Large Principal Quantum Numbers Research Articles

Dissociation of ultracold cesium Rydberg-ground molecules.

We report the experimental measurements of the decay rate of polar cesium nD5/2 - 6S1/2 Rydberg-ground molecules with a large principal quantum number range of 35 ≤ n ≤ 40. Rydberg molecules are prepared employing the method of two-photon photoassociation and the molecular (atomic) ions, due to autoionization (blackbody photoionization), are detected with a microchannel plate detector. The decay rate Γ of the vibrational ground state of the deep and shadow bound molecules for triplet (TΣ) and mixed singlet-triplet (S,TΣ) are measured by fitting the molecular population with the exponential function. Comparing with the parent atom, the decay rate of the polar Rydberg-ground molecule shows an obvious increase with a magnitude of a few μs. The possible dissociation mechanism of polar Rydberg-ground molecules including a collisional decay, blackbody induced decay, and coupling of adjacent Rydberg states and tunneling decay are discussed in detail. The theoretical model is induced to simulate the measurements, showing agreement.

Highly-excited Rydberg excitons in synthetic thin-film cuprous oxide

Cuprous oxide (hbox {Cu}{}_2hbox {O}) has recently emerged as a promising material in solid-state quantum technology, specifically for its excitonic Rydberg states characterized by large principal quantum numbers (n). The significant wavefunction size of these highly-excited states (proportional to n^2) enables strong long-range dipole-dipole (proportional to n^4) and van der Waals interactions (proportional to n^{11}). Currently, the highest-lying Rydberg states are found in naturally occurring hbox {Cu}_2hbox {O}. However, for technological applications, the ability to grow high-quality synthetic samples is essential. The fabrication of thin-film hbox {Cu}{}_2hbox {O} samples is of particular interest as they hold potential for observing extreme single-photon nonlinearities through the Rydberg blockade. Nevertheless, due to the susceptibility of high-lying states to charged impurities, growing synthetic samples of sufficient quality poses a substantial challenge. This study successfully demonstrates the CMOS-compatible synthesis of a hbox {Cu}{}_2hbox {O} thin film on a transparent substrate that showcases Rydberg excitons up to n = 8 which is readily suitable for photonic device fabrications. These findings mark a significant advancement towards the realization of scalable and on-chip integrable Rydberg quantum technologies.

Effects of the noninteger-cycle pulse and the initial phase on the Magnus approximation to study Rydberg atoms in intense laser fields

The Magnus expansion method is popular for the study of Rydberg atoms in intense laser fields. In such studies, the pulse length is usually set as an integer multiple of wavelength, at the same time, the initial phase of the laser pulse is usually set as zero, i.e., without considering the effect of the initial phase in the calculation. However, this will result in some items multiplied by zero. Then, contributions from these items will be lost. Here, we investigated the effects of the noninteger-cycle pulse and initial phase of the laser on the calculated transition probability of Rydberg atoms in intense laser fields. Our calculation results show that these effects are trivial when the nondipole approximation is adopted. In dipole approximation i.e., when the wavelength of the laser field exceeds the characteristic size of atomic or molecular orbitals, these effects are trivial only in the case of a long pulse duration and a large principal quantum number, however for ultrashort laser pulses (pulse duration that lasts less than five light cycles), these effects are evident.

Cold ion chemistry within a Rydberg-electron orbit: test of the spectator role of the Rydberg electron in the He(n) + CO → C(n′) + O + He reaction

