"Single-shot" ultrafast spectroscopy based on the frequency encoding of transient absorbance kinetics using chirped probe pulses is analyzed theoretically. FDSS has an advantage over pump-probe spectroscopy in a situation where the "noise" is dominated by amplitude variations of the signal. Unlike "single-shot" techniques based on spatial encoding of the kinetics, no a priori knowledge of the excitation profile of the pump is needed. FDSS spectroscopy can be used for many types of samples, liquid or solid, including those comparable in thickness to the wavelength of the probe light. Another advantage is that due to the interference of quasimonochromatic components of the chirped probe pulse, an oscillation pattern near the origin of the FDSS kinetics emerges. This interference pattern is unique and can be used to determine the complex dielectric function of the photogenerated species.
Single-shot ultrafast absorbance spectroscopy based on the frequency encoding of the kinetics is analyzed theoretically and implemented experimentally. In Part II of the series, arbitrary thickness sample is analysed theroretically. The model is then used to simulate the results for a-Si:H films.
Single-shot ultrafast absorbance spectroscopy based on the frequency encoding of the kinetics is analyzed theoretically and implemented experimentally. The kinetics are sampled in the frequency domain using linearly chirped, amplified 33 fs FWHM pulses derived from a Ti:sapphire laser. A variable length grating pair compressor is used to achieve the time resolution of 500-1000 channels per a 2-to-160 ps window with sensitivity > 5x10-4. In terms of the acquisition time, FDSS has an advantage over the pump-probe spectroscopy in a situation when the "noise" is dominated by amplitude variations o…
Single-shot ultrafast spectroscopy based on the frequency encoding of transient absorbance kinetics (FDSS) is demonstrated. These kinetics are sampled spectrally using linearly chirped pulses derived from a Ti:sapphire laser. A variable length grating pair compressor is used to provide group velocity dispersion out to -1.6 ps^2 and achieve the sampling of 512 channels per a 2-to-160 ps window with sensitivity > 5e-4. The possibilities of FDSS are illustrated with studies of three photon ionization of liquid water and one-photon excitation of a thin-film
It is critical to characterize the carrier and instantaneous frequency distribution variation in ultrafast processes, all of which are determined by the optical phase. Nevertheless, there is no method that can single-shot record the intro-pulse phase evolution of pico/femtosecond signals, to date. By analogying holographic principle in space to the time domain and using the time-stretch method, we propose the dispersive temporal holography to single-shot recover the phase and amplitude of ultrafast signals. It is a general and comprehensive technology and can be applied to analyze ultrafast si…
We have developed a single-shot imaging technique that can capture ultrafast events occurring on femtosecond to picosecond time scales. The technique is based on an optical pump-probe method, in which multiple time-delayed femtosecond pulses simultaneously probe a pump-excited sample. Here we use two sets of 2-by-2 mirror arrays for spatial/temporal division and routing of multiple probe pulses. This single-shot scheme is successfully applied to capture femtosecond ionization fronts propagating at the speed of light in air, as well as laser-induced ablation of solid targets.
Precise measurement of multi-parameters of ultrafast lasers is vital both in scientific investigations and technical applications, such as, optical field manipulation, pulse shaping, sample characteristics test, and biomedical imaging. Tremendous progress in parameter measurement of ultrafast laser has been made, including single-shot spectra acquired by time-stretch dispersive Fourier transform in spectral domain, and pulse magnification or compression realized by time lens in temporal domain. Nevertheless, single-shot measurement of frequency-resolved states of polarization (SOPs) of ultrafa…
Single-shot ultrafast optical imaging plays a very important role in the detection of transient scenes, especially in capturing irreversible or stochastic dynamic scenes. To break the limit of time response speed of electronic devices, such as charge-coupled device (CCD) or complementary metal-oxide-semiconductor (CMOS) detectors, ultrafast optical imaging techniques usually convert the time information of a transient scene into the wavelength, angle, space or spatial frequency of the illumination light in previous studies. In this work, we propose a novel polarization-resolved ultrafast mappi…
We present a method for acquiring a sequence of time-resolved images in a single shot, called Single-Shot Non-Synchronous Array Photography (SNAP). In SNAP, a pulsed laser beam is split by a diffractive optical element into an array of angled beamlets whose illumination fronts remain perpendicular to the optical axis. Different time delays are imparted to each beamlet by an echelon, enabling them to probe a scene in rapid succession. The beamlets are then imaged onto different regions of a camera by a lenslet array. Because the illumination fronts remain flat (head-on) independently of beamlet…
