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At least 145 records · Page 8

Atomic Force Microscopy-Based Force Spectroscopy and Multiparametric Imaging of Biomolecular and Cellular Systems

During the last three decades, a series of key technological improvements turned atomic force microscopy (AFM) into a nanoscopic laboratory to directly observe and chemically characterize molecular and cell biological systems under physiological conditions. In this work, we review key technological improvements that have established AFM as an analytical tool to observe and quantify native biological systems from the micro- to the nanoscale. Native biological systems include living tissues, cells, and cellular components such as single or complexed proteins, nucleic acids, lipids, or sugars. We showcase the procedures to customize nanoscopic chemical laboratories by functionalizing AFM tips and outline the advantages and limitations in applying different AFM modes to chemically image, sense, and manipulate biosystems at (sub)nanometer spatial and millisecond temporal resolution. We further discuss theoretical approaches to extract the kinetic and thermodynamic parameters of specific biomolecular interactions detected by AFM for single bonds and extend the discussion to multiple bonds. Finally, we highlight the potential of combining AFM with optical microscopy and spectroscopy to address the full complexity of biological systems and to tackle fundamental challenges in life sciences.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Five-second STEM dislocation tomography for 300 nm thick specimen assisted by deep-learning-based noise filtering

Scanning transmission electron microscopy (STEM) is suitable for visualizing the inside of a relatively thick specimen than the conventional transmission electron microscopy, whose resolution is limited by the chromatic aberration of image forming lenses, and thus, the STEM mode has been employed frequently for computed electron tomography based three-dimensional (3D) structural characterization and combined with analytical methods such as annular dark field imaging or spectroscopies. However, the image quality of STEM is severely suffered by noise or artifacts especially when rapid imaging, in the order of millisecond per frame or faster, is pursued. Here we demonstrate a deep-learning-assisted rapid STEM tomography, which visualizes 3D dislocation arrangement only within five-second acquisition of all the tilt-series images even in a 300 nm thick steel specimen. The developed method offers a new platform for various in situ or operando 3D microanalyses in which dealing with relatively thick specimens or covering media like liquid cells are required.

47 OTHER INSTRUMENTATION↗

Thermal Stability of Quasi-1D NbS 3 Nanoribbons and Their Transformation to 2D NbS 2 : Insights from in Situ Electron Microscopy and Spectroscopy

Here in situ electron microscopy imaging and spectroscopy enabled us to study the evolution of quasi-1D NbS 3 -IV nanoribbons with respect to morphology and chemical structure at temperatures between room temperature and 1000 °C. Scanning transmission electron microscopy (STEM) experiments included imaging in the secondary electron, (transmitted) bright field, and high-angle annular dark-field modes while operating in the low kV regime. The results showed that NbS 3 -IV samples transform dramatically from smooth nanoribbons into highly textured configurations featuring polyhedral divots and steps. Similar in situ heating experiments conducted with aberration-corrected STEM revealed that bilayers of NbS 3 -IV chains convert topotactically into aligned 2H-NbS 2 sheets upon loss of sulfur. Atomic resolution imaging, fast Fourier transform analysis, and electron energy loss spectroscopy confirmed these chemical changes, from which we propose an atomistic mechanism for the NbS 3 -IV → 2H-NbS 2 conversion.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Photodetachment spectroscopy and resonant photoelectron imaging of cryogenically cooled 1-pyrenolate

We report an investigation of the 1-pyrenolate anion (PyO - ) and the 1-pyrenoxy radical (PyO) using photodetachment spectroscopy and resonant photoelectron imaging of cryogenically-cooled anions. The electron affinity of PyO is measured to be 2.4772(4) eV (19,980 ± 3 cm -1 ) from high-resolution photoelectron spectroscopy. Photodetachment spectroscopy reveals a dipole-bound state (DBS) for PyO - 280 cm-1 below the detachment threshold, as well as a broad and intense valence excited state (shape resonance) 1,077 cm-1 above the detachment threshold. The shape resonance with an excitation energy of 21,055 cm -1 is due to excitation of an electron from the highest occupied molecular orbital of PyO - to its lowest unoccupied molecular orbital in the continuum. Twenty-nine vibrational levels of the DBS are observed, including twenty-seven above-threshold vibrational levels (vibrational Feshbach resonances). Twenty-seven resonant photoelectron spectra are obtained by tuning the detachment laser to the vibrational Feshbach resonances, resulting in highly non-Franck-Condon photoelectron spectra and rich vibrational information. In total, the frequencies of twenty-one vibrational modes are obtained for the PyO radical by the combination of the photodetachment and resonant photoelectron spectroscopy, including thirteen out-of-plane bending modes.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Photodetachment spectroscopy and resonant photoelectron imaging of the 2-naphthoxide anion via dipole-bound excited states

