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 mapping photography (PUMP) technique by converting the time information into the polarization. Here, the spatiotemporal information of a dynamic scene is loaded into a rotationally polarized illumination laser pulse, and a polarization filtering in imaging detection and a deconvolution algorithm in image reconstruction are used to extract the original dynamic scene. In our PUMP system, the temporal resolution is 850 fs, the spatial resolution is 28.5 lp/mm at 700 micrometer by 700 micrometer field of view, and the number of frames is 16. By using PUMP, a spatiotemporal dynamics of femtosecond laser ablation in an indium tin oxide film on glass substrate is successfully captured. PUMP provides a new solution for measuring the transient scenes in a snapshot, which will bring a very wide range of applications in the field of ultrafast science.
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…
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,…
A flexible and accurate total variation and cascaded denoisers-based image reconstruction algorithm for hyperspectrally compressed ultrafast photography
Cameras capable of capturing videos at a trillion frames per second allow to freeze light in motion, a very counterintuitive capability when related to our everyday experience in which light appears to travel instantaneously. By combining this capability with computational imaging techniques, new imaging opportunities emerge such as three dimensional imaging of scenes that are hidden behind a corner, the study of relativistic distortion effects, imaging through diffusive media and imaging of ultrafast optical processes such as laser ablation, supercontinuum and plasma generation. We provide an…
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…
Enabling control over a spontaneous dynamic process is a very complicated task in practice because of its statistical nature, and electro-optic (E-O) relaxation dynamic in a nematic liquid crystal (NLC) system is not an exception. Controlling E-O relaxation time requires an appropriate microscopic visualization. For that, a time-resolved diffusing wave spectroscopy (TR-DWS) is developed first time, and further demonstrated with that the linear E-O relaxation time of a NLC can be improved typically, from 25msec to 350μsec at room temperature, by controlling the orientational ordering of NLC. Ap…
We explore a planar GaAs/AlAs photonic microcavity using pump-probe spectroscopy. Free carriers are excited in the GaAs with short pump pulses. The time-resolved reflectivity is spectrally resolved short probe pulses. We show experimentally that the cavity resonance and its width depend on the dynamic refractive index of both the lambda-slab and the lambda/4 GaAs mirrors. We clearly observe a double exponential relaxation of both the the cavity resonance and its width, which is due to the different recombination timescales in the lambda-slab and the mirrors. In particular, the relaxation time …
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 …
We have measured time-resolved the photon storage time and the quality factor of an ultrafast photonic cavity using an autocorrelator. The cavity consists of a $λ$-thick GaAs layer sandwiched between GaAs/AlAs distributed Bragg reflectors and resonates at 985 nm wavelength. The inverse relative linewidth measured with white light reflectivity is 830, while the quality factor obtained from the time resolved measurements is 1500. The photon storage time in the cavity is 0.78 ps. We show that the difference between the quality factor and the inverse relative linewidth results from inhomogeneous b…
We investigate the valley related carrier dynamics in monolayer MoS2 using helicity resolved non-degenerate ultrafast pump-probe spectroscopy at the vicinity of the high-symmetry K point under the temperature down to 78 K. Monolayer MoS2 shows remarkable transient reflection signals, in stark contrast to bilayer and bulk MoS2 due to the enhancement of many-body effect at reduced dimensionality. The helicity resolved ultrafast time-resolved result shows that the valley polarization is preserved for only several ps before scattering process makes it undistinguishable. We suggest that the dynamic…
Imaging with ultrashort exposure times is generally achieved with a crossed-beam geometry. In the usual arrangement, an off-axis gating pulse induces birefringence in a medium exhibiting a strong Kerr response (commonly carbon disulfide) which is followed by a polarizer aligned to fully attenuate the on-axis imaging beam. By properly timing the gate pulse, imaging light experiences a polarization change allowing time-dependent transmission through the polarizer to form an ultrashort image. The crossed-beam system is effective in generating short gate times, however, signal transmission through…
As a key component for next-generation wireless communications (6G and beyond), terahertz (THz) electronic oscillators are being actively developed. Precise and dynamic phase control of ultrafast THz waveforms is essential for high-speed beam steering and high-capacity data transmission. However, measurement of such ultrafast dynamic process is beyond the scope of electronics due to the limited bandwidth of the electrical measuring instruments. Here we surpass this limit by applying photonic technology. Using a femtosecond laser, we generate offset-free THz pulses to phase-lock the electronic …
Ultrafast Oscillations of a Ballistically Propagating Polariton Condensate Driven by Inter-mode Coherent Energy Transfer
Wuhan National High Magnetic Field Center and School of Physics, Huazhong University of Science and Technology（华中科技大学物理学院、武汉国家高磁场科学中心）；State Key Laboratory of Precision Spectroscopy, School of Physics and Electronic Science, East China Normal University（华东师范大学精密光谱科学与技术国家重点实验室、物理与电子科学学院）
Transient field-resolved spectroscopy enables studies of ultrafast dynamics in molecules, nanostructures, or solids with sub-cycle resolution, but previous work has so far concentrated on extracting the dielectric response at frequencies below 50\,THz. Here, we implemented transient field-resolved reflectometry at 50-100\,THz (3-6\,$μ$m) with MHz repetition rate employing 800\,nm few-cