We report the creation of heteronuclear ultralong-range Rydberg-molecule dimers by excitation of minority $^{88}\text{Sr}$ atoms to $5sns\,^3S_1$ Rydberg states ($n=31-39$) in a dense background of $^{84}\text{Sr}$. We observe an isotope shift of the $ν=0$ vibrational state over this range of $n$ and compare our measurements with a theoretical prediction and a simple scaling argument. With the appropriate choice of principal quantum number the isotope shift is sufficiently large to produce heteronuclear dimers with almost perfect fidelity. When the spectral selectivity is limited, we obtain a lower bound on the ratio of heteronuclear to homonuclear excitation probability of 30 to 1 by measuring the scaling of the molecular excitation rate with varying relative densities of $^{88}\text{Sr}$ and $^{84}\text{Sr}$ in the ultracold mixture.
We present the formation of homonuclear Cs2, K2, and heteronuclear CsK long-range Rydberg molecules in a dual-species magneto-optical trap for 39K and 133Cs by one-photon UV photoassociation. The different ground-state-density dependence of homo- and heteronuclear photoassociation rates and the detection of stable molecular ions resulting from auto-ionization provide an unambiguous assignment. We perform bound-bound millimeter-wave spectroscopy of long-range Rydberg molecules to access molecular states not accessible by one-photon photoassociation. Calculations based on the most recent theoret…
Due to the intrinsic strong blockaded interaction shifting the energy level of Rydberg state, the steady Rydberg probability may be substantially restrained to a low level, especially for atoms suffering from weak drivings. We report an exotic excitation facilitation using strong blockaded energy shifting the double excitation state, leading to the weakly-driven atom deterministically excited by a significantly improved fraction even at far off-resonant regimes. This phenomenon is attributed to the effective induction of a reduced detuning to the weakly-driven atom by optimizing parameters of …
We report the observation of a dimer-dimer inelastic collision resonance for ultracold Feshbach molecules made of bosonic sodium and rubidium atoms. This resonance, which we attribute to the crossing of the dimer-dimer threshold with a heteronuclear tetramer state, manifests itself as a pronounced inelastic loss peak of dimers when the interspecies scattering length between the constituent atoms is tuned. Near this resonance, a strong modification of the temperature dependence of the dimer-dimer scattering is observed. Our result provides insight into the heteronuclear four-body system consist…
We present a comprehensive study of the diverse properties of heteronuclear Rydberg molecules, placing a special emphasis on those composed of the light alkali atoms, Li, Na, and K. Electron-atom scattering phase shifts, which determine the strength of the molecular bond, are calculated at very low energy and then used in a spin-dependent theoretical model to calculate accurate Rydberg molecule potential energy curves. The wide parameter range accessible by combining the various properties of different alkali atoms often leads to hybridized electronic states accessible via one or two photon ex…
We report on the production of ultracold heteronuclear YbLi* molecules in a dual-species magneto-optical trap by photoassociation (PA). The formation of the electronically excited molecules close to dissociation was observed by trap loss spectroscopy. We find 4 rovibrational states within a range of $250\,$GHz below the Yb($^1S_0$) + Li($^2P_{1/2}$) asymptote and observe isotopic PA line shifts in mixtures of $^6$Li with $^{174}$Yb, $^{172}$Yb, and $^{176}$Yb. We also describe our theoretical ab-initio calculation for the relevant electronic potentials and utilize it to analyze and identify th…
We investigate the formation of weakly bound, electronically excited, heteronuclear 6Li40K* molecules by single-photon photoassociation in a magneto-optical trap. We performed trap loss spectroscopy within a range of 325 GHz below the Li(2S_(1/2))+K(4P_(3/2)) and Li(2S_(1/2))+K(4P_(1/2)) asymptotic states and observed more than 60 resonances, which we identify as rovibrational levels of 7 of 8 attractive long-range molecular potentials. The long-range dispersion coefficients and rotational constants are derived. We find large molecule formation rates of up to ~3.5x10^7s^(-1), which are shown t…
