High-lying Rydberg States Research Articles

Spectral Signatures of Vibronic Coupling in Trapped Cold Ionic Rydberg Systems.

Atoms and ions confined with electric and optical fields form the basis of many current quantum simulation and computing platforms. When excited to high-lying Rydberg states, long-ranged dipole interactions emerge which strongly couple the electronic and vibrational degrees of freedom through state-dependent forces. This vibronic coupling and the ensuing hybridization of internal and external degrees of freedom manifest through clear signatures in the many-body spectrum. We illustrate this by considering the case of two trapped Rydberg ions, for which the interaction between the relative vibrations and Rydberg states realizes a quantum Rabi model. We proceed to demonstrate that the aforementioned hybridization can be probed by radio frequency spectroscopy and discuss observable spectral signatures at finite temperatures and for larger ion crystals.

Sensitive detection and imaging of H2O density through Rydberg resonant femtosecond laser induced photofragmentation fluorescence.

A femtosecond laser induced photofragmentation fluorescence (fs-LIPF) scheme for the sensitive detection and imaging of water vapor is presented. Two photons of 244.3nm excite water to the D̃ state and produce hydroxyl radicals in the fluorescing à state. Two more photons promote electrons from the D̃ state to a neutral Rydberg state of the (1b2)-1 ionic core through a 2 + 2 doubly resonant process. The resulting high-lying Rydberg state undergoes neutral dissociation, and the energetic hydrogen fragments are detected from their Balmer series fluorescence. These channels (in the low-pressure limit) have detection sensitivities around 1012 molecules per cubic centimeters, orders of magnitude more sensitive than laser-induced fluorescence based approaches, allowing for sensitive non-invasive detection and imaging of water density for many important processes.

Electron impact electronic excitation of benzene: Theory and experiment.

We report experimental differential cross sections (DCSs) for electron impact excitation of bands I to V of benzene at incident energies of 10, 12.5, 15, and 20eV. They are compared to calculations using the Schwinger multichannel method while accounting for up to 437 open channels. For intermediate scattering angles, the calculations reveal that the most intense band (V) emerges from surprisingly similar contributions from all its underlying states (despite some preference for the dipole-allowed transitions). They further shed light on intricate multichannel couplings between the states of bands I to V and higher-lying Rydberg states. In turn, the measurements support a vibronic coupling mechanism for excitation of bands II and IV and also show an unexpected forward peak in the spin-forbidden transition accounting for band III. Overall, there is decent agreement between theory and experiment at intermediate angles and at lower energies and in terms of the relative DCSs of the five bands. Discrepancies between the present and previous experiment regarding bands IV and V draw attention to the need of additional experimental investigations. We also report measured DCSs for vibrational excitation of combined C-H stretching modes.

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.

Maximally entangled Rydberg-atom pairs via Landau-Zener sweeps

We analyze the formation of maximally entangled Rydberg atom pairs subjected to Landau-Zener sweeps of the atom-light detuning. Though the populations reach a steady value at longer times, the phases evolve continuously, leading to periodic oscillations in the entanglement entropy. The local unitary equivalence between the obtained maximally entangled states and the Bell states is verified by computing the polynomial invariants. Finally, we study the effect of spontaneous emission from the Rydberg state of rubidium atoms on the correlation dynamics and show that the oscillatory dynamics persists for high-lying Rydberg states. Our study may offer novel ways to generate maximally entangled states, quantum gates and exotic quantum matter in arrays of Rydberg atoms through Landau Zener sweeps.

Ultrafast Imaging of the Jahn–Teller Topography in Carbon Tetrachloride

We report the direct time-domain observation of ultrafast dynamics driven by the Jahn-Teller effect. Using time-resolved photoelectron spectroscopy with a vacuum-ultraviolet femtosecond source to prepare high-lying Rydberg states of carbon tetrachloride, our measurements reveal the local topography of a Jahn-Teller conical intersection. The pump pulse prepares a configurationally mixed superposition of the degenerate 1T2 4p-Rydberg states, which then distorts through spontaneous symmetry breaking that we identify to follow the t2 bending motion. Photoionization of these states to three cationic states 2T1, 2T2, and 2E reveals a shift in the center-of-mass of the photoelectron peaks associated with the 2Tn states which reveals the local topography of the Jahn-Teller conical intersection region prepared by the pump pulse. Time-dependent density functional theory calculations confirm that the dominant nuclear motion observed in the spectrum is the CCl4 t2 bending mode. The large density of states in the VUV spectral region at 9.33 eV of carbon tetrachloride and strong vibronic coupling result in ultrafast decay of the excited-state signal with a time constant of 75(4) fs.

