Rydberg States Research Articles

Rydberg excitation through detuned microwave transition in rubidium

We study the excitation of Rydberg states in warm rubidium vapor. Using an inverted wavelength excitation scheme, we observe the effect of microwave coupling between Rydberg states through electromagnetically induced transparency. We observe AC stark shifts of the Rydberg states from the microwave coupling, and demonstrate detuned excitation to a secondary Rydberg state. These results show flexibility in the excitation process and state selection necessary for a variety of wave-mixing processes using Rydberg states.

Shepherd electron effects in multiple ionization of rubidium by circularly polarized intense laser fields

Nonsequential double/multiple ionization (NSDI/NSMI) of atoms in strong laser fields is a paradigm system for studying field-intervened electron-electron correlation. However, there exists a long-standing debated topic as to how NSDI/NSMI is triggered in a circularly-polarized laser field. In this contribution, it is shown counter-intuitively that the NSMI of alkali atoms is strongly enhanced due to a mechanism induced by their intrinsic shell structure, coined as the shepherd electron effect. Specifically, we find that the early-released outermost electron (the shepherd electron) can be stabilized on the Rydberg states even after dislodging some other inner-shell electrons and thus lead to the emergence of a transient hollow atom. Experimental signatures of the shepherd electron effect and its real-time observation with the attoclock technique are discussed. These results have substantially enriched our understanding of NSMI, beyond the well-accepted cascade recollision picture. They might have applications in coherent extreme-ultraviolet (XUV) light amplification.

XUV fluorescence as a probe of laser-induced helium nanoplasma dynamics

XUV fluorescence spectroscopy provides information on energy absorption and dissipation processes taking place in the interaction of helium clusters with intense femtosecond laser pulses. The present experimental results complement the physical picture derived from previous electron and ion spectroscopic studies of the generated helium nanoplasma. Here, the broadband XUV fluorescence emission from high-lying Rydberg states that covers the spectral region from at 53.0 eV all the way to photon energies corresponding to the ionization potential of He+ ions at 54.4 eV is observed directly. The cluster size-dependent population of these states in the expanding nanoplasma follows the well-known bottleneck model. The results support previous findings and highlight the important role of Rydberg states in the energetics and dynamics of laser-generated nanoplasma.

Leveling the Mountain Range of Excited-State Benchmarking through Multistate Density Functional Theory.

The performance of multistate density functional theory (MSDFT) with nonorthogonal state interaction (NOSI) is assessed for 100 vertical excitation energies against the theoretical best estimates extracted to the full configuration interaction accuracy on the database developed by Loos et al. in 2018 (Loos2018). Two optimization techniques, namely, block-localized excitation and target state optimization, are examined along with two ways of estimating the transition density functional (TDF) for the correlation energy of the Hamiltonian matrix density functional. The results from the two optimization methods are similar. It was found that MSDFT-NOSI using the spin-multiplet degeneracy constraint for the TDF of spin-coupling interaction, along with the M06-2X functional, yields a root-mean-square error (RMSE) of 0.22 eV, which performs noticeably better than time-dependent density functional theory (DFT) at an RMSE of 0.43 eV using the same functional and basis set on the Loos2018 database. In comparison with wave function theory, NOSI has smaller errors than CIS(D∞), LR-CC2, and ADC(3) all of which have an RMSE of 0.28 eV, but somewhat greater than STEOM-CCSD (RMSE of 0.14 eV) and LR-CCSD (RMSE of 0.11 eV) wave function methods. In comparison with Kohn-Sham (KS) DFT calculations, the multistate DFT approach has little double counting of correlation. Importantly, there is no noticeable difference in the performance of MSDFT-NOSI on the valence, Rydberg, singlet, triplet, and double-excitation states. Although the use of another hybrid functional PBE0 leads to a greater RMSE of 0.36 eV, the deviation is systematic with a linear regression slope of 0.994 against the results with M06-2X. The present benchmark reveals that density functional approximations developed for KS-DFT for the ground state with a noninteracting reference may be adopted in MSDFT calculations in which the state interaction is key.

