Time-resolved Imaging Technique Research Articles

Unraveling the Nanosheet Zeolite-Catalyzed Combustion of Aluminum Nanoparticles-Doped exo-Tetrahydrodicyclopentadiene (JP-10) Energetic Fuel.

Nanosheet MFI zeolites (Zeolite Socony Mobil, five) have grown in popularity in cracking catalysis considering their tunability in porous topologies, acidic sites, and sheet thickness, thus allowing them to selectively adsorb molecules of specific sizes, shapes, and polarities, resulting in improved cracking performance for a specific fuel. Five different MFI zeolites in the form of a mesoporous nanosheet structure with a controlled concentration of acidic sites denoted as NSMFI(y), where y is Si/Al ratio, have been synthesized. The effects of the relative acidity content of these NSMFI(y) samples on the zeolite-catalyzed combustion of aluminum nanoparticles (AlNPs)-aided exo-tetrahydrodicyclopentadiene (JP-10) mixed energetic fuel droplets levitated in an oxygen-argon atmosphere were investigated using time-resolved imaging (optical and thermal infrared) and spectroscopic techniques (UV-vis and FTIR). The addition of 1.0 wt % of NSMFI(y) zeolites to AlNPs-JP-10 fluid fuel results in critically reduced ignition delays (9 ± 2 ms), elevated ignition temperatures (2800 ± 170 K), and prolonged burning times (60 ± 10 ms) with an enhanced combustion efficiency. The NSMFI(y) zeolites, which possess high acidity and significant mesoporosity, play a crucial role in improving the combustion efficiency by effectively catalyzing the chemical activation of JP-10 and prolonging the burning of the igniting droplet. The NSMFI (60) variant with the highest acidic site content achieved a maximum combustion efficiency of 80 ± 6%. A comprehensive catalytic combustion mechanism has been elucidated based on the detected reactive intermediates such as hydroxyl radical (OH) and aluminum monoxide (AlO). These findings will help to critically advance the development of next-generation, sustainable, and innovative mixed nanofluid fuels.

A Novel Fit-Flexible Fluorescence Soft Imager: Tri-Sensing of Intensity, Fall-Time, and Life Profile.

Time-resolved fluorescence imaging techniques, like confocal fluorescence lifetime imaging microscopy, are powerful photonic instrumentation tools of modern science with diverse applications, including: biology, medicine, and chemistry. However, complexities of the systems, both at specimen and device levels, cause difficulties in quantifying soft biomarkers. To address the problems, we first aim to understand and model the underlying photophysics of fluorescence decay curves. For this purpose, we provide a set of mathematical functions, called "life models", fittable with the real temporal recordings of histogram of photon counts. For each model, an equivalent electrical circuit, called a "life circuit", is derived for explaining the whole process. In confocal endomicroscopy, the components of excitation laser, specimen, and fluorescence-emission signal as the histogram of photon counts are modelled by a power source, network of resistor-inductor-capacitor circuitry, and multimetre, respectively. We then design a novel pixel-level temporal classification algorithm, called a "fit-flexible approach", where qualities of "intensity", "fall-time", and "life profile" are identified for each point. A model selection mechanism is used at each pixel to flexibly choose the best representative life model based on a proposed Misfit-percent metric. A two-dimensional arrangement of the quantified information detects some kind of structural information. This approach showed a potential of separating microbeads from lung tissue, distinguishing the tri-sensing from conventional methods. We alleviated by 7% the error of the Misfit-percent for recovering the histograms on real samples than the best state-of-the-art competitor. Codes are available online.

Time-resolved Laser Speckle Contrast Imaging (TR-LSCI) of Cerebral Blood Flow.

