Search arXiv⌕ Search
Home/Archive/arXiv

arXiv · 2410.01601

Measurement of ionization delays in atomic REMPI using photoelectron vortices

D. Köhnke·T. Bayer·M. Wollenhaupt
View original source ↗Read source document ↗Export metadata ↓

Abstract

We study time-delays in atomic multiphoton ionization (MPI) using the phase-sensitive detection of photoelectron vortices. Photoelectron vortices are created by MPI with counter-rotating circularly polarized (CRCP) ultrashort double pulse sequences. The vortices are characterized by a spiral-shaped photoelectron momentum distribution (PMD) resulting from the Ramsey-type interference of the partial photoelectron wave packets created by each pulse. The slope of the spiral arms encodes the time-delay between the partial wave packets with interferometric precision. We study the ionization time-delay in the (1+2) resonance-enhanced multiphoton ionization (REMPI) of potassium atoms using femtosecond CRCP white-light supercontinuum pulses. Pairwise interference of the partial wave packets with a reference wave packet gives rise to vortices of different rotational symmetry, which are superimposed to form the total PMD. The PMD is reconstructed tomographically and decomposed into the vortices using 3D Fourier analysis. From the energy-dependent spectral phases of the vortices, we retrieve a resonant ionization delay in the order of 1 fs, much shorter than the pulse duration. Our results demonstrate the power of photoelectron vortices for the accurate determination of photoionization time-delays and open up new perspectives for photoelectron chronoscopy including the measurement of ionization delays on the attosecond timescale.

Explore related subjects

physics.atom-ph

Keep this discovery

Explore connections, maps & timelines

BibTeXRIS

D. Köhnke, T. Bayer, M. Wollenhaupt. 2024-10-02. Measurement of ionization delays in atomic REMPI using photoelectron vortices. https://doi.org/10.1103/physreva.110.063111

Cite the original work for its findings. Save a collection to share your selection of sources.

KEEP EXPLORING

Related papers

arXiv2026

Effective Conservation and Bistability of Atomic Alignment under Strong Spin~Exchange

We present a phenomenological model of anomalous alignment signals in dense cesium vapor under linearly polarized pumping and fast spin exchange near zero magnetic field. Despite the absence of a conservation law for rank-2 angular momentum, our recent experiments reveal anisotropic narrow resonances, hysteresis, and bistability. We attribute these effects to a stretched state forming a collective mode in which orientation and alignment are bidirectionally coupled. This mode acts as a reservoir, preserving the essential properties of alignment despite rapid spin exchange.

physics.atom-ph↗
arXiv2026

$LS/LSJ$ Hybrid Coupling Framework for Auger Angular Distributions of Experimentally Unresolved Multiplets with Isolated Fine-Structure

We present a hybrid $LS/LSJ$ coupling framework for treating state multiplets in the regime $ΔE_\text{int}\sim\hbar/τ_\text{int} \ggΔE_\text{FS}\ggΓ$, where $τ_\text{int}$ is the collision interaction time, $ΔE_\text{FS}$ the fine-structure splitting, and $Γ$ the natural width. In this regime, the collision interaction is fast compared with fine-structure evolution, whereas the individual $J$ levels are well isolated on the scale of their natural widths. The produced multiplet's alignment is therefore described in $LS$ coupling and then projected onto the individual fine-structure $J$ levels before their subsequent decay, described by $LSJ$ coupling. Applied to the multi-open-shell $1s2s2p\,^4\!P_J$ manifold, which closely satisfies these conditions, the hybrid treatment reveals strong suppression and inversion of the Auger angular-distribution anisotropy relative to the traditional pure-$LS$ treatment. It substantially improves agreement with absolute experimental data while using the same $LS$ production cross sections. This hybrid $LS/LSJ$ framework thus provides the appropriate treatment of state multiplets with isolated fine-structure levels, as it retains the $J$-dependent decay dynamics missing from the traditional pure-$LS$ treatment.

physics.atom-ph↗
arXiv2026

Optical Ion Clock with Engineered Immunity to Motion-Induced Frequency Shifts

Spectroscopic frequency shifts due to residual motion of the probed atoms significantly contribute to the uncertainty budgets of state-of-the-art optical ion clocks. For clock transitions with second-order Doppler and quadratic Stark shifts of opposite signs, it is possible to configure electrodynamic ion confinement such that these two shift effects become anticorrelated causing zero net shift. Here, we introduce a spectroscopic interrogation protocol which leads, for systems with unknown and varying motional energy gain rates, to first-order auto-suppression of corresponding frequency shifts without requiring the opposite-sign configuration. We experimentally demonstrate the proposed method on a new ytterbium ion optical clock probing the 467 nm electric octupole (E3) transition, where the combined fractional uncertainty contribution from motion-induced frequency shifts is reduced from $1.3\times10^{-18}$ to $0.3\times10^{-18}$. An interleaved optical frequency ratio measurement against ytterbium's electric quadrupole transition (E2) at 435 nm delivers an E3/E2 frequency ratio of $0.932 \,829 \,404 \,530 \,965 \, 340 (39)$. Combined with previously published ratio data this leads to a limit for a potential fractional temporal variation of the fine-structure constant of $2.4 (2.7) \times 10^{-19}/$yr, in agreement with existing bounds.

physics.atom-ph↗