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At least 37 records · Page 2

Revealing ultrafast proton-transfer-mediated autoionization as a source of low-energy electrons in hydrogen-bonded systems

Ionizing radiation can trigger ultrafast proton transfer, a central mechanism in many chemical and biological functions, that in turn can enable or suppress electron relaxation processes and consequently cause abrupt changes in the reaction pathway. This study combines theory and experiment to probe ultrafast relaxation and dissociation in water dimers following inner- and outer-valence photoionization. By tracking electron and nuclear motion simultaneously, we reveal competing fragmentation pathways that produce low-energy electrons, which are key agents in radiation-induced chemistry, including DNA damage. While low-energy electrons are known to arise via intermolecular Coulombic decay, here we identify a faster relaxation mechanism gated by proton transfer following inner-valence ionization, which we call proton-transfer-mediated autoionization. Occurring within 10 femtoseconds, this process alters fragmentation outcomes, yielding either D 3 O + + OD + or D 2 O + + D 2 O + , depending on the interplay of proton migration and hydrogen back-transfer. Our findings underscore the intricate coupling between electronic and nuclear dynamics in hydrogen-bonded systems and establish proton-transfer-mediated autoionization as a significant pathway for low-energy electron generation.

Atomic and molecular interactions with photons

Optomechanical self-organization in a mesoscopic atom array

Increasing the number of particles in a system often leads to qualitative changes in its properties, such as breaking of symmetries and the appearance of phase transitions. This renders a macroscopic system fundamentally different from its individual microscopic constituents. Lying between these extremes, mesoscopic systems exhibit microscopic fluctuations that influence behaviour on longer length scales, leading to critical phenomena and dynamics. Therefore, tracing the properties of well-controlled mesoscopic systems can help bridge the gap between an exact description of few-body microscopic systems and the emergent description of many-body systems. Here we explore the mesoscopic signatures of an optomechanical self-organization phase transition using arrays of cold atoms inside an optical cavity. By precisely engineering atom–cavity interactions, we reveal how critical behaviour depends on the atom number, identify characteristic dynamical behaviours in the self-organized regime and observe a finite optomechanical susceptibility at the critical point. These findings advance our understanding of particle-number- and time-resolved properties of phase transitions in mesoscopic systems.

Atomic and molecular interactions with photons

Photoerosion and the abundances of the light elements

The abundances of the rare light elements H-2, He-3, Li-7, and B-11 are shown to be potentially affected by photoerosion. That process, involving the interaction of high energy photons from galactic centers with atomic nuclei, will increase the abundances of H-2, He-3, and B-11 while lowering slightly those of Li-7 and He-4. In some regions of galaxies the effects may be large enough to impact their chemical evolution. In particular this process may have enhanced the H-2 and He-3 abundances near the center of our galaxy over and above those from the big bang, as well as the galactic B-11 abundance over that from cosmic-ray spallation.

Boyd, Richard N.

Photoerosion and the abundances of the light elements

The abundances of the rare light elements H-2, He-3, Li-7, and B-11 are shown to be potentially affected by photoerosion. That process, involving the interaction of high energy photons from galactic centers with atomic nuclei, will increase the abundances of H-2, He-3, and B-11 while lowering slightly those of Li-7 and He-4. In some regions of galaxies the effects may be large enough to impact their chemical evolution. In particular, this process may have enhanced the H-2 and He-3 abundances near the center of our galaxy over and above those from the big bang, as well as the galactic B-11 abundance over that from cosmic-ray spallation.

Boyd, Richard N.

Formation of cosmic structure by Doppler instability

A new mechanism is described which can create an instability in homogeneous gaseous matter at very low density. When an isotropic background radiation field has, near an electronic resonance, a spectral feature for which photon occupation number increases with frequency, moving atoms increase their speed by taking energy from the photon distribution. In a cosmological setting, a sufficiently intense spectral feature can interact with neutral atomic gas, after recombination, to generate protogalactic perturbations of the scale and magnitude needed to explain large-scale cosmic structure.

Hogan, Craig J.

