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At least 127 records · Page 7

Coherent diffractive imaging with twisted X-rays: Principles, applications, and outlook

Recent technological breakthroughs in synchrotron and x-ray free electron laser facilities have revolutionized nanoscale structural and dynamic analyses in condensed matter systems. This review provides a comprehensive overview of the advancements in coherent scattering and diffractive imaging techniques, which are now at the forefront of exploring materials science complexities. These techniques, notably Bragg coherent diffractive imaging and x-ray photon correlation spectroscopy, x-ray magnetic dichroism, and x-ray correlation analysis leverage beam coherence to achieve volumetric three-dimensional imaging at unprecedented sub-nanometer resolutions and explore dynamic phenomena within sub-millisecond timeframes. Such capabilities are critical in understanding and developing advanced materials and technologies. Simultaneously, the emergence of chiral crystals—characterized by their unique absence of standard inversion, mirror, or other roto-inversion symmetries—presents both challenges and opportunities. These materials exhibit distinctive interactions with light, leading to phenomena such as molecular optical activity, chiral photonic waveguides, and valley-specific light emissions, which are pivotal in the burgeoning fields of photonic and spintronic devices. This review elucidates how novel x-ray probes can be leveraged to unravel these properties and their implications for future technological applications. A significant focus of this review is the exploration of new avenues in research, particularly the shift from conventional methods to more innovative approaches in studying these chiral materials. Inspired by structured optical beams, the potential of coherent scattering techniques utilizing twisted x-ray beams is examined. This promising direction not only offers higher spatial resolution but also opens the door to previously unattainable insights in materials science. By contextualizing these advancements within the broader scientific landscape and highlighting their practical applications, this review aims to chart a course for future research in this rapidly evolving field.

Physics↗

Hidden vibronic and excitonic structure and vibronic coherence transfer in the bacterial reaction center

We report two-dimensional electronic spectroscopy (2DES) experiments on the bacterial reaction center (BRC) from purple bacteria, revealing hidden vibronic and excitonic structure. Through analysis of the coherent dynamics of the BRC, we identify multiple quasi-resonances between pigment vibrations and excitonic energy gaps, and vibronic coherence transfer processes that are typically neglected in standard models of photosynthetic energy transfer and charge separation. We support our assignment with control experiments on bacteriochlorophyll and simulations of the coherent dynamics using a reduced excitonic model of the BRC. We find that specific vibronic coherence processes can readily reveal weak exciton transitions. While the functional relevance of such processes is unclear, they provide a spectroscopic tool that uses vibrations as a window for observing excited state structure and dynamics elsewhere in the BRC via vibronic coupling. Vibronic coherence transfer reveals the upper exciton of the “special pair” that was weakly visible in previous 2DES experiments.

59 BASIC BIOLOGICAL SCIENCES↗

Collection and processing of data from a phase-coherent meteor radar

An analysis of the measurement accuracy requirement of a high resolution meteor radar for observing short period, atmospheric waves is presented, and a system which satisfies the requirements is described. A medium scale, real time computer is programmed to perform all echo recognition and coordinate measurement functions. The measurement algorithms are exercised on noisy data generated by a program which simulates the hardware system, in order to find the effects of noise on the measurement accuracies.

Backof, C. A., Jr.↗

Beamforming in an acoustic shadow

The sound field deep within an acoustic shadow region is less well understood than that outside the shadow region. Signal levels are substantially lower within the shadow, but beamforming difficulties arise for other reasons such as loss of spatial coherence. Based on analysis of JAPE-91 data, and other data, three types of characteristic signals within acoustic shadow regions are identified. These signal types may correspond to different, intermittent signal propagation conditions. Detection and classification algorithms might take advantage of the signal characteristics. Frequency coherence is also discussed. The extent of coherence across frequencies is shown to be limited, causing difficulties for source classification based on harmonic amplitude relationships. Discussions emphasize short-term characteristics on the order of one second. A video presentation on frequency coherence shows the similarity, in the presence of atmospheric turbulence, between the received signal from a stable set of harmonics generated by a loudspeaker and that received from a helicopter hovering behind a hill.

