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At least 487 records · Page 27

Production and transfer of UV photons in non-homogeneous spherical clouds

Due to screening by dust particles, the UV radiation field of interstellar origin is practically inexistent within very dense interstellar clouds. However, it appears possible that the cosmic-ray excitation of the Lyman and Werner systems of the hydrogen molecule could originate a chemically-significant flux of UV photons even within such dense clouds. Computations of photon fluxes were carried out for two different models of radial density distribution inside the cloud (gas and dust densities were assumed to have the same density distribution). The result strongly support the suggestion that the low energy cosmic rays may generate inside dense interstellar clouds UV radiation fields that may significantly contribute to the gas and dust evolution.

Aiello, Santi↗

Scientific applications of frequency-stabilized laser technology in space

A synoptic investigation of the uses of frequency-stabilized lasers for scientific applications in space is presented. It begins by summarizing properties of lasers, characterizing their frequency stability, and describing limitations and techniques to achieve certain levels of frequency stability. Limits to precision set by laser frequency stability for various kinds of measurements are investigated and compared with other sources of error. These other sources include photon-counting statistics, scattered laser light, fluctuations in laser power, and intensity distribution across the beam, propagation effects, mechanical and thermal noise, and radiation pressure. Methods are explored to improve the sensitivity of laser-based interferometric and range-rate measurements. Several specific types of science experiments that rely on highly precise measurements made with lasers are analyzed, and anticipated errors and overall performance are discussed. Qualitative descriptions are given of a number of other possible science applications involving frequency-stabilized lasers and related laser technology in space. These applications will warrant more careful analysis as technology develops.

Schumaker, Bonny L.↗

Accuracy of the Independent Pixel Approximation at Absorbing Wavelengths

In order to correctly interpret shortwave cloud radiation measured by satellites and ground-based radiometers, or by two aircraft flying above and below clouds, we need to better understand interactions between inhomogeneous clouds and solar radiation. The discrepancies between shortwave absorption inferred from measurements and predicted by models, between cloud optical depths estimated from satellites and ground measurements, between single scattering albedo retrieved from in situ radiation measurements and computed from measured droplet size distribution, among others, are strongly affected by cloud horizontal inhomogeneity. Net horizontal photon transport (i. e., horizontal fluxes) are a direct consequence of the inhomoqeneity in cloud structure. Horizontal fluxes and their effect on the accuracy of the pixel-by-pixel one-dimensional (1 D) radiative transfer calculations has recently undergone close scrutiny for conservative scattering. However, the properties and magnitude of horizontal fluxes in absorbing wavelengths are still poorly understood. As far as we are aware, only Ackerman and Cox and Titov discussed correlations between horizontal fluxes at absorbing wavelengths, though these were far from comprehensive. This paper partly fills this gap. We discuss here of whether the accuracy of the Independent Pixel Approximation (IPA), a 1 D radiative transfer approximation for each pixel, is a better model for multiple scattering at conservative or at absorbing wavelengths. Issues addressed here are: (1) dependence of net horizontal fluxes on single scattering albedo; (2) connection between pixel-by-pixel accuracy of the IPA and horizontal fluxes and (3) radiative smoothing and horizontal fluxes at absorbing wavelengths. In contrast to the traditional understanding of IPA, we study IPA accuracies not only for reflectance but also for transmittance and absorptance at both conservative and absorbing wavelengths. In spite of the apparent similarity between the three processes, dependence of IPA accuracies on single-scattering albedo is completely different. As a result, cloud optical properties retrieved from high resolution satellite images and ground-based measurements using IPA at absorbing channels will have different accuracies.

Marchak, Alexander↗

Cloud Droplet Measurement System for the ARM Tethered Balloon System (TBS) Field Campaign Report