We study the association and dissociation dynamics of weakly bound heteronuclear Feshbach molecules using transverse RF-fields for expected parameters accessible through the microgravity environment of NASA's Cold Atom Laboratory (CAL) aboard the International Space Station, including temperatures at or below nK and atomic densities as low as $10^8$/cm$^3$. We show that under such conditions, thermal and loss effects can be greatly suppressed resulting in high efficiency in both association and dissociation of Feshbach molecules with mean size exceeding 10$^4a_0$, and allowing for the coherenc…
We report on two-photon photoassociation (PA) spectroscopy of ultracold heteronuclear LiRb molecules. This is used to determine the binding energies of the loosely bound levels of the electronic ground singlet and the lowest triplet states of LiRb. We observe strong two-photon PA lines with power broadened line widths greater than 20 GHz at relatively low laser intensity of 30 W/cm$^{2}$. The implication of this observation on direct atom to molecule conversion using stimulated Raman adiabatic passage (STIRAP) is discussed and the prospect for electronic ground state molecule production is the…
Ultra-cold RbCs molecules in high-lying vibrational levels of the a$^3Σ^+$ ground electronic state are confined in an optical trap. Inelastic collision rates of these molecules with both Rb and Cs atoms are determined for individual vibrational levels, across an order of magnitude of binding energies. A simple model for the collision process is shown to accurately reproduce the observed scattering rates.
We report on the observation of ultracold heteronuclear Feshbach molecules. Starting with a $^{87}$Rb BEC and a cold atomic gas of $^{85}$Rb, we utilize previously unobserved interspecies Feshbach resonances to create up to 25,000 molecules. Even though the $^{85}$Rb gas is non-degenerate we observe a large molecular conversion efficiency due to the presence of a quantum degenerate $^{87}$Rb gas; this represents a key feature of our system. We compare the molecule creation at two different Feshbach resonances with different magnetic-field widths. The two Feshbach resonances are located at $265…
The relation between high-harmonic spectra and the geometry of the molecular orbitals in position and momentum space is investigated. In particular we choose two isoelectronic pairs of homonuclear and heteronuclear molecules, such that the highest occupied molecular orbital of the former exhibit at least one nodal plane. The imprint of such planes is a strong suppression in the harmonic spectra, for particular alignment angles. We are able to identify two distinct types of nodal planes. If the nodal planes are determined by the atomic wavefunctions only, the angle for which the yield is suppre…
We demonstrate a generally applicable technique for mixing two-species quantum degenerate bosonic samples in the presence of an optical lattice, and we employ it to produce low-entropy samples of ultracold 87Rb133Cs Feshbach molecules with a lattice filling fraction exceeding 30%. Starting from two spatially separated Bose-Einstein condensates of Rb and Cs atoms, Rb-Cs atom pairs are efficiently produced by using the superfluid-to-Mott insulator quantum phase transition twice, first for the Cs sample, then for the Rb sample, after nulling the Rb-Cs interaction at a Feshbach resonance's zero cr…
We study frustrated double ionization in a strongly-driven heteronuclear molecule HeH$^{+}$ and compare with H$_2$. We compute the probability distribution of the sum of the final kinetic energies of the nuclei for strongly-driven HeH$^{+}$. We find that this distribution has more than one peak for strongly-driven HeH$^{+}$, a feature we do not find to be present for strongly-driven H$_{2}$. Moreover, we compute the probability distribution of the n quantum number of frustrated double ionization. We find that this distribution has several peaks for strongly-driven HeH$^{+}$, while the respecti…
Vibrational dynamics in conventional molecules usually takes place on a timescale of picoseconds or shorter. A striking exception are ultralong-range Rydberg molecules, for which dynamics is dramatically slowed down as a consequence of the huge bond length of up to several micrometers. Here, we report on the direct observation of vibrational dynamics of a recently observed Rydberg-atom-ion molecule. By applying a weak external electric field of a few mV/cm, we are able to control the orientation of the photoassociated ultralong-range Rydberg molecules and induce vibrational dynamics by quenchi…
