Single-pulse Imaging Research Articles

Single-pulse real-time billion-frames-per-second planar imaging of ultrafast nanoparticle-laser dynamics and temperature in flames

Unburnt hydrocarbon flames produce soot, which is the second biggest contributor to global warming and harmful to human health. The state-of-the-art high-speed imaging techniques, developed to study non-repeatable turbulent flames, are limited to million-frames-per-second imaging rates, falling short in capturing the dynamics of critical species. Unfortunately, these techniques do not provide a complete picture of flame-laser interactions, important for understanding soot formation. Furthermore, thermal effects induced by multiple consecutive pulses modify the optical properties of soot nanoparticles, thus making single-pulse imaging essential. Here, we report single-shot laser-sheet compressed ultrafast photography (LS-CUP) for billion-frames-per-second planar imaging of flame-laser dynamics. We observed laser-induced incandescence, elastic light scattering, and fluorescence of soot precursors - polycyclic aromatic hydrocarbons (PAHs) in real-time using a single nanosecond laser pulse. The spatiotemporal maps of the PAHs emission, soot temperature, primary nanoparticle size, soot aggregate size, and the number of monomers, present strong experimental evidence in support of the theory and modeling of soot inception and growth mechanism in flames. LS-CUP represents a generic and indispensable tool that combines a portfolio of ultrafast combustion diagnostic techniques, covering the entire lifecycle of soot nanoparticles, for probing extremely short-lived (picoseconds to nanoseconds) species in the spatiotemporal domain in non-repeatable turbulent environments. Finally, LS-CUP’s unparalleled capability of ultrafast wide-field temperature imaging in real-time is envisioned to unravel mysteries in modern physics such as hot plasma, sonoluminescence, and nuclear fusion.

Research progress of ultra-high spatiotemporally resolved microscopy

High-resolution microscopy has opened the door to the exploration of the micro-world, while femtosecond laser has provided a measurement method for detecting ultrafast physical/chemical phenomena. Combination of these two techniques can produce new microscopic techniques with both ultra-high spatial resolution and ultra-fast temporal resolution, and thus has great importance in exploring new scientific phenomena and mechanisms on an extremely small spatial scale and temporal scale. This paper reviews the basic principles and properties of main microscopic techniques with ultra-high temporal resolution and spatial resolution, and introduces the latest research progress of their applications in various fields such as characterizing optoelectronic materials and devices, monitoring femtosecond laser micromachining, and detecting surface plasmon excitation dynamics. In order to conduct these researches systematically, we group these techniques based on time dimension and space dimension, including the near-field multi-pulse imaging techniques, the far-field multi-pulse imaging techniques, and the far-field single-pulse imaging techniques. In Section 2, we introduce the principles and characteristics of the ultra-high spatiotemporally resolved microscopic techniques. The near-field multi-pulse spatiotemporally microscopic techniques based on nano-probe are described in Subsection 2.1, in which is shown the combination of common near-field imaging techniques such as atomic force microscopy (AFM), near-field scanning optical microscopy (NSOM), scanning tunneling microscope (STM), and the ultra-fast temporal detection of pump-probe technique. In Subsection 2.2, we introduce the far-field multi-pulse spatiotemporal microscopic techniques. In contrast to near-field cases, the far-field spatiotemporal microscopic techniques have lower spatial resolution but possess more advantages of being non-invasive and non-contact, wider field of view, and faster imaging speed. In Subsection 2.3 we introduce the far-field single-pulse spatiotemporal microscopic techniques, in which is used a single ultrafast light pulse to capture dynamic processes at different moments in time, thereby enabling real-time imaging of ultrafast phenomena. In Section 3 , the advances in the application of the ultra-high spatiotemporal resolved microscopic techniques are introduced in many frontier areas, including the monitoring of femtosecond laser micromachining in Subsection 3.1, the detection of optoelectronic materials/devices in Subsection 3.2, and the characterization of surface plasmon dynamics in Subsection 3.3. Finally, in Section 4, we summarize the features of all above-mentioned spatiotemporal microscopic techniques in a table, including the spatial resolution and temporal resolution, advantages and disadvantages of each technique, and we also provide an outlook on future development trend in this research field. Looking forward to the future, ultra-high spatiotemporally resolved microscopy will develop rapidly toward the goal of "smaller, faster, smarter and more extensive". Its development not only promotes the research of the microscopy technology, but also provides a powerful tool for various practical applications such as precision machining, two-dimensional material dynamics, optoelectronic device design and characterization.