The Mesa Photonics' cloud droplet measurement system (CDMS) performs in situ measurement of droplet size distribution and droplet number density in clouds. These characteristics are important cloud microphysical properties that are critical input parameters for atmospheric models and are also useful for proper calibration and validation of performance of other atmospheric measurement instrumentation. This small campaign was the first project (out of two) that involved integration of the CDMS into the U.S. Department of Energy (DOE) Atmospheric Radiation Measurement (ARM) user facility’s tethered balloon system (TBS) and its initial testing at the ARM Southern Great Plains (SGP) atmospheric observatory. The follow-up campaign (AFC07016) involved testing of the CDMS under relevant conditions at the third ARM Mobile Facility (AMF3) at Oliktok Point, Alaska and making in situ measurements in clouds. The goal of this small field campaign was to deploy the CDMS on the ARM TBS, demonstrate its integrity and compatibility with the TBS, and test the wireless telecommunication system in preparation for subsequent in-cloud measurements at ARM’s North Slope of Alaska (NSA) observatory at Utqiagvik (formerly Barrow). The specific technical objectives included: (1) Integration of the Mesa Photonics' CDMS into the ARM TBS, (2) testing of the wireless telecommunication system of the CDMS, (3) evaluating the data acquisition software and image processing algorithms especially under high-background-illumination conditions, and (4) testing the ruggedness of the instrument's optical alignment and other performance characteristics. All objectives have been successfully met. The mounting hardware was designed and built mostly at Sandia National Laboratories (SNL), which allowed reliable mounting of the CDMS on the TBS and co-locating the CDMS with other instruments. The field tests were performed by the principal investigator (PI) in collaboration with the TBS operational crew led by D. Dexheimer. The field testing demonstrated good compatibility of the CDMS with the TBS. During the TBS flights, the crew did not experience any operational issues with the CDMS. The instrument demonstrated reliable operational characteristics, including sufficient battery life and good thermal management. The wireless telecommunication system has been successfully tested at TBS flight altitudes of up to 1000 m. During all flights, the CDMS raw data were wirelessly transmitted to the ground station and processed in real time. The ruggedness of the instrument's optical alignment was evaluated by performing calibration of the CDMS (using Mesa Photonics' fixed-size monodisperse droplet generator) before and after the campaign. The calibration was stable within the instrument's measurement precision. In summary, the campaign demonstrated good compatibility of the Mesa Photonics' CDMS with the ARM TBS. The flight tests confirmed the mechanical integrity of the CDMS and stability of its optical layout, as well as reliability of the wireless telecommunication system. Successful completion of this campaign provided a solid basis for the next campaign (AFC07016, November 2020), that involved testing of the CDMS during in-cloud TBS flights at AMF3 at Oliktok Point.

54 ENVIRONMENTAL SCIENCES↗

The application of the principles of invariance to the radiative transfer equation in plant canopies

Solutions of the radiative transfer equation describing photon interactions with vegetation canopies are important in remote sensing since they provide the canopy reflectance distribution required in the interpretation of satellite acquired information. The general one-dimensional two-angle transport problem for a finite copy of arbitrary leaf angle distribution is considered. Analytical solutions are obtained in terms of generalized Chandrasekhar's X- and Y-functions by invoking the principles of invariance. A critical step in the formulation involves the decomposition of the integral of the scattering phase function into a product of known functions of the incident and scattered photon directions. Several simplified cases previously considered in the literature are derived from the generalized solution. Various symmetries obeyed by the scattering operator and reciprocity relations are formally proved.

Ganapol, B. D.↗

Single-Photon Generation: Materials, Techniques, and the Rydberg Exciton Frontier

Due to their quantum nature, single-photon emitters (SPE) generate individual photons in bursts or streams. They are paramount in emerging quantum technologies such as quantum key distribution, quantum repeaters, and measurement-based quantum computing. Many such systems have been reported in the last three decades, from rubidium atoms coupled to cavities to semiconductor quantum dots and color centers implanted in waveguides. This review article highlights different solid-state and atomic systems with on-demand and controlled single-photon generation. We discuss and compare the performance metrics, such as purity and indistinguishability, for these sources and evaluate their potential for different applications. Finally, a new potential single-photon source, based on the Rydberg exciton in solid-state metal oxide thin films, is introduced, where we discuss its promising features and unique advantages in fabricating quantum chips for quantum photonic applications.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

High-Energy X-ray Diffraction Microscopy for Nuclear Forensics FY2022 Project Report