To address many of the deficiencies in optical neuroimaging technologies, such as poor tempo-spatial resolution, low penetration depth, contact-based measurement, and time-consuming image reconstruction, a novel, noncontact, portable, time-resolved laser speckle contrast imaging (TR-LSCI) technique has been developed for continuous, fast, and high-resolution 2D mapping of cerebral blood flow (CBF) at different depths of the head. TR-LSCI illuminates the head with picosecond-pulsed, coherent, widefield near-infrared light and synchronizes a fast, high-resolution, gated single-photon avalanche diode camera to selectively collect diffuse photons with longer pathlengths through the head, thus improving the accuracy of CBF measurement in the deep brain. The reconstruction of a CBF map was dramatically expedited by incorporating convolution functions with parallel computations. The performance of TR-LSCI was evaluated using head-simulating phantoms with known properties and in-vivo rodents with varied hemodynamic challenges to the brain. TR-LSCI enabled mapping CBF variations at different depths with a sampling rate of up to 1 Hz and spatial resolutions ranging from tens/hundreds of micrometers on rodent head surfaces to 1-2 millimeters in deep brains. With additional improvements and validation in larger populations against established methods, we anticipate offering a noncontact, fast, high-resolution, portable, and affordable brain imager for fundamental neuroscience research in animals and for translational studies in humans.

Insights into ultrafast decay dynamics of electronically excited pyridine-N-oxide.

The ultrafast decay dynamics of pyridine-N-oxide upon excitation in the near-ultraviolet range of 340.2-217.6 nm is investigated using the femtosecond time-resolved photoelectron imaging technique. The time-resolved photoelectron spectra and photoelectron angular distributions at all pump wavelengths are carefully analyzed and the following view is derived: at the longest pump wavelengths (340.2 and 325.6 nm), pyridine-N-oxide is excited to the S1(1ππ*) state with different vibrational levels. The depopulation rate of the S1 state shows a marked dependence on vibrational energy and mode, and the lifetime is in the range of 1.4-160 ps. At 289.8 and 280.5 nm, both the second 1ππ* state and the S1 state are initially prepared. The former has an extremely short lifetime of ∼60 fs, which indicates that the ultrafast deactivation pathway such as a rapid internal conversion to one close-lying state is its dominant decay channel, while the latter is at high levels of vibrational excitation and decays within the range of 380-520 fs. At the shortest pump wavelengths (227.3 and 217.6 nm), another excited state of Rydberg character is mostly excited. We assign this state to the 3s Rydberg state which has a lifetime of 0.55-2.2 ps. This study provides a comprehensive picture of the ultrafast excited-state decay dynamics of the photoexcited pyridine-N-oxide molecule.

Hidden-information extraction from layered structures through terahertz imaging down to ultralow SNR.

Noninvasive inspection of layered structures has remained a long-standing challenge for time-resolved imaging techniques, where both resolution and contrast are compromised by prominent signal attenuation, interlayer reflections, and dispersion. Our method based on terahertz (THz) time-domain spectroscopy overcomes these limitations by offering fine resolution and a broadband spectrum to efficiently extract hidden structural and content information from layered structures. We exploit local symmetrical characteristics of reflected THz pulses to determine the location of each layer, and apply a statistical process in the spatiotemporal domain to enhance the image contrast. Its superior performance is evidenced by the extraction of alphabetic characters in 26-layer subwavelength papers as well as layer reconstruction and debonding inspection in the conservation of Terra-Cotta Warriors. Our method enables accurate structure reconstruction and high-contrast imaging of layered structures at ultralow signal-to-noise ratio, which holds great potential for internal inspection of cultural artifacts, electronic components, coatings, and composites with dozens of submillimeter layers.