Prototype X-ray and Gamma Detection with Cyclotron Radiation Emission Spectroscopy

Cyclotron radiation emission spectroscopy, or CRES, is a novel approach to measuring the energy of an electron. By trapping a free electron in a high magnetic field, it undergoes cyclotron motion and emits radiofrequency (RF) waves. The frequency of this RF radiation is directly related to the energy of the electron. Because many cycles of the RF emission are recorded, the energy resolution of the CRES system is on the order of a single electron volt. To make a CRES system sensitive to photons, a target gas is used to induce a photoelectric effect, producing the electron that is subsequently trapped. By adding the binding energy of the target atom, the energy of the incident photon may be reconstructed. Using a xenon target gas, photoelectric interactions dominate up to approximately 300 keV, covering not only all atomic shell X-rays of the elements, but many low-lying nuclear states as well, including key transuranic elements related to nuclear security. CRES holds the potential of maintaining single-eV resolution up to this 300-keV range, thereby surpassing current state-of-the-art detectors by a factor of 10-100. The instrumental resolution of the system is limited by the uniformity of the applied magnetic field.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND

Flow Property Measurement Using Laser-Induced Fluorescence in the NASA Ames Interaction Heating Facility

The spectroscopic diagnostic technique of two photon absorption laser-induced fluorescence (TALIF) of atomic species has been applied to single-point measurements of velocity and static temperature in the NASA Ames Interaction Heating Facility (IHF) arc jet. Excitation spectra of atomic oxygen and nitrogen were recorded while scanning a tunable dye laser over the absorption feature. Thirty excitation spectra were acquired during 8 arc jet runs at two facility operating conditions; the number of scans per run varied between 2 and 6. Curve fits to the spectra were analyzed to recover their Doppler shifts and widths, from which the flow velocities and static temperatures, respectively, were determined. An increase in the number of independent flow property pairs from each as-measured scan was obtained by extracting multiple lower-resolution scans. The larger population sample size enabled the mean property values and their uncertainties for each run to be characterized with greater confidence. The average plus or minus 2 sigma uncertainties in the mean velocities and temperatures for all 8 runs were plus or minus 1.4% and plus or minus 11%, respectively.

Grinstead, Jay Henderson

Coherent Magnon–Photon Coupling in the Magnetic Semiconductor CrSBr

Magnon-based hybrid quantum systems are promising candidates for quantum interconnects and quantum sensors, and they offer a rich platform for exploring nonlinear magnonics and cavity–photon interactions. Two-dimensional (2D) van der Waals magnets provide a compact, atomically flat geometry that can be easily integrated into existing quantum circuits, such as superconducting resonators and qubits. Among various 2D magnets, the magnetic semiconductor CrSBr is particularly unique due to its strong spin–exciton, spin–lattice, and magnon–exciton interactions. In this work, we demonstrate coherent coupling between antiferromagnetic (AFM) magnons in CrSBr and microwave photons in a niobium-(Nb)-based-on-chip resonator. We tuned the magnon–photon coupling strength by changing the number of CrSBr flakes integrated into the Nb microwave photon resonators. Furthermore, this work demonstrates the first step toward integrating layered van der Waals 2D magnets into superconducting microwave circuits, with full access for microwave and optical probing.

Electromagnetic radiation

Calculating the X-Ray Fluorescence from the Planet Mercury Due to High-Energy Electrons

The least-studied terrestrial planet is Mercury due to its proximity to the Sun, which makes telescopic observations and spacecraft encounters difficult. Our lack of knowledge about Mercury should change in the near future due to the recent launching of MESSENGER, a Mercury orbiter. Another mission (BepiColombo) is currently being planned. The x-ray spectrometer on MESSENGER (and planned for BepiColombo) can characterize the elemental composition of a planetary surface by measuring emitted fluorescent x-rays. If electrons are ejected from an atom s inner shell by interaction with energetic particles such as photons, electrons, or ions, electrons from an outer shell can transfer to the inner shell. Characteristic x-rays are then emitted with energies that are the difference between the binding energy of the ion in its excited state and that of the ion in its ground state. Because each element has a unique set of energy levels, each element emits x-rays at a unique set of energies. Electrons and ions usually do not have the needed flux at high energies to cause significant x-ray fluorescence on most planetary bodies. This is not the case for Mercury where high-energy particles were detected during the Mariner 10 flybys. Mercury has an intrinsic magnetic field that deflects the solar wind, resulting in a bow shock in the solar wind and a magnetospheric cavity. Electrons and ions accelerated in the magnetosphere tend to follow its magnetic field lines and can impact the surface on Mercury s dark side Modeling has been done to determine if x-ray fluorescence resulting from the impact of high-energy electrons accelerated in Mercury's magnetosphere can be detected by MESSENGER. Our goal is to understand how much bulk chemical information can be obtained from x-ray fluorescence measurements on the dark side of Mercury.