Morphological information on nuclear material has been identified using visible light and scanning electron microscopy. These identify qualitative differences in particle morphology. Three-dimensional imaging of materials through alternating scanning electron microscopy imaging and focused ion beam milling has also been used. Unfortunately, these techniques are time- and labor-intensive, with significant sample preparation required and lengthy analysis times. Further, the resulting 3D images are qualitative, require manual identification, and do not capture statistically-representative populations. High energy X-ray 3D imaging using a direct-beam or diffracted-beam (High-Energy Diffraction Microscopy) have been developed at the Advanced Photon Source and can produce quantitative information on grains (phase, location, etc.) and pores (size distribution, sphericity) in a material. These techniques require only minutes to characterize a sample volume and are non-destructive, thus suitable for a wide range of existing samples and for confirmatory analyses to be carried out using conventional microscopy techniques. In this first year of the project, all uranium oxide samples were synthesized and characterized using conventional analyses by the analytical chemistry laboratory. Conventional analysis methods included powder x-ray diffraction, scanning electron microscopy, impurity analysis via inductively coupled plasma mass spectrometry, and infrared spectroscopy. Impurity analysis shows a drop in boron content from UO 3 to the lowest U 3 O 8 calcination temperature, but otherwise no appreciable difference in any sample. Analysis of diffraction data shows a flip of peaks from UO 3 dominated for the 600 °C calcined sample to U 3 O 8 dominated at 700 °C and 800 °C. Analysis of scanning electron microscopy images shows that with increased calcination temperature the size distribution of particles seems to increase and broaden. Both of these last findings are in line with previously published data, though this work used significantly fewer particles to simply show similar trends instead of getting truly quantitative particle analysis. Infrared analysis similarly shows ingrowth of U 3 O 8 as calcination temperature is increased, along with depression of peaks associated with UO 3 and water. Samples were prepared for analysis at the Advanced Photon Source at beamline 1-ID. It is anticipated that analysis will occur in November of 2022. AI/ML techniques to de-noise data coming out of 1-ID during the analyses was also developed during this time using previously gathered data. Preliminary results using a self-supervision technique called Noise2Selfshow good de-noising of data. Once the uranium oxide samples are analyzed, real data will be used to test the de-noising and other AI/ML techniques that may be developed in the second year of the project.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Two-photon annihilation of thermal pairs in strong magnetic fields

The annihilation spectrum of pairs with 1-D thermal distributions in the presence of a strong magnetic field is calculated. Numerical analysis of the spectrum are performed for mildly relativistic temperatures and for different angles of emission with respect to field lines. Teragauss magnetic fields are assumed so that conditions are typical of gamma ray burst and pulsar environments. The spectra at each viewing angle reveal asymmetric line profiles that are signatures of the magnetic broadening and red shifting of the line: these asymmetries are more prominent for small viewing angles. Thermal Doppler broadening tends to dominate in the right wing of the line and obscures the magnetic broadening more at high temperatures and smaller viewing angles. This angular dependence of the line asymmetry may prove a valuable diagnostic tool. For low temperatures and magnetic field strengths, useful analytic expressions are presented for the line width, and also for the annihilation spectrum at zero viewing angle. The results presented find application in gamma ray burst and pulsar models, and may prove very helpful in deducing field strengths and temperatures of the emission regions of these objects from line observations made by Compton GRO and future missions.

Baring, Matthew G.↗

Carbon in photon dominated regions: C II/C I/CO observations of NGC 2024

We present observations of the large-scale distribution of the major forms of carbon, neutral and singly ionized atomic carbon and carbon monoxide, in the NGC 2024/Orion B cloud. The overall extent and morphology of the different types of emission are similar, consistent with a picture in which the atomic carbon lies on the UV-illuminated surfaces of molecular clumps throughout the cloud. However, emission from ionized carbon extends considerably farther to the west than the CO emission. Integrated over the region mapped in the 158 mu m (C II) line, about half of the gas-phase carbon is in a form other than CO.

Jaffe, Dan T.↗

Constraints on the galactic distribution of cosmic rays from the COS-B gamma-ray data

The diffuse component of the galactic high energy gamma rays results mainly from the interaction of CR nuclei and electrons with the nuclei of the interstellar gas. An additional contribution is obtained from the interaction of CR electrons with the interstellar photons through the inverse-Compton (IC) process. Gamma ray astronomy therefore offers an excellent means to study the distribution of CR particles throughout the Galaxy, but it is essential to know the distribution of the target interstellar gas particles, the major constituents being atomic and molecular hydrogen. Large scale millimeter wave surveys of the CO molecule covering more than half of the Milky Way, obtained with the Columbia 1.2 m telescopes, are currently available and are used to trace the H2; the COS-B observations have sufficient resolution and sensitivity to constrain the relation between the integrated CO line intensity and the molecular hydrogen column density.

