high angular momentum Rydberg electron scatters off of a ground-state atom. Their unique electronic structure and highly oscillatory potential energy curves support a rich variety of dynamical effects yet to be explored. We analyze the vibrational motion of these molecules using a framework of adiabatic wave-packet propagation dynamics and observe that for appropriate initial states, the trilobite potential acts as molecular diffraction grating. The quantum dynamic effects observed are explained using a Fourier analysis of the scattering potential and the associated scattered wave packet. Furthermore, vibrational ground states of the low angular momentum ultralong-range Rydberg molecules are found to be particularly suitable to prepare the relevant wave packets. Hence, we propose a time-resolved pump-probe scheme designed for the realization of the effect in question, and advertise the utilization of a single diatomic Rydberg molecule as a test bed for the study of exaggerated quantum dynamical phenomena.
We investigate the non-adiabatic quantum dynamics of ultralong-range Rydberg molecules using a vibronically coupled two-channel treatment. The two-channels are composed of coupled trilobite and butterfly electronic states, formed as a result of SSS-wave and PPP-wave scattering of high angular momentum Rydberg electrons with perturbing ground state atoms. Within the Born-Oppenheimer treatment, the PPP-wave scattering channel introduces an adiabatic decay pathway that affects the stability and lifetimes of trilobite states. Our numerical results show that the vibronic coupling is dependent on the principal quantum number nnn, and for certain nnn there is non-adiabatic stabilization against internal molecular decay, facilitating previously studied dynamical effects in pure trilobite molecules. Apart from the internal diffraction effect caused by the backscattering of vibrational wavepackets from the trilobite potential, we also observe interesting multi-well tunneling effects during low-energy oscillations for a range of nnn-values. Our work serves to highlight that the unique vibrational coordinate dependent electronic structure of these polar molecules, along with high level densities, promise many exciting dynamical effects.
Abstract This PhD tutorial discusses ultra-long-range Rydberg molecules, the exotic bound states of a Rydberg atom and one or more ground state atoms immersed in the Rydberg electron’s wave function. This novel chemical bond is distinct from an ionic or covalent bond, and is accomplished by a very different mechanism: the Rydberg electron, elastically scattering off of the ground state atoms, exerts a weak attractive force sufficient to form the molecule in long-range oscillatory potential wells. In the last decade this topic has burgeoned into a vibrant and mature subfield of atomic and molecular physics following the rapidly developing capability of experiment to observe and manipulate these molecules. This tutorial focuses on three areas where this experimental progress has demanded more sophisticated theoretical descriptions: the structure of polyatomic molecules, the influence of electronic and nuclear spin, and the behavior of these molecules in external fields. The main results are a collection of potential energy curves and electronic wave functions which together describe the physics of Rydberg molecules. Additionally, to facilitate future progress in this field, this tutorial provides a general overview of the current state of experiment and theory.
We investigate the impact of combined electric and magnetic fields on the structure of ultralong-range polar Rydberg molecules. Our focus is hereby on the parallel as well as the crossed field configuration, taking into account both the s -wave and p -wave interactions of the Rydberg electron and the neutral ground state atom. We show the strong impact of the p -wave interaction on the ultralong-range molecular states for a pure B -field configuration. In the presence of external fields, the angular degrees of freedom acquire vibrational character, and we encounter two- and three-dimensional oscillatory adiabatic potential energy surfaces for the parallel and crossed field configuration, respectively. The equilibrium configurations of local potential wells can be controlled via the external field parameters for both field configurations depending on the specific degree of electronic excitation. This allows us to tune the molecular alignment and orientation. The resulting electric dipole moment is in the order of several kDebye, and the rovibrational level spacings are in the range of 2– . Both properties are analyzed with varying field strengths.
We investigate triatomic molecules that consist of two ground-state atoms and a highly excited Rydberg atom, bound at large internuclear distances of thousands of angstroms. In the molecular state the Rydberg electron is in a superposition of high angular momentum states whose probability densities resemble the form of trilobite fossils. The associated potential-energy landscape has an oscillatory shape and supports a rich variety of stable geometries with different bond angles and bond lengths. Based on an electronic structure investigation we analyze the molecular geometry systematically and develop a simple building principle that predicts the triatomic equilibrium configurations. As a representative example we focus on 87Rb^{87}\mathrm{Rb}87Rb trimers correlated to the n=30n=30n=30 Rydberg state. Using an exact diagonalization scheme we determine and characterize localized vibrational states in these potential minima with energy spacings on the order of 100 $\mathrm{MHz}\ifmmode\times\else\texttimes\fi{}h$.