Comparison of precision frequency measurements to quantum electrodynamics (QED) predictions for Rydberg states of hydrogen-like ions can yield information on values of fundamental constants and test theory. With the results of a calculation of a key QED contribution reported here, the uncertainty in the theory of the energy levels is reduced to a level where such a comparison can yield an improved value of the Rydberg constant.
We report on the observation of interactions between ultracold Rydberg atoms and ions in a Paul trap. The rate of observed inelastic collisions, which manifest themselves as charge transfer between the Rydberg atoms and ions, exceeds that of Langevin collisions for ground state atoms by about three orders of magnitude. This indicates a huge increase in interaction strength. We study the effect of the vacant Paul trap's electric fields on the Rydberg excitation spectra. To quantitatively describe the exhibited shape of the ion loss spectra, we need to include the ion-induced Stark shift on the …
The triatomic hydrogen ion (H$_3^+$) has spurred tremendous interest in astrophysics in recent decades, and Rydberg states of H$_3$ have also maintained an important role for understanding H$_3^+$ experiments. In a previous study [J. Chem. Phys. \textbf{133}, 234302 (2010)], radiative transitions between neutral H$_3$ Rydberg states were calculated at wavelengths near 7 microns, and could be compared with mid-infrared laser lines observed in hydrogen/rare gas discharges. The present study extends the investigation to wavelengths near 10 -- 13 microns. Rydberg states of D$_3$ are also treated.
The nature of the theory of circular Rydberg states of hydrogenlike ions allows highly-accurate predictions to be made for energy levels. In particular, uncertainties arising from the problematic nuclear size correction which beset low angular-momentum states are negligibly small for the high angular-momentum states. The largest remaining source of uncertainty can be addressed with the help of quantum electrodynamics (QED) calculations, including a new nonperturbative result reported here. More stringent tests of theory and an improved determination of the Rydberg constant may be possible if p…
We present a Rydberg hydrogen beamline developed to commission techniques of stimulated deexcitation for application in antihydrogen experiments at CERN's Antiproton Decelerator. The stimulation of spontaneous decay is a key technology to enhance the number of ground-state anti-atoms available in a beam toward precision spectroscopy and gravity measurements.
We investigate the Rydberg states generation of Hydrogen atoms with intense laser pulses, by solving the time-dependent Schrödinger equation and by means of classical trajectory monte-carlo simulations. Both linearly polarized multi-cycle pulses and pairs of optical half cycle pulses are used. Comparisons between these methods show that both the Coulomb force and initial lateral momentum, which have effects on the $n$-distribution and $l$-distribution of the population of excited states, are important in the generation of Rydberg states.
We report a theoretical scheme using a B-spline basis set to improve the poor computational accuracy of circular Rydberg states of hydrogen atoms in the intermediate magnetic field. This scheme can produce high accuracy energy levels and valid for an arbitrary magnetic field. Energy levels of hydrogen are presented for circular Rydberg states with azimuthal quantum numbers $|m|$ = 10 - 70 as a function of magnetic field strengths ranging from zero to 2.35 $\times$ 10$^9$ T. The variation of spatial distributions of electron probability densities with magnetic field strengths is discussed and c…
Triple photoionization of Xe3+, Xe4+ and Xe5+ ions has been studied in the energy range 670-750 eV, including the 3d ionization threshold. The photon-ion merged-beam technique was used at a synchrotron light source to measure the absolute photoionization cross sections. These cross sections exhibit a progressively larger number of sharp resonances as the ion charge state is increased. This clearly visualizes the re-ordering of the $ε$f continuum into a regular series of (bound) Rydberg orbitals as the ionic core becomes more attractive. The energies and strengths of the resonances are extracte…
We present a method for measuring the polarizability of Rydberg ions confined in the harmonic potential of a Paul trap. For a highly excited electronic state, the coupling between the electronic wave function and the trapping field modifies the excitation probability depending on the motional state of the ion. This interaction strongly depends on the polarizability of the excited state and manifests itself in the state-dependent secular frequencies of the ion. We initialize a single trapped $^{40}$Ca$^+$ ion from the motional ground state into coherent states with $|α|$ up to 12 using electric…
In this chapter, we present an overview of experiments with trapped Rydberg ions and outline the advantages and challenges of developing applications of this new platform for quantum computing, sensing and simulation. Trapped Rydberg ions feature several important properties, unique in their combination: they are tightly bound in a harmonic potential of a Paul trap, in which their internal and external degrees of freedom can be controlled in a precise fashion. High fidelity state preparation of both internal and motional states of the ions has been demonstrated, and the internal states have be…
We introduce a scheme to entangle Rydberg ions in a linear ion crystal, using the high electric polarizability of the Rydberg electronic states in combination with mutual Coulomb coupling of ions that establishes common modes of motion. After laser-initialization of ions to a superposition of ground- and Rydberg-state, the entanglement operation is driven purely by applying a voltage pulse that shuttles the ion crystal back and forth. This operation can achieve entanglement on a sub-$μ$s timescale, more than two orders of magnitude faster than typical gate operations driven by continuous-wave …