Bloemen, J. B. G. M.↗

Radio to Gamma-Ray Emission from Shell-Type Supernova Remnants: Predictions from Non-Linear Shock Acceleration Models

Supernova remnants (SNRs) are widely believed to be the principal source of galactic cosmic rays, produced by diffusive shock acceleration in the environs of the remnant's expanding blast wave. Such energetic particles can produce gamma-rays and lower energy photons via interactions with the ambient plasma. The recently reported observation of TeV gamma-rays from SN1006 by the CANGAROO Collaboration, combined with the fact that several unidentified EGRET sources have been associated with known radio/optical/X-ray-emitting remnants, provides powerful motivation for studying gamma-ray emission from SNRs. In this paper, we present results from a Monte Carlo simulation of non-linear shock structure and acceleration coupled with photon emission in shell-like SNRs. These non-linearities are a by-product of the dynamical influence of the accelerated cosmic rays on the shocked plasma and result in distributions of cosmic rays which deviate from pure power-laws. Such deviations are crucial to acceleration efficiency considerations and impact photon intensities and spectral shapes at all energies, producing GeV/TeV intensity ratios that are quite different from test particle predictions.

Baring, Matthew G.↗

A Novel Technique for Distributed Measuring of Strain in the Vadose Zone

Characterizing water content and pressure changes in the vadose zone is important to understanding a variety of geologic processes, ranging from permeability, to evapotranspiration, and aquifer recharge. Changes in water content, or pressure, cause strain in the solid porous medium of the vadose zone, and it is possible that measuring those strains could be used a characterization tool. The Coherence-length-gated Microwave Photonics Interferometry (CMPI) technique measures strain at high resolution along many intervals defined by pairs of reflectors distributed along an optical fiber. This technique has recently been developed at Clemson University, and it has the spatial, and temporal resolution to characterize the strains that are expected to occur with hydrologic changes in the vadose zone. However, the technique has never been used to measure strain in porous media, so its capabilities remain uncertain. The objective of this thesis is to evaluate the ability of using CMPI to measure strain changes in the vadose zone. The research approach consists of conducting laboratory tests using a column filled with sand that was subjected to changes in water content and pressure. An optical fiber with CMPI reflectors was deployed in a high surface area ribbon and used to measure strain along the axis of the column. The column was made from 8-inch, Schedule 40 PVC pipe (75 cm tall, 20 cm inner diameter) and filled with medium-grained sand (K = 2.5x10-6 m/s, porosity = 0.28, Coefficient of Uniformity = 2, van Genuchten (n = 4.34 and  = 0.00039 m-1), Young’s Modulus = 18 – 47 MPa). Five pressure and four temperature sensors attached to probes inserted into the wall. The optical fiber includes five reflectors spaced 10 cm apart on the inside and outside of the column along the vertical axis. Strain measurements are made between pairs of reflectors. The reflectors are created in 250-micron-diameter acrylate-coated single mode Corning SMF28e+ optical fiber using a femtosecond laser. The optical fiber was laminated between two pieces of polyester film creating a large surface area to transfer strain from the porous media to the optical fiber. The experiments were conducted by filling the column from the bottom or infiltrating water from the top. The water was allowed to equilibrate to room temperature prior to each test in order to limit thermoelastic strain. Five injection tests with a rate of 250 ml/min and three infiltration tests at varying rates were conducted, and the results show patterns of strain and pressure are generally similar. Hydrologic conditions define three zones based on the pressure magnitude and distribution. 1.) Ambient Zone where the pressure heads are quasi-static and the pressure gradient is roughly unity (head gradient of zero). This is the uppermost zone and is characterized by negative pressures. 2.) Transition Zone where the pressures increase from ambient to zero, are changing relatively rapidly and the pressure gradient is relatively steep (pressure head gradients of 2). The Transition zone is 10 to 15 cm thick. 3.) Positive Pressure Zone where the pressure is positive, the rate of change is slower than in the transition zone and the gradient is flatter (pressure head gradient 1.1 to 1.2). This is the lowest zone in the column. Injection of water causes the pressure to increase and the three zones to move upward. The Transition zone moves at a rate of approximately 0.0002 m/s +/- .00005, according to analyses of pressure profiles. This is the same as the average velocity of the water calculated as volumetric flux/effective porosity =5.4x10-5 m/s/0.28. Strain signals in the range of 10s  were observed with a noise level of generally less than 0.1  (signal to noise ratio of greater than 100) during injection and drainage. The spatial and temporal distributions of strain caused by injection depend on the location of the moving pressure zones. The locations of the different pressure zones were determined from pressure profiles at different times and these data were transferred to strain time series. This showed that strain in the Ambient pressure zone is either unchanged or slightly compressive, whereas strain in Transition zone is tensile and roughly proportional to the pressure change, and strain ranges from tensile to compressive in the Positive Pressure zone. In general, the strain is variable at the top of the Positive Pressure zone, but it appears to be consistently tensile lower in the zone. The spatial distribution of strain causes three distinct stages in the strain times series measured between pairs of CMPI reflectors. The strain is unchanged or slightly compressive during Stage 1, it increases (positive strain is tensile) approximately linearly at a rate of 0.02 to 0.03 μ/s during the Stage 2, and then flattens out in Stage 3. The strain increases again during Stage 4 of the time series. The pressure also changes in stages. It is unchanged during Stage 1 and then increases relatively rapidly at a rate of between 4 and 10 Pa/s during Stage 2 and continues to increase during Stages 3 and 4, but at a rate slightly slower than during Stage 2 (from 2.5 to 3.5 Pa/s). The rates of pressure and strain change are consistent with basic analyses. The rate of pressurization is similar to the calculated velocity of flow in the saturated zone, and this is similar to the measured velocity of the strain increase. The ratio of the pressurization rate and strain rate during Stage 2 (2.5 (Pa/s) /0.03 (μ/s)) is 80 MPa, which is approximately equal to the upper range expected considering the uniaxial compression and the Young’s Modulus of the sand. An interesting effect occurs when the upper surface of the sand becomes saturated. Significant compression (several 10s of ) occurs as the pressure and saturation increase at the upper surface. Compression occurs throughout the column, but the effect is greatest at the top of the column. The rate of compression is fastest slightly before ponding occurs, but it slows markedly and nearly stops when water starts to accumulate at the surface (ponding). This effect reverses when the surface of the sand is drained, resulting in tension throughout the column. The compression caused by this effect can be as large or larger than the tensile strain that accumulated during filling. This effect was unexpected because increasing pressure is normally associated with tensile strain. Nevertheless, this effect was observed consistently in all tests where the pressure changes at the upper surface, including tests where water was injected from below or infiltrated from above. This effect behaves as if the pore pressure at the upper surface of the sand exerts a normal force on the boundary (increasing pore pressure exerts a downward compression on the boundary). The results of these laboratory experiments indicate that CMPI can measure strain caused by fluid pressure changes in the vadose zone with a signal to noise ratio of 100 or more. Injection and drainage cause a strain signal that is complex, but repeatable. The magnitudes of the strain signal are consistent with magnitudes that are expected based on poroelastic calculations using independently measured properties of the sand. These results indicate that the CMPI technique with an optical fiber laminated in a polyester ribbon generates data that represent the strain distribution during hydrologic processes of imbibition and drainage in variably saturated sand. This suggests that distributed strain measurements using CMPI could be a viable approach for evaluating processes in the vadose zone, laying the groundwork for future field implementation.