We report a photodetachment spectroscopy and high-resolution resonant photoelectron imaging study of cryogenically-cooled 2-naphthoxide anions (C 10 H 7 O - ). The photodetachment spectrum revealed a dipole-bound state (DBS) 202(4) cm -1 below the detachment threshold and thirty-eight resonances corresponding to the vibrational levels of the DBS. By tuning the detachment laser to these above-threshold resonances, we obtained thirty-eight resonantly-enhanced photoelectron spectra, which were highly non-Franck-Condon as a result of mode-selective vibrational auto-detachment from the DBS. The resonances were assigned by comparing the resonant and non-resonant photoelectron spectra, assisted by the computed vibrational frequencies. Specifically, vibrational features with low Franck-Condon factors or from Franck-Condon-forbidden vibrational modes were significantly enhanced in the resonant photoelectron spectra, resulting in much richer spectroscopic information. The electron affinity of the 2-naphthoxy radical was measured accurately to be 19,387(4) cm -1 or 2.4037(5) eV. In addition, a total of seventeen vibrational frequencies were obtained for the 2-naphthoxy radical. In particular, seven Franck-Condon-forbidden out-of-plane bending modes, including the two lowest frequency modes (ν 48 at 102 cm -1 and ν47 at 171 cm -1 ), were observed, demonstrating the advantages of combining photodetachment spectroscopy and resonant photoelectron spectroscopy in obtaining vibrational information for polar radical species via DBS.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

On the redistribution of charge in La 0.7 Sr 0.3 CrO 3 /La 0.7 Sr 0.3 MnO 3 multilayer thin films

The atomic and electronic structures of La 0.7 Sr 0.3 MnO 3 (LSMO)/La 0.7 Sr 0.3 CrO 3 (LSCO) multilayer thin films are investigated using aberration corrected scanning transmission electron microscopy (STEM) imaging and spectroscopy. Atomic resolution high angle annular dark-field reveals that LSMO layers have an expanded out-of-plane lattice parameter compared to compressed LSCO layers, contrasting with x-ray diffraction measurements. The expansion is found to result from preferential oxygen vacancy formation in LSMO during STEM sample preparation as determined by electron energy-loss spectroscopy. The La/Sr atom column intensity is also found to oscillate by about 4% between the LSMO and LSCO layers, indicative of La/Sr concentration variation. Using energy-dispersive x-ray spectroscopy in combination with image simulations, we confirm the La/Sr inhomogeneity and elucidate the origin of charge redistribution within the multilayer. These results illuminate the sensitivity of the technique to subtle structural, chemical, and electronic features that can arise to compensate charge imbalances in complex oxide heterostructures.

36 MATERIALS SCIENCE↗

Enhanced spatial resolution of Eljen-204 plastic scintillators for use in rep-rated proton diagnostics

A pixelated scintillator has been designed, fabricated, and tested using a laser-accelerated proton source for use in proton diagnostics at rep-rated laser facilities. The work presented here demonstrates the enhanced spatial resolution of thin, organic scintillators through a novel pixelation technique. Furthermore, experimental measurements using laser-generated protons incident onto 130 μm-thick scintillators indicate a >20% reduction in the scintillator point spread function (PSF) for the detectors tested. The best performing pixelated detector reduced the ~200 μm PSF of the stock material to ~150 μm. The fabrication technique may be tailored to reduce the pixel size and achieve higher spatial resolutions.