Control of the Longitudinal Compression and Transverse Focus of Ultrafast Electron Beam for Detecting the Transient Evolution of Materials.

Ultrafast detection is an effective method to reveal the transient evolution mechanism of materials. Compared with ultra-fast X-ray diffraction (XRD), the ultra-fast electron beam is increasingly adopted because the larger scattering cross-section is less harmful to the sample. The keV single-shot ultra-fast electron imaging system has been widely used with its compact structure and easy integration. To achieve both the single pulse imaging and the ultra-high temporal resolution, magnetic lenses are typically used for transverse focus to increase signal strength, while radio frequency (RF) cavities are generally utilized for longitudinal compression to improve temporal resolution. However, the detection signal is relatively weak due to the Coulomb force between electrons. Moreover, the effect of RF compression on the transverse focus is usually ignored. We established a particle tracking model to simulate the electron pulse propagation based on the 1-D fluid equation and the 2-D mean-field equation. Under considering the relativity effect and Coulomb force, the impact of RF compression on the transverse focus was studied by solving the fifth-order Rung–Kutta equation. The results show that the RF cavity is not only a key component of longitudinal compression but also affects the transverse focusing. While the effect of transverse focus on longitudinal duration is negligible. By adjusting the position and compression strength of the RF cavity, the beam spot radius can be reduced from 100 m to 30 m under the simulation conditions in this paper. When the number of single pulse electrons remains constant, the electrons density incident on the sample could be increased from to , which is 11 times the original. The larger the electron density incident on the sample, the greater the signal intensity, which is more conducive to detecting the transient evolution of the material.

Rigorous single pulse imaging for ultrafast interferometric observation.

We discuss how to realize rigorous single pulse imaging using a fiber mode-locked laser for the purpose of ultrafast interferometric observation of fast varying dynamic objects. Sub-picosecond pulses are readily picked up in synchronization with the camera operation, allocating one pulse per frame, but rigorous ultrashort single pulse imaging is disturbed by the accumulation of amplified spontaneous emission (ASE) over the exposure time of the camera. Here, we propose four distinct methods to eliminate the ASE-accumulated disruption in the ultrashort optical gating by pulse interferometry and then evaluate their merits and limitations individually by experiments. The proposed four methods are referred to respectively as the time averaged phase modulation, unbalanced pulse overlapping, tandem pulse picking, and second harmonic generation.

Four-Dimensional Probing of Phase-Reaction Dynamics in Au/GaAs Nanowires.

Nanoeutectic phase reaction covers the fundamental study of a chemical and physical reaction of multiple phases at the nanoscale. Here, we report the direct visualization of phase-reaction dynamics in Au/GaAs nanowires (NWs) using four-dimensional (4D) electron microscopy. The NW phase reactions were initiated with a pump laser pulse, while the following dynamics in the Au/GaAs NW was probed by a precisely time-delayed electron pulse. Single-pulse imaging reveals that the cubic zinc-blende NW presents a transient length increase within the time duration of ∼150 ns, giving the appearance of intermediate phase reactions at an early stage. A final length reduction of the NW is observed after the phase reactions have fully ended. In contrast, only length reduction is seen throughout the entire process in GaAs/AlGaAs core-shell and hexagonal wurtzite GaAs NWs. The reasons for the above intriguing phenomena are discussed. The eutectic-related phenomena in both zinc-blende and wurtzite materials offer a comprehensive understanding of phase-reaction dynamics in polytypic structures commonly available in compound semiconductors.

Superposition of streamer and glow discharges in single pulse mode of sliding discharge burning in Ne

Numerical simulation of streamer development following the 1D ‘classic fluid model’ of ionization wave front propagation is applied to analyze the previously observed superposition of streamer- and glow-type discharges, in experiments with Ne using a single pulse sliding discharge setup at voltage amplitudes below the threshold of the spark gas breakdown. Experimental results are presented using single pulse images of spatial discharge plasma distribution between two parallel strip electrodes placed above the alumina ceramics substrate, at Ne pressures of 30 and 100 kPa and with the applied voltage rise time of 20–25 ns. A comparison of electron density values, calculated behind the wave front and estimated from the experiments, resulted in the conclusion that discharge formation in the gap begins from the development and propagation of the ionization wave. Its formation starts from the high voltage electrode at faster temporal dynamics as compared to the glow discharge, whose slower development begins from the cathode. The structure of the visual discharge plasma depends on the discharge voltage and polarity, as well as the gas pressure. In particular, at relatively low voltage the wave propagation may stop somewhere in the gap and then the rest of the gap is occupied by the glow discharge only, as was observed in positive polarity experiments at a gas pressure of 100 kPa.

First functionality tests of a 64 × 64 pixel DSSC sensor module connected to the complete ladder readout

The European X-ray Free Electron Laser (XFEL.EU) will provide every 0.1 s a train of 2700 spatially coherent ultrashort X-ray pulses at 4.5 MHz repetition rate. The Small Quantum Systems (SQS) instrument and the Spectroscopy and Coherent Scattering instrument (SCS) operate with soft X-rays between 0.5 keV–6 keV. The DEPFET Sensor with Signal Compression (DSSC) detector is being developed to meet the requirements set by these two XFEL.EU instruments. The DSSC imager is a 1 mega-pixel camera able to store up to 800 single-pulse images per train. The so-called ladder is the basic unit of the DSSC detector. It is the single unit out of sixteen identical-units composing the DSSC-megapixel camera, containing all representative electronic components of the full-size system and allows testing the full electronic chain. Each DSSC ladder has a focal plane sensor with 128× 512 pixels. The read-out ASIC provides full-parallel readout of the sensor pixels. Every read-out channel contains an amplifier and an analog filter, an up-to 9 bit ADC and the digital memory. The ASIC amplifier have a double front-end to allow one to use either DEPFET sensors or Mini-SDD sensors. In the first case, the signal compression is a characteristic intrinsic of the sensor; in the second case, the compression is implemented at the first amplification stage. The goal of signal compression is to meet the requirement of single-photon detection capability and wide dynamic range. We present the first results of measurements obtained using a 64× 64 pixel DEPFET sensor attached to the full final electronic and data-acquisition chain.

High resolution corneal and single pulse imaging with line field spectral domain optical coherence tomography.

We report the development of a Spectral Domain Line Field Optical Coherence Tomography (LF-OCT) system, using a broad bandwidth and spatial coherent Super-Continuum (SC) source. With conventional quasi-Continuous Wave (CW) setup we achieve axial resolutions up to 2.1 μm in air and 3D volume imaging speeds up to 213 kA-Scan/s. Furthermore, we report the use of a single SC pulse, of 2 ns duration, to temporally gate an OCT B-Scan image of 70 A-Scans. This is the equivalent of 35 GA-Scans/s. We apply the CW setup for high resolution imaging of the fine structures of a human cornea sample ex-vivo. The single pulse setup is applied to imaging of a coated pharmaceutical tablet. The fixed pattern noise due to spectral noise is removed by subtracting the median magnitude A-Scan. We also demonstrate that the Fourier phase can be used to remove aberration caused artefacts.

