Submicrosecond Time Scale Research Articles

Electrical properties of different materials studied by sub-microsecond underwater electrical explosions of single wires

Results of an experimental research and one-dimensional hydrodynamical simulations of critically damped sub-microsecond timescale underwater electrical explosions of wires made of 12 different materials are presented. Using current and voltage waveforms, streak shadow images of the shocks generated in water and wire expansion obtained by one-dimensional hydrodynamic simulations, the maximal values of the energy density, energy density deposition rates, and specific action integrals were determined. It is shown that for all study materials, the deposited energy density significantly exceeds the energy density required for the solid–liquid phase transition but is substantially smaller to induce a full liquid–vapor phase transition of the wire. At the time when the maximal value of the deposited power is realized, the deposited energy densities were found to be larger than the atomization energy for all materials. Estimates of the plasma parameters show that the explosion of the wires can be characterized by a high resistance and lowly ionized weakly coupled plasma. Three groups of materials were distinguished by either decrease, plateau, or increase in the resistance after the maximum of the deposited power. It was confirmed that the observed maximum Planckian temperature for all wire material does not exceed 6000 K due to the “bath” effect and that there is a correlation between the wire radial expansion and the strong shock wave velocities.

Conceptual design of a high reactive-power ferroelectric fast reactive tuner

We present a novel design of a ferroelectric fast reactive tuner (FE-FRT) capable of modulating mega-VAR reactive power on a submicrosecond timescale. The high reactive power capability of our design extends the range of applications of reactive tuners to numerous applications. We present a detailed analytical model of the performance of a megawatt-class reactive power device and benchmark it against finite-element method eigenmode and frequency domain electromagnetic simulations. We introduce new features, including an annulus design for the ferroelectric capacitors and capacitive window coupling to the cavity. We consider thermal design issues and nonlinear effects in the ferroelectric. The model covers several configurations, allowing control of the frequency of superconducting and normal-conducting cavities in a variety of applications and frequencies. We calculate that the FE-FRT designed should be capable of handling around 0.45 MVAR of reactive power with around 3 kW of resistive losses, providing a frequency tuning range of 8 kHz in an example of 400 MHz cavity geometry. Published by the American Physical Society 2024

Modeling allosteric mechanisms of eukaryotic type II topoisomerases

Type II topoisomerases (TopoIIs) are ubiquitous enzymes that are involved in crucial nuclear processes such as genome organization, chromosome segregation, and other DNA metabolic processes. These enzymes function as large, homodimeric complexes that undergo a complex cycle of binding and hydrolysis of two ATP molecules in their ATPase domains, which regulates the capture and passage of one DNA double-helix through a second, cleaved DNA molecule. This process requires the transmission of information about the state of the bound nucleotide over vast ranges in the TopoII complex. How this information is transmitted at the molecular level to regulate TopoII functions and how protein substitutions disrupt these mechanisms remains largely unknown. Here, we employed extensive microsecond-scale molecular dynamics simulations of the yeast TopoII enzyme in multiple nucleotide-bound states and with amino acid substitutions near both the N and C termini of the complex. Simulation results indicate that the ATPase domains are remarkably flexible on the sub-microsecond timescale and that these dynamics are modulated by the identity of the bound nucleotides and both local and distant amino acid substitutions. Network analyses point toward specific allosteric networks that transmit information about the hydrolysis cycle throughout the complex, which include residues in both the protein and the bound DNA molecule. Amino acid substitutions weaken many of these pathways. Together, our results provide molecular level details on how the TopoII catalytic cycle is controlled through nucleotide binding and hydrolysis and how mutations may disrupt this process.

Real-time swelling-collapse kinetics of nanogels driven by XFEL pulses.