We demonstrate that a near-dissociation photoassociation resonance can be used to create a deeply bound molecular sample of ultracold NaCs. To probe the resulting vibrational distribution of the sample, we use a new technique that can be applied to any ultracold molecular system. We utilize a tunable pulsed dye laser to produce efficient spectroscopic scans ($\sim700$ cm$^{-1}$ at a time) in which we observe the $1^{1} Σ^{+}\rightarrow 2^{1}Σ^{+}-2^{3}Π$ vibrational progression, as well as the dissociation limit to the Cs 6$^{2}$P$_{3/2}$ asymptote. We assign $1^{1} Σ^{+}$$(\emph{v}$ = 4, 5, 6…
We describe a quantum information architecture consisting of a hybrid array of optically-trapped molecules and atoms. This design leverages the large transition dipole moments of Rydberg atoms to mediate fast, high-fidelity gates between qubits encoded in coherent molecular degrees of freedom. Error channels of detuning, decay, pulse area noise, and leakage to other molecular states are discussed. The molecule-Rydberg interaction can also be used to enable nondestructive molecule detection and rotational state readout. We consider a specific near-term implementation of this scheme using NaCs m…
Promising pathways for photoassociative formation of ultracold heteronuclear alkali metal dimers in their lowest rovibronic levels (denoted X(0,0)) are examined using high quality ab initio calculations of potential energy curves currently available. A promising pathway for KRb, involving the resonant coupling of the $2 ^1Π$ and $1 ^1Π$ states just below the lowest excited asymptote (K($4s$)+Rb($5p_{1/2}$)), is found to occur also for RbCs and less promisingly for KCs as well. The resonant coupling of the $3 ^1 Σ^+ $ and $1 ^1Π$ states, also just below the lowest excited asymptote, is found to…
Recently, the quest for an ultracold and dense ensemble of polar molecules has attracted strong interest. Polar molecules have bright prospects for novel quantum gases with long-range and anisotropic interactions, for quantum information science, and for precision measurements. However, high-density clouds of ultracold polar molecules have so far not been produced. Here, we report a key step towards this goal. Starting from an ultracold dense gas of heteronuclear 40K-87Rb Feshbach molecules with typical binding energies of a few hundred kHz and a negligible dipole moment, we coherently transfe…
The lifetimes and decay channels of ultralong-range Rydberg molecules created in a dense BEC are examined by monitoring the time evolution of the Rydberg population using field ionization. Studies of molecules with values of principal quantum number, $n$, in the range $n=49$ to $n=72$ that contain tens to hundreds of ground state atoms within the Rydberg electron orbit show that their presence leads to marked changes in the field ionization characteristics. The Rydberg molecules have lifetimes of $\sim1-5\,μ$s, their destruction being attributed to two main processes: formation of Sr$^+_2$ ion…
We present experimental evidence for spin-orbit interaction of an electron as it scatters from a neutral atom. The scattering process takes place within a Rb$_2$ ultralong-range Rydberg molecule, consisting of a Rydberg atomic core, a Rydberg electron, and a ground state atom. The spin-orbit interaction leads to characteristic level splittings of vibrational molecular lines which we directly observe via photoassociation spectroscopy. We benefit from the fact that molecular states dominated by resonant $p$-wave interaction are particularly sensitive to the spin-orbit interaction. Our work paves…
The level structure of negative-ions near the electron detachment limit dictates the low-energy scattering of an electron with the parent neutral atom. We demonstrate that a single ultracold atom bound inside a Rydberg orbit forming an ultralong-range Rydberg molecule provides an atomic-scale system which is highly sensitive to electron-neutral scattering and thus allows for detailed insights into the underlying near-threshold anion states. Our measurements reveal the so far unobserved fine structure of the $^3P_J$ triplet of Rb$^-$ and allow us to extract parameters of the associated $p$-wave…