Energy loss of monopolium in a medium

We study the energy loss of excited monopolium in an atomic medium. We perform a classical calculation in line with a similar calculation performed for charged particles which leads in the non-relativistic limit to the Bethe–Bloch formula except for the density dependence of the medium, which we do not consider in this paper. Our result shows that for maximally deformed Rydberg states, the ionization of monopolium in a light atomic medium is similar to that of light ions.

Microwave Radiation in the Environment and Its Impact on the State of Living Organisms

In the early 1990s [1], we proposed a new agent of the impact of geocosmos on a set of processes in the lower atmosphere and biosphere - the microwave radiation of the earth's ionosphere, emitted by all its atoms, molecules and their ions when high-energy (Rydberg) states are excited by photo- and secondary electrons mainly during solar flares and geomagnetic storms. This made it possible to solve the main problem of the physics of solar-terrestrial relations, since it opened a previously unknown channel for the constant influence of space weather factors on terrestrial processes and the state of the human body. In addition, we proposed to take into account the existence of such a factor when assessing the safety of manned space flights beyond the Earth's magnetosphere [2,10,12], including during the operation of the Moon. In our approach - supramolecular physics of supramolecular structures of molecules with high affinity for the proton (including water in a living organism), we took into account the pioneering works [14,15], in which the possibility of the formation of "polyatomic Rydberg molecules" in such cases was found. Their existence, including in the biological molecules, was discussed in [18]. Here we used the analogy with molecular protonics considered for the biomedium within the framework of supramolecular chemistry [16]. In our studies of the geocosmic contribution to terrestrial processes, we proposed for the first time to take into account the role of microwave emission from the ionosphere in studying the problem of global warming. Such an emission causes the generation of optically thin upper clouds from water-containing associates, which delays the escape of thermal radiation from the surface atmosphere [4]. This was confirmed when interpreting the data of meteorological observations at an altitude of 2100 meters at the Kislovodsk station of the Leningrad University in 2003 [3].

Tunable Rydberg–Rydberg transitions in helium with reduced sensitivity to dc electric fields by two-colour microwave dressing

The difference in the static electric dipole polarizabilities of the and Rydberg levels in helium has been eliminated by dressing the atom with a microwave field near resonant with the single-photon transition. For an amplitude dressing field, detuned by from the zero-field transition frequency, the dc Stark shift of the two-photon transition between these states remained within for electric fields up to . This transition was probed by single-color two-photon microwave spectroscopy, and by two-color two-photon spectroscopy with one strong additional dressing field and a weak probe field. For all measurements, the transition frequencies and Stark shifts were compared, and found to be in excellent quantitative agreement with the results of Floquet calculations of the energy-level structure of the Rydberg states in the presence of the dressing fields and applied dc electric fields. The two-color microwave dressing scheme demonstrated, with one field applied to null the differential polarizability of the Rydberg–Rydberg transition, and the second exploited to allow the two-photon transition to be employed to achieve tunable absorption of single-photons from a weak probe field, will facilitate improved coherence times and tunable single-photon absorption in hybrid cavity QED experiments with Rydberg atoms and superconducting microwave circuits.

New atomic data for C i Rydberg states compared with solar UV spectra

ABSTRACT We use the Breit–Pauli R-matrix method to calculate accurate energies and radiative data for states in C i up to n = 30 and with l ≤ 3. We provide the full data set of decays to the five 2s2 2p2 ground configuration states 3P0,1,2, 1D2, and 1S0. This is the first complete set of data for transitions from n ≥ 5. We compare oscillator strengths and transition probabilities with the few previously calculated values for such transitions, finding generally good agreement (within 10 per cent) with the exception of values recently recommended by National Institute of Standards and Technology, where significant discrepancies are found. We then calculate spectral line intensities originating from the Rydberg states using typical chromospheric conditions and assuming local thermal equilibrium, and compare them with well-calibrated Solar and Heliospheric Observatory Solar Ultraviolet Measurements of Emitted Radiation ultraviolet (UV) spectra of the quiet Sun. The relative intensities of the Rydberg series are in excellent agreement with observation, which provides firm evidence for the identifications and blends of nearly 200 UV lines. Such comparison also resulted in a large number of new identifications of C i lines in the spectra. We also estimate optical depth effects and find that these can account for much of the absorption noted in the observations. The atomic data can be applied to model a wide range of solar and astrophysical observations.