Recently, a new method has been introduced to study ion-molecule reactions at very low collision energies, down to below k B ⋅ 1 K (Allmendinger et al 2016 ChemPhysChem 17 3596). To eliminate the acceleration of the ions by stray electric fields in the reaction volume, the reactions are observed within the orbit of a Rydberg electron with large principal quantum number n > 20. This electron is assumed not to influence the reaction taking place between the ion core and the neutral molecules. This assumption is tested here with the example of the He(n) + CO → C(n′) + O + He reaction, which is expected to be equivalent to the He+ + CO → C+ + O + He reaction, using a merged-beam approach enabling measurements of relative reaction rates for collision energies E coll in the range from 0 to about k B ⋅ 25 K with a collision-energy resolution of ∼k B ⋅ 200 mK at E coll = 0. In contrast to the other ion-molecule reactions studied so far with this method, the atomic ion product (C+) is in its electronic ground state and does not have rotational and vibrational degrees of freedom so that the corresponding Rydberg product [C(n′)] cannot decay by autoionization. Consequently, one can investigate whether the principal quantum number is effectively conserved, as would be expected in the spectator Rydberg-electron model. We measure the distribution of principal quantum numbers of the reactant He(n) and product C(n′) Rydberg atoms by pulsed-field ionization following initial preparation of He(n) in states with n values between 30 and 45 and observe that the principal quantum number of the Rydberg electron is conserved during the reaction. This observation indicates that the Rydberg electron is not affected by the reaction, from which we can conclude that it does not affect the reaction either. This conclusion is strengthened by measurements of the collision-energy-dependent reaction yields at n = 30, 35 and 40, which exhibit the same behavior, i.e. a marked decrease below E coll ≈ k B ⋅ 5 K.

Measuring the Electric Field Strength of Microwave Radiation at the Frequency of the Radiation Transition Between Rydberg States of Atoms 85Rb

The spectral characteristics of the resonance effect of the electromagnetic-induced transparency (EIT) of rubidium atomic vapors induced by intense radiation with a wavelength in the region from 479 to 486 nm in the presence of microwave radiation at a frequency of 1 to 300 GHz, which splits the energy of transition of the atom from the resonant 5P3/2 states into the Rydberg nD5/2 state, are determined. The magnitude of the splitting of the EIT peak is proportional to the electric field intensity of the microwave radiation. Simple approximation expressions are obtained for the numerical calculation of the transition amplitude between Rydberg nD5/2 and (n + 1)P3/2 states with large principal quantum numbers n. A setup has been developed for measuring the electric field intensity of microwave radiation based on measuring the frequency of splitting of the resonance of an electron microscope in the absorption spectrum of probe radiation.

Laser spectroscopy of pionic helium atoms.

Charged pions1 are the lightest and longest-lived mesons. Mesonic atoms are formed when an orbital electron in an atom is replaced by a negatively charged meson. Laser spectroscopy of these atoms should permit the mass and other properties of the meson to be determined with high precision and could place upper limits on exotic forces involving mesons (as has been done in other experiments on antiprotons2-9). Determining the mass of the π- meson in particular could help to place direct experimental constraints on the mass of the muon antineutrino10-13. However, laser excitations of mesonic atoms have not been previously achieved because of the small number of atoms that can be synthesized and their typically short (less than one picosecond) lifetimes against absorption of the mesons into the nuclei1. Metastable pionic helium (π4He+) is a hypothetical14-16 three-body atom composed of a helium-4 nucleus, an electron and a π- occupying a Rydberg state of large principal (n≈16) and orbital angular momentum (l≈n-1) quantum numbers. The π4He+ atom is predicted to have an anomalously long nanosecond-scale lifetime, which could allow laser spectroscopy to be carried out17. Its atomic structure is unique owing to the absence of hyperfine interactions18,19 between the spin-0 π- and the 4He nucleus. Here we synthesize π4He+ in a superfluid-helium target and excite the transition (n,l)=(17,16)→(17,15) of the π--occupied π4He+ orbital at anear-infrared resonance frequency of 183,760 gigahertz. The laser initiates electromagnetic cascade processes that end with the nucleus absorbing the π- and undergoing fission20,21. The detection of emerging neutron, proton and deuteron fragments signals the laser-induced resonance in the atom, thereby confirming the presence of π4He+. This work enables the use of theexperimental techniques of quantum opticsto study ameson.

The rule of radius averaging in hydrogen atom

According to quantum mechanics, electrons do not have a fixed position in an atom, and therefore orbitals have no definite radii. However, electrons have characteristic wave functions from which the radius of their orbits can be calculated or averaged. Depending on the average method, there are three most popular expressions for orbital radius, namely the average radius, the root mean square (rms) radius, and the most probable radius. Unfortunately, for hydrogen atom, none of those three radii is equal to the classical radius, even for large principal quantum numbers called the classical regime. Here, by using energy analysis, we propose a harmonic radius and show that the results well agree with the classical radius for each principal and orbital quantum numbers.

Interatomic interactions and thermally induced shifts and broadenings of energy levels of atoms in circular Rydberg states

Analytical expressions are obtained for the constants determining the energy of the long-range (at large distances exceeding the LeRoy radius RLR ≈ 4n2) polarisation interaction of the multipole electric moments of two atoms in identical Rydberg states with large principal (n) and maximum orbital (l) and magnetic (m) quantum numbers (|m| = l = n − 1). Asymptotic expansions in powers of n are found for the components of the van der Waals interaction tensor, which determine the dependence of the dispersion energy on the orientation of the interatomic axis. The spontaneous and thermally induced broadenings of the energy levels of circular states are represented analytically as functions of the principal quantum number and temperature. It is found that analytical formulae for the sum of spontaneous and thermally induced line widths in the region of high temperatures and large principal quantum numbers (assuming n3kBT >> 1) do not contain a temperature-independent contribution of the spontaneous part of the broadening. Closed analytical expressions are also obtained for the Farley − Wing function and for the n- and T-dependent corrections to the asymptotic behaviour of the thermally induced shift.

Two-body entanglement in a dilute gas of Rydberg atoms

Since the establishment of quantum mechanics, quantum entanglement has become one of the most important realms in quantum physics. On the one hand, it reflects some of the most fascinating features, such as quantum coherence, probability and non-locality and so on. On the other hand, it proves to be an indispensable resource of quantum information processing and quantum computation, which is considered to greatly promote the development of human science and technology. In the past decades, inspired by advances in quantum information theory and quantum physics, people have been searching for suitable systems with great enthusiasm to prepare the robust and manipulable quantum entanglement. Recently, Rydberg atoms have been considered to be a good candidate for many quantum information and quantum computation tasks. Compared with general neutral atoms, Rydberg atoms with large principal quantum number have several advantages in the quantum information and computation service. Firstly, they have finite lifetimes much larger than general neutral atoms, which indicates that the long-time entanglement between Rydberg atoms can be achieved. Secondly, due to the high-excitation level, Rydberg-excitation atoms have long-ranged dipole-dipole interaction much stronger than ground state atoms. This strong atomic interaction leads to the so-called blockade effect: when one atom is excited to Rydberg level, the excitation of the neighboring atoms will be strictly suppressed due to the energy shift induced by the strong atomic interaction. On the contrast, if the energy shift is compensated for by the detuning between the energy levels and the driven laser field, these atoms can be excited with higher probability simultaneously. These effects imply that Rydberg atoms provide an excellent platform for investigating the quantum information and quantum computation process, and many important achievements based on them have been achieved. Encouraged by these researches on entanglement and Rydberg atoms, in this paper, we study the steady-state and transient dynamical properties of two-body entanglement and the Rydberg-excitation properties in a dilute gas of Rydberg atoms, which can be represented by a tetrahedrally arranged interacting four-atom model. By solving numerically the master equation of four atoms involving Rydberg level, we investigate the higher-order Rydberg excitations and bipartite entanglement, which is estimated by concurrence. Our results show that the bipartite entanglement can only achieve its maximal value in the strongest dipole blockade regime rather than anti-blockade one (the high-order Rydberg excitations). Furthermore, the physical essence of quantum entanglement is analyzed theoretically in relevant regimes. Our work can naturally extend to more complicated atomic space structures, and might be treated as a good platform for fulfilling many quantum information tasks by employing the quantum entanglement.

Annulled van der Waals interaction and fast Rydberg quantum gates

A pair of neutral atoms separated by several microns and prepared in identical s-states of large principal quantum number experience a van der Waals interaction. If microwave fields are used to generate a superposition of s-states with different principal quantum numbers, a null point may be found at which a specific superposition state experiences no van der Waals interaction. An application of this novel Rydberg state in a quantum controlled-Z gate is proposed, which takes advantage of GHz rate transitions to nearby Rydberg states. A gate operation time in the tens of nanoseconds is predicted.