47 OTHER INSTRUMENTATION↗

Ultrafast method for scanning tunneling spectroscopy

A scanning tunneling microscope (STM) combines unique capabilities in imaging and spectroscopy with atomic precision, and it can obtain energy-resolved spectroscopic data with atomic resolution. In this paper, we utilize a recently proposed modification to the STM feedback control loop to acquire high quality d 2 I/dV 2 images. We have developed a constant differential conductance imaging method by closing the STM feedback loop with a high precision dI/dV measurement. In this mode, the tip’s vertical position is adjusted so as to keep the differential conductance constant during raster scanning of the surface. Based on this imaging mode, we propose a new technique to acquire fast and reliable scanning tunneling spectroscopy (STS) data simultaneously with the imaging.

47 OTHER INSTRUMENTATION↗

RapidEELS: machine learning for denoising and classification in rapid acquisition electron energy loss spectroscopy

Recent advances in detectors for imaging and spectroscopy have afforded in situ, rapid acquisition of hyperspectral data. While electron energy loss spectroscopy (EELS) data acquisition speeds with electron counting are regularly reaching 400 frames per second with near-zero read noise, signal to noise ratio (SNR) remains a challenge owing to fundamental counting statistics. In order to advance understanding of transient materials phenomena during rapid acquisition EELS, trustworthy analysis of noisy spectra must be demonstrated. In this study, we applied machine learning techniques to denoise high frame rate spectra, benchmarking with slower frame rate “ground truths”. The results provide a foundation for reliable use of low SNR data acquired in rapid, in-situ spectroscopy experiments. Such a tool-set is a first step toward both automation in microscopy as well as use of these methods to interrogate otherwise poorly understood transformations.

36 MATERIALS SCIENCE↗

Applications of ultrafast nano-spectroscopy and nano-imaging with tip-based microscopy

Innovation in microscopy has often been critical in advancing both fundamental science and technological progress. Notably, the evolution of ultrafast near-field optical nano-spectroscopy and nano-imaging has unlocked the ability to image at spatial scales from nanometers to ångströms and temporal scales from nanoseconds to femtoseconds. This approach revealed a plethora of fascinating light-matter states and quantum phenomena, including various species of polaritons, quantum phases, and complex many-body effects. This review focuses on the working principles and state-of-the-art development of ultrafast tip-enhanced and near-field microscopy, integrating diverse optical pump-probe methods across the terahertz (THz) to ultraviolet (UV) spectral ranges. It highlights their utility in examining a broad range of materials, including two-dimensional (2D), organic molecular, and hybrid materials. The review concludes with a spatio-spectral-temporal comparison of ultrafast nano-imaging techniques, both within already well-defined domains, and offering an outlook on future developments of ultrafast tip-based microscopy and their potential to address a wider range of materials.

Zhao, Zhichen [Tongji University, Shanghai (China)↗

In planta single-molecule imaging and holographic force spectroscopy to study real-time, multimodal turnover dynamics of polysaccharides and associated carbohydrate metabolites

Cellular production of polysaccharides from simple sugar molecules serves critical roles in a variety of metabolic processes essential to the survival of every living organism. In the context of photosynthetically fixed carbon, cell wall polysaccharides synthesis is particularly of interest for increased biomass accumulation for human food, animal feed, and bioenergy related applications. Despite a long history of research in plant cell biology, our understanding of in planta cell wall biosynthesis and its regulation is far from complete due to lack of a comprehensive microscopy toolkit that encompass the multiple spatial and temporal scales in which cell wall polysaccharides fibrils are synthesized and assembled into intricate cell wall networks. In this project, a multidisciplinary team of scientists from Rutgers University, Vanderbilt University, and Oak Ridge National Laboratory carried out innovative multimodal, multiscale microscopy studies of cell wall synthesis using single-molecule force-spectroscopy, super-resolution fluorescence microscopy, and in vivo live cell imaging. Our novel multimodal and holistic imaging approach revealed plant cell wall polysaccharides synthesis processes in unprecedented detail across multiple spatiotemporal scales, from a single-molecule to a single-cell. Besides, the team has made technical and scientific innovations across multiple research fields—microscopy, bioengineering, single-molecule biophysics, and plant biology, etc.—to accomplish the goals. The results from this project will greatly advance the mechanistic and holistic understanding of in planta cell wall synthesis, which will accelerate the development of better transgenic crops for bioenergy applications. Moreover, the new toolbox, combining powerful advanced microscopy assays with cell/protein engineering, will have broader impacts on molecular and cellular biology fields by paving the way for studying cellular processes occurring across multiple physical scales with multimodal microscopy methodologies.