We report the production of a high phase-space density mixture of $^{87}$Rb and $^{133}$Cs atoms in a levitated crossed optical dipole trap as the first step towards the creation of ultracold RbCs molecules via magneto-association. We present a simple and robust experimental setup designed for the sympathetic cooling of $^{133}$Cs via interspecies elastic collisions with $^{87}$Rb. Working with the $|F=1, m_F=+1 >$ and the $|3, +3 >$ states of $^{87}$Rb and $^{133}$Cs respectively, we measure a high interspecies three-body inelastic collision rate $\sim 10^{-25}-10^{-26} \rm{cm}^{6}\rm{s}^{-1}…
We explore the electronic structure of ultralong-range pentaatomic Rydberg molecules from a merger of a Rydberg atom and two ground state heteronuclear diatomic molecules. Our focus is on the interaction of Rb($23s$) and Rb($n=20$, $l\ge 3$) Rydberg states with ground and rotationally excited KRb diatomic polar molecules. For symmetric and asymmetric configurations of the pentaatomic Rydberg molecule, we investigate the metamorphosis of the Born-Oppenheimer potential curves, essential for the binding of the molecule, with varying distance from the Rydberg core and analyze the alignment and ori…
We present photo-excitation of ultra-long-range Rydberg molecules as a probe of spatial correlations in quantum gases. Rydberg molecules can be created with well-defined internuclear spacing, set by the radius of the outer lobe of the Rydberg electron wavefunction $R_n$. By varying the principal quantum number $n$ of the target Rydberg state, the molecular excitation rate can be used to map the pair-correlation function of the trapped gas $g^{(2)}(R_n)$. We demonstrate this with ultracold Sr gases and probe pair-separation length scales ranging from $R_n = 1400 - 3200$ $a_0$, which are on the …
We study properties of two different atoms at a single optical lattice site at a heteronuclear atomic Feshbach resonance. We calculate the energy spectrum, the efficiency of rf association and the lifetime as a function of magnetic field and compare the results with the experimental data obtained for K-40 and Rb-87 [C. Ospelkaus et al., Phys. Rev. Lett. 97, 120402 (2006)]. We treat the interaction in terms of a regularized delta function pseudopotential and consider the general case of particles with different trap frequencies, where the usual approach of separating center-of-mass and relative…
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…
We propose an experimentally realizable scheme to produce triatomic ultralong-range Rydberg molecules (TURM), formed in ultracold KRb traps. A near resonant coupling of the non-zero quantum defect Rydberg levels with the KRb molecule in N=0 and N=2 rotational levels, is engineered which exploits the unique Rydberg electron-molecule anisotropic dipole interaction. This near resonant coupling enhances the TURM binding and produces favorable Franck-Condon factors. Schemes for both postassium and rubidium excitations are demonstrated.
We explore the electronic structure and rovibrational properties of an ultralong-range triatomic Rydberg molecule formed by a Rydberg atom and a ground state heteronuclear diatomic molecule. We focus here on interaction of Rb($27s$) Rydberg atom with KRb($N=0$) diatomic polar molecule. There's significant electronic hybridization of Rb($n=24$, $l\ge 3$) degenerate manifold. The polar diatomic molecule is allowed to rotate in the electric fields generated by the Rydberg electron and core as well as an external field. We investigate the metamorphosis of the Born-Oppenheimer potential curves, ess…
We report the production of ultracold heteronuclear 7Li85Rb molecules in excited electronic states by photoassociation (PA) of ultracold 7Li and 85Rb atoms. PA is performed in a dual-species 7Li-85Rb magneto-optical trap (MOT) and the PA resonances are detected using trap loss spectroscopy. We identify several strong PA resonances below the Li (2s 2S1/2) + Rb (5p 2P3/2) asymptote and experimentally determine the long range C6 dispersion coefficients. We find a molecule formation rate (P_LiRb) of 3.5x10^7 s^-1 and a PA rate coefficient (K_PA) of 1.3x10^-10 cm^3/s, the highest among heteronuclea…
Ultracold Rydberg molecules have been extensively studied both theoretically and ex-perimentally. Here the authors review the recent realizations of various ultralong-range Rydberg molecules and macrodimers, and explore their potential for current and future applications in spectroscopy, few- and many-body interactions and quantum information processing.