Electromagnetically induced transparency of a cesium Rydberg atom in weak radio-frequency field

Rydberg atoms are highly excited atoms with large principal quantum number n, big sizes (~n2) and long lifetimes (~n3). Rydberg atoms are very sensitive to an external field due to the large polarizabilities of Rydberg atoms (~n7). Electromagnetically induced transparency (EIT) of Rydberg atom provides an ideal method to detect Rydberg atoms without destroying atoms, and can be used to measure the external direct current and radio frequency (RF) field. In this paper, we study the EIT effect of a cesium ladder-type three-level atom involving Rydberg state exposed to a weak RF field. The ground state (6S1/2), the excited state (6P3/2) and Rydberg state (48D5/2) constitute the Rydberg three-level system, in which the probe laser couples 6S1/2(F=4)6P3/2(F'=5) transition, whereas the coupling laser scans across the 6P3/248D5/2 Rydberg transition. The coupling laser (510 nm laser, propagating in the z-axis direction and linear polarization in the y-axis direction) and the probe laser (852 nm laser, linear polarization in the y-axis direction) counter-propagate through a 50-mm-long cesium vapor cell at room temperature, yielding Rydberg EIT spectra. Rydberg EIT signal is detected as a function of the detuning of the coupling laser. When a weak RF (80 MHz) electric field polarized in the x-axis direction is applied to a pair of electrode plates located on both sides of the cesium cell, the EIT spectrum of Rydberg 48D5/2 shows the Stark splitting and the even order harmonic sidebands. The experimental results are analyzed by using the Floquet theory. The simulation results accord well with the experimentally measured results. Furthermore, we also investigate the influence of the self-ionization effect of Rydberg atom on the Stark spectrum by changing the RF frequency. We put forward a proposal to avoid the effect of ionization by placing electrode plates in the cesium cell. In the weak RF-field domain, mj=5/2 Stark line crosses mj=1/2, 3/2 sidebands, these cross points provide an antenna-free method of accurately calibrating the RF electric field based on Rydberg atoms.

Electric dipole polarizabilities of Rydberg states of alkali-metal atoms

Calculations of the static electric-dipole scalar and tensor polarizabilities are presented for two alkali atoms, Rb and Cs, for the $nS$, $nP_{1/2, 3/2}$, and $nD_{3/2, 5/2}$ states with large principal quantum numbers up to $n = 50$. The calculations are performed within an effective one-electron approximation, based on the Dirac-Fock Hamiltonian with a semi-empirical core-polarization potential. The obtained results are compared with those from a simpler semi-empirical approach and with available experimental data.

Spectrum, radial wave functions, and hyperfine splittings of the Rydberg states in heavy alkali-metal atoms

We calculate the bound state spectrum of the highly excited valence electron in the heavy alkali atoms solving the radial Schr\"odinger eigenvalue problem numerically with an accurate spectral collocation algorithm that applies also for a large principal quantum number $n\gg1$. As an effective single-particle potential we favor the reputable potential of Marinescu \emph{et al}., {[}Phys. Rev.A \textbf{49}, 982(1994){]}. Recent quasiclassical calculations of the quantum defect of the valence electron agree for orbital angular momentum $l=0,1,2,...$ overall remarkably well with the results of the numerical calculations, but for the Rydberg states of rubidium and also cesium with $l=3$ this agreement is less fair. The reason for this anomaly is that the potential acquires for $l=3$ deep inside the ionic core a tiny second classical region, thus invalidating a standard WKB calculation with two widely spaced turning points. Comparing then our numerical solutions of the radial Schr\"odinger eigenvalue problem with the uniform analytic WKB approximation of Langer we observe everywhere a remarkable agreement, apart from a tiny region around the inner turning point. With help of an ansatz proposed by Fock we obtain for the \emph{s}-states a second uniform analytic approximation to the radial wave function complementary to the WKB approximation of Langer, which is exact for $r\to0^{+}$. The value of the radial \emph{s}-wave function at $r=0$ is analytically found, thus validating the Fermi-Segr\`e formula for the magnetic dipole interaction constant $A_{n,j,0}^{\left(\mathrm{HFS}\right)}$.

Spin–charge separation of dark-state polaritons in a Rydberg medium

The propagation of light fields through a quasi one-dimensional cold atomic gas, exciting atomic Rydberg levels of large principal quantum number under conditions of electromagnetically induced transparency, can lead to a stable two-mode Luttinger liquid system. Atomic van der Waals interactions induce a coupling of bosonic field modes that display both photonic and atomic character, the Rydberg dark-state polaritons (RDPs). It is shown that by tunable control of the van der Waals coupling, the RDP may decouple into independent ‘spin’ and ‘charge’ fields which propagate at different speeds, analogous to spin–charge separation of electrons in a one-dimensional metal.