We provide a detailed theoretical and conceptual study of a planned experiment to excite Rydberg states of ions trapped in a Paul trap. The ultimate goal is to exploit the strong state dependent interactions between Rydberg ions to implement quantum information processing protocols and to simulate the dynamics of strongly interacting spin systems. We highlight the promises of this approach when combining the high degree of control and readout of quantum states in trapped ion crystals with the novel and fast gate schemes based on interacting giant Rydberg atomic dipole moments. We discuss antic…
We demonstrate the excitation of ions to the Rydberg state $22F$ by vacuum ultraviolet radiation at a wavelength of $123\,\text{nm}$ combined with the coherent manipulation of the optical qubit transition in $^{40}\text{Ca}^+$. With a tightly focused beam at $729\,\text{nm}$ wavelength we coherently excite a single ion from a linear string into the metastable $3D_{5/2}$ state before a VUV pulse excites it to the Rydberg state. In combination with ion shuttling in the trap, we extend this approach to the addressed excitation of multiple ions. The coherent initialization as well as the addressed…
We present a theoretical analysis of the implementation of an entangling quantum gate between two trapped Ca$^+$ ions which is based on the dipolar interaction among ionic Rydberg states. In trapped ions the Rydberg excitation dynamics is usually strongly affected by mechanical forces due to the strong couplings between electronic and vibrational degrees of freedom in inhomogeneous electric fields. We demonstrate that this harmful effect can be overcome by using dressed states that emerge from the microwave coupling of nearby Rydberg states. At the same time these dressed states exhibit long r…
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 theoretically study trapped ions that are immersed in an ultracold gas of Rydberg-dressed atoms. By off-resonant coupling on a dipole-forbidden transition, the adiabatic atom-ion potential can be made repulsive. We study the energy exchange between the atoms and a single trapped ion and find that Langevin collisions are inhibited in the ultracold regime for these repulsive interactions. Therefore, the proposed system avoids recently observed ion heating in hybrid atom-ion systems caused by coupling to the ion's radio frequency trapping field and retains ultracold temperatures even in the pr…
The quadrupole interaction between the Rydberg electronic states of a Rydberg ion and the radio frequency electric field of the ion trap is analyzed. Such a coupling is negligible for the lowest energy levels of a trapped ion but it is important for a trapped Rydberg ion due to its large electric dipole moment. This coupling cannot be neglected by the standard rotating-wave approximation because it is comparable to the frequency of the trapping electric field. We investigate the effect of the quadrupole coupling by performing a suitable effective representation of the Hamiltonian. For a single…
Energy-conserving, angular momentum-changing collisions between protons and highly excited Rydberg hydrogen atoms are important for precise understanding of atomic recombination at the photon decoupling era, and the elemental abundance after primordial nucleosynthesis. Early approaches to $\ell$-changing collisions used perturbation theory for only dipole-allowed ($Δ\ell=\pm 1$) transitions. An exact non-perturbative quantum mechanical treatment is possible, but it comes at computational cost for highly excited Rydberg states. In this note we show how to obtain a semi-classical limit that is a…
Anomalously enhanced lifetimes of low angular momentum Rydberg states in singly charged alkaline-earth metal ions
Institut für Theoretische Physik and Center for Integrated Quantum Science and Technology, Universität Tübingen（蒂宾根大学理论物理研究所与集成量子科学与技术中心）；School of Physics and Astronomy and Centre for the Mathematics and Theoretical Physics of Quantum Non-Equilibrium Systems, The University of Nottingham（诺丁汉大学物理与天文学学院及量子非平衡系统数学与理论物理中心）
Trapped Rydberg ions are a promising new system for quantum information processing. They have the potential to join the precise quantum operations of trapped ions and the strong, long-range interactions between Rydberg atoms. Technically, the ion trap will need to stay active while exciting the ions into the Rydberg state, else the strong Coulomb repulsion will quickly push the ions apart. Thus, a thorough understanding of the trap effects on Rydberg ions is essential for future applications. Here we report the observation of two fundamental trap effects. First, we investigate the interaction …
Precision spectroscopy of the fine and hyperfine structures of high molecular Rydberg-Stark states: Metrology of molecular hydrogen ions
ETH Zürich（苏黎世联邦理工学院）；Vrije Universiteit Amsterdam（阿姆斯特丹自由大学）；Université Paris-Saclay（巴黎萨克雷大学）；Centre National de la Recherche Scientifique（法国国家科学研究中心）
We propose a hardware architecture and protocol for connecting many local quantum processors contained within an optical cavity. The scheme is compatible with trapped ions or Rydberg arrays, and realizes teleported gates between any two qubits by distributing entanglement via single-photon transfers through a cavity. Heralding enables high-fidelity entanglement even for a cavity of moderate quality. For processors composed of trapped ions in a linear chain, a single cavity with realistic parameters successfully transfers photons every few $μ$s, enabling the any-to-any entanglement of 20 ion ch…