Stimuli-responsive polymers are an important class of materials with many applications in nanotechnology and drug delivery. The most prominent one is poly-N-isopropylacrylamide (PNIPAm). The characterization of the kinetics of its change after a temperature jump is still a lively research topic, especially at nanometer-length scales where it is not possible to rely on conventional microscopic techniques. Here, we measured in real time the collapse of a PNIPAm shell on silica nanoparticles with megahertz x-ray photon correlation spectroscopy at the European XFEL. We characterize the changes of the particles diffusion constant as a function of time and consequently local temperature on sub-microsecond timescales. We developed a phenomenological model to describe the observed data and extract the characteristic times associated to the swelling and collapse processes. Different from previous studies tracking the turbidity of PNIPAm dispersions and using laser heating, we find collapse times below microsecond timescales and two to three orders of magnitude slower swelling times.

Oxygen-evolving photosystem II structures during S1–S2–S3 transitions

Photosystem II (PSII) catalyses the oxidation of water through a four-step cycle of Si states (i = 0–4) at the Mn4CaO5 cluster1–3, during which an extra oxygen (O6) is incorporated at the S3 state to form a possible dioxygen4–7. Structural changes of the metal cluster and its environment during the S-state transitions have been studied on the microsecond timescale. Here we use pump-probe serial femtosecond crystallography to reveal the structural dynamics of PSII from nanoseconds to milliseconds after illumination with one flash (1F) or two flashes (2F). YZ, a tyrosine residue that connects the reaction centre P680 and the Mn4CaO5 cluster, showed structural changes on a nanosecond timescale, as did its surrounding amino acid residues and water molecules, reflecting the fast transfer of electrons and protons after flash illumination. Notably, one water molecule emerged in the vicinity of Glu189 of the D1 subunit of PSII (D1-E189), and was bound to the Ca2+ ion on a sub-microsecond timescale after 2F illumination. This water molecule disappeared later with the concomitant increase of O6, suggesting that it is the origin of O6. We also observed concerted movements of water molecules in the O1, O4 and Cl-1 channels and their surrounding amino acid residues to complete the sequence of electron transfer, proton release and substrate water delivery. These results provide crucial insights into the structural dynamics of PSII during S-state transitions as well as O–O bond formation.

What determines sub-diffusive behavior in crowded protein solutions?

The aqueous environment inside cells is densely packed. A typical cell has a macromolecular concentration in the range 90–450 g/L, with 5%–40% of its volume being occupied by macromolecules, resulting in what is known as macromolecular crowding. The space available for the free diffusion of metabolites and other macromolecules is thus greatly reduced, leading to so-called excluded volume effects. The slow diffusion of macromolecules under crowded conditions has been explained using transient complex formation. However, sub-diffusion noted in earlier works is not well characterized, particularly the role played by transient complex formation and excluded volume effects. We have used Brownian dynamics simulations to characterize the diffusion of chymotrypsin inhibitor 2 in protein solutions of bovine serum albumin and lysozyme at concentrations ranging from 50 to 300 g/L. The predicted changes in diffusion coefficient as a function of crowder concentration are consistent with NMR experiments. The sub-diffusive behavior observed in the sub-microsecond timescale can be explained in terms of a so-called cage effect, arising from rattling motion in a local molecular cage as a consequence of excluded volume effects. By selectively manipulating the nature of interactions between protein molecules, we determined that excluded volume effects induce sub-diffusive dynamics at sub-microsecond timescales. These findings may help to explain the diffusion-mediated effects of protein crowding on cellular processes.

Real-time imaging of acoustic waves in bulk materials with X-ray microscopy

The dynamics of lattice vibrations govern many material processes, such as acoustic wave propagation, displacive phase transitions, and ballistic thermal transport. The maximum velocity of these processes and their effects is determined by the speed of sound, which therefore defines the temporal resolution (picoseconds) needed to resolve these phenomena on their characteristic length scales (nanometers). Here, we present an X-ray microscope capable of imaging acoustic waves with subpicosecond resolution within mm-sized crystals. We directly visualize the generation, propagation, branching, and energy dissipation of longitudinal and transverse acoustic waves in diamond, demonstrating how mechanical energy thermalizes from picosecond to microsecond timescales. Bulk characterization techniques capable of resolving this level of structural detail have previously been available on millisecond time scales-orders of magnitude too slow to capture these fundamental phenomena in solid-state physics and geoscience. As such, the reported results provide broad insights into the interaction of acoustic waves with the structure of materials, and the availability of ultrafast time-resolved dark-field X-ray microscopy opens a vista of new opportunities for 3D imaging of materials dynamics on their intrinsic submicrosecond time scales.

Direct observation of 890 ns dynamics of carbon black and polybutadiene in rubber materials using diffracted x-ray blinking

Dynamic behavior in soft matter physics, biology, and nanoscience frequently occurs on submicrosecond timescales. Diffracted x-ray blinking (DXB) is a unique method that can provide a broad range of spatial scale information and is becoming an attractive tool for use at high repetition rate x-ray facilities. In this study, we performed DXB experiments with 890 ns time resolution at the European X-ray Free-Electron Laser Facility to obtain dynamic information about rubber samples that are typically used in automobile tires. Time-resolved scattering was simultaneously recorded for two samples that mainly consisted of carbon black (CB) and polybutadiene (PB). These samples contained either graphitized or non-graphitized CB and displayed significantly different dynamics. A clear interaction between CB and PB was observed, indicating that the mobility of PB was changed by the introduction of CB. Restricted polymer motion was observed in the q-range of 0.78–1.58 Å−1 regions. Our results suggest that the particle network can be flexibly controlled without impairing the mechanical strength of the rubber.

Examining the molecular origins of anomalously high H2O generation at oxide-passivated metal surfaces for plasma applications

Elucidating the mechanisms responsible for sub-microsecond desorption of water and other impurities from electrode surfaces at high heating rates is crucial for understanding pulsed-power behavior and optimizing its efficiency. Ionization of desorbed impurities in the vacuum regions may create parallel loads and current loss. Devising methods to limit desorption during the short time duration of pulsed-power will significantly improve the power output. This problem also presents an exciting challenge to and paradigm for molecular length-scale modeling and theories. Previous molecular modeling studies have strongly suggested that, under high vacuum conditions, the amount of water impurity adsorbed on oxide surfaces on metal electrodes is at a sub-monolayer level, which appears insufficient to explain the observed pulsed-power losses at high current densities. Based on density functional theory (DFT) calculations, we propose that hydrogen trapped inside iron metal can diffuse into iron (III) oxide on the metal surface in sub-microsecond time scales, explaining the extra desorbed inventory. These hydrogen atoms react with the oxide to form Fe(II) and desorbed H2O at elevated temperatures. Cr2O3 is found to react more slowly to form Cr(II). H2 evolution is also predicted to require higher activation energies, so H2 may be evolved at later times than H2O. A one-dimensional diffusion model, based on DFT results, is devised to estimate the water outgassing rate under different conditions. This model explains outgassing above 1 ML for surface temperatures of 1 eV often assumed in pulsed-power systems. Finally, we apply a suite of characterization techniques to demonstrate that when iron metal is heated to 650 ∘C, the dominant surface oxide component becomes α-Fe2O3. We propose such specially-prepared samples will lead to convergence between atomic modeling and measurements like temperature-programmed desorption.

Lightning Interferometry with the Long Wavelength Array

The Long Wavelength Array is a radio telescope array located at the Sevilleta National Wildlife Refuge in La Joya, New Mexico, well suited and situated for the observation of lightning. The array consists of 256 high-sensitivity dual polarization antennas arranged in a 100 m diameter. This paper demonstrates some of the capabilities that the array brings to the study of lightning. Once 32 or more antennas are used to image lightning radio sources, virtually every integration period longer than the impulse response of the array includes at least one identifiable lightning emitter, independent of the integration period used. The use of many antennas also allows multiple simultaneous lightning radio sources to be imaged at sub-microsecond timescales; for the flash examined, 51% of the images contained more than one lightning source. Finally, by using many antennas to image lightning sources, the array is capable of locating sources fainter than the galactic background radio noise level, yielding possibly the most sensitive radio maps of lightning to date. This incredible sensitivity enables, for the first time, the emissions originating from the positive leader tips of natural in-cloud lightning to be detected and located. The tip emission is distinctly different from needle emission and is most likely due to positive breakdown.

Extreme dynamics in a biomolecular condensate.

