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 Multi-Configurational 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 intra-well and inter-well 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.
Trilobites are exotic giant dimers with enormous dipole moments. They consist of a Rydberg atom and a distant ground-state atom bound together by short-range electron-neutral attraction. We show that highly polar, polyatomic trilobite states unexpectedly persist and thrive in a dense ultracold gas of randomly positioned atoms. This is caused by perturbation-induced quantum scarring and the localization of electron density on randomly occurring atom clusters. At certain densities these states also mix with a s-state, overcoming selection rules that hinder the photoassociation of ordinary trilob…
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 Ångstroms. 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…
We observe that when an ultracold ground state cesium (Cs) atom becomes bound within the electronic cloud of an extended Cs electronic orbit, ultralong-range molecules with giant (kilo-Debye) permanent electric dipole moments form. Large molecular permanent electric dipole moments are challenging to experimentally realize. Meeting this challenge has garnered significant interest because permanent electric dipole moments are important for understanding symmetry breaking in molecular physics, control of chemical reactions and realization of strongly correlated many-body quantum systems. These ne…
A few-body approach relying on static line broadening theory is developed to treat the spectroscopy of a single Rydberg excitation to a trilobite-like state immersed in a high density ultracold medium. The present theoretical framework implements the compact treatment of polyatomic Rydberg molecules by Eiles et al. [arXiv:1601.06881], allowing for an accurate treatment of a large number of perturbers within the Rydberg orbit. This system exhibits two unique spectral signatures: its lineshape depends on the Rydberg quantum number $n$ but, strikingly, is independent of the density of the medium,…
We observe "trilobite-like" states of ultracold 85Rb2 molecules, in which a ground-state atom is bound by the electronic wavefunction of its Rydberg-atom partner. We populate these states through the ultraviolet excitation of weakly-bound molecules, and access a regime of trilobite-like states at low principal quantum numbers and with vibrational turning points around 35 Bohr radii. This demonstrates that, unlike previous studies that used free-to-bound transitions, trilobite-like states can also be excited through bound-to-bound transitions. This approach provides high excitation probabilitie…
We report on a novel method for photo-association of strongly polar trilobite Rydberg molecules. This exotic ultralong-range dimer, consisting of a ground-state atom bound to the Rydberg electron via electron-neutral scattering, inherits its polar character from the admixture of high angular momentum electronic orbitals. The absence of low-$L$ character hinders standard photo-association techniques. Here, we show that for suitable principal quantum numbers resonant coupling of the orbital motion with the nuclear spin of the perturber, mediated by electron-neutral scattering, hybridizes the tri…
Ultralong-range Rydberg molecules provide an exciting testbed for molecular physics at exaggerated scales. In the so-called trilobite and butterfly Rydberg molecules, the Born-Oppenheimer approximation can fail due to strong non-adiabatic couplings arising from the combination of radial oscillations and rapid energy variations in the adiabatic potential energy curves. We utilize an accurate coupled-channel treatment of the vibronic system to observe the breakdown of Born-Oppenheimer physics, such as non-adiabatic trapping and decay of molecular states found near pronounced avoided crossings in…
We have studied electron-induced ion-pair dissociation dynamics of CO using the state-of-art velocity map imaging technique in combination with a time-of-flight-based two-field mass spectrometer. Extracting the characteristics for O$^-$/CO nascent atomic anionic fragments from the low energy (25 - 45 eV) electron-molecule scattering, first-time, we have directly detected the existence of S-wave resonated Trilobite resembling a novel molecular binding energy mechanism, as predicted by Greene \textit{et al.} \cite{greene2000creation}. The energy balance demands ion-pair dissociation (IPD) lie wi…
This Ph.D. 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 ph…
A generalized class of ultra-long-range Rydberg molecules is proposed which consist of a multichannel Rydberg atom whose outermost electron creates a chemical bond with a distant ground state atom. Such multichannel Rydberg molecules exhibit favorable properties for laser excitation, because states exist where the quantum defect varies strongly with the principal quantum number. The resulting occurrence of near degeneracies with states of high orbital angular momentum promotes the admixture of low $l$ into the high $l$ deeply bound `trilobite' molecule states, thereby circumventing the usual d…
A ground state atom immersed in the wave function of the valence electron of a Rydberg atom can generate a long-range Rydberg molecule (LRRM). In this work, using the multipole expansion of the electrostatic interaction in prolate spheroidal coordinates, approximate and compact expressions of the electrostatic potential that determine the chemistry of trilobite and butterfly LRRM are explored. It is shown that even the spheroidal monopole term can be used to describe general features of the potential generated by a LRRM at short distances. It is also shown that even at long separations that al…