Copper bromide vapor brightness amplifiers with 100 kHz pulse repetition frequency

The paper presents a laser monitor with 10μs time-resolution based on a high-frequency copper bromide vapor brightness amplifier. A sync circuit has been designed for single-pulse imaging. The analysis of amplifying characteristics of the active elements and active optical system (laser monitor) parameters allowed to determine the optimal concentration of HBr at which the images can be obtained with minimum distortions. For the active element operating at high frequencies (more than 50kHz) as a brightness amplifier, the concentration of HBr must be lower than that needed for obtaining the maximum output power. The limiting brightness temperature of the background radiation which does not affect the image quality is determined. The potential feasibility of using a proposed brightness amplifier for visualizing processes blocked from viewing by the background radiation with the brightness temperature up to 8000K is demonstrated.

Detector developments at DESY.

With the increased brilliance of state-of-the-art synchrotron radiation sources and the advent of free-electron lasers (FELs) enabling revolutionary science with EUV to X-ray photons comes an urgent need for suitable photon imaging detectors. Requirements include high frame rates, very large dynamic range, single-photon sensitivity with low probability of false positives and (multi)-megapixels. At DESY, one ongoing development project - in collaboration with RAL/STFC, Elettra Sincrotrone Trieste, Diamond, and Pohang Accelerator Laboratory - is the CMOS-based soft X-ray imager PERCIVAL. PERCIVAL is a monolithic active-pixel sensor back-thinned to access its primary energy range of 250 eV to 1 keV with target efficiencies above 90%. According to preliminary specifications, the roughly 10 cm × 10 cm, 3.5k × 3.7k monolithic sensor will operate at frame rates up to 120 Hz (commensurate with most FELs) and use multiple gains within 27 µm pixels to measure 1 to ∼100000 (500 eV) simultaneously arriving photons. DESY is also leading the development of the AGIPD, a high-speed detector based on hybrid pixel technology intended for use at the European XFEL. This system is being developed in collaboration with PSI, University of Hamburg, and University of Bonn. The AGIPD allows single-pulse imaging at 4.5 MHz frame rate into a 352-frame buffer, with a dynamic range allowing single-photon detection and detection of more than 10000 photons at 12.4 keV in the same image. Modules of 65k pixels each are configured to make up (multi)megapixel cameras. This review describes the AGIPD and the PERCIVAL concepts and systems, including some recent results and a summary of their current status. It also gives a short overview over other FEL-relevant developments where the Photon Science Detector Group at DESY is involved.

TH-C-17A-03: Dynamic Visualization and Dosimetry of IMRT and VMAT Treatment Plans by Video-Rate Imaging of Cherenkov Radiation in Pure Water

Purpose: A novel optical dosimetry technique for the QA and verification of intensity-modulated radiation therapy (IMRT) and volumetric-modulated arc therapy (VMAT) radiotherapy plans was investigated for the first time by capturing images of the induced Cherenkov radiation in water. Methods: An intensified CCD camera (ICCD) was used to acquire a two-dimensional (2D) projection image of the Cherenkov radiation induced by IMRT and VMAT plans, based on the Task Group 119 C-Shape geometry. Plans were generated using the Varian Eclipse treatment planning system (TPS) and delivered using 6 MV x-rays from a Varian TrueBeam Linear Accelerator (Linac) incident on a water tank. The ICCD acquisition was gated to the Linac, operated for single pulse imaging, and binned to a resolution of 512×512 pixels. The resulting videos were analyzed temporally for regions of interest (ROI) covering the planning target volume (PTV) and organ at risk (OAR) and summed to obtain an overall light distribution, which was compared to the expected dose distribution from the TPS using a gammaindex analysis. Results: The chosen camera settings resulted in data at 23.5 frames per second. Temporal intensity plots of the PTV and OAR ROIs confirmed the preferential delivery of dose to the PTV versus the OAR, and the gamma analysis yielded 95.2% and 95.6% agreement between the light distribution and expected TPS dose distribution based upon a 3% / 3 mm dose difference and distance-to-agreement criterion for the IMRT and VMAT plans respectively. Conclusion: The results from this initial study demonstrate the first documented use of Cherenkov radiation for optical dosimetry of dynamic IMRT and VMAT treatment plans. The proposed modality has several potential advantages over alternative methods including the real-time nature of the acquisition, and upon future refinement may prove to be a robust and novel dosimetry method with both research and clinical applications. NIH R01CA109558 and R21EB017559.

