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arXiv:2502.15911

Time-resolved 3D momentum spectroscopy in continuous wave atomic photoionization

K. L. Romans, B. P. Acharya, A. H. Nishshanka. C. De Silva, Foster, Kyle, O. Russ, Fischer, Daniel

Published Feb 21, 2025• 0 citations
arXivHTMLPDF

Abstract

An experimental continuous-wave (cw) pump-probe scheme is demonstrated by investigating the population and photoionization dynamics of an atomic system. Specifically, $^6$Li atoms are initially prepared in optically pumped $2^{2}S_{1/2}$ and $2^{2}P_{3/2}$ states before being excited via multi-photon absorption from a tunable femtosecond laser. The subsequent cascade back to the ground state is analyzed by ionizing the atoms in the field of a cw optical dipole trap laser. Conventional spectroscopic methods such as standard cold-target recoil-ion momentum spectroscopy (COLTRIMS) or velocity map imaging (VMI) cannot provide simultaneous momentum and time-resolved information on an event-by-event basis for the system investigated here. The new approach overcomes this limitation by leveraging electron-recoil ion coincidences, momentum conservation, and the cyclotron motion of the photoelectron in the magnetic spectrometer field. This enables the reconstruction of ionization times and time-of-flight of the charged target fragments with nanosecond resolution. As a result, not only can three-dimensional photoelectron momentum vectors be determined, but the (incoherent) population dynamics of the atomic system also become accessible. Future applications exploring coherent atomic dynamics on the nanosecond timescale would not only expand the scope of time-resolved spectroscopy but can also aid in developing coherent control schemes for precise atomic manipulation.