Oscillator Strengths and Cross Sections of the Valence-Shell Excitations of HBr Studied by Fast Electron Impact.

The oscillator strengths and cross sections of the valence-shell excitations of HBr were determined by fast electron scattering with an incident electron energy of 1500 eV and an energy resolution of 80 meV. The momentum transfer dependence behaviors of the generalized oscillator strengths have been used to elucidate the transition characteristics. The present results show that the strong spin-orbital interaction results in the observation of some triplet states in the (Λ, S) coupling and the constant generalized oscillator strength ratios for the pair states with the same electronic configuration and quantum number Ω, and the quantitative spin-orbit coupling coefficients of b3Π1(v = 0) and C1Π(v = 0) are determined. The optical oscillator strengths of the valence-shell excitations were obtained by extrapolating the generalized oscillator strengths to the limit of zero squared momentum transfer. The present optical oscillator strengths give an independent cross-check of the previous experimental and theoretical results, and the comparison shows that the line-saturation effect is more severe for the high Rydberg states with large intensities and narrow natural widths. The integral cross sections of the valence-shell excitations of HBr were obtained from the excitation threshold to 5000 eV by the BE-scaling method. The present oscillator strengths and cross sections supplement the fundamental molecular database of HBr and can be used for modeling in the semiconductor industry, astrophysics, and atmospheric chemistry.

Precise determination of adiabatic ionisation energies of large polyatomic molecules: p-diaminobenzene

We present a procedure, based on established principles, to accurately determine the ionisation energies of medium-sized to large polyatomic molecules in supersonic beams. The method combines single-photon excitation from the electronic ground state using tunable vacuum-ultraviolet laser radiation, the delayed pulsed-field ionisation of high Rydberg states with sequences of pulsed electric fields, and the modelling of the lineshapes from calculations of the field-ionisation dynamics of high Rydberg states and of the rotational contours of the photoelectron bands. The method is illustrated by a measurement of the adiabatic ionisation energy of p-diaminobenzene (p-DB), for which we obtain the value of 54,617.47(15) cm , which represents a more than 20-fold accuracy improvement over previous determinations.

Photodissociation dynamics of the ethyl radical via the Ã2A'(3s) state: H-atom product channels and ethylene product vibrational state distribution.

The photodissociation dynamics of jet-cooled ethyl radical (C2H5) via the Ã2A'(3s) states are studied in the wavelength region of 230-260nm using the high-n Rydberg H-atom time-of-flight (TOF) technique. The H + C2H4 product channels are reexamined using the H-atom TOF spectra and photofragment translational spectroscopy. A prompt H + C2H4(X̃1Ag) product channel is characterized by a repulsive translational energy release, anisotropic product angular distribution, and partially resolved vibrational state distribution of the C2H4(X̃1Ag) product. This fast dissociation is initiated from the 3s Rydberg state and proceeds via a H-bridged configuration directly to the H + C2H4(X̃1Ag) products. A statistical-like H + C2H4(X̃1Ag) product channel via unimolecular dissociation of the hot electronic ground-state ethyl (X̃2A') after internal conversion from the 3s Rydberg state is also examined, showing a modest translational energy release and isotropic angular distribution. An adiabatic H + excited triplet C2H4(ã3B1u) product channel (a minor channel) is identified by energy-dependent product angular distribution, showing a small translational energy release, anisotropic angular distribution, and significant internal excitation in the C2H4(ã3B1u) product. The dissociation times of the different product channels are evaluated using energy-dependent product angular distribution and pump-probe delay measurements. The prompt H + C2H4(X̃1Ag) product channel has a dissociation time scale of <10ps, and the upper bound of the dissociation time scale of the statistical-like H + C2H4(X̃1Ag) product channel is <5ns.