Laser monitor for non-destructive testing of materials and processes shielded by intensive background lighting

A single-pulse imaging laser projection system (laser monitor) is proposed for real-time monitoring high-speed processes shielded by the intensive background lighting. The brightness temperature of the lighting can reach thousands or even tens of thousands of degrees, which makes it difficult to observe the processes with the naked eye. The estimates of limiting temperatures show that the use of the proposed instrument allows to view the objects when the equivalent brightness temperature of the background lighting is up to 45,000 K. The results of visualization of some bright objects and processes using high-speed copper bromide vapor laser monitor are presented.

Motion clustering for deblurring multispectral optoacoustic tomography images of the mouse heart

Cardiac imaging in small animals is a valuable tool in basic biological research and drug discovery for cardiovascular disease. Multispectral optoacoustic tomography (MSOT) represents an emerging imaging modality capable of visualizing specific tissue chromophores at high resolution and deep in tissues in vivo by separating their spectral signatures. Whereas single-wavelength images can be acquired by multielement ultrasound detection in real-time imaging, using multiple wavelengths at separate times can lead to image blurring due to motion during acquisition. Therefore, MSOT imaging of the heart results in degraded resolution because of the heartbeat. In this work, we applied a clustering algorithm, k-means, to automatically separate a sequence of single-pulse images at multiple excitation wavelengths into clusters corresponding to different stages of the cardiac cycle. We then performed spectral unmixing on each cluster to obtain images of tissue intrinsic chromophores at different cardiac stages, showing reduced sensitivity to motion compared to signal averaging without clustering. We found that myocardium images of improved resolution and contrast can be achieved using MSOT motion clustering correction. The correction method presented could be generally applied to other MSOT imaging applications prone to motion artifacts, for example, by respiration and heartbeat.

X-ray holographic microscopy with zone plates applied to biological samples in the water window using 3rd harmonic radiation from the free-electron laser FLASH

The imaging of hydrated biological samples - especially in the energy window of 284-540 eV, where water does not obscure the signal of soft organic matter and biologically relevant elements - is of tremendous interest for life sciences. Free-electron lasers can provide highly intense and coherent pulses, which allow single pulse imaging to overcome resolution limits set by radiation damage. One current challenge is to match both the desired energy and the intensity of the light source. We present the first images of dehydrated biological material acquired with 3rd harmonic radiation from FLASH by digital in-line zone plate holography as one step towards the vision of imaging hydrated biological material with photons in the water window. We also demonstrate the first application of ultrathin molecular sheets as suitable substrates for future free-electron laser experiments with biological samples in the form of a rat fibroblast cell and marine biofouling bacteria Cobetia marina.

Ultra-intense X-ray Induced Non-linear Processes in Molecular Nitrogen

Sequential multiple photoionization of the prototypical molecule N2 is studied with femtosecond time resolution using the Linac Coherent Light Source (LCLS). A detailed picture of intense x-ray induced ionization and dissociation dynamics is revealed, including a molecular mechanism of frustrated absorption that suppresses the formation of high charge states at short pulse durations. The inverse scaling of the average target charge state with x-ray peak brightness has possible implications for single pulse imaging applications. Moreover, we investigate the creation of double K-shell holes in N2 molecules via sequential absorption of two photons on a timescale shorter than the core-hole lifetime by using intense x-ray pulses from the LCLS. The production and decay of these states is characterized by photoelectron spectroscopy and Auger electron spectroscopy. In molecules, two types of double core holes are expected, the first with two core holes on the same N atom, and the second with one core hole on each N atom. We report the first direct observations of the former type of core hole in a molecule, in good agreement with theory, and provide an experimental upper bound for the relative contribution of the latter type.