Havelock, David↗

Two-Dimensional Distribution of Volatiles in the Lunar Regolith from Space Weathering Simulations

We present simulations of space weathering effects on ice deposits in regions of permanent shadow on the Moon. These Monte Carlo simulations follow the effects of space weathering processes on the distribution of the volatiles over time. The model output constrains the coherence of volatile deposits with depth, lateral separation, and time. The results suggest that ice sheets become broken and buried with time. As impacts begin to puncture an initially coherent surficial ice sheet, small areas with a deficit of ice compared to surrounding areas are formed first. As time progresses, holes become prevalent and the anomalous regions are local enhancements of ice concentration in a volume. The 3-D distribution is also heterogeneous because the ice is buried to varying depths in different locations. Analysis of the coherence of ice on 10 cm scales predicts that putative ice sheets in anomalous radar craters are < 100 Myr old. Surface frost becomes homogenized within 20 Myr. The simulations show the data from the LCROSS impact and surrounding region are consistent with the ice deposit in Cabeus being >1000 Myr old. For future in situ analysis of cold trap volatiles, a horizontal range of 10 m is sufficient to acquire surface-based measurements of heterogeneously distributed ice. These results also support previous analyses that Mercury's cold traps are young.

Hurley, Dana M.↗

Quantification of Oxygen Vacancies in SrFe0.5Cr0.5O3−δ Thin Films: Correlating Lattice Expansion with Oxidation State Variability

Oxygen vacancies (VO), even in the dilute regime, can significantly impact the physical and chemical properties of complex oxides. It is however challenging to reliably detect and adequately quantify such defects in thin film samples where the VO concentration and distribution may further vary in response to interfacial strain. Here, we present a method to quantify VO concentrations in SrFe0.5Cr0.5O3−δ (SFCO) epitaxial thin films. Through coherent Bragg rod analysis, X-ray absorption spectroscopy, and theoretical modeling, we systematically correlate the c-axis lattice expansion detected in SFCO films with a VO concentration gradient. Our results reveal a nearly linear relationship between oxygen off-stoichiometry and out-of-plane lattice expansion in coherently strained SFCO films, with δ increasing from 0.32 to 0.52 and the lattice expanding by ∼1.0%. Moreover, a significant decrease in Cr oxidation state (from Cr5+ to Cr3+) is observed as the VO concentration increases, while the Fe oxidation state remains fixed at Fe3+. Our findings provide a reliable way to quantify oxygen stoichiometry in complex oxides, offering a pathway to design materials with precisely tailored structure–property relationships.

Hossain, Mohammad Delower↗

Investigations of tilt measurements using shallow borehole tiltmeters

An array of shallow borehole tiltmeters has been operated at Pinon Flat Observatory since early in 1977. The data from this array are examined for coherence between the individual instruments and compared with the corresponding data from three 732-m laser strainmeters. In general, there is no significant coherence between the signals from the tiltmeters outside the microseismic and tidal bands even though they are spaced as closely as 10 m apart. Comparisons with the strain records show that the observed tilt noise power exceeds the strain noise power by 25-40 dB over the band from 0.000001 to 1 Hz. Analysis of the coherence estimates establishes the necessity for an unacceptably large (approximately 1000) array of instruments in order to determine the common tectonic signals. The observed secular tilt rates are from 40 to 450 times the observed secular strain rates for the same period. The theoretical noise power limit of the tilt transducer renders the instrument incapable of recording background noise at a quiet site over the band from 0.0001 to 0.1 Hz.

Wyatt, F.↗

On the Curious Pulsation Properties of the Accreting Millisecond Pulsar IGR J17379-3747

(NICER) monitoring campaign of the 468 Hz accreting millisecond X-ray pulsar IGR J17379–3747. From a detailed spectral and timing analysis of the coherent pulsations we find that they show a strong energy dependence, with soft thermal emission lagging about 640 μs behind the hard, Comptonized emission. Additionally, we observe uncommonly large pulse fractions, with measured amplitudes in excess of 20% sinusoidal fractional amplitude across the NICER passband and fluctuations of up to ∼70%. Based on a phase-resolved spectral analysis, we suggest that these extreme properties might be explained if the source has an unusually favorable viewing geometry with a large magnetic misalignment angle. Due to these large pulse fractions, we were able to detect pulsations down to quiescent luminosities (~5 x 10(exp 33) erg/s).