Robust Ramsey interferometer based on a single Rydberg polariton

We demonstrate a robust single-photon Ramsey interferometer based on a single Rydberg excitation, where the photon is stored as a Rydberg polariton in an ensemble of atoms. This coherent conversion of the photon to Rydberg polariton enables to split an incoming photon into a superposition state of two Rydberg states by applying microwave fields, which constructs two paths of interferometer. Ramsey interference fringes are demonstrated when we scan either the detuning of the microwave or the free evolution time, from which we can obtain the resonant transition frequency of two Rydberg states. We use the Ramsey-like sequence to demonstrate coherent manipulation of the stored single-photon to construct different interference patterns. In addition, the robustness of the Ramsey interferometer to the fluctuation of incoming photon numbers and optical depth (OD) of the atomic ensemble is tested, showing that the coherent of Ramsey interferometer is preserved for input photon number in a range of R in &lt; 15 and for OD varying from 1.0 to 4.0. The robust interferometer will find its applications in quantum precision measurement.

Ultrafast Proton Transfer and Contact Ion-Pair Formation in Formic Acid Clusters.

The ultrafast proton transfer dynamics of homogeneous formic acid clusters (FA)n, n < 10, are investigated with femtosecond time-resolved mass spectrometry. We monitor the proton transfer pathway following Rydberg state electronic relaxation and find that successful ion pair formation increases logarithmically with cluster size. Ab initio calculations demonstrate similar excitation/relaxation behavior for each cluster, revealing a contact ion pair forms between two molecules composing the cluster before finally a formate anion (HCOO-) is dissociated by the probe pulse. The sub-ps time scale for rearrangement and proton transfer increases almost linearly with cluster size, requiring ∼67 fs per additional formic acid molecule and ranging from 213 ± 51 fs for the trimer to 667 ± 116 fs for FA9. The near-linear trends measured for both rearrangement lifetime and ion pair formation suggest that proton transfer is unlikely in the formic acid dimer but becomes prominent in small clusters.

Excited-State-Specific Pseudoprojected Coupled-Cluster Theory.

We present an excited-state-specific coupled-cluster approach in which both the molecular orbitals and cluster amplitudes are optimized for an individual excited state. The theory is formulated via a pseudoprojection of the traditional coupled-cluster wavefunction that allows correlation effects to be introduced atop an excited-state mean field starting point. The approach shares much in common with ground-state CCSD, including size extensivity and an N6 cost scaling. Preliminary numerical tests show that, when augmented with N5 cost perturbative corrections for key terms, the method can improve over excited-state-specific second-order perturbation theory in valence, charge transfer, and Rydberg states.

Imaging-Assisted Single-Photon Doppler-Free Laser Spectroscopy and the Ionization Energy of Metastable Triplet Helium.

Skimmed supersonic beams provide intense, cold, collision-free samples of atoms and molecules and are one of the most widely used tools in atomic and molecular laser spectroscopy. High-resolution optical spectra are typically recorded in a perpendicular arrangement of laser and supersonic beams to minimize Doppler broadening. Typical Doppler widths are nevertheless limited to tens of MHz by the residual transverse-velocity distribution in the gas-expansion cones. We present an imaging method to overcome this limitation that exploits the correlation between the positions of the atoms and molecules in the supersonic expansion and their transverse velocities, and thus their Doppler shifts. With the example of spectra of (1s)(np) ^{3}P_{0-2}←(1s)(2s) ^{3}S_{1} transitions to high Rydberg states of metastable triplet He, we demonstrate the suppression of the residual Doppler broadening and a reduction of the full linewidths at half maximum to only about 1MHz in the UV. Using a retroreflection arrangement for the laser beam and a cross-correlation method, we determine Doppler-free spectra without any signal loss from the selection, by imaging, of atoms within ultranarrow transverse-velocity classes. As an illustration, we determine the ionization energy of triplet metastable He and confirm the significant discrepancy between recent experimental [G. Clausen etal., Phys. Rev. Lett. 127, 093001 (2021)PRLTAO0031-900710.1103/PhysRevLett.127.093001] and high-level theoretical [V. Patkós etal., Phys. Rev. A 103, 042809 (2021)PLRAAN2469-992610.1103/PhysRevA.103.042809] values of this quantity.

Controlled‐NOT Gate Based on the Rydberg States of Surface Electrons

AbstractDue to the long coherence time and efficient manipulation, the surface electron (SE) provides a perfect 2D platform for quantum computation and quantum simulation. In this work, a theoretical scheme to realize the controlled‐NOT gate is proposed, where the two‐qubit system is encoded on the four‐level Rydberg structure of SE. The state transfer is achieved by a three‐level structure with an intermediate level. By simultaneously driving the SE with two external electromagnetic fields, the dark state in the electromagnetically induced transparency effect is exploited to suppress the population of the most dissipative state and increase the robustness against dissipation. The fidelity of the scheme is 0.9989 with experimentally achievable parameters.