Vibrational properties of ultralong Rydberg Cs$_2$ molecules are investigated on corresponding potential curves obtained by perturbation theory. The Rydberg Cs$_2$ molecules are associated by a Rydberg Cs($nS/nP$) atom $(n=30-70)$ and a ground state Cs($6s$) atom. The starting point for the perturbation treatment of corresponding Rydberg molecular potential curves is to generate accurate atomic Rydberg states from realistic {\it ab initio} effective core potential. The calculated results have similar characteristics with available experimental and theoretical investigations on Rydberg Rb$_2$ m…
We calculate vibrational spectra of ultralong-range Cs(32p) Rydberg molecules which form in an ultracold gas of Cs atoms. We account for the partial-wave scattering of the Rydberg electrons from the ground Cs perturber atoms by including the full set of spin-resolved ${}^{1,3}S_J$ and ${}^{1,3}P_J$ scattering phase shifts, and allow for the mixing of singlet (S=0) and triplet (S=1) spin states through Rydberg electron spin-orbit and ground electron hyperfine interactions. Excellent agreement with observed data in Saßmannshausen et al. [Phys. Rev. Lett. 113, 133201(2015)] in line positions and …
We present a novel binding mechanism where a neutral Rydberg atom and an atomic ion form a molecular bound state at large internuclear distance. The binding mechanism is based on Stark shifts and level crossings which are induced in the Rydberg atom due to the electric field of the ion. At particular internuclear distances between Rydberg atom and ion, potential wells occur which can hold atom-ion molecular bound states. Apart from the binding mechanism we describe important properties of the long-range atom-ion Rydberg molecule, such as its lifetime and decay paths, its vibrational and rotati…
The internal electric field of a Rydberg atom electron can bind a polar molecule to form a giant ultralong-range stable polyatomic molecule. Such molecules not only share their properties with Rydberg atoms, they possess huge permanent electric dipole moments and in addition allow for coherent control of the polar molecule orientation. In this work, we include additional Rydberg manifolds which couple to the nearly degenerate set of Rydberg states employed in [S. T. Rittenhouse and H. R. Sadeghpour, Phys. Rev. Lett. 104, 243002 (2010)]. The coupling of a set of $(n+3)s$ Rydberg states with the…
We show that the excitation of long-range Rydberg molecules in a three-dimensional optical lattice can be used as a position- and time-sensitive probe of the site occupancy in the system. To this end, we detect the ions which are continuously generated by the decay of the formed Rydberg molecules. While a superfluid gas shows molecule formation for all parameters, a Mott insulator with $n=1$ filling reveals a strong suppression of the number of formed molecules. In the limit of weak probing, the technique can be used to probe the superfluid to Mott-insulator transition in real-time. Our method…
We propose an experiment to demonstrate a novel blockade mechanism caused by long-range anisotropic interactions in an ultracold dipolar gas composed of the recently observed "butterfly" Rydberg molecules. At the blockade radius, the strong intermolecular interaction between two adjacent molecules shifts their molecular states out of resonance with the photoassociation laser, preventing their simultaneous excitation. When the molecules are prepared in a quasi-one-dimensional (Q1D) trap, the interaction's strength can be tuned via a weak external field. The molecular density thus depends strong…