Bult, Peter↗

Exploratory Analysis of Carbon Dioxide Levels, Ultrasound and Optical Coherence Tomography Measures of the Eye During ISS Missions

Carbon dioxide (CO2) levels on board the International Space Station (ISS) have typically averaged 2.3 to 5.3 mmHg, with large fluctuations occurring over periods of hours and days. CO2 has effects on cerebral vascular tone, resulting in vasodilation and alteration of cerebral blood flow (CBF). Increased CBF leads to elevated intracranial pressure (ICP), a factor leading to visual disturbances, headaches, and other central nervous system symptoms. Ultrasound of the optic nerve and optical coherence tomography (OCT) provide surrogate measurements of ICP; in-flight measurements of both were implemented as enhanced screening tools for the Visual Impairment/Intracranial Pressure (VIIP) syndrome. This analysis examines the relationships between ambient CO2 levels on ISS, ultrasound and OCT measures of the eye in an effort to understand how CO2 may possibly be associated with VIIP and to inform future analysis of in-flight VIIP data.

Schaefer, C.↗

Nonresonant coherent amplitude transfer in attosecond four-wave-mixing spectroscopy

Attosecond four-wave mixing (FWM) spectroscopy using an extreme ultraviolet (XUV) pulse and two noncollinear near-infrared (NIR) pulses is employed to measure Rydberg wave packet dynamics resulting from XUV excitation of a 3s electron in atomic argon into a series of autoionizing 3s –1 np Rydberg states ~29 eV. The emitted signals from individual Rydberg states exhibit oscillatory structure and persist well beyond the expected lifetimes of the emitting Rydberg states. These results reflect substantial contributions of longer-lived Rydberg states to the FWM emission signals of each individually detected state. A wave packet decomposition analysis reveals that coherent amplitude transfer occurs predominantly from photoexcited 3s –1 (n + 1) p states to the observed 3s –1 np Rydberg states. The experimental observations are reproduced by time-dependent Schrödinger equation simulations using electronic structure and transition moment calculations. Finally, the theory highlights that coherent amplitude transfer is driven nonresonantly to the 3s –1 np states by the NIR light through 3s –1 (n + 1)s and 3s –1 (n – 1)d dark states during the FWM process.

74 ATOMIC AND MOLECULAR PHYSICS↗

Understanding of bacterial lignin extracellular degradation mechanisms by Pseudomonas putida KT2440 via secretomic analysis

Abstract Background Bacterial lignin degradation is believed to be primarily achieved by a secreted enzyme system. Effects of such extracellular enzyme systems on lignin structural changes and degradation pathways are still not clearly understood, which remains as a bottleneck in the bacterial lignin bioconversion process. Results This study investigated lignin degradation using an isolated secretome secreted by Pseudomonas putida KT2440 that grew on glucose as the only carbon source. Enzyme assays revealed that the secretome harbored oxidase and peroxidase/Mn 2+ -peroxidase capacity and reached the highest activity at 120 h of the fermentation time. The degradation rate of alkali lignin was found to be only 8.1% by oxidases, but increased to 14.5% with the activation of peroxidase/Mn 2+ -peroxidase. Gas chromatography–mass spectrometry (GC–MS) and two-dimensional 1 H– 13 C heteronuclear single-quantum coherence (HSQC) NMR analysis revealed that the oxidases exhibited strong C–C bond ( β-β , β -5, and β -1) cleavage. The activation of peroxidases enhanced lignin degradation by stimulating C–O bond ( β -O-4) cleavage, resulting in increased yields of aromatic monomers and dimers. Further mass spectrometry-based quantitative proteomics measurements comprehensively identified different groups of enzymes particularly oxidoreductases in P. putida secretome, including reductases, peroxidases, monooxygenases, dioxygenases, oxidases, and dehydrogenases, potentially contributed to the lignin degradation process. Conclusions Overall, we discovered that bacterial extracellular degradation of alkali lignin to vanillin, vanillic acid, and other lignin-derived aromatics involved a series of oxidative cleavage, catalyzed by active DyP-type peroxidase, multicopper oxidase, and other accessory enzymes. These results will guide further metabolic engineering design to improve the efficiency of lignin bioconversion. Graphical Abstract