DOI
10.48550/arxiv.2502.15911

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An experimental continuous-wave (cw) pump-probe scheme is demonstrated by investigating the population and photoionization dynamics of an atomic system. Specifically, 6^66Li atoms are initially prepared in optically pumped 22S1/22^{2}S_{1/2}22S1/2​ and 22P3/22^{2}P_{3/2}22P3/2​ states before being excited via multi-photon absorption from a tunable femtosecond laser. The subsequent cascade back to the ground state is analyzed by ionizing the atoms in the field of a cw optical dipole trap laser. Conventional spectroscopic methods such as standard cold-target recoil-ion momentum spectroscopy (COLTRIMS) or velocity map imaging (VMI) cannot provide simultaneous momentum and time-resolved information on an event-by-event basis for the system investigated here. The new approach overcomes this limitation by leveraging electron-recoil ion coincidences, momentum conservation, and the cyclotron motion of the photoelectron in the magnetic spectrometer field. This enables the reconstruction of ionization times and time-of-flight of the charged target fragments with nanosecond resolution. As a result, not only can three-dimensional photoelectron momentum vectors be determined, but the (incoherent) population dynamics of the atomic system also become accessible. Future applications exploring coherent atomic dynamics on the nanosecond timescale would not only expand the scope of time-resolved spectroscopy but can also aid in developing coherent control schemes for precise atomic manipulation.
An experimental continuous-wave (cw) pump-probe scheme is demonstrated by investigating the population and photoionization dynamics of an atomic system. In particular, 6Li atoms are initially prepared in optically pumped 22S1/2 and 22P3/2 states before being excited via multi-photon absorption from a tunable femtosecond laser. The subsequent cascade back to the ground state is analyzed by ionizing the atoms in the field of a cw optical dipole trap laser. Conventional spectroscopic methods, such as standard cold-target recoil ion momentum spectroscopy or velocity map imaging, cannot provide simultaneous momentum and time-resolved information on an event-by-event basis for the system investigated here. The new approach overcomes this limitation by leveraging electron-recoil ion coincidences, momentum conservation, and the cyclotron motion of the photoelectron in the magnetic spectrometer field. This enables the reconstruction of ionization times and time-of-flight of the charged target fragments with nanosecond resolution. As a result, not only can three-dimensional photoelectron momentum vectors be determined, but the (incoherent) population dynamics of the atomic system also become accessible. Future applications exploring coherent atomic dynamics on the nanosecond timescale would not only expand the scope of time-resolved spectroscopy but can also aid in developing coherent control schemes for precise atomic manipulation.
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Rydberg atoms are in the focus of intense research due to the peculiar properties which make them interesting candidates for quantum optics and quantum information applications. In this work we study the ionization of Rydberg atoms due to their interaction with a trapping laser field, and a reaction microscope is used to measure photoelectron angular and energy distributions. Reaction microscopes are excellent tools when brandished against atomic photoionization processes involving pulsed lasers; the timing tied to each pulse is crucial in solving the subsequent equations of motion for the atomic fragments in the spectrometer field. However, when used in pump-probe schemes, which rely on continuous wave probe lasers, vital information linked to the time of flight is lost. This study reports on a method in which the standard ReMi technique is extended in time through coincidence measurements. This is then applied to the photoionization of 6^66Li atoms initially prepared in optically pumped 22S1/22^{2}S_{1/2}22S1/2​ and 22P3/22^{2}P_{3/2}22P3/2​ states. Multi-photon excitation from a tunable femtosecond laser is exploited to produce Rydberg atoms inside an infrared optical dipole trap; the structure and dynamics of the subsequent cascade back towards ground is evaluated.
In this work, we study the coherent dynamics of an atomic Zeeman wave packet using a continuous pump--probe scheme. A polarized wave packet is generated via few-photon excitation by a femtosecond laser pulse, creating a state with a magnetic moment tilted relative to an external magnetic field. The subsequent Larmor precession of the atoms is probed by continuous ionization in the field of an optical dipole trap (ODT) laser. Photoelectrons and photoions are detected in coincidence using a cold target recoil ion momentum spectrometer (COLTRIMS). While the addition of the ODT enables further cooling of the atomic ensemble, it removes the pulsed timing reference typically used to extract photoelectron momentum distributions in COLTRIMS. Here, we present a method that extends the standard COLTRIMS technique by exploiting redundancy in the measured data to reconstruct the time of ionization. The resulting time-dependent ionization signal reflects the coherent precession of the atomic magnetic moment, enabling real-time access to atomic dynamics on nanosecond timescales.
Photoionization induced by trapping and auxiliary laser fields is an inherent feature of many laser-cooling and optical trapping experiments, yet its microscopic dynamics are rarely investigated directly. In this work, we employ a reaction microscope implementing an event-by-event photoionization time retrieval technique to extend momentum-resolved photoelectron spectroscopy to continuous-wave laser--atom interactions. We investigate low-intensity multicolor photoionization of laser-cooled lithium atoms confined in an all-optical trap. Complete three-dimensional electron momentum distributions and kinetic-energy spectra recorded for different laser wavelengths and polarization configurations identify resonant excitation of the 5p5p5p and 5f5f5f states and reveal an additional ionization channel following spontaneous decay from the 5f5f5f to the 4d4d4d state. A pronounced polarization dependence of the photoionization yield is explained by magnetic-sublevel selection rules and the coherent interference of different virtual excitation pathways. These results demonstrate that reaction microscopy combined with event-by-event time reconstruction provides a powerful approach for investigating microscopic electronic dynamics in laser-cooled atomic systems and offers new insight into photoionization processes occurring during optical trapping.
Coherent control provides a quantum interference based method for controlling atomic and molecular dynamics. We report two experimental observations of different ways to achieve such a control in atomic photoionization continuum. One is the photoionization of sodium atoms, initially prepared in the 3P1/2 excited state, by a non resonant three-photon interaction with 1064-nm laser light and by a one-photon interaction with the third-harmonic field, at 355 nm. Interference between the two transition paths allows the control of the total ionization rate by varying the relative phase of the laser fields. The second experiment is the observation of the modification of the ionization continua of xenon through laser induced continuum structure (LICS). The multiphoton radiative decay of the xenon ground state into the two electronic continua, that correspond to the two fine structure levels of the ground state of the xenon ion, is varied by electromagnetically embedding a bound state of the atom into the two continua. Both experiments are performed on an atomic beam apparatus which uses a time-of-flight spectrometer for energy analyzing the emitted photoelectrons.