Synthesis of ZnO/C Nanocomposites via Liquid-Assisted Laser Ablation in an Applied Electric Field for Supercapacitor Applications

The formation of nonspherical anisotropic nanoparticles having a large surface area by pulsed laser ablation in liquids (PLAL) still remains a challenge. In this work, to expand the capabilities of the PLAL technique, an approach was developed based on pulsed laser ablation in liquids with an external voltage applied to the target. This approach allowed shape-controlled preparation of nonspherical ZnO/C composite nanomaterials providing additional possibilities for tuning of the particles’ morphology that was found to depend on the applied voltage and polarity. The positive polarity on the Zn target allowed obtaining nanodisk structures, whereas application of negative polarity to the target enabled the formation of flower-like nanostructures proven by scanning (SEM) and transmission electron microscopy (TEM) studies. The optimal conditions for the nanoflower formation were found with the voltage set to be 200 V. A time-resolved imaging technique was applied to study plasma propagation evolution and lifetime that allows suggesting the mechanisms of nanoflower formation. Furthermore, utilizing the developed approach in a carbon nanoparticle colloid, sponge-like composites were obtained having a developed surface that showed promising capacitance and charge storage behavior in preliminary electrochemical tests. The ZnO/C composite structures were evidenced by SEM and TEM studies as well as by EDX mapping, X-ray diffraction, Raman, infrared, and optical absorption spectroscopy measurements. In addition, the production of particles in the presence of an electric field leads to the deposition of the formed nanostructures on the cathode surface that can serve as a tool for assembling the resulting particles into ordered structures for subsequent supercapacitor applications.

New perspectives in time-resolved laser-induced electron diffraction

Imaging the microscopic world in real space and real time is a grand challenge of science. In the landscape of time-resolved imaging techniques, laser-induced electron diffraction (LIED) has recently shown to be a promising candidate to push the frontiers of ultrafast molecular imaging. In this work, we review the main achievements of LIED research in terms of experimental results and advanced modelling. We also envision interesting perspectives toward the future advancement of time-resolved LIED imaging.

Optical Creation of Skyrmions by Spin Reorientation Transition in Ferrimagnetic CoHo Alloys.

Manipulating magnetic skyrmions by means of a femtosecond (fs) laser pulse has attracted great interest due to their promising applications in efficient information-storage devices with ultralow energy consumption. However, the mechanism underlying the creation of skyrmions induced by an fs laser is still lacking. As a result, a key challenge is to reveal the pathway for the massive reorientation of magnetization from trivial to nontrivial topological states. Here, we studied a series of ferrimagnetic CoHo alloys and investigated the effect of a single laser pulse on the magnetic states. Thanks to the time-resolved magneto-optical Kerr effect and imaging techniques, we demonstrate that the laser-induced phase transitions from single domains into a topological skyrmion phase are mediated by the transient in-plane magnetization state, in real time and space domains, respectively. Combining experiments and micromagnetic simulations, we propose a two-step process for creating skyrmions through laser pulse irradiation: (i) the electron temperature enhancement induces a spin reorientation transition on a picosecond (ps) timescale due to the suppression of perpendicular magnetic anisotropy (PMA) and (ii) the PMA slowly restores, accompanied by out-of-plane magnetization recovery, leading to the generation of skyrmions with the help of spin fluctuations. This work provides a route to control skyrmion patterns using an fs laser, thereby establishing the foundation for further exploration of topological magnetism at ultrafast timescales.

Behavior of 355 nm laser-induced damage growth in fused silica

The behavior of morphology and crack propagation during damage growth on the rear surface of fused silica is studied using a time-resolved shadow imaging technique. The mechanism and distribution characteristics of the plasma caused by energy deposition during the damage growth process and the effect on crack extension are studied. Finally, the properties of shock and stress waves and their effects on the damage growth are discussed. The results indicate that the damage growth process leads to significant differences in the transmission of shock and stress waves. The growth size of the damage site leads to a significant energy concentration deposition effect, which induces a local enhancement of the plasma that subsequently affects the crack distribution. It contributes to the transition from radial to circumferential crack and also further accelerates the damage growth process. The results could contribute to experimental support for further understanding of the physical mechanism of fused silica damage and the fundamental principles of damage growth.

Motion-corrected 3D-EPTI with efficient 4D navigator acquisition for fast and robust whole-brain quantitative imaging.