59 BASIC BIOLOGICAL SCIENCES↗

Chlorine and potassium enrichment in the Cassiopeia A supernova remnant

The elements in the Universe are synthesized primarily in stars and supernovae, where nuclear fusion favours the production of even-Z elements. In contrast, odd-Z elements are less abundant and their yields are highly dependent on detailed stellar physics, making theoretical predictions of their cosmic abundance uncertain. In particular, the origin of odd-Z elements such as phosphorus (P), chlorine (Cl) and potassium (K), which are important for planet formation and life, is poorly understood. While the abundances of these elements in Milky Way stars are close to solar values, supernova explosion models systematically underestimate their production by up to an order of magnitude, indicating that key mechanisms for odd-Z nucleosynthesis are currently missing from theoretical models. Here we report the observation of P, Cl and K in the Cassiopeia A supernova remnant using high-resolution X-ray spectroscopy with X-Ray Imaging and Spectroscopy Mission data, with the detection of K at above the 6σ level being the most significant finding. Supernova explosion models of normal massive stars cannot explain the element abundance pattern, especially the high abundances of Cl and K, while models that include stellar rotation, binary interactions or shell mergers agree closely with the observations. Our observations suggest that such stellar activity plays an important role in supplying these elements to the Universe.

Astronomy and AstroPhysics↗

Studies of localized mix and asymmetry caused by the stalk in inertial fusion experiments at OMEGA

In an inertially confined fusion experiment, a capsule of fusion fuel is compressed to high temperatures and densities using lasers, creating a hot plasma in which thermonuclear fusion reactions take place. To achieve efficient conversion of laser energy to fuel heating, the implosion must be as spherically symmetric as possible. One common source of asymmetry that degrades performance is the stalk and glue spot that hold the capsule in place before the experiment. The exact nature and magnitude of this perturbation had not been previously quantified. In this work, inertially confined fusion experiments were executed with an additional stalk on the capsule to measure and quantify the effect of the stalk and glue spot on the symmetry and performance. It is found that the stalk drives low-mode asymmetry by shadowing the laser drive on the part of the shell near the glue spot, enhancing the hot-spot velocity toward the stalk by 40–80 km/s and elongating the hot-spot along the stalk axis. It is also found that localized mix due to the additional stalk has a negligible effect on implosion performance. Two-dimensional radiation-hydrodynamic simulations using the xRAGE code reproduce the direction of the experimentally observed change to hot-spot velocity and implosion performance metrics, but not the observed elongation, suggesting that this feature results from an interaction between stalk perturbations and other preexisting asymmetry seeds, such as laser drive asymmetry.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

The Mass-loss History of the Red Hypergiant VY CMa

Imaging and spectroscopy of the knots, clumps, and extended arcs in the complex ejecta of VY CMa confirm a record of high mass-loss events over the past few hundred years. Hubble Space Telescope/Space Telescope Imaging Spectrograph spectroscopy of numerous small knots close to the star allow us to measure their radial velocities from the strong K i emission and determine their separate motions, spatial orientations, and time since ejecta. Their ages concentrate around 70, 120, 200, and 250 yr ago. A K i emission knot only 50 mas from the star ejected as recently as 1985–1995 may coincide with an H{sub 2}O maser. Comparison with VY CMa’s historic light curve from 1800 to the present shows several knots with ejection times that correspond with extended periods of variability and deep minima. The similarity of this correspondence in VY CMa with the remarkable recent dimming of Betelgeuse and an outflow of gas is apparent. The evidence for similar outflows from the surface of a more typical red supergiant suggests that discrete ejections are more common and surface or convective activity is a major source of mass loss for red supergiants.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