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Rydberg-state ionization dynamics and tunnel ionization rates in strong electric fields
摘要： Tunnel ionization rates of triplet Rydberg states in helium with principal quantum numbers close to 37 have been measured in electric fields at the classical ionization threshold of ～197 V/cm. The measurements were performed in the time domain by combining high-resolution continuous-wave laser photoexcitation and pulsed electric field ionization. The observed tunnel ionization rates range from 105 to 107 s?1 and have, together with the measured atomic energy-level structure in the corresponding electric fields, been compared to the results of calculations of the eigenvalues of the Hamiltonian matrix describing the atoms in the presence of the fields to which complex absorbing potentials have been introduced. The comparison of the measured tunnel ionization rates with the results of these, and additional calculations for hydrogenlike Rydberg states performed using semiempirical methods, have allowed the accuracy of these methods of calculation to be tested. For the particular eigenstates studied the measured ionization rates are ～5 times larger than those obtained from semiempirical expressions.
关键词： Rydberg states,tunnel ionization,electric field ionization,complex absorbing potentials,helium
更新于2025-09-23 15:22:29
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Quantum computing with neutral atoms
摘要： The power of quantum computation derives from algorithmic methods that exploit the availability of quantum superposition and entanglement to perform computations that are intractable with classical devices. The race is on to develop hardware that will unleash the promise of quantum algorithms. A handful of different types of hardware are currently being developed with the greatest efforts directed at superconducting, quantum-dot, trapped-ion, photonic, and neutral-atom approaches [1]. While all approaches have strengths and weaknesses, and are at different stages of development, the challenge of creating a practical design that can be scaled to a million or more qubits has not yet been met with any of the existing platforms.
关键词： neutral atoms,Rydberg states,Quantum computing,quantum error correction,qubits
更新于2025-09-23 15:21:21
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Pathways to excitation of atoms with bicircular laser pulses
摘要： We study the excitation of the hydrogen atom by bichromatic circularly polarized laser pulses using numerical solutions of the time-dependent Schr?dinger equation. The results are in agreement with the selection rules for multiphoton processes in such fields, namely, excited states are populated in which orbital angular momentum and magnetic quantum numbers are either both odd or both even, independent of the relative helicity, peak intensity, and pulse duration of the pulses. For co-rotating pulses the results show that excitation predominantly proceeds to states with magnetic quantum number of the same helicity as the laser pulses. Besides pathways via direct photon absorption from the ground state our results indicate that a transfer of population among the Rydberg states occurs via (cid:2)-type transitions. In the case of counter-rotating pulses the largest excitation probability is found for Rydberg states that differ in magnetic quantum number by (cid:3)m = ±3. This pattern allows us to estimate how many photons from each of the two bichromatic fields have been absorbed. Finally, we confirm that a population in Rydberg states beyond a maximum orbital angular quantum number is unlikely.
关键词： Rydberg states,hydrogen atom,bichromatic circularly polarized laser pulses,time-dependent Schr?dinger equation,multiphoton processes
更新于2025-09-23 15:21:01
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The Oscillatory Photoelectron Signal of <i>N</i> -Methylmorpholine as a Test Case for the Algebraic-Diagrammatic Construction Method of Second Order
摘要： Motivated by recent progress in the application of time-resolved photoelectron spectroscopy (TRPES) to molecular Rydberg states, we report herein a detailed assessment of the performance of the second-order algebraic diagrammatic construction (ADC(2)) method in the simulation of their TRPES spectra. As the test case, we employ the tertiary aliphatic amine N -methylmorpholine (NMM), which is notable for the fact that the signal of its 3s state exhibits long-lived oscillations along the electron binding energy axis. The relaxation process of photoexcited NMM is simulated via the Born-Oppenheimer molecular dynamics method, and the resulting TRPES spectrum is generated basing on ionization energies and approximate Dyson orbital norms calculated with the continuum orbital technique. On the whole, the simulated TRPES spectrum achieves satisfactory agreement with experiment, which suggests that the ADC(2) method provides a realistic description of the potential energy surfaces of the relevant excited and ionized states. In particular, the simulations reproduce the ?ne oscillatory structure of the signal of the 3s state, and provide evidence to the e?ect that it results from a coherent vibrational wavepacket evolving along the deformation modes of the six-membered ring. However, it is found that ADC(2) underestimates of electron binding energies by up to a few tenths of an electronvolt. The case of NMM demonstrates the usefulness of ADC(2) as a tool to aid the interpretation of the TRPES spectra of large organic molecules.
关键词： Dyson orbital,TRPES,ADC(2),time-resolved photoelectron spectroscopy,NMM,N-methylmorpholine,Rydberg states,Born-Oppenheimer molecular dynamics,continuum orbital technique,algebraic diagrammatic construction
更新于2025-09-23 15:21:01
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Laser Trapping of Circular Rydberg Atoms
摘要： Rydberg atoms are remarkable tools for quantum simulation and computation. They are the focus of an intense experimental activity, mainly based on low-angular-momentum Rydberg states. Unfortunately, atomic motion and levels lifetime limit the experimental timescale to about 100 μs. Here, we demonstrate two-dimensional laser trapping of long-lived circular Rydberg states for up to 10 ms. Our method is very general and opens many opportunities for quantum technologies with Rydberg atoms. The 10 ms trapping time corresponds to thousands of interaction cycles in a circular-state-based quantum simulator. It is also promising for quantum metrology and quantum information with Rydberg atoms, by bringing atom-field interaction times into unprecedented regimes.