09 BIOMASS FUELS↗

Crystallographic registry in epitaxial V3O5 thin films

Crystallographic orientation plays a central role in determining transport properties in correlated oxides with low-hysteresis metal–insulator transitions. Here, V3O5 thin films were grown on Al2O3 (0001) and their crystallographic registry was evaluated using x-ray diffraction and cross-sectional transmission electron microscopy. θ–2θ measurements show a single out-of-plane orientation defined by the (202) reflection. Azimuthal φ-scans of the V3O5 (310) reflection exhibit twelve discrete maxima over 360°, indicating a finite set of in-plane orientations imposed by the substrate symmetry. High-resolution TEM and fast Fourier transform analysis confirm crystallographic coherence at the film–substrate interface. The electrical conductivity exhibits a metal–insulator transition at TMIT ≈ 423 K with no measurable thermal hysteresis and a total change of ~1.6 orders of magnitude between 300 and 480 K. These results establish crystallographic registry in epitaxial V3O5 thin films and provide a structurally well-defined system for future studies of orientation-dependent transport.\r\nT

36 MATERIALS SCIENCE↗

Coherent Detection of High-Rate Optical PPM Signals

A method of coherent detection of high-rate pulse-position modulation (PPM) on a received laser beam has been conceived as a means of reducing the deleterious effects of noise and atmospheric turbulence in free-space optical communication using focal-plane detector array technologies. In comparison with a receiver based on direct detection of the intensity modulation of a PPM signal, a receiver based on the present method of coherent detection performs well at much higher background levels. In principle, the coherent-detection receiver can exhibit quantum-limited performance despite atmospheric turbulence. The key components of such a receiver include standard receiver optics, a laser that serves as a local oscillator, a focal-plane array of photodetectors, and a signal-processing and data-acquisition assembly needed to sample the focal-plane fields and reconstruct the pulsed signal prior to detection. The received PPM-modulated laser beam and the local-oscillator beam are focused onto the photodetector array, where they are mixed in the detection process. The two lasers are of the same or nearly the same frequency. If the two lasers are of different frequencies, then the coherent detection process is characterized as heterodyne and, using traditional heterodyne-detection terminology, the difference between the two laser frequencies is denoted the intermediate frequency (IF). If the two laser beams are of the same frequency and remain aligned in phase, then the coherent detection process is characterized as homodyne (essentially, heterodyne detection at zero IF). As a result of the inherent squaring operation of each photodetector, the output current includes an IF component that contains the signal modulation. The amplitude of the IF component is proportional to the product of the local-oscillator signal amplitude and the PPM signal amplitude. Hence, by using a sufficiently strong local-oscillator signal, one can make the PPM-modulated IF signal strong enough to overcome thermal noise in the receiver circuits: this is what makes it possible to achieve near-quantum-limited detection in the presence of strong background. Following quantum-limited coherent detection, the outputs of the individual photodetectors are automatically aligned in phase by use of one or more adaptive array compensation algorithms [e.g., the least-mean-square (LMS) algorithm]. Then the outputs are combined and the resulting signal is processed to extract the high-rate information, as though the PPM signal were received by a single photodetector. In a continuing series of experiments to test this method (see Fig. 1), the local oscillator has a wavelength of 1,064 nm, and another laser is used as a signal transmitter at a slightly different wavelength to establish an IF of about 6 MHz. There are 16 photodetectors in a 4 4 focal-plane array; the detector outputs are digitized at a sampling rate of 25 MHz, and the signals in digital form are combined by use of the LMS algorithm. Convergence of the adaptive combining algorithm in the presence of simulated atmospheric turbulence for optical PPM signals has already been demonstrated in the laboratory; the combined output is shown in Fig. 2(a), and Fig. 2(b) shows the behavior of the phase of the combining weights as a function of time (or samples). We observe that the phase of the weights has a sawtooth shape due to the continuously changing phase in the down-converted output, which is not exactly at zero frequency. Detailed performance analysis of this coherent free-space optical communication system in the presence of simulated atmospheric turbulence is currently under way.