Driven by many applications in a wide span of scientific fields, a myriad of advanced ultrafastimaging techniques have emerged in the last decade, featuring record-high imaging speeds abovea trillion-frame-per-second with long sequence depths. Although bringing remarkable insights invarious ultrafast phenomena, their application out of a laboratory environment is however limitedin most cases, either by the cost, complexity of operation or by an heavy data processing. We thenreport a flexible single-shot imaging technique combining sequentially-timed all-optical mappingphotography (STAMP) with …
Ultrafast lasers have revolutionized material processing, opening a wealth of new applications in many areas of science. A recent technology that allows the cleaving of transparent materials via non-ablative processes is based on focusing and translating a high-intensity laser beam within a material to induce a well-defined internal stress plane. This then enables material separation without debris generation. Here, we use a non-diffracting beam engineered to have a transverse elliptical spatial profile to generate high aspect ratio elliptical channels in glass of dimension 350 nm x 710 nm, an…
We present a laboratory system for single-shot magneto-optical (MO) imaging of ultrafast magnetization dynamics with high-sensitivity of MO rotation. We create a stack of MO images repeatedly employing a single pair of a pump and defocused probe pulses to induce and visualize MO changes in the sample. Both laser beams are independently wavelength-tunable allowing for a flexible, resonant adjustable two-color pump and probe scheme. To increase the MO contrast the probe beam is spatially filtered. We performed the all-optical switching experiment in Co-doped yttrium iron garnet films (YIG:Co) to…
Ultrafast imaging is a powerful tool for studying space-time dynamics in photonic material, plasma physics, living cells, and neural activity. Pushing the imaging speed to the quantum limit could reveal extraordinary scenes about the questionable quantization of life and intelligence, or the wave-particle duality of light. However, previous designs of ultrafast photography are intrinsically limited by framing speed. Here, we introduce a new technique based on a multiple non-collinear optical parametric amplifier principle (MOPA), which readily push the frame rate into the area of ten trillion …
Temporal imaging systems are outstanding tools for single-shot observation of optical signals that have irregular and ultrafast dynamics. They allow long time windows to be recorded with femtosecond resolution, and do not rely on complex algorithms. However, simultaneous recording of amplitude and phase remains an open challenge for these systems. Here we present a new heterodyne time-lens arrangement that efficiently records both the amplitude and phase of complex signals, while keeping the performances of classical time-lens systems ($\sim 200$~fs) and field of view (tens of ps). Phase and t…
The discovery and understanding of many ultrafast dynamical processes are often invaluable. This paper is the first report to apply optical parametric amplification to implement single-shot ultrafast imaging with high space and time resolutions. Our setup breaks the constraints usually occurring among the time resolution, frame number, frame interval and spatial resolution in existing single-shot femtosecond imagers, so its performance can be greatly improved by using laser pulses with higher power and shorter time durations. Our setup has provided the highest experimental record of the frame …
Mode-locked lasers, which produce ultrashort pulses in the picosecond and femtosecond range, have enabled some of the most precise measurements. However, despite significant recent progress, resolving the temporal behavior of their short pulses is still a challenge. State-of-the-art oscilloscopes with tens of picosecond resolution prevent time-resolved observations in mode-locked lasers and limit the real-time pulse evolution tracking of ultrafast lasers. Here, using the time-lens technique with a Raman amplifier, we implement an ultrafast single-shot time-microscope (TM) with a high temporal …
We report here an experimental setup to perform three-pulse pump-probe measurements over a wide wavelength and temperature range. By combining two pump pulses in the visible (650-900 nm) and mid-IR (5-20 $μ$m) range, with a broadband supercontinuum white-light probe, our apparatus enables both the combined selective excitation of different material degrees of freedom and a full time-dependent reconstruction of the non-equilibrium dielectric function of the sample. We describe here the optical setup, the cryogenic sample environment and the custom-made acquisition electronics capable of referen…