47 OTHER INSTRUMENTATION↗

High-efficiency microwave-optical quantum transduction based on a cavity electro-optic superconducting system with long coherence time

Abstract Frequency conversion between microwave and optical photons is a key enabling technology to create links between superconducting quantum processors and to realize distributed quantum networks. We propose a microwave-optical transduction platform based on long-coherence time superconducting radio-frequency (SRF) cavities coupled to electro-optic optical cavities to mitigate the loss mechanisms that limit the attainment of high conversion efficiency. We optimize the microwave-optical field overlap and optical coupling losses in the design while achieving long microwave and optical photon lifetime at milli-Kelvin temperatures. This represents a significant enhancement of the transduction efficiency up to 50% under incoming pump power of 140 μW, which allows the conversion of few-photon quantum signals. Furthermore, this scheme exhibits high resolution for optically reading out the dispersive shift induced by a superconducting transmon qubit coupled to the SRF cavity. We also show that low microwave losses enhance the fidelity of heralded entanglement generation between two remote quantum systems. Finally, high precision in quantum sensing can be reached below the standard quantum limit.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Visualization of a Limonene Synthesis Metabolon Inside Living Bacteria by Hyperspectral SRS Microscopy

Abstract Monitoring biosynthesis activity at single‐cell level is key to metabolic engineering but is still difficult to achieve in a label‐free manner. Using hyperspectral stimulated Raman scattering imaging in the 670–900 cm −1 region, localized limonene synthesis are visualized inside engineered Escherichia coli . The colocalization of limonene and GFP‐fused limonene synthase is confirmed by co‐registered stimulated Raman scattering and two‐photon fluorescence images. The finding suggests a limonene synthesis metabolon with a polar distribution inside the cells. This finding expands the knowledge of de novo limonene biosynthesis in engineered bacteria and highlights the potential of SRS chemical imaging in metabolic engineering research.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Large field-of-view event-mode camera for high-precision epithermal neutron resonance imaging