Molecular Dynamics in Rydberg Tweezer Arrays: Spin-Phonon Entanglement and Jahn-Teller Effect.

Atoms confined in optical tweezer arrays constitute a platform for the implementation of quantum computers and simulators. State-dependent operations are realized by exploiting electrostatic dipolar interactions that emerge, when two atoms are simultaneously excited to high-lying electronic states, so-called Rydberg states. These interactions also lead to state-dependent mechanical forces, which couple the electronic dynamics of the atoms to their vibrational motion. We explore these vibronic couplings within an artificial molecular system in which Rydberg states are excited under so-called facilitation conditions. This system, which is not necessarily self-bound, undergoes a structural transition between an equilateral triangle and an equal-weighted superposition of distorted triangular states (Jahn-Teller regime) exhibiting spin-phonon entanglement on a micrometer distance. This highlights the potential of Rydberg tweezer arrays for the study of molecular phenomena at exaggerated length scales.

Wavelength Dependence of Atomic Excitation for Ar Subject to Intense Midinfrared Laser Pulses

We report experimental and theoretical investigations of wavelength dependence of Rydberg state excitation (RSE) process of Ar subject to intense laser fields. By simultaneously measuring ionization and RSE yields of Ar atoms subject to strong laser fields at a series of wavelengths, we obtain the wavelength scaling law of the ratio of Ar* over Ar+ with respect to the laser intensity, and this result can be well reproduced by a nonadiabatic model, but not by the classical-trajectory Monte Carlo model. Our results indicate that the nonadiabatic corrections of the photoelectron tunneling exit and tunneling probability play a significant role at shorter wavelengths. Analysis shows that the wavelength dependence phenomenon is due to the interplay of the nonadiabatic effect, wave-packet diffusion and Coulomb focusing effect of the liberated electron.

Landau-Forbidden Quantum Criticality in Rydberg Quantum Simulators.

The Landau-Ginzburg-Wilson theory of phase transitions precludes a continuous transition between two phases that spontaneously break distinct symmetries. However, quantum mechanical effects can intertwine the symmetries, giving rise to an exotic phenomenon called deconfined quantum criticality (DQC). In this Letter, we study the ground state phase diagram of a one-dimensional array of individually trapped neutral atoms interacting strongly via Rydberg states, and demonstrate through extensive numerical simulations that it hosts a variety of symmetry-breaking phases and their transitions including DQC. We show how an enlarged, emergent continuous symmetry arises at the DQCs, which can be experimentally observed in the joint distribution of two distinct order parameters, obtained within measurement snapshots in the standard computational basis. Our findings highlight quantum simulators of Rydberg atoms not only as promising platforms to experimentally realize such exotic phenomena, but also as unique ones allowing access to physical properties not obtainable in traditional experiments.

Satellite radio detection via dual-microwave Rydberg spectroscopy

Rydberg electric field sensors exploit the large number of Rydberg resonances to provide sensitivity over a broad range of the electromagnetic spectrum. However, due to the difficulty of accessing resonant Rydberg states at ultra-high frequency (UHF) and below, ubiquitous bands in the world's current wireless communications infrastructure, they currently fall, short in sensitivity in this range. We present a resonant Rydberg electric field sensor operating in the UHF band using a dual-optical dual-microwave spectroscopy scheme. Adding an additional microwave photon allows us to access transitions between Rydberg states with higher angular momentum (L=3→4), which have lower resonant frequencies than transitions typically used in Rydberg sensors. We discuss the applicability of this type of sensor across the UHF band and below and measure the resonant sensitivity of our system at 2.3 GHz to be 70(5) μV m−1 Hz−1∕2, 57 times better than the measured sensitivity with a far off-resonant probing scheme at this frequency. We also show the effectiveness of this sensing scheme by measuring Sirius XM satellite radio (2.320–2.345 GHz) received outside the laboratory and rebroadcast onto the atoms.