Ultrafast manipulation of magnetic order has challenged our understanding the fundamental and dynamic properties of magnetic materials. So far single shot magnetic switching has been limited to ferrimagnetic alloys and multilayers. In ferromagnetic (FM)/antiferromagnetic (AFM) bilayers, exchange bias (He) arises from the interfacial exchange coupling between the two layers and reflects the microscopic orientation of the antiferromagnet. Here we demonstrate the possibility of single shot switching of the antiferromagnet (change of the sign and amplitude of He) with a single femtosecond laser pu…
We present a framing integration ultrafast photography (FIP), which integrates the framing structure, codes a dynamic event by an inversed 4f system (I4F) and decodes regionally with high spatial resolution. In the experiment about laser-induced plasma, FIP achieved a framing rate of 5.3*1012 frames per second (fps) and an intrinsic spatial resolution of 110.4 lp/mm. It has an excellent spatio-temporal resolution and a compact and flexible structure. Hence, it can probe unrepeatable ultrafast intra- and inter-atomic/molecular dynamics, different in size and duration with high-quality. Besides,…
Transition metal dichalcogenides are known to possess large optical nonlinearities and driving these materials at high intensities is desirable for many applications. Understanding their optical responses under repetitive intense excitation is essential to improve the performance limit of these strong-field devices and to achieve efficient laser patterning. Here, we report the incubation study of monolayer MoS${}_{2}$ and WS${}_{2}$ induced by 160 fs, 800 nm pulses in air to examine how their ablation threshold scales with the number of admitted laser pulses. Both materials were shown to outpe…
We have developed a method for producing spatially stable micron-scale liquid targets of flexible shapes at kilohertz repetition rate for use in air and vacuum, by perturbing 5 and 30 μm diameter streams with femtosecond laser pulses and monitoring the temporal development of the perturbation. Using water, we have produced features such as 2.1 μm diameter droplet and 1.3 μm diameter neck with less than 0.3 μm shot-to-shot variation, with prospects for further reduction in size and variability. The use of such micron-scale targets can be expected to prevent conductive heat dissipation, enhance …
We vary the time-frequency mode structure of ultrafast pulse-pumped modulational instability (MI) twin beams in an argon-filled hollow-core kagomé-style PCF by adjusting the pressure, pump pulse chirp, fiber length and parametric gain. Compared to solid-core systems, the pressure dependent dispersion landscape brings increased flexibility to the tailoring of frequency correlations and we demonstrate that the pump pulse chirp can be used to tune the joint spectrum of femtosecond-pumped sources. We also characterize the resulting mode content, not only by measuring the multimode second-order cor…
Although ultrafast laser materials processing has advanced at a breakneck pace over the last two decades, most applications have been developed with laser pulses at near-IR or visible wavelengths. Recent progress in mid-infrared (MIR) femtosecond laser source development may create novel capabilities for material processing. This is because, at high intensities required for such processing, wavelength tuning to longer wavelengths opens the pathway to a special regime of laser-solid interactions. Under these conditions, due to the $λ^2$ scaling, the ponderomotive energy of laser-driven electron…
Femtosecond-scale ultrafast imaging is an essential tool for visualizing ultrafast dynamics in molecular biology, physical chemistry, atomic physics, and fluid dynamics. Pump-probe imaging and a streak camera are the most widely used techniques, but they are either demanding the repetitions of the same scene or sacrificing the number of imaging dimensions. Many interesting single-shot ultrafast imaging techniques have been developed in recent years for recording non-repetitive dynamic scenes. Nevertheless, there are still weaknesses in the number of frames, the number of image pixels, or spati…
Time-bin qudits have emerged as a promising encoding platform in many quantum photonic applications. However, the requirement for efficient single-shot measurement of time-bin qudits instead of reconstructive detection has restricted their widespread use in experiments. Here, we propose an efficient method to measure arbitrary superposition states of time-bin qudits and confirm it up to dimension 4. This method is based on encoding time bins at the picosecond time scale, also known as ultrafast time bins. By doing so, we enable the use of robust and phase-stable single spatial mode temporal in…
Mid-infrared spectroscopy is often used to identify material. Thousands of spectral points are measured in a time-consuming process using expensive table-top instrument. However, material identification is a sparse problem, which in theory could be solved with just a few measurements. Here we exploit the sparsity of the problem and develop an ultra-fast, portable, and inexpensive method to identify materials. In a single-shot, a mid-infrared camera can identify materials based on their spectroscopic signatures. This method does not require prior calibration, making it robust and versatile in h…