The theoretical treatment of Rydberg states in one-electron ions is facilitated by the virtual absence of the nuclear-size correction, and fundamental constants like the Rydberg constant may be in the reach of planned high-precision spectroscopic experiments. The dominant nuclear effect that shifts transition energies among Rydberg states therefore is due to the nuclear mass. As a consequence, spectroscopic measurements of Rydberg transitions can be used in order to precisely deduce nuclear masses. A possible application of this approach to the hydrogen and deuterium, and hydrogen-like lithium…
Generating quantum entanglement in large systems on time scales much shorter than the coherence time is key to powerful quantum simulation and computation. Trapped ions are among the most accurately controlled and best isolated quantum systems with low-error entanglement gates operated via the vibrational motion of a few-ion crystal within tens of microseconds. To exceed the level of complexity tractable by classical computers the main challenge is to realise fast entanglement operations in large ion crystals. The strong dipole-dipole interactions in polar molecule and Rydberg atom systems all…
Conical intersections between electronic potential energy surfaces are paradigmatic for the study of non-adiabatic processes in the excited states of large molecules. However, since the corresponding dynamics occurs on a femtosecond timescale, their investigation remains challenging and requires ultrafast spectroscopy techniques. We demonstrate that trapped Rydberg ions are a platform to engineer conical intersections and to simulate their ensuing dynamics on larger length and time scales of the order of nanometers and microseconds, respectively; all this in a highly controllable system. Here,…
We theoretically investigate trapped ions interacting with atoms that are coupled to Rydberg states. The strong polarizabilities of the Rydberg levels increases the interaction strength between atoms and ions by many orders of magnitude, as compared to the case of ground state atoms, and may be mediated over micrometers. We calculate that such interactions can be used to generate entanglement between an atom and the motion or internal state of an ion. Furthermore, the ion could be used as a bus for mediating spin-spin interactions between atomic spins in analogy to much employed techniques in …
We measure strong radio-frequency (RF) electric fields using rubidium Rydberg atoms prepared in a room-temperature vapor cell as field sensors. Electromagnetically induced transparency is employed as an optical readout. We RF-modulate the 60$S_{1/2}$ and 58$D_{5/2}$ Rydberg states with 50~MHz and 100~MHz fields, respectively. For weak to moderate RF fields, the Rydberg levels become Stark-shifted, and sidebands appear at even multiples of the driving frequency. In high fields, the adjacent hydrogenic manifold begins to intersect the shifted levels, providing rich spectroscopic structure suitab…
It has been argued that precise measurements of optical transition frequencies between Rydberg states of hydrogen-like ions could be used to obtain an improved value of the Rydberg constant and even to test Quantum Electrodynamics (QED) theory more accurately, by avoiding the uncertainties about the proton radius. Motivated by this perspective, we investigate the influence of the gravitational interaction on the energy levels of Hydrogen-like ions in Rydberg states within the context of the braneworld models. As it is known, in this scenario, the gravitational interaction is amplified in short…
The charge transfer (ionization) of hydrogen Rydberg atoms (principal quantum number $n=25-34$) incident at a Cu(100) surface is investigated. Unlike fully metallic surfaces, where the Rydberg electron energy is degenerate with the conduction band of the metal, the Cu(100) surface has a projected bandgap at these energies, and only discrete image states are available through which charge transfer can take place. Resonant enhancement of charge transfer is observed at hydrogen principal quantum numbers for which the Rydberg energy matches the energy of one of the image states. The integrated sur…
Trapped Rydberg ions represent a flexible platform for quantum simulation and information processing which combines a high degree of control over electronic and vibrational degrees of freedom. The possibility to individually excite ions to high-lying Rydberg levels provides a system where strong and long-range interactions between pairs of excited ions can be engineered and tuned via external laser fields. We show that the coupling between Rydberg pair interactions and collective motional modes gives rise to effective long-range multi-body interactions, consisting of two, three, and four-body …
Theoretical calculations of the Lamb shift provide the basis required for the determination of the Rydberg constant from spectroscopic measurements in hydrogen. The recent high-precision determination of the proton charge radius drastically reduced the uncertainty in the hydrogen Lamb shift originating from the proton size. As a result, the dominant theoretical uncertainty now comes from the two- and three-loop QED effects, which calls for further advances in their calculations. We review the present status of theoretical calculations of the Lamb shift in hydrogen and light hydrogen-like ions …
The static dipole polarizability for the hydrogen molecular ions H$_2^+$, HD$^+$, and D$_2^+$ are calculated. These new data for polarizability takes into account the leading order relativistic corrections to the wave function of the three-body system resulted from the Breit-Pauli Hamiltonian of $mα^4$ order. Our study covers a wide range of rotational ($L=0-5$) and vibrational ($v=0-10$) states, which are of practical interest for precision spectroscopy of the hydrogen molecular ions.