The "trilobite" type of molecule, predicted in 2000 and observed experimentally in 2015, arises when a Rydberg electron exerts a weak attractive force on a neutral ground state atom. Such molecules have bond lengths exceeding 100 nm. The ultra-long-range chemical bond between the two atoms is a nonperturbative linear combination of the many degenerate electronic states associated with high principal quantum numbers, and the resulting electron probability distribution closely resembles a fossil trilobite from antiquity. We show how to coherently engineer this same long-range orbital through a s…
Rydberg molecules, often exemplified by long-range "trilobite" molecules, are a subject of much recent interest at high principal quantum number $n$. States that use the same bonding mechanism can exist at much lower $n$ and less-extreme internuclear separations that are still quite long range. We use a high-resolution pulsed amplifier to study previously-detected transitions to a low-$n$ Rydberg molecular state near the $5s+7p$ asymptote in $^{85}$Rb$_2$. The observed line structure is modeled using precise ground-state positions and a lower bound of $τ> 1.1 \times 10^{-9}$ s is set on the ex…
We introduce the Rydberg Composite, a new class of Rydberg matter where a single Rydberg atom is interfaced with a dense environment of neutral ground state atoms. The properties of the Composite depend on both the Rydberg excitation, which provides the gross energetic and spatial scales, and on the distribution of ground state atoms within the volume of the Rydberg wave function, which sculpt the electronic states. The latter range from the "trilobites", for small numbers of scatterers, to delocalized and chaotic eigenstates for disordered scatterer arrays, culminating in the dense scatterer …
The preparation of low-entropy starting conditions is a key requirement for many experiments involving neutral atoms. Here, we propose a method to autonomously assemble arbitrary spatial configurations of atoms within arrays of optical tweezers or lattice sites, enabled by a combination of tunneling and ground-state laser cooling. In contrast to previous methods, our protocol does not rely on either imaging or evaporative cooling. This circumvents limitations associated with imaging fidelity and loss, especially in systems with small spatial scales, while providing a substantial improvement in…
We present an experimental system for Rydberg tweezer arrays with ytterbium (Yb) atoms featuring internal state manipulation between the ground ${}^1$S$_0$ and the metastable ${}^3$P$_2$ states, and single-photon excitation from the ${}^3$P$_2$ to Rydberg states. In the experiments, single Yb atoms are trapped in two-dimensional arrays of optical tweezers and are detected by fluorescence imaging with the intercombination ${}^1$S$_0 \leftrightarrow {}^3$P$_1$ transition, and the defect-free single atom arrays are prepared by the rearrangement with the feedaback. We successfully perform high-res…
Recent developments toward the production and laboratory use of pulses of high intensity, and/or of very high frequency, and/or of ultrashort duration, make possible experiments which can produce time-resolved data on ultrafast transformations involving motions of electrons. The formulation, quantitative understanding and prediction of related new phenomena entail the possibility of computing and applying solutions of the many-electron time-dependent Schroedinger equation, for arbitrary electronic structures, including the dominant effects of Rydberg series, of multiply excited states and of t…
Radiative and collisional constants of excited atoms contain the matrix elements of the dipole transitions and when they are blocked one can expect occurring a number of interesting phenomena in radiation-collisional kinetics. In recent astrophysical studies of IR emission spectra it was revealed a gap in the radiation emitted by Rydberg atoms ($RA$) with values of the principal quantum number of $n\approx10$. Under the presence of external electric fields a rearrangement of $RA$ emission spectra is possible to associate with manifestations of the Stark effect. The threshold for electric field…
Many-body systems relaxing to equilibrium can exhibit complex dynamics even if their steady state is trivial. At low temperatures or high densities their evolution is often dominated by steric hindrances affecting particle motion [1,2,3]. Local rearrangements are highly constrained, giving rise to collective - and often slow - relaxation.This dynamics can be difficult to analyse from first principles, but the essential physical ingredients are captured by idealized lattice models with so- called kinetic constraints [4]. Here we experimentally realize a many-body system exhibiting manifest kine…
The generation of long-lived entanglement on an optical clock transition is a key requirement to unlocking the promise of quantum metrology. Arrays of neutral atoms constitute a capable quantum platform for accessing such physics, where Rydberg-based interactions may generate entanglement between individually controlled and resolved atoms. To this end, we leverage the programmable state preparation afforded by optical tweezers along with the efficient strong confinement of a 3d optical lattice to prepare an ensemble of strontium atom pairs in their motional ground state. We engineer global sin…