Laser-induced transient opacity in helium nanodroplets probed by single-shot coherent diffraction
ETH Zurich（苏黎世联邦理工学院）；University of Rostock（罗斯托克大学）；Max Born Institute for Nonlinear Optics and Short Pulse Spectroscopy（马克斯·玻恩非线性光学和超快光谱研究所）；Technical University of Berlin（柏林工业大学）
Here we introduce three-dimensional single-shot ptychography (3DSSP). 3DSSP leverages an additional constraint unique to the single-shot geometry to deconvolve multiple 2D planes of a 3D object. Numeric simulations and analytic calculations demonstrate that 3DSSP reconstructs multiple planes in an extended 3D object with a minimum separation consistent with the depth of field for a conventional microscope. We experimentally demonstrate 3DSSP by reconstructing orthogonal hair strands axially separated by 5 mm. Three-dimensional single-shot ptychography provides a pathway towards volumetric imag…
The measurement of transient optical fields has proven critical to understanding the dynamical mechanisms underlying ultrafast physical and chemical phenomena, and is key to realizing higher speeds in electronics and telecommunications. Complete characterization of optical waveforms, however, requires an optical oscilloscope capable of resolving the electric field oscillations with sub-femtosecond resolution and with single-shot operation. Here, we show that strong-field nonlinear excitation of photocurrents in a silicon-based image sensor chip can provide the sub-cycle optical gate necessary …
We demonstrate a novel, single-shot ultrafast diagnostic, based on the dispersion-scan (d-scan) technique. In this implementation, rather than scanning wedges to vary the dispersion as in standard d-scan, the pulse to be measured experiences a spatially varying amount of dispersion in a Littrow prism. The resulting beam is then imaged into a second-harmonic generation crystal and an imaging spectrometer is used to measure the two-dimensional trace, which is analyzed using the d-scan retrieval algorithm. We compare the single-shot implementation with the standard d-scan for the measurement of s…
Visualizing ultrafast dynamics at the atomic scale requires time-resolved pump-probe characterization with femtosecond temporal resolution. For single-shot ultrafast electron diffraction (UED) with fully relativistic electron bunch probes, existing techniques are limited by the achievable electron probe bunch length, charge, and timing jitter. We present the first experimental demonstration of pump-probe UED with THz-driven compression and time-stamping that enable UED probes with unprecedented temporal resolution. This technique utilizes two counter-propagating quasi-single-cycle THz pulses g…
We introduce photonic kernel machines, a scheme for ultrafast spectral analysis of noisy radio-frequency signals from single-shot optical intensity measurements. The approach combines the versatility of machine learning and the speed of photonic hardware to reach unprecedented throughput rates. We theoretically describe some of the key underlying principles, and then numerically illustrate the reached performances on a photonic lattice-based implementation. We apply the technique both to picosecond pulsed radio-frequency signals, on energy-spectral-density estimation and a shape classification…
A femtosecond pump-probe setup is described that is optimised for broadband transient reflectivity experiments on solid samples over a wide range of temperatures. By combining a temporal resolution of 45 fs and a broad detection range between 1.75 and 2.85 eV, this apparatus can provide insightful information on the interplay between coherent collective modes and high-energy electronic excitations, which is one of the distinctive characteristics of strongly interacting and correlated quantum systems. The use of a single-shot readout CMOS array detector at frame rates up to 10 kHz allows to res…
Shot-noise-limited few-cycle mid-infrared frequency comb with attosecond phase stability
Wrocław University of Science and Technology（弗罗茨瓦夫理工大学）；University of Warsaw（华沙大学）；Center for Molecular Fingerprinting Research（分子指纹研究中心）；Max-Planck-Institute of Quantum Optics（马克斯·普朗克量子光学研究所）
We reconstructed the 3D Fourier intensity distribution of mono-disperse prolate nano-particles using single-shot 2D coherent diffraction patterns collected at DESY's FLASH facility when a bright, coherent, ultrafast X-ray pulse intercepted individual particles of random, unmeasured orientations. This first experimental demonstration of cryptotomography extended the Expansion-Maximization-Compression (EMC) framework to accommodate unmeasured fluctuations in photon fluence and loss of data due to saturation or background scatter. This work is an important step towards realizing single-shot diffr…
Single-shot laser-pulse-induced magnetization reversal in CoFeB/MgO-based magnetic tunnel junctions
Université de Lorraine, CNRS, IJL（洛林大学）；National Institute of Advanced Industrial Science and Technology（产业技术综合研究所）；Tohoku University（东北大学）；Inamori Research Institute for Science（稻盛科学研究所）