To develop a motion estimation and correction method for motion-robust three-dimensional (3D) quantitative imaging with 3D-echo-planar time-resolved imaging. The 3D-echo-planar time-resolved imaging technique was designed with additional four-dimensional navigator acquisition (x-y-z-echoes) to achieve fast and motion-robust quantitative imaging of the human brain. The four-dimensional-navigator is inserted into the relaxation-recovery deadtime of the sequence in every pulse TR (∼2s) to avoid extra scan time, and to provide continuous tracking of the 3D head motion and B0 -inhomogeneity changes. By using an optimized spatiotemporal encoding combined with a partial-Fourier scheme, the navigator acquires a large central k-t data block for accurate motion estimation using only four small-flip-angle excitations and readouts, resulting in negligible signal-recovery reduction to the 3D-echo-planar time-resolved imaging acquisition. By incorporating the estimated motion and B0 -inhomogeneity changes into the reconstruction, multi-contrast images can be recovered with reduced motion artifacts. Simulation shows the cost to the SNR efficiency from the added navigator acquisitions is <1%. Both simulation and in vivo retrospective experiments were conducted, that demonstrate the four-dimensional navigator provided accurate estimation of the 3D motion and B0 -inhomogeneity changes, allowing effective reduction of image artifacts in quantitative maps. Finally, in vivo prospective undersampling acquisition was performed with and without head motion, in which the motion corrupted data after correction show close image quality and consistent quantifications to the motion-free scan, providing reliable quantitative measurements even with head motion. The proposed four-dimensional navigator acquisition provides reliable tracking of the head motion and B0 change with negligible SNR cost, equips the 3D-echo-planar time-resolved imaging technique for motion-robust and efficient quantitative imaging.

SNR-efficient distortion-free diffusion relaxometry imaging using accelerated echo-train shifted echo-planar time-resolving imaging (ACE-EPTI).

To develop an efficient acquisition technique for distortion-free diffusion MRI and diffusion-relaxometry. A new accelerated echo-train shifted echo-planar time-resolved imaging (ACE-EPTI) technique is developed to achieve high-SNR, distortion-free diffusion, and diffusion-relaxometry imaging. ACE-EPTI uses a newly designed variable density spatiotemporal encoding with self-navigators for phase correction, that allows for submillimeter in-plane resolution using only 3-shot. Moreover, an echo-train-shifted acquisition is developed to achieve minimal TE, together with an SNR-optimal readout length, leading to ∼30% improvement in SNR efficiency over single-shot EPI. To recover the highly accelerated data with high image quality, a tailored subspace image reconstruction framework is developed, that corrects for odd/even-echo phase difference, shot-to-shot phase variation, and the B0 field changes because of field drift and eddy currents across different dynamics. After the phase-corrected subspace reconstruction, artifacts-free high-SNR diffusion images at multiple TEs are obtained with varying T2 * weighting. Simulation, phantom, and in vivo experiments were performed, which validated the 3-shot spatiotemporal encoding provides accurate reconstruction at submillimeter resolution. The use of echo-train shifting and optimized readout length improves the SNR-efficiency by 27%-36% over single-shot EPI. The level of image distortion was also evaluated, which shows no noticeable susceptibility and eddy-current distortions in ACE-EPTI images that are common in EPI. The time-resolved acquisition of ACE-EPTI also provides multi-TE images for diffusion-relaxometry analysis. ACE-EPTI was demonstrated to be an efficient and powerful technique for high-resolution diffusion imaging and diffusion-relaxometry, which provides high SNR, distortion- and blurring-free, and time-resolved multi-echo images by a fast 3-shot acquisition.

Time-resolved imaging of ultrasound waveform with synchronized laser illumination

We present a synchronous time delay technique to precisely control the illuminating laser pulses and the ultrasonic wave generation to visualize the ultrasound waveform through the Schlieren imaging method. The proposed time-resolved imaging technique offers the two-dimensional mapping of ultrasound waveform in a temporally evolved manner. The critical physical parameters, such as speed and spatial pulse length of ultrasonic waves, are visualized and calculated from image analysis. Our results suggest a protocol in characterizing ultrasound waveform, and it has the potential to reconstruct the acoustic field by accumulating the time-lapse waveforms.