Ultrafast dissociation of nitromethane from the 3p Rydberg state

ABSTRACT We report the time-resolved observation of the ultrafast dissociation of the 3p Rydberg state manifold of nitromethane, which decays with a time constant of 53 ± 5 fs. We access this manifold using a femtosecond high-harmonic-generation source, allowing us to track the dynamics of high-lying Rydberg states. Combining ultrafast VUV/UV pump-probe ultrafast photoelectron spectroscopy with ab initio non-adiabatic surface-hopping calculations, we find that a major channel of this ultrafast relaxation is NO bond cleavage. In contrast to previous literature, we find that intersystem crossing is not necessary to explain the dynamics, as the multiplicity of the system is retained along the reaction pathway. The photoinduced homolytic fission results in the formation of a nitrosomethane radical, with possible implications for atmospheric chemistry.

Many-Body Radiative Decay in Strongly Interacting Rydberg Ensembles.

When atoms are excited to high-lying Rydberg states they interact strongly with dipolar forces. The resulting state-dependent level shifts allow us to study many-body systems displaying intriguing nonequilibrium phenomena, such as constrained spin systems, and are at the heart of numerous technological applications, e.g., in quantum simulation and computation platforms. Here, we show that these interactions also have a significant impact on dissipative effects caused by the inevitable coupling of Rydberg atoms to the surrounding electromagnetic field. We demonstrate that their presence modifies the frequency of the photons emitted from the Rydberg atoms, making it dependent on the local neighborhood of the emitting atom. Interactions among Rydberg atoms thus turn spontaneous emission into a many-body process which manifests, in a thermodynamically consistent Markovian setting, in the emergence of collective jump operators in the quantum master equation governing the dynamics. We discuss how this collective dissipation-stemming from a mechanism different from the much studied superradiance and subradiance-accelerates decoherence and affects dissipative phase transitions in Rydberg ensembles.

Laser photo-ionization study of nat Ag using opto-galvanic signal at SPES offline laser lab

Resonant Ionization Laser Ion Source (RILIS) is one of the most advancing techniques for the production of radioactive ion beams (RIBs) in ISOL facilities. SPES project at INFN-LNL is a second generation ISOL facility which aims to produce several isotopes in a couple of years. Within the framework of this project, resonant photo-ionization schemes of several elements are studied in the offline laser lab, to be later implemented in the SPES Laser Ion Source. Silver is one of the elements being studied for the stated purpose. In this article, we report a resonant photo-ionization scheme of silver tested with a hollow cathode lamp (HCL). Evidence of high lying Rydberg states around 60945.32 cm−1 has also been observed by studying the fast opto-galvanic signal detected.

Quantum watch and its intrinsic proof of accuracy

We have investigated the rich dynamics of complex wave packets composed of multiple high-lying Rydberg states in He. A quantitative agreement is found between theory and time-resolved photoelectron spectroscopy experiments. We show that the intricate time dependence of such wave packets can be used for investigating quantum defects and performing artifact-free timekeeping. The latter relies on the unique fingerprint that is created by the time-dependent photoionization of these complex wave packets. These fingerprints determine how much time has passed since the wave packet was formed and provide an assurance that the measured time is correct. Unlike any other clock, this quantum watch does not utilize a counter and is fully quantum mechanical in its nature. The quantum watch has the potential to become an invaluable tool in pump-probe spectroscopy due to its simplicity, assurance of accuracy, and ability to provide an absolute timestamp, i.e., there is no need to find time zero.