Light carrying spatiotemporal orbital angular momentum (ST-OAM) makes possible new types of optical vortices arising from transverse OAM. ST-OAM pulses exhibit novel properties during propagation, transmission, refraction, diffraction, and nonlinear conversion, attracting growing experimental and theoretical interest and studies. However, one major challenge is the lack of a simple and straightforward method for characterizing ultrafast ST-OAM pulses. Using spatially resolved spectral interferometry, we demonstrate a simple, stationary, single-frame method to quantitatively characterize ultras…
We propose a simple all-in-line single-shot scheme for diagnostics of ultrashort laser pulses, consisting of a multi-mode fiber, a nonlinear crystal and a CCD camera. The system records a 2D spatial intensity pattern, from which the pulse shape (amplitude and phase) are recovered, through a fast Deep Learning algorithm. We explore this scheme in simulations and demonstrate the recovery of ultrashort pulses, robustness to noise in measurements and to inaccuracies in the parameters of the system components. Our technique mitigates the need for commonly used iterative optimization reconstruction …
In strong-field physics experiments with intense lasers, it is of paramount importance to single-shot diagnose the temporal contrast between laser pulse peak and its noise pedestal. This allows fast optimization of pulse contrast and meaningful comparison with theory for each pulse shot, and it can help new outcomes from clean laser-plasma interactions. Thus far, high contrast ratios up to ~10^10, required by present petawatt (PW) class lasers, have been accessible in both generation and single-shot characterization. However, ultrahigh contrast ~10^13, required by the planned 200-PW lasers, ch…
Single-shot supercontinuum spectral interferometry (SSSI) is an optical technique that can measure ultrafast transients in the complex index of refraction. This method uses chirped supercontinuum reference/probe pulses that need to be pre-characterized prior to use. Conventionally, the spectral phase (or chirp) of those pulses can be determined from a series of phase or spectral measurements taken at various time delays with respect to a pump-induced modulation. Here we propose a novel method to simplify this process and characterize reference/probe pulses up to the third order dispersion from…
Direct single-shot imaging of time-resolved terahertz vector fields
École de technologie supérieure (ÉTS)（高等电力技术学院）；INRS – EMT Institut national de recherche scientifique（国家科学研究所）；National Institute for Research and Development in Microtechnologies IMT（微技术研究与开发国家研究所）；Université de Bordeaux, CNRS, Laboratoire Ondes et Matière d’Aquitaine (LOMA)（波多大学、法国国家科学研究中心、阿基坦波与物质实验室）
Cold atom electron sources are a promising alternative to traditional photocathode sources for use in ultrafast electron diffraction due to greatly reduced electron temperature at creation, and the potential for a corresponding increase in brightness. Here we demonstrate single-shot, nanosecond electron diffraction from monocrystalline gold using cold electron bunches generated in a cold atom electron source. The diffraction patterns have sufficient signal to allow registration of multiple single-shot images, generating an averaged image with significantly higher signal-to-noise ratio than obt…
Coherent diffractive imaging of individual free nanoparticles has opened novel routes for the in-situ analysis of their transient structural, optical, and electronic properties. So far, single-shot single-particle diffraction was assumed to be feasible only at extreme ultraviolet (XUV) and X-ray free-electron lasers, restricting this research field to large-scale facilities. Here we demonstrate single-shot imaging of isolated helium nanodroplets using XUV pulses from a femtosecond-laser driven high harmonic source. We obtain bright wide-angle scattering patterns, that allow us to uniquely iden…
Single-shot pulse retrieval of femtosecond bright squeezed vacuum
Technion – Israel Institute of Technology（以色列理工学院）；Solid State Institute（固态研究所）；Helen Diller Quantum Center（海伦·迪勒量子中心）；The Russell Berrie Nanotechnology Institute（罗素·贝里纳米技术研究所）；Max Planck Institute for the Science of Light（马克斯·普朗克光科学研究所）；Friedrich–Alexander Universität Erlangen–Nürnberg（埃尔朗根-纽伦堡弗里德里希-亚历山大大学）
Robust biexciton preparation for entangled photon-pair generation by single-shot Floquet driving
Zhejiang University（浙江大学）；National University of Singapore（新加坡国立大学）；Universität Bayreuth（拜罗伊特大学）；Ruhr University Bochum（波鸿鲁尔大学）；Hangzhou City University（杭州城市学院）
Single-shot 3D characterization the spatiotemporal optical vortex via a spatiotemporal wavefront sensor (STWFS)
Key Laboratory of High Power Laser and Physics, Shanghai Institute of Optics and Fine Mechanics, Chinese Academy of Sciences（中国科学院上海光学精密机械研究所高功率激光物理重点实验室）；Center of Materials Science and Optoelectronics Engineering, University of Chinese Academy of Sciences（中国科学院大学材料科学与光电技术研究中心）；School of Physics, Xi'an Jiaotong University（西安交通大学物理学院）；College of Information Science and Technology, Donghua University（东华大学信息科学与技术学院）