Ultrafast decay dynamics of 2-hydroxypyridine excited to S1 electronic state

The S1 state decay dynamics of 2-hydroxypyridine following UV excitation at a wavelength range of 276.9−250.0 nm is investigated using femtosecond time-resolved photoelectron imaging technique. Based on pump wavelength dependence of the decay dynamics, a refined decay picture is proposed. At pump wavelength of 276.9 nm, the S1 state is depopulated through intersystem crossing to lower triplet state(s). At 264.0 nm, both intersystem crossing to lower triplet state(s) and internal conversion to the ground state are in operation. At 250.0 nm, internal conversion to the ground state becomes dominated.

Time-Resolved Scanning Ion Conductance Microscopy for Three-Dimensional Tracking of Nanoscale Cell Surface Dynamics.

Nanocharacterization plays a vital role in understanding the complex nanoscale organization of cells and organelles. Understanding cellular function requires high-resolution information about how the cellular structures evolve over time. A number of techniques exist to resolve static nanoscale structure of cells in great detail (super-resolution optical microscopy, EM, AFM). However, time-resolved imaging techniques tend to either have a lower resolution, are limited to small areas, or cause damage to the cells, thereby preventing long-term time-lapse studies. Scanning probe microscopy methods such as atomic force microscopy (AFM) combine high-resolution imaging with the ability to image living cells in physiological conditions. The mechanical contact between the tip and the sample, however, deforms the cell surface, disturbs the native state, and prohibits long-term time-lapse imaging. Here, we develop a scanning ion conductance microscope (SICM) for high-speed and long-term nanoscale imaging of eukaryotic cells. By utilizing advances in nanopositioning, nanopore fabrication, microelectronics, and controls engineering, we developed a microscopy method that can resolve spatiotemporally diverse three-dimensional (3D) processes on the cell membrane at sub-5-nm axial resolution. We tracked dynamic changes in live cell morphology with nanometer details and temporal ranges of subsecond to days, imaging diverse processes ranging from endocytosis, micropinocytosis, and mitosis to bacterial infection and cell differentiation in cancer cells. This technique enables a detailed look at membrane events and may offer insights into cell–cell interactions for infection, immunology, and cancer research.

Time-resolved fluorescence imaging technique for rat brain tumors analysis

The paper presents a new approach to assessing the state of tissues that differ in phenotype and in the degree of immunocompetent cells activity using photosensitizers (PS) and time-resolved fluorescence analysis methods. The main attention is paid to the detection of differences between tumor cells and tumor-associated macrophages (TAM) using spectroscopic and microscopic methods by the fluorescent kinetics signal and the difference in the accumulation of PS (the accumulation is several times greater in macrophages). The results of the PS photoluminescence study were obtained using two different techniques: time-resolved spectroscopy and time-resolved fluorescence microscopy (FLIM). Time-resolved spectroscopic analysis of the PS fluorescence lifetime was performed on adult female rats with induced C6 glioma in vivo. 5-ALA-induced Pp IX, which is widely used in clinical practice for carrying out effective conduction photodiagnostics and PDT, was used as the PS.

Analysis of Molecular Disordering Processes in the Phase Transition of Liquid Crystals Observed by Patterned-Illumination Time-Resolved Phase Microscopy.

The initial processes of the phase transition dynamics of liquid crystals (LCs) subject to UV pulse irradiation were clarified using a nanosecond time-resolved imaging technique called pattern-illumination time-resolved phase microscopy (PI-PM). Two types of LCs were studied: a photo-responsive LC and dye-doped LCs. We found two steps of molecular disordering processes in the phase transition, namely local disordering proceeding anisotropically, followed by the spreading of the isotropic phase. These two processes were separated for a photo-responsive LC while being simultaneously observed for the dye-doped LCs. It was found that the photomechanical dyes induced the phase transition process faster than the photothermal dyes.