Proteins and nucleic acids can phase-separate in the cell to form concentrated biomolecular condensates1-4. The functions of condensatesspan many length scales: they modulate interactions and chemical reactions at the molecular scale5, organize biochemical processes at the mesoscale6 and compartmentalize cells4. Understanding the underlying mechanisms of these processeswill require detailed knowledge of the rich dynamics across these scales7. The mesoscopic dynamics of biomolecular condensates have been extensively characterized8, but their behaviour at the molecular scale has remained more elusive. Here, as an example of biomolecular phase separation, we study complexcoacervates of two highly and oppositely charged disordered human proteins9. Their dense phase is 1,000 times more concentrated than the dilute phase, and the resulting percolated interaction network10 leads to a bulk viscosity 300 times greater than that of water. However, single-molecule spectroscopy optimized for measurements within individual droplets reveals that at the molecular scale, the disordered proteins remain exceedingly dynamic, with their chain configurations interconverting on submicrosecond timescales. Massive all-atom moleculardynamics simulations reproduce the experimental observations and explain this apparent discrepancy: the underlying interactions between individual charged side chains are short-lived and exchange on a pico- to nanosecond timescale. Our results indicate that, despite the high macroscopic viscosity of phase-separated systems, local biomolecular rearrangements required for efficient reactions at the molecular scale can remain rapid.

Direct Spectroscopic Observation of Cross-Plane Heat Transfer in a Two-Dimensional Van der Waals Heterostructure

Two-dimensional (2D) transition metal chalcogenides (TMDs) have drawn significant attention in recent years due to their extraordinary optical and electronic properties. As heat transfer plays an important role in device performance, various methods such as optothermal Raman spectroscopy and time-domain thermoreflectance have been developed to measure the thermal conductivity and interfacial thermal conductance in 2D van der Waals (vdW) heterostructures. Here, we employ the vibrational-pump-visible-probe (VPVP) spectroscopy to directly visualize the heat transfer process in a heterostructure of multilayer h-BN and monolayer WS2. Following an impulsive vibrational excitation of h-BN in the mid-infrared, we probe the heat transfer from h-BN through WS2 and finally to the substrate from the subpicosecond to the submicrosecond timescale. The interfacial thermal conductance of the h-BN/WS2 and WS2/SiO2 interfaces is obtained by corroborating the experiments with heat transfer calculations based on the Fourier’s law of heat conduction. Our study demonstrates an alternative, time-resolved optical method to measure cross-plane heat dissipation and opens up a new pathway to investigate the interlayer electron–phonon and phonon–phonon interactions in vdW heterostructures.

Binding of the peptide deformylase on the ribosome surface modulates the exit tunnel interior

Proteosynthesis on ribosomes is regulated at many levels. Conformational changes of the ribosome, possibly induced by external factors, may transfer over large distances and contribute to the regulation. The molecular principles of this long-distance allostery within the ribosome remain poorly understood. Here, we use structural analysis and atomistic molecular dynamics simulations to investigate peptide deformylase (PDF), an enzyme that binds to the ribosome surface near the ribosomal protein uL22 during translation and chemically modifies the emerging nascent peptide. Our simulations of the entire ribosome-PDF complex reveal that the PDF undergoes a swaying motion on the ribosome surface at the submicrosecond timescale. We show that the PDF affects the conformational dynamics of parts of the ribosome over distances of more than 5 nm. Using a supervised-learning algorithm, we demonstrate that the exit tunnel is influenced by the presence or absence of PDF. Our findings suggest a possible effect of the PDF on the nascent peptide translocation through the ribosome exit tunnel.

Thermal effects of beam profiles on X-ray photon correlation spectroscopy at megahertz X-ray free-electron lasers.

X-ray free-electron lasers (XFELs) with megahertz repetition rates enable X-ray photon correlation spectroscopy (XPCS) studies of fast dynamics on microsecond and sub-microsecond time scales. Beam-induced sample heating is one of the central concerns in these studies, as the interval time is often insufficient for heat dissipation. Despite the great efforts devoted to this issue, few have evaluated the thermal effects of X-ray beam profiles. This work compares the effective dynamics of three common beam profiles using numerical methods. Results show that under the same fluence, the effective temperatures increase with the nonuniformity of the beam, such that the Gaussian beam profile yields a higher effective temperature than the donut-like and uniform profiles. Moreover, decreasing the beam sizes is found to reduce beam-induced thermal effects, in particular the effects of beam profiles.