Burbine, T. H.

Realization of three- and four-body interactions between momentum states in a cavity

Spin Hamiltonians in condensed matter and quantum sensing typically utilize pairwise or two-body interactions between constituents in the material or ensemble. However, there is growing interest in exploring more general n-body interactions for n > 2. In this study, we realized an effective n = 3-body Hamiltonian interaction using an ensemble of laser-cooled atoms in a high-finesse optical cavity with the pseudospin 1/2 encoded by two atomic momentum states. We applied two dressing tones that induce the atoms to exchange photons via the cavity to realize a virtual six-photon process; lower-order interactions destructively interfered. We also observed signatures of a n = 4-body interaction mediated by a virtual eight-photon process. Our approach may be extensible to three-body interactions in multilevel systems or to even higher-order interactions.

Luo, Chengyi [University of Colorado, Boulder, CO

Cooperative effects in thin dielectric layers: Long-range Dicke superradiance

The realization and control of collective quantum effects so far have predominantly focused on cold atomic ensembles. Quantum photonic platforms, with their engineered Green's functions and integration capability of advanced solid-state quantum emitters, provide opportunities to explore regimes of light-matter interaction beyond the scope of atomic systems. In this work, we demonstrate that embedding quantum emitters within a thin dielectric layer fundamentally alters their collective radiative behavior. The optical modes in the dielectric layer mediate long-range dipole-dipole interactions between emitters, enabling both total and directional superradiance between emitters separated by several wavelengths. Crucially, this mechanism supports Dicke superradiance even in parameter regimes where standard settings fail to support an interaction, unveiling a dimensionality-driven enhancement of cooperative effects. By bridging many-body quantum optics and photonic engineering, our work reveals a distinct interplay between surrounding dimensionality and collective quantum dynamics. Experimental realization of these predictions, readily achievable in solid-state quantum optics platforms, paves the way for scalable, directional quantum light sources and frontiers in many-body quantum optics.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC

Populating excited states of incoherent atoms using coherent light.

Study of the influence of various experimental parameters on the interaction between a multimode high-intensity laser light and the absorbing atoms of an atomic gas. Using a simplified treatment of line broadening which does not include correlations between momentum-changing collisions and pressure-broadening collisions, expressions are obtained that show the effect of pressure, laser-pulse length, and intensity on the excitation. It is found that, as long as the dephasing time of the atomic system is sufficiently short, the interaction reduces to a two-body collision between the atoms and photons, where coherence effects do not occur.

Mcilrath, T. J.

Gamma rays, cosmic rays, and galactic structure

Observations of cosmic and gamma radiation by SAS-2 satellite are summarized and analyzed to determine processes responsible for producing observed galactic radiation. In addition to the production of gamma rays in discrete galactic objects such as pulsars, there are three main mechanisms by which high-energy (greater than 100 MeV) radiation is produced by high-energy interactions involving cosmic rays in interstellar space. These processes, which produce what may be called diffuse galactic gamma-rays, are: (1) the decay of pi mesons produced by interactions of cosmic ray nucleons with interstellar gas nuclei; (2) the bremsstrahlung radiation produced by cosmic ray electrons interacting in the Coulomb fields of nuclei of interstellar gas atoms; and (3) Compton interactions between cosmic ray electrons and low-energy photons in interstellar space.

Stecker, F. W.