Vilnrotter, Victor↗

Advanced light source-Upgrade accumulator-ring gas bremsstrahlung production

Lawrence Berkeley National Laboratory is designing a new electron synchrotron for scientific research using synchrotron radiation. An upgrade of the Advanced Light Source (ALS) would position the nation to retain its international competitiveness in the soft X-ray sciences. The ALS is a 1.9 GeV storage ring operating at 500 mA of beam current. It is optimized to produce intense beams of soft X-rays, which offer spectroscopic contrast, nanometer-scale resolution, and broad temporal sensitivity. Upgrading the ALS storage ring from a triple-bend-achromat to a multibend-achromat (MBA) lattice design will provide a soft X-ray source that is up to 100–1,000 times brighter than today’s ALS and will provide a significantly higher fraction of coherent light in the soft X-ray region than is currently available at the ALS. Further, the upgraded ALS will offer the highest coherent flux of any existing or planned storage-ring facility, worldwide, up to a photon energy of 3.5 keV. The addition of an accumulator ring that enables on-axis, swap-out, recovery, and exchange of bunch trains is required to achieve this coherence and brightness. Analysis of the radiation generated and shielding required by the addition of this new accelerator is presented in this paper.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Topochemical Oxidation of Ruddlesden–Popper Nickelates Reveals Distinct Structural Family: Oxygen-Intercalated Layered Perovskites

Layered perovskites─including the Dion–Jacobson, Ruddlesden–Popper, and Aurivillius families─exhibit a wide range of correlated electron phenomena, from high-temperature superconductivity to multiferroicity. Here, in this study, we report a new family of layered perovskites realized through topochemical oxidation of La n+1 Ni n O 3n+1+δ (n = 1–4) Ruddlesden–Popper nickelate thin films. Postgrowth ozone annealing induces a substantial c-axis expansion─17.8% for La 2 NiO 4+δ (n = 1)─that monotonically decreases with increasing n. Surface synchrotron X-ray diffraction and coherent Bragg rod analysis (COBRA) reveal that this structural expansion arises from the intercalation of approximately δ ≈ 0.7–1.0 oxygen atoms into interstitial sites within the rock salt spacer layers, far exceeding the previous record of δ ≈ 0.3 for any Ruddlesden–Popper oxide. These oxygen-intercalated phases form a new class of layered perovskites with a spacer layer composition intermediate between the Ruddlesden–Popper and Aurivillius phases. Furthermore, oxygen intercalation induces metallicity, enhances nickel–oxygen hybridization, and suppresses oxygen octahedral rotations, a feature associated with high-temperature superconductivity in Ruddlesden–Popper nickelates. Our work establishes topochemical oxidation as a powerful approach to accessing highly oxidized, metastable phases across a broad range of layered oxide systems, offering new platforms to engineer electronic properties via intercalation chemistry.

Ferenc Segedin, Dan [Harvard Univ., Cambridge, MA ↗

Solvent Polarity Independent Symmetry-Breaking Charge Separation in a Slip-Stacked Covalent Terrylene Monoimide Dimer

The design of organic materials capable of efficient photoinduced charge separation in low-polarity environments is a critical challenge for advancing organic photovoltaics. Symmetry-breaking charge separation (SB-CS) offers a promising route to efficient charge separation with minimal energy loss; however, in conventional organic materials this process typically relies on polar solvents to stabilize the charge-separated state. Here, we investigate a slip-stacked terrylene monoimide dimer (TMI 2 ) engineered with intrinsic electronic asymmetry to circumvent this limitation. We demonstrate through a comprehensive suite of ultrafast spectroscopic techniques that TMI 2 undergoes remarkably efficient SB-CS regardless of solvent polarity enabled by the permanent dipole moment of TMI and the accessible intramolecular charge-transfer (ICT) character of its monomer units. Furthermore, analysis of vibronic coherences reveals that the initial state mixing is actively driven by a 193 cm –1 intermolecular mode, while the final SB-CS state is marked by a distinct vibrational fingerprint of the radical ion pair product. Our findings reveal how the intrinsic electronic asymmetry of the TMI monomers that constitute TMI 2 creates an efficient charge separation pathway that precludes the need for external stabilization from a polar solvent. Here, this work establishes a powerful molecular design principle for leveraging intrinsic monomeric asymmetry to achieve efficient charge separation in low-dielectric environments, with significant implications for the development of next-generation organic optoelectronic materials.

Aromatic compounds↗