Global Dynamics of a Protein on the Surface of Anisotropic Lipid Nanoparticles Derived from Relaxation-Based NMR Spectroscopy.

The global motions of ubiquitin, a model protein, on the surface of anisotropically tumbling 1-palmitoyl-2-oleoyl-sn-glycero-3-phospho-(1'-rac-glycerol) (POPG):1,2-dihexanoyl-sn-glycero-3-phosphocholine (DHPC) bicelles are described. The shapes of POPG:DHPC bicelles prepared with high molar ratios q of POPG to DHPC can be approximated by prolate ellipsoids, with the ratio of ellipsoid dimensions and dimensions themselves increasing with higher values of q. Adaptation of the nuclear magnetic resonance (NMR) relaxation-based approach that we previously developed for interactions of ubiquitin with spherical POPG liposomes (Ceccon, A. J. Am. Chem. Soc. 2016, 138, 5789-5792) allowed us to quantitatively analyze the variation in lifetime line broadening of NMR signals (ΔR2) measured for ubiquitin in the presence of q = 2 POPG:DHPC bicelles and the associated transverse spin relaxation rates (R2,B) of bicelle-bound ubiquitin. Ubiquitin, transiently bound to POPG:DHPC bicelles, undergoes internal rotation about an axis orthogonal to the surface of the bicelle and perpendicular to the principal axis of its rotational diffusion tensor on the low microsecond time scale (∼3 μs), while the rotation axis itself wobbles in a cone on a submicrosecond time scale (≤ 500 ns).

Quasi-real-time dual-comb spectroscopy with 750-MHz Yb:fiber combs.

We present quasi-real-time dual-comb spectroscopy (DCS) using two Yb:fiber combs with ∼750 MHz repetition rates. A computational coherent averaging technique is employed to correct timing and phase fluctuations of the measured dual-comb interferogram (IGM). Quasi-real-time phase correction of 1-ms long acquisitions occurs every 1.5 seconds and is assisted by coarse radio frequency (RF) phase-locking of an isolated RF comb mode. After resampling and global offset phase correction, the RF comb linewidth is reduced from 200 kHz to ∼1 kHz, while the line-to-floor ratio increases 13 dB in power in 1 ms. Using simultaneous offset frequency correction in opposite phases, we correct the aliased RF spectrum spanning three Nyquist zones, which yields an optical coverage of ∼180 GHz around 1.035 µm probed on a sub-microsecond timescale. The absorption profile of gaseous acetylene is observed to validate the presented technique.

Simultaneous Multiple Timescale Imaging For High-Speed Accelerometry Using The FRAME-Method

Fast transient events, such as the disintegration of liquid bodies or chemical reactions between radical species, involve various processes that may occur at different timescales. Currently, there are two alternatives for monitoring such events: burst- or high-speed imaging. Burst imaging at ultra-high speeds (~ 100 MHz - THz) allows the fastest processes to be captured but only for a narrowly confined period of time and under the condition that the onset can be predicted. To monitor long lasting events with existing high-speed imaging technology, the frame rate must be reduced (~ kHz - 1 MHz) and thus processes occurring on sub-microsecond timescales cannot be observed. To date, no imaging technology is capable of visualizing detailed sub-microsecond dynamics over a long period of time. In this manuscript we present a solution to this technological gap by combining multiplexed imaging with high-speed sensor technology resulting in temporally resolved image series at two simultaneous timescales. We demonstrate its unique capability of tracking structures at MHz burst rates over a long time by, for the first time, extracting 2D accelerometry data acting upon liquid bodies at kHz frame-rates.