Quantum-brachistochrone approach to the conversion from W to Greenberger-Horne-Zeilinger states for Rydberg-atom qubits

Using the quantum-brachistochrone formalism, we address the problem of finding the fastest possible (time-optimal) deterministic conversion between $W$ and Greenberger-Horne-Zeilinger (GHZ) states in a system of three identical and equidistant neutral atoms that are acted upon by four external laser pulses. Assuming that all four pulses are close to being resonant with the same internal (atomic) transition---the one between the atomic ground state and a high-lying Rydberg state---each atom can be treated as an effective two-level system ($gr$-type qubit). Starting from an effective system Hamiltonian, which is valid in the Rydberg-blockade regime and defined on a four-state manifold, we derive the quantum-brachistochrone equations pertaining to the fastest possible $W$-to-GHZ state conversion. By numerically solving these equations, we determine the time-dependent Rabi frequencies of external laser pulses that correspond to the time-optimal state conversion. In particular, we show that the shortest possible $W$-to-GHZ state-conversion time is given by ${T}_{\text{QB}}=6.8\phantom{\rule{0.222222em}{0ex}}\ensuremath{\hbar}/E$, where $E$ is the total laser-pulse energy used, this last time being significantly shorter than the state-conversion times previously found using a dynamical-symmetry-based approach [${T}_{\text{DS}}=(1.33\ensuremath{-}1.66)\phantom{\rule{0.222222em}{0ex}}{T}_{\text{QB}}$].

Simulation of many-body dynamics using Rydberg excitons

The recent observation of high-lying Rydberg states of excitons in semiconductors with relatively high binding energy motivates exploring their applications in quantum nonlinear optics and quantum information processing. Here, we study Rydberg excitation dynamics of a mesoscopic array of excitons to demonstrate its application in simulation of quantum many-body dynamics. We show that the -ordered phase can be reached using physical parameters available for cuprous oxide (Cu2O) by optimizing driving laser parameters such as duration, intensity, and frequency. In an example, we study the application of our proposed system to solving the maximum independent set problem based on the Rydberg blockade effect.

A field ionizer for photodetachment studies of negative ions.

In this paper, we present an apparatus for studies into the photodetachment process of atomic negative ions. State-selective detection of the residual atom following the initial photodetachment step is achieved by combining resonant laser excitation of the photo-detached atom with electric field ionization. The resonance ionization technique in combination with a co-linear ion-laser beam geometry gives an experimental apparatus that has both high selectivity and sensitivity. In addition to measurements of a single selected partial photodetachment channel, the apparatus also can be used to study a manifold of photodetachment channels in which the residual atom is left in a high-lying Rydberg state and for investigation of the double electron-detachment process. Ion-optical simulations in SIMION are used to illustrate the operation of the apparatus for studying such processes. Successful performance of the apparatus against the simulation is demonstrated by a high resolution study of the photodetachment of cesium, where the sharp s-wave threshold of the photodetachment processes leaving the residual atom in the excited 6p state was investigated.

Probing the Atomic Structure of Californium by Resonance Ionization Spectroscopy

The atomic structure of californium is probed by two-step resonance ionization spectroscopy. Using samples with a total amount of about 2×1010 Cf atoms (ca. 8.3 pg), ground-state transitions as well as transitions to high-lying Rydberg states and auto-ionizing states above the ionization potential are investigated and the lifetimes of various atomic levels are measured. These investigations lead to the identification of efficient ionization schemes, important for trace analysis and nuclear structure investigations. Most of the measurements are conducted on 250Cf. In addition, the isotope shift of the isotopic chain 249−252Cf is measured for one transition. The identification and analysis of Rydberg series enables the determination of the first ionization potential of californium to EIP=50,666.76(5)cm−1. This is about a factor of 20 more precise than the current literature value.

Detection of transitions between high-lying Rydberg states of Ca-40 using the effect of autoionization, optical and microwave radiation

Detection of transitions between high-lying Rydberg states of Ca-40 using the effect of autoionization, optical and microwave radiation

Advanced Laser-Photoionization Scheme of Separation of Heavy Isotopes in the Gases Separator Devices

An effective approach to determining the parameters of the optimal schemes of the method of laser selective photoionization of atoms (elements and isotopes) with finite ionization due to collisions, ionization by a pulsed electric field, ionization through high (Rydberg) states and narrow autoionization resonances for the separation of heavy isotopes has been proposed. in gas separator devices. On the basis of the theory of optimal control and previously developed quantum models for calculating the characteristics of elementary atomic processes, optimization models of isotope separation are numerically implemented in the scheme of selective laser photoionization with ionization due to collisions in gas mixtures, ionization by a pulsed electric field, autoionization, etc. etc. The data obtained quantitatively confirm the promise of the method of laser photoionization with finite ionization due to collisions, ionization by a pulsed electric field, ionization through high-lying (Rydberg) states and narrow autoionization resonances and give a set of parameters for the desired optimal schemes, in particular, the laser pulse optimal shape for rubidium and uranium isotopes.