Electromagnetically induced transparency of Rydberg atoms in modulated laser fields

Rydberg atoms, with large principal quantum number n, have been widely investigated in recent years due to their peculiar properties, such as big sizes, long lifetimes and strong interactions with fields and other Rydberg atoms. Rydberg atoms are very sensitive to external fields due to their large polarizabilities scaling as n7.These make Rydberg atoms an ideal candidate for the quantum information, the many-body interaction, etc.In this work, we investigate the Rydberg atoms using electromagneticlly induced transparency (EIT) in a ladder three-level system. The EIT is a quantum interference effect between two excitation path-ways driven by two laser fields. The main idea is performed in a room temperature cesium vapor cell, where the probe laser frequency is modulated. The ground state (6P1/2), excited state (6P3/2), and Rydberg state (nS1/2) constitute a Rydberg three-level system, in which the probe laser is fixed to the 6S1/2 (F = 4)6P3/2 (F = 5) transition by saturated absorption spectrum technique, whereas the coupling laser is scanned across the 6P3/249S1/2 transition. We detect the demodulated EIT signal with the lock-in amplifier (SR830). The modulated EIT signal shows a two-peak structure. The measured spacing between two peaks increases with the frequency detuning, caused by the modulation amplitude, and half the spacing between the peak-to-peak is nearly 1.67 times the modulation amplitude of the probe laser; the measured result shows that the splitting is independent of the modulation frequency. The experimental results are in agreement with the theoretical calculations. The results in our work can be used for real-time monitoring of the laser-line profiles and the fluctuation of laser frequency.

Two-photon radio frequency spectroscopy of 49S Rydberg state

Rydberg atoms, with large principal quantum number, exhibit certain properties, such as long lifetimes and strong interactions with fields and other atoms, which have been extensively investigated recently. One of the properties is the electromagnetically induced transparency (EIT) of Rydberg ladder system, which can be used to measure the radio frequency (RF) field with high sensitivity. In this paper, we investigate the quantum coherent effect of cesium Rydberg atom in a three-level ladder system involving the ground state (6S1/2), the excited state (6P3/2) and 49S1/2 Rydberg state in room temperature vapor cell. The probe laser (852 nm) drives the transition of 6S1/2(F=4)→6P3/2(F'=5), while the coupling laser (510 nm) couples the Rydberg transition of 6P3/2 (F'=5)→nS1/2. A typical electromagnetically induced transparency spectrum is obtained when the weak probe laser is scanned through the transition of 6S1/2(F=4)→6P3/2(F'=5) and the coupling laser tuning to Rydberg transition. The two-photon RF spectra are observed when the RF field with a frequency of ～16.9 GHz couples the Rydberg transition of 49S1/2→47D3/2, where the EIT signal is split into two EIT peaks due to the interaction between the RF field and Rydberg atoms. The dependences of EIT splitting on the power of RF field are investigated. The results show that the EIT splitting increases with the power of RF field, which can inversely be used to measure the RF field with a higher spatial resolution in the future.

Potentials of long-range cesium Rydberg molecule

Rydberg atom, with a large principal quantum number n, has big size, long lifetime, strong long-range interactions, and so on. These properties make Rydberg atoms potential candidate of quantum gate and single-photon source. Rydberg electron can interact with nearby ground-state atom, which is polarized by the Rydberg electron and is bound to the orbit of Rydberg electrons forming Rydberg molecule. As the kinetic energy of the Rydberg electron is very low, only the lowest partial waves will contribute to the molecular potential.#br#In this paper, the low electron-atom scattering with the semi-classical approximation is introduced, and the pseudopotential of interaction between Rydberg electron and ground-state atom is used to describe the long-range Rydberg molecular potential. Molecular potential curves for cesium (nS, n=30-60) are plotted according to the results of numerical computation, from which the outermost potential depth De and the equilibrium distance r0 of long-range cesium Rydberg molecule are deduced. Potential curves of cesium Rydberg molecules are consistent with the distribution curves in radial probability densities of cesium Rydberg electrons. Dependences of De and r0 on the principal quantum number n are investigated, this has an important role for the experimental measurements. The size of a Rydberg molecule depends on the equilibrium distance r0 and is proportional to the square of effective principal quantum number (n-δ )2. The calculated outermost potential depth De of Rydberg molecule becomes smaller with the increase of principal quantum number n. Rydberg molecule is very sensitive to the external field and can be used to measure and monitor weak signals.