Simultaneous multiple time scale imaging for kHz–MHz high-speed accelerometry

Fast transient events, such as the disintegration of liquid bodies or chemical reactions between radical species, involve various processes that may occur at different time scales. Currently, there are two alternatives for monitoring such events: burst- or high-speed imaging. Burst imaging at ultrahigh speeds ( ∼ 100 MHz to THz ) allows for the capture of nature’s fastest processes but only for a narrowly confined period of time and at a repetition rate of ∼ 10 Hz . Monitoring long lasting, rapidly evolving transient events requires a significantly higher repetition rate, which is met by existing ∼ kHz to 1 MHz high-speed imaging technology. However, the use of such systems eliminates the possibility to observe dynamics occurring on the sub-microsecond time scale. In this paper, we present a solution to this technological gap by combining multiplexed imaging with high-speed sensor technology, resulting in temporally resolved, high-spatial-resolution image series at two simultaneous time scales. We further demonstrate how the collection of such data opens up the tracking of rapidly evolving structures up to MHz burst rates over long durations, allowing, for the first time, to our knowledge, the extraction of acceleration fields acting upon the liquid bodies of an atomizing spray in two dimensions at kHz frame rates.

Influence of surface roughness on the transient interfacial phenomena in laser impact welding

Presented is an investigation into laser impact welding (LIW) wherein experimentally measured surface profiles of the flyer and target foils are incorporated to study their effects on the transient physical phenomena that occur during this rapid, collision-based joining process. During LIW, thermal response, plastic strains, and shear stresses evolve over a sub-microsecond timescale, which necessitates the use of computational modeling to predict the influence that surface roughness has on the material response and resulting joint morphology. White light interferometry is used to experimentally characterize the surface profiles of an aluminum 1100 flyer foil and a stainless steel 304 target foil. The profiles are mapped to material volumes within a plane strain, thermomechanical simulation employing an Eulerian framework. A spatially and temporally varying laser-induced plasma pressure is applied to the flyer foil, and the resulting transient phenomena are analyzed at timeframes ranging from initial contact through complete weld formation. To reveal effects of the rough foil surfaces, results from the same computational model using smooth foil surfaces are also obtained. When the rough surface profiles are included, it is found that significant differences in the thermal response and plastic strains are observed, and these differences are hypothesized to arise from the effects of discontinuous surface contact along the collision path. The incorporation of rough surface asperities also reveals two distinct regions prior to the weld initiation point; the first where elastic rebound occurs at a negligible collision angle, leaving interfacial voids, and the second where superficial shear deformation flattens the surfaces without mutual ablation and jetting. The work represents the first study in which measured surface profiles of the flyer and target foils are incorporated into a computational model of laser impact welding.

Microphysiological Modeling of the Structure and Function of Neuromuscular Transmitter Release Sites.

The general mechanism of calcium-triggered chemical transmitter release from neuronal synapses has been intensely studied, is well-known, and highly conserved between species and synapses across the nervous system. However, the structural and functional details within each transmitter release site (or active zone) are difficult to study in living tissue using current experimental approaches owing to the small spatial compartment within the synapse where exocytosis occurs with a very rapid time course. Therefore, computer simulations offer the opportunity to explore these microphysiological environments of the synapse at nanometer spatial scales and on a sub-microsecond timescale. Because biological reactions and physiological processes at synapses occur under conditions where stochastic behavior is dominant, simulation approaches must be driven by such stochastic processes. MCell provides a powerful simulation approach that employs particle-based stochastic simulation tools to study presynaptic processes in realistic and complex (3D) geometries using optimized Monte Carlo algorithms to track finite numbers of molecules as they diffuse and interact in a complex cellular space with other molecules in solution and on surfaces (representing membranes, channels and binding sites). In this review we discuss MCell-based spatially realistic models of the mammalian and frog neuromuscular active zones that were developed to study presynaptic mechanisms that control transmitter release. In particular, these models focus on the role of presynaptic voltage-gated calcium channels, calcium sensors that control the probability of synaptic vesicle fusion, and the effects of action potential waveform shape on presynaptic calcium entry. With the development of these models, they can now be used in the future to predict disease-induced changes to the active zone, and the effects of candidate therapeutic approaches.