Gamma-ray observations of Ophiuchus with EGRET: The diffuse emission and point sources

Observations of the Ophiuchus region made with the Energetic Gamma-Ray Experiment Telescope (EGRET) on the Compton Gamma Ray Observatory (CGRO) during the first 2 1/2 years of operation show the diffuse emission from the interstellar gas in Ophiuchus as well as variable emission from two point sources. The gamma-ray emission is modeled in terms of cosmic-ray interactions with atomic and molecular hydrogen in Ophiuchus and with low-energy photons along the line of sight. The model also includes the flux from the two point sources and an isotropic diffuse contribution. The cosmic-ray density is assumed to be uniform. The derived ratio of molecular hydrogen column density to integrated CO intensity is (1.1 +/- 0.2) x 10(exp 20) H-mols/sq cm (K km/s)(exp -1). At the sensitivity and resolution of the gamma-ray data, no variation of this ratio over the modeled region is discernible, nor are any regions of enhanced cosmic-ray density apparent. The model was fitted to seven narrow energy bands to obtain the energy depedence of the gamma-ray production function and the spectra of the point sources. The derived production function is in good agreement with theoretical calculations and the local cosmic-ray electron and proton spectra. The positions of the point sources were determined from maximum likelihood analysis of the gamma-ray emission observed in excess of the diffuse model. We identify one point source with the quasar PKS 1622-253, which has an average flux, E greater than 100 MeV, of (2.5 +/- 0.5) x 10(exp -7) photons/sq cm/s and photon spectral index -1.9 +/- 0.3. The other source, denoted GRO J1631-27, has not yet been identified at other wavelengths. Its average flux, E greater than 100 MeV, is (1.1 +/- 0.4) x 10(exp -7) photons/sq cm/s; however, its spectral index is poorly determined. The spectral index and intensity of the isotropic contribution to the model agree well with the extragalactic diffuse emission derived from the SAS 2 data.

Hunter, S. D.

Ultrafast studies of elusive chemical reactions in the gas phase

The chemical composition of the interstellar medium and planetary atmospheres is constantly in flux as atoms and molecules collide and interact with high-energy particles such as electrons, protons, and photons. These transformative processes ultimately lead to the coalescence of molecules and eventually the birth of stars. Our understanding of these chemical ecosystems relies on models that synthesize data from gas-phase experiments, providing insights into reaction cross sections. This Review examines efforts to delve into the fundamental bond-forming and bond-breaking dynamics that occur during bimolecular and electron-initiated reactions. Furthermore, these experiments involve clever approaches to establish a time reference and the collision geometry necessary for tracking atomic motion with femtosecond time resolution. Findings from these efforts enhance present models and improve predictions for molecule-molecule and electron-molecule collisions.

74 ATOMIC AND MOLECULAR PHYSICS

Research on the properties and interactions of simple atomic and ionic systems

Simple ionic systems were studied, such as metastable autoionizing states of the negative He ion, two-photon decay spectrum of metastable He ion, optical excitation with low energy ions, and lifetime measurements of singly ionized Li and metastable He ion. Simple atomic systems were also investigated. Metastable autoionizing atomic energy levels in alkali elements were included, along with lifetime measurements of Cr-53, group 2A isotopes, and alkali metal atoms using level crossing and optical double resonance spectroscopy.

Novick, R.

Indistinguishable photons from an artificial atom in silicon photonics

Silicon is the ideal material for building electronic and photonic circuits at scale. Integrated photonic quantum technologies in silicon offer a promising path to scaling by leveraging advanced semiconductor manufacturing and integration capabilities. However, the lack of deterministic quantum light sources and strong photon-photon interactions in silicon poses a challenge to scalability. In this work, we demonstrate an indistinguishable photon source in silicon photonics based on an artificial atom. We show that a G center in a silicon waveguide can generate high-purity telecom-band single photons. We perform high-resolution spectroscopy and time-delayed two-photon interference to demonstrate the indistinguishability of single photons emitted from a G center in a silicon waveguide. Our results show that artificial atoms in silicon photonics can source single photons suitable for photonic quantum networks and processors.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC

General properties of quantum optical systems in a strong field limit

We investigate the dynamics of an arbitrary atomic system (n-level atoms or many n-level atoms) interacting with a resonant quantized mode of an em field. If the initial field state is a coherent state with a large photon number then the system dynamics possesses some general features, independently of the particular structure of the atomic system. Namely, trapping states, factorization of the wave function, collapses and revivals of the atomic energy oscillations are discussed.

Chumakov, S. M.