Digital in-line X-ray holography with zone plates

Single pulse imaging with radiation provided by free-electron laser sources is a promising approach towards X-ray microscopy, which is expected to provide high resolution images of biological samples unaffected by radiation damage. One fully coherent imaging technique for this purpose is digital in-line holography. Key to its successful application is the creation of X-ray point sources with high photon flux. In this study we applied zone plates to create such point sources with synchrotron radiation provided by the storage ring BESSY II. The obtained, divergent light cone is applied to holographic microscopy of biological objects such as critical point dried Navicula perminuta diatoms and human cells using photons with an energy of 250 eV. Compared to conventional experiments employing pinholes, exposure times are reduced by two orders of magnitude.

Femtosecond pulse x-ray imaging with a large field of view

Femtosecond pulse x-ray imaging is demonstrated in a sample-multiplexed Fourier transform holography scheme. Parallel imaging of multiple samples over an extended field of view is achieved by exploiting the coherence properties of the free-electron laser (FEL) source and the large profile of the unfocused x-ray pulse. The resulting photon flux density per pulse allows for damage-free single-pulse imaging with moderate image resolution. We envision the application of the method for femtosecond time-resolved pump–probe experiments with the feasibility of recording multiple steps in time with a single pulse. Furthermore, the scheme presented allows for a characterization of FEL radiation pulse parameters.

Ultraintense X-Ray Induced Ionization, Dissociation, and Frustrated Absorption in Molecular Nitrogen

Sequential multiple photoionization of the prototypical molecule N2 is studied with femtosecond time resolution using the Linac Coherent Light Source (LCLS). A detailed picture of intense x-ray induced ionization and dissociation dynamics is revealed, including a molecular mechanism of frustrated absorption that suppresses the formation of high charge states at short pulse durations. The inverse scaling of the average target charge state with x-ray peak brightness has possible implications for single-pulse imaging applications.

Quantifying transient states in materials with the dynamic transmission electron microscope

The dynamic transmission electron microscope (DTEM) offers a means of capturing rapid evolution in a specimen through in situ microscopy experiments by allowing 15-ns electron micrograph exposure times. The rapid exposure time is enabled by creating a burst of electrons at the emitter by ultraviolet pulsed laser illumination. This burst arrives at a specified time after a second laser initiates the specimen reaction. The timing of the two Q-switched lasers is controlled by high-speed pulse generators with a timing error much less than the pulse duration. Both diffraction and imaging experiments can be performed, just as in a conventional TEM. The brightness of the emitter and the total current control the spatial and temporal resolutions. We have demonstrated 7-nm spatial resolution in single 15-ns pulsed images. These single-pulse imaging experiments have been used to study martensitic transformations, nucleation and crystallization of an amorphous metal and rapid chemical reactions. Measurements have been performed on these systems that are possible by no other experimental approaches currently available.

Doppler Compensation & Single Pulse Imaging using Adaptive Pulse Compression

The effects of target Doppler are addressed in relation to adaptive receive processing for radar pulse compression. To correct for Doppler-induced filter mismatch over a single pulse, the Doppler-compensated adaptive pulse compression (DC-APC) algorithm is presented whereby the respective Doppler shifts for large target returns are jointly estimated with the illuminated range profile and subsequently incorporated into the original APC adaptive receive filter formulation. As a result, the Doppler-mismatch-induced range sidelobes can be suppressed thereby regaining a significant portion of the sensitivity improvement that is possible when applying adaptive pulse compression (APC) without the existence of significant Doppler mismatch. In contrast, instead of compensating for Doppler mismatch, the single pulse imaging (SPI) algorithm generalizes the APC formulation for a bank of Doppler-shifted matched filters thereby producing a sidelobe-suppressed range-Doppler image from the return signal of a single radar pulse which is applicable for targets with substantial variation in Doppler. Both techniques are based on the recently proposed APC algorithm and its generalization, the multistatic adaptive pulse compression (MAPC) algorithm, which have been shown to be effective for the suppression of pulse compression range sidelobes thus dramatically increasing the sensitivity of pulse compression radar.