We consider the role of high-lying Rydberg states of simple atomic systems such as $^1$H in setting constraints on physics beyond the Standard Model. We obtain highly accurate bound states energies for a hydrogen atom in the presence of an additional force carrier (the energy levels of the Hellmann potential). These results show that varying the size and shape of the Rydberg state by varying the quantum numbers provides a way to probe the range of new forces. By combining these results with the current state-of-the-art QED corrections, we determine a robust global constraint on new physics tha…
In this work, analytical formulas for the static multipole polarizabilities of hydrogen-like ions are derived by using the analytical wave functions and the reduced Green function and by applying a numerical fitting procedure. Our results are then applied to the studies of blackbody radiation shifts to atomic energy levels at different temperatures. Our analytical results can be served as a benchmark for other theoretical methods.
Polarization properties of the photons emitted in the two-photon decay of hydrogen-like ions are studied within the framework of the density matrix and second-order perturbation theory. In particular, we derive the polarization correlation function that gives the probability of the (two-photon) coincidence measurement performed by polarization-sensitive detectors. Detailed calculations of this function are performed for the $2s_{1/2} \to 1s_{1/2}$ transition in neutral hydrogen as well as Xe$^{53+}$ and U$^{91+}$ ions. The obtained results allow us to understand the influence of relativistic a…
One- and two-photon transitions in the hydrogen atom are analytically evaluated in the absence and in the presence of an external electric field. The emission probabilities are different for the hydrogen and anti-hydrogen atoms due to the existence of contributions, linear in electric field. The magnitude of these contributions is evaluated within the nonrelativistic limit. The Coulomb Green function method is applied. Different nonrelativistic "forms" for the decay probabilities in combination with different gauge choices are considered. The three-photon E1E1E1 2p-1s transition probability is…
Thin metallic films have a 1D quantum well along the surface normal direction, which yields particle-in-a-box style electronic quantum states. However the quantum well is not infinitely deep and the wavefunctions of these states penetrate outside the surface where the electron is bound by its own image-charge attraction. Therefore a series of discrete, vacant states reach out from the thin film into the vacuum increasing the probability of electron transfer from an external atom or molecule to the thin film, especially for the resonant case where the quantum well energy matches that of the Ryd…
We develop {\it ab initio} relativistic QED theory for elastic electron scattering on hydrogen-like highly charged ions for impact energies where, in addition to direct (Coulomb) scattering, the process can also proceed via formation and consequent Auger decay of autoionizing states of the corresponding helium-like ions. Even so the primary goal of the theory is to treat electron scattering on highly charged ions, a comparison with experiment shows that it can also be applied for relatively light ions covering thus a very broad range of the scattering systems. Using the theory we performed cal…
Two--photon decay of hydrogen--like ions is studied within the framework of second--order perturbation theory, based on relativistic Dirac's equation. Special attention is paid to the effects arising from the summation over the negative--energy (intermediate virtual) states that occurs in such a framework. In order to investigate the role of these states, detailed calculations have been carried out for the $2s_{1/2} - 1s_{1/2}$ and $2p_{1/2} - 1s_{1/2}$ transitions in neutral hydrogen H as well as for hydrogen--like xenon Xe$^{53+}$ and uranium U$^{91+}$ ions. We found that for a correct evalu…
Approximate scaling laws with respect to the nuclear charge are introduced for the time-dependent Dirac equation describing hydrogen-like ions subject to laser fields within the dipole approximation. In particular, scaling relations with respect to the laser wavelengths and peak intensities are discussed. The validity of the scaling relations is investigated for two-, three-, four-, and five-photon ionization of hydrogen-like ions with the nuclear charges ranging from $Z=1$ to $92$ by solving the corresponding time-dependent Dirac equations adopting the properly scaled laser parameters. Good a…
The possible use of high-resolution rovibrational spectroscopy of the hydrogen molecular ions H + 2 and HD + for an independent determination of several fundamental constants is analyzed. While these molecules had been proposed for metrology of nuclear-to-electron mass ratios, we show that they are also sensitive to the radii of the proton and deuteron and to the Rydberg constant at the level of the current discrepancies colloquially known as the proton size puzzle. The required level of accuracy, in the 10 --12 range, can be reached both by experiments, using Doppler-free two-photon spectrosc…