Dynamic, Time-Resolved Computed Tomography Angiography Technique to Characterize Aortic Endoleak Type, Inflow and Provide Guidance for Targeted Treatment

Purpose: To illustrate dynamic, time-resolved CTA (d-CTA) imaging technique in characterizing aortic endoleak type/inflow using quantitative parameters and its value in providing image guidance for targeted treatment approach. Technique: Dedicated endoleak protocol involved acquiring multiple time-resolved contrast enhanced scans using third-generation CT scanner (Somatom Force®, Siemens Healthineers). Parameters such as scan field of view (FOV), kV, number/timing of scans were customized based on patient’s body-mass-index, timing bolus, and prior imaging findings. D-CTA image datasets were evaluated qualitatively and quantitatively using time-attenuation curves (TAC) analysis after motion correction using a dedicated software (syngo.via®, Siemens). D-CTA findings from 4 illustrative cases demonstrating type I, type II (inferior mesenteric and lumbar artery inflow), and type III endoleak were illustrated. TAC analysis with time to peak parameter enabled better characterization of endoleak type and inflow. During endoleak intervention, target vessels from d-CTA images were electronically annotated and overlaid on fluoroscopy using 2D−3D image fusion to provide image guidance for targeted treatment. Conclusion: D-CTA imaging with TAC analysis characterizes aortic endoleak type and inflow, in addition to providing image guidance for targeted endoleak treatment. Such dynamic, time-resolved imaging techniques may provide further insights into understanding aortic endoleak that remains an Achilles heel for endovascular aortic aneurysm repair.

Substituent Effects on the Vibrational Properties of the CN Stretch Mode of Aromatic Nitriles: IR Probes Useful for Time-resolved IR Spectroscopy.

Developing ideal IR probes is essential to understand the structure and dynamics of biomolecules with time-resolved IR spectroscopies and imaging techniques. Especially, nitrile (CN) group has recently been proposed to serve as IR probes of the local environment of proteins. Herein, we investigated the effect of a substituent on the vibrational properties of the benzonitrile. The electron-donating and withdrawing character of p-substituent on benzonitrile are expected to modulate the vibrational frequency, molar extinction coefficient, and vibrational lifetime of CN probe. FT-IR revealed the positive correlation between electron-donating character and the molar extinction coefficient of CN stretch mode. Infrared pump-probe (IR-PP) measurements showed that the vibrational lifetime of CN stretch mode exhibits a relatively weak correlation with the electron-donating strength. Among the investigated samples, 4-dimethylamino benzonitrile with the strongest electron-donating strength shows enhanced absorption and extended vibrational lifetime. Utilizing substituent effects will be a practical strategy to improve the performance of the IR probe.

Time-resolved imaging techniques applied to femtosecond laser material processing

Time-resolved imaging techniques applied to femtosecond laser material processing

Giant enhancement of THz-frequency optical nonlinearity by phonon polariton in ionic crystals

The field of nonlinear optics has grown substantially in past decades, leading to tremendous progress in fundamental research and revolutionized applications. Traditionally, the optical nonlinearity for a light wave at frequencies beyond near-infrared is observed with very high peak intensity, as in most materials only the electronic nonlinearity dominates while ionic contribution is negligible. However, it was shown that the ionic contribution to nonlinearity can be much larger than the electronic one in microwave experiments. In the terahertz (THz) regime, phonon polariton may assist to substantially trigger the ionic nonlinearity of the crystals, so as to enhance even more the nonlinear optical susceptibility. Here, we experimentally demonstrate a giant second-order optical nonlinearity at THz frequency, orders of magnitude higher than that in the visible and microwave regimes. Different from previous work, the phonon-light coupling is achieved under a phase-matching setting, and the dynamic process of nonlinear THz generation is directly observed in a thin-film waveguide using a time-resolved imaging technique. Furthermore, a nonlinear modification to the Huang equations is proposed to explain the observed nonlinearity enhancement. This work brings about an effective approach to achieve high nonlinearity in ionic crystals, promising for applications in THz nonlinear technologies.