Controlling the interactions of a few cold Rb Rydberg atoms by radio-frequency-assisted Förster resonances

Long-range interactions between cold Rydberg atoms, which are used in many important applications, can be enhanced using F\"orster resonances between collective many-body states controlled by an external electric field. Here we report on the first experimental observation of highly-resolved radio-frequency-assisted F\"orster resonances in a few cold Rb Rydberg atoms. We also observed radio-frequency-induced F\"orster resonances which cannot be tuned by a dc electric field. They imply an efficient transition from van der Waals to resonant dipole-dipole interaction due to Floquet sidebands of Rydberg levels appearing in the rf-field. This method can be applied to enhance the interactions of almost arbitrary Rydberg atoms with large principal quantum numbers.

Giant Rydberg excitons in the copper oxide Cu2O.

A highly excited atom having an electron that has moved into a level with large principal quantum number is a hydrogen-like object, termed a Rydberg atom. The giant size of Rydberg atoms leads to huge interaction effects. Monitoring these interactions has provided insights into atomic and molecular physics on the single-quantum level. Excitons--the fundamental optical excitations in semiconductors, consisting of an electron and a positively charged hole--are the condensed-matter analogues of hydrogen. Highly excited excitons with extensions similar to those of Rydberg atoms are of interest because they can be placed and moved in a crystal with high precision using microscopic energy potential landscapes. The interaction of such Rydberg excitons may allow the formation of ordered exciton phases or the sensing of elementary excitations in their surroundings on a quantum level. Here we demonstrate the existence of Rydberg excitons in the copper oxide Cu2O, with principal quantum numbers as large as n = 25. These states have giant wavefunction extensions (that is, the average distance between the electron and the hole) of more than two micrometres, compared to about a nanometre for the ground state. The strong dipole-dipole interaction between such excitons is indicated by a blockade effect in which the presence of one exciton prevents the excitation of another in its vicinity.

On the calculation of line strengths, oscillator strengths and lifetimes for very large principal quantum numbers in hydrogenic atoms and ions by the McLean–Watson formula

As a sequel to an earlier study (Hey 2009 J. Phys. B: At. Mol. Opt. Phys. 42 125701), we consider further the application of the line strength formula derived by Watson (2006 J. Phys. B: At. Mol. Opt. Phys. 39 L291) to transitions arising from states of very high principal quantum number in hydrogenic atoms and ions (Rydberg–Rydberg transitions, n > 1000). It is shown how apparent difficulties associated with the use of recurrence relations, derived (Hey 2006 J. Phys. B: At. Mol. Opt. Phys. 39 2641) by the ladder operator technique of Infeld and Hull (1951 Rev. Mod. Phys. 23 21), may be eliminated by a very simple numerical device, whereby this method may readily be applied up to n ≈ 10 000. Beyond this range, programming of the method may entail greater care and complexity. The use of the numerically efficient McLean–Watson formula for such cases is again illustrated by the determination of radiative lifetimes and comparison of present results with those from an asymptotic formula. The question of the influence on the results of the omission or inclusion of fine structure is considered by comparison with calculations based on the standard Condon–Shortley line strength formula. Interest in this work on the radial matrix elements for large n and n′ is related to measurements of radio recombination lines from tenuous space plasmas, e.g. Stepkin et al (2007 Mon. Not. R. Astron. Soc. 374 852), Bell et al (2011 Astrophys. Space Sci. 333 377), to the calculation of electron impact broadening parameters for such spectra (Watson 2006 J. Phys. B: At. Mol. Opt. Phys. 39 1889) and comparison with other theoretical methods (Peach 2014 Adv. Space Res. in press), to the modelling of physical processes in H II regions (Roshi et al 2012 Astrophys. J. 749 49), and the evaluation bound–bound transitions from states of high n during primordial cosmological recombination (Grin and Hirata 2010 Phys. Rev. D 81 083005, Ali-Haïmoud and Hirata 2010 Phys. Rev. D 82 063521, Ali-Haïmoud 2013 Phys. Rev. D 87 023526).