关键词： circular Rydberg states,quantum computation,Rydberg atoms,quantum simulation,laser trapping
更新于2025-09-23 15:19:57
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How the methyl group position influences the ultrafast deactivation in aromatic radicals
摘要： Excited xylyl (methyl–benzyl) radical isomers have been studied by femtosecond time-resolved photoelectron spectroscopy and mass spectrometry. Depending on the substitution we find different deactivation channels after excitation into the D3(2A00) state (310 nm, 4 eV). While the ortho and para isomer exhibit deactivation rates similar to the benzyl radical, meta-xylyl sticks out and depletes twice as fast into the vibrationally hot ground state. We found that a ring deformation mode rather than the methyl pseudorotation enables access to a conical intersection, which is responsible for the faster deactivation. Transitions in the photoelectron spectrum can be assigned to several Rydberg series with mostly d angular momentum components. Absorption of two 4 eV photons triggers hydrogen loss reactions on a femtosecond timescale.
关键词： photoelectron spectroscopy,mass spectrometry,conical intersection,Rydberg states,femtosecond spectroscopy,ultrafast deactivation,xylyl radicals
更新于2025-09-19 17:15:36
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Rydberg-State-Resolved Resonant Energy Transfer in Cold Electric-Field-Controlled Intrabeam Collisions of NH <sub/>3</sub> with Rydberg He Atoms
摘要： The resonant transfer of energy from the inversion sublevels in NH3 to He atoms in triplet Rydberg states with principal quantum number n = 38 has been controlled using electric fields below 15 V/cm in intrabeam collisions at translational temperatures of ～1 K. The experiments were performed in pulsed supersonic beams of NH3 seeded in He at a ratio of 1:19. The He atoms were prepared in the metastable 1s2s 3S1 level in a pulsed electric discharge in the trailing part of the beams. The velocity slip between the heavy NH3 and the lighter metastable He was exploited to perform collision studies at center-of-mass collision speeds of ～70 m/s. Resonant energy transfer in the atom?molecule collisions was identified by Rydberg-state-selective electric-field ionization. The experimental data have been compared to a theoretical model of the resonant dipole?dipole interactions between the collision partners based on the impact parameter method.
关键词： NH3,resonant energy transfer,cold collisions,electric-field control,Rydberg states,He
更新于2025-09-12 10:27:22
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Symmetry of molecular Rydberg states revealed by XUV transient absorption spectroscopy
摘要： Transient absorption spectroscopy is utilized extensively for measurements of bound- and quasibound-state dynamics of atoms and molecules. The extension of this technique into the extreme ultraviolet (XUV) region with attosecond pulses has the potential to attain unprecedented time resolution. Here we apply this technique to aligned-in-space molecules. The XUV pulses are much shorter than the time during which the molecules remain aligned, typically <100 fs. However, transient absorption is not an instantaneous probe, because long-lived coherences re-emit for picoseconds to nanoseconds. Due to dephasing of the rotational wavepacket, it is not clear if these coherences will be evident in the absorption spectrum, and whether the properties of the initial excitations will be preserved. We studied Rydberg states of N2 and O2 from 12 to 23 eV. We were able to determine the polarization direction of the electronic transitions, and hence identify the symmetry of the final states.
关键词： transient absorption spectroscopy,extreme ultraviolet,attosecond pulses,molecular alignment,Rydberg states
更新于2025-09-11 14:15:04
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Photoluminescence properties of the entire excitonic series in
摘要： We investigated the photoluminescence spectra of Cu2O under photoexcitation at 3.05 eV across the violet band gap. The following three features were found: photoluminescence from blue and violet excitons; photoluminescence from yellow excitons of s, d, and f states in addition to p states with a quantum number up to ten; and emissions associated with the inelastic collision of the 1s yellow excitons. The first process is relevant for the separation of radiative and nonradiative decay rates. The second process likely indicates radiative enhancement of high Rydberg yellow excitons. The last process verifies up-conversion of 1s yellow paraexcitons into higher Rydberg states, which is a critical factor impeding the realization of a high-density paraexciton gas towards transition to the Bose-Einstein condensation.
关键词： photoluminescence,Rydberg states,excitons,Bose-Einstein condensation,Cu2O
更新于2025-09-10 09:29:36
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Improving the state selectivity of field ionization with quantum control
摘要： The electron signals from the ?eld ionization of two closely spaced Rydberg states of rubidium-85 are separated using quantum control. In selective ?eld ionization, the state distribution of a collection of Rydberg atoms is measured by ionizing the atoms with a ramped electric ?eld. Generally, atoms in higher energy states ionize at lower ?elds, so ionized electrons which are detected earlier in time can be correlated with higher energy Rydberg states. However, the resolution of this technique is limited by the Stark effect. As the electric ?eld is increased, the electron encounters numerous avoided Stark level crossings which split the amplitude among many states, thus broadening the time-resolved ionization signal. Previously, a genetic algorithm has been used to control the signal shape of a single Rydberg state. The present work extends this technique to separate the signals from the 34s and 33p states of rubidium-85, which are overlapped when using a simple ?eld ramp as in selective ?eld ionization.
关键词： quantum control,Rydberg states,field ionization,genetic algorithm,rubidium-85
更新于2025-09-04 15:30:14