We explore the external electric field control of a species of ultralong-range molecules that emerge from the interaction of a ground state polar molecule with a Rydberg atom. The external field mixes the Rydberg electronic states and therefore strongly alters the electric field seen by the polar diatomic molecule due to the Rydberg electron. As a consequence, the adiabatic potential energy curves responsible for the molecular binding can be tuned in such a way that an intersection with neighboring curves occurs. The latter leads to admixture of s-wave character in the Rydberg wave function an…
We study the impact of Rydberg molecule formation on the storage and retrieval of Rydberg polaritons in an ultracold atomic medium. We observe coherent revivals appearing in the retrieval efficiency of stored photons that originate from simultaneous excitation of Rydberg atoms and Rydberg molecules in the system with subsequent interference between the possible storage paths. We show that over a large range of principal quantum numbers the observed results can be described by a two-state model including only the atomic Rydberg state and the Rydberg dimer molecule state. At higher principal qua…
We predict that ultralong-range Rydberg bi-molecules form in collisions between polar molecules in cold and ultracold settings. The collision of $Λ$-doublet nitric oxide (NO) with long-lived Rydberg NO($nf$, $ng$) molecules forms ultralong-range Rydberg bi-molecules with GHz energies and kilo-Debye permanent electric dipole moments. The Hamiltonian includes both the anisotropic charge-molecular dipole interaction and the electron-NO scattering. The rotational constant for the Rydberg bi-molecules is in the MHz range, allowing for microwave spectroscopy of rotational transitions in Rydberg bi-m…
We study the possibility to use interaction between a polar molecule in the ground electronic and vibrational state and a Rydberg atom to construct two-qubit gates between molecular qubits and to coherently control molecular states. A polar molecule within the electron orbit in a Rydberg atom can either shift the Rydberg state, or form Rydberg molecule. Both the atomic shift and the Rydberg molecule states depend on the initial internal state of the polar molecule, resulting in molecular state dependent van der Waals or dipole-dipole interaction between Rydberg atoms. Rydberg atoms mediated in…
We propose a scheme to realize a heavy Rydberg system (HRS), a bound pair of oppositely charged ions, from a gas of ultracold atoms. The intermediate step to achieve large internuclear separations is the creation of a unique class of ultra-long-range Rydberg molecules bound in a stairwell potential energy curve. Here, a ground-state atom is bound to a Rydberg atom in an oscillatory potential emerging due to attractive singlet $p$-wave electron scattering. The utility of our approach originates in the large electronic dipole transition element between the Rydberg- and the ionic molecule, while …
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…
It is common knowledge that atoms can form molecules if they attract each other. Here, we show that it is possible to create molecules where bound states of the atoms are not the result of attractive interactions but have the topological origin. That is, the bound states of the atoms correspond to the topologically protected edge states of a topological model. Such topological molecules can be realized if the interaction strength between ultra-cold atoms is properly modulated in time. A similar mechanism allows one to realize topologically protected localization of an electron on a classical o…
The formation of ultralong-range Rydberg molecules is a result of the attractive interaction between Rydberg electron and polarizable ground state atom in an ultracold gas. In the nondegenerate case the backaction of the polarizable atom on the electronic orbital is minimal. Here we demonstrate, how controlled degeneracy of the respective electronic orbitals maximizes this backaction and leads to stronger binding energies and lower symmetry of the bound dimers. Consequently, the Rydberg orbitals hybridize due to the molecular bond.