A large-area event-mode camera system coupled with a 6 LiF-ZnS:Ag scintillator is applied for neutron resonance imaging (NRI) on the energy-resolved neutron imaging (ERNI) flight path, also known as Flight Path 5 (FP5), at the Los Alamos Neutron Science Center (LANSCE). This novel neutron imaging system, featuring a 120 x 120 mm 2 field of view, efficiently captures resonance information across the entire image in a single acquisition, significantly reducing beam time requirements compared to conventional energy-resolved neutron imaging systems. High-quality neutron radiographs with enhanced spatial resolution are achieved through the reconstruction of neutron events based on observations of individual photons emitted from the scintillator. The system demonstrates reduced background through neutron/gamma discrimination capabilities while maintaining sharpness across a large fields of view. In the measurements presented here, a spatial resolution of approximately 340 μm was achieved using center-of-gravity photon cluster centroiding. We demonstrate the system’s capability for quantitatively determining isotopic distributions in various thin samples, as well as automatically reconstructing complex scenes with overlapping resonances from diverse samples. These results are obtained using standard data analysis tools, despite the relatively slow 6 LiF-ZnS:Ag scintillator, which may not be optimal for absorption resonance detection. The capabilities demonstrated here offer a valuable, versatile, and cost-effective solution for high spatial and temporal resolution, large field-of-view energy-resolved neutron imaging, with potential applications across various scientific and industrial domains.

36 MATERIALS SCIENCE↗

Ionization of helium by an ultrashort extreme-ultraviolet laser pulse

We theoretically study photoelectron angular distributions and related anisotropy parameters for the competition of one- and two-photon ionization of He in an ultrashort extreme-ultraviolet laser pulse, using numerical results from the time-dependent Schrödinger equation. We explore the transition between the two processes for variation of the pulse duration, peak intensity, and central frequency or photoelectron energy. In the results obtained for fixed pulse parameters the transition and interference between the processes can be observed in the even (β 2 , β 4 ) and odd (β 1 , β 3 ) parameters, respectively, while the onset of the impact of three-photon ionization is observed via β5 at high peak intensities. Lastly, we show that the transition can be observed via the even anisotropy parameters in pulses without carrier-to-envelope stabilization as well as in free-electron laser pulses with fluctuating pulse shape.

74 ATOMIC AND MOLECULAR PHYSICS↗

Resonance-enhanced x-ray multiple ionization of a polyatomic molecule

Extremely high charge states of atoms and molecules can be created when they are irradiated by intense x-ray pulses. At certain x-ray photon energies, electron ejection from atoms can be drastically enhanced by transient resonances created during the sequential ionization process. In this study we report on the observation of such resonance effects in a molecule, CH 3 I, and show the photon-energy-dependent shift of resonance-induced structures in ion charge state distributions. By comparing the ion charge state distribution of CH 3 I with that from ionization of atomic xenon, molecule-specific features are observed, which can be attributed to ultrafast intramolecular charge rearrangement. In addition, we experimentally demonstrate that the charge-rearrangement-enhanced x-ray ionization of molecules, previously found with hard x rays, also plays a role in the soft x-ray regime.

74 ATOMIC AND MOLECULAR PHYSICS↗

Rephasing spectral diffusion in time-bin spin-spin entanglement protocols

Generating high-fidelity spin-spin entanglement is an essential task of quantum repeater networks for the distribution of quantum information across long distances. Solid-state-based spin-photon interfaces are promising candidates to realize nodes of a quantum network, but are often limited by spectral diffusion of the optical transition, which results in phase errors on the entangled states. Here, we introduce a method to correct phase errors from quasi-static frequency fluctuations after the entangled state is generated, by shelving the emitters in the excited state to refocus the unknown phase. For quasi-static frequency fluctuations, the fidelity is determined only by the lifetime of the excited state used for shelving, making it particularly suitable for systems with a long-lived shelving state with correlated spectral diffusion. Such a shelving state may be found in Kramers doublet systems such as rare-earth emitters and color centers in Si or SiC interfaced with nanophotonic cavities with a strongly frequency-dependent Purcell enhancement. Furthermore, the protocol can be used to generate high-fidelity entangled spin pairs without reducing the rate of entanglement generation.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