High-lying Rydberg atoms surviving intense laser fields

In this work, we have experimentally and theoretically investigated the high-lying Rydberg state excitation for noble gas atoms subject to an intense near-infrared laser field. To obtain the signal of these high-lying Rydberg atoms which are further ionized by a constant electric field $({F}_{c})$, coincident detection of the photoelectrons and photoions with well-chosen arrival times is performed. Based on a fitting to the time dependence of the coincidently measured photofragment yields with a semiempirical formula, we can extract a principal quantum number distribution (PQND) of the population of the excited states in a range closely related to the strength of ${F}_{c}$. The extracted valid PQND is in qualitative agreement with a semiclassical model calculation. Our work thus provides a method to extract the PQND and study the ultrafast high-lying Rydberg state excitation.

Innovative mass spectrometer for high-resolution ion spectroscopy.

Conventional ion spectroscopy is inapplicable for ions produced in low concentrations or with low spectral resolutions. Hence, we constructed a high-resolution vacuum ultraviolet mass-analyzed threshold ionization (HR VUV-MATI) spectrometer composed of a four-wave frequency mixing cell capable of generating long-lasting and intense VUV laser pulses of ∼1 × 1010 photons/pulse at wavelengths of 123.6-160.0nm, a space-focused linear time-of-flight photoionization chamber with a new ion-source assembly, and a compact molecular beam chamber with a temperature-controlled pulsed nozzle for ion spectroscopy. The ion-source assembly and pulsing schemes enabled an ∼15-μs-delayed but extremely weak pulsed-field-ionization of the molecules in the zero-kinetic-energy (ZEKE) states and first-order space focusing of the generated MATI ions. These ZEKE states were effectively generated by a minute electric jitter from the high-lying Rydberg states, which were initially prepared via VUV photoexcitation. The spectral and mass resolutions (∼5cm-1 and 2400, respectively) and the signal strength were simultaneously enhanced using this spectrometer. Moreover, it could be used to measure the fine vibrational spectrum from the zero-pointlevel of the cation and the exact adiabatic ionization energy of the neutral molecule. Additionally, it could be used to measure the appearance energies of the photoproducts and elucidate the vibrational structures of the cationic isotopomers, utilizing other pulsing schemes. Furthermore, this spectrometer could be used to analyze the congested vibrational spectrum of a cation with multiple conformations. Thus, the HR VUV-MATI spectrometer-a potential alternative to photoelectron spectrometers-can be used to analyze the conformational structure-dependent reactivities.

Orbital effects in strong-field Rydberg state excitation of N2, Ar, O2 and Xe

Rather than being freed to the continuum, the strong-field tunneled electrons can make a trajectory driven by the remaining laser fields and have certain probability to be captured by the high lying Rydberg states of the parent atoms or molecules. To explore the effect of molecular orbital on Rydberg state excitation, the ellipticity dependence of Rydberg state yields of N2 and O2 molecules are experimentally investigated using cold target recoil ion momentum spectroscopy and are compared with their counterpart atoms Ar and Xe with comparable ionization potentials. We found the generation probability of the neutral Rydberg fragment O2* was orders of magnitude higher than that of Xe* due to the butterfly-shaped highest occupied molecular orbital of O2. Meanwhile, our experimental and simulation results reveal that it is the initial momentum distribution (determined by the detailed characteristics of orbitals) that finally leads to the tendency that the Rydberg state yield of O2 (Ar) decreased slower than that obtained for Xe (N2) when the ellipticity of the excitation laser field is increased.

Rydberg excitons in synthetic cuprous oxide Cu2O

High-lying Rydberg states of Mott-Wannier excitons are receiving considerable interest due to the possibility of adding long-range interactions to the physics of exciton-polaritons. Here, we study Rydberg excitation in bulk synthetic cuprous oxide grown by the optical float zone technique and compare the result with natural samples. X-ray characterization confirms both materials are mostly single crystal, and mid-infrared transmission spectroscopy revealed little difference between synthetic and natural material. The synthetic samples show principal quantum numbers up to $n=10$, exhibit additional absorption lines, plus enhanced spatial broadening and spatial inhomogeneity. Room temperature and cryogenic photoluminescence measurements reveal a significant excess of copper vacancies in the synthetic material. These measurements provide a route towards achieving \mbox{high-$n$} excitons in synthetic crystals, opening a route to scalable quantum devices.