We predict the existence of a class of ultracold giant molecules formed from trapped ultracold Rydberg atoms and polar molecules. The interaction which leads to the formation of such molecules is the anisotropic charge-dipole interaction ($a/R^2$). We show that prominent candidate molecules such as KRb and deuterated hydroxyl (OD) should bind to Rydberg rubidium atoms, with energies $E_b\simeq 5-25$ GHz at distances $R\simeq 0.1-1 \ μ$m. These molecules form in double wells, mimicking chiral molecules, with each well containing a particular dipole orientation. We prepare a set of correlated dr…
We investigate polyatomic ultralong-range Rydberg molecules consisting of three ground state atoms bound to a Rydberg atom via $s$- and $p$-wave interactions. By employing the finite basis set representation of the unperturbed Rydberg electron Green's function we reduce the computational effort to solve the electronic problem substantially. This method is subsequently applied to determine the potential energy surfaces of triatomic systems in electronic $s$- and $p$-Rydberg states. Their molecular geometry and resulting vibrational structure are analyzed within an adiabatic approach that separa…
Observation of resonant monopole-dipole energy transfer between Rydberg atoms and polar molecules
University College London（伦敦大学学院）；Department of Physics, Harvard University（哈佛大学物理系）；Instituto Carlos I de Física Teórica y Computacional, and Departamento de Física Atómica, Molecular y Nuclear, Universidad de Granada（格拉纳达大学理论计算物理卡洛斯一世研究所及原子、分子和核物理系）；Department of Physics and Astronomy, University College London（伦敦大学学院物理与天文系）
The lifetimes of the lower-lying vibrational states of ultralong-range strontium Rydberg molecules comprising one ground-state 5s2 1S0 atom and one Rydberg atom in the 5s38s 3S1 state are reported. The molecules are created in an ultracold gas held in an optical dipole trap and their numbers determined using field ionization, the product electrons being detected by a microchannel plate. The measurements show that, in marked contrast to earlier measurements involving rubidium Rydberg molecules, the lifetimes of the low-lying molecular vibrational states are very similar to those of the parent R…
We report on the formation of ultralong-range Rydberg D-state molecules via photoassociation in an ultracold cloud of rubidium atoms. By applying a magnetic offset field on the order of 10 G and high resolution spectroscopy, we are able to resolve individual rovibrational molecular states. A full theory, using the Born-Oppenheimer approximation including s- and p-wave scattering, reproduces the measured binding energies. The calculated molecular wavefunctions show that in the experiment we can selectively excite stationary molecular states with an extraordinary degree of alignment or anti-alig…
We observe long-range homonuclear diatomic $nD$ Rydberg molecules photoassociated out of an ultracold gas of $^{87}$Rb atoms for 34$\le n \le$40. The measured ground-state binding energies of $^{87}$Rb$(nD-5S_{1/2})$ molecular states are larger than those of their $^{87}$Rb$(nS-5S_{1/2})$ counterparts, showing the dependence of the molecular bond on the angular momentum of the Rydberg atom. We exhibit the transition of $^{87}$Rb$(nD-5S_{1/2})$ molecules from a molecular-binding-dominant regime at low $n$ to a fine-structure-dominant regime at high $n$ [akin to Hund's cases (a) and (c), respect…
We present a new mechanism contributing to the detection of photoassociated long-range Rydberg molecules via pulsed-field ionization: ionic products, created by the decay of a long-range Rydberg molecule, modify the excitation spectrum of surrounding ground-state atoms and facilitate the excitation of further atoms into Rydberg states by the photoassociation light. Such an ion-mediated excitation mechanism has been previously called "Coulomb anti-blockade". Pulsed-field ionisation typically doesn't discriminate between the ionization of a long-range Rydberg molecule and an isolated Rydberg ato…
Long-range metastable molecules consisting of two cesium atoms in high Rydberg states have been observed in an ultracold gas. A sequential three-photon two-color photoassociation scheme was employed to form these molecules in states which correlate to $np(n+1)s$ dissociation asymptotes. Spectral signatures of bound molecular states are clearly resolved at the positions of avoided crossings between long-range van der Waals potential curves. The experimental results are in agreement with simulations based on a detailed model of the long-range multipole-multipole interactions of Rydberg-atom pair…
We investigate the electronic structure of a triatomic Rydberg molecule formed by a Rydberg atom and two neutral ground-state atoms. Taking into account the $s$-wave and $p$-wave interactions we perform electronic structure calculations and analyze the adiabatic electronic potentials evolving from the Rb$(n=35, l\ge 3)$ Rydberg degenerate manifold. We hereby focus on three different classes of geometries of the Rydberg molecules, including symmetric, asymmetric and planar configurations. The metamorphosis of these potential energy surfaces in the presence of an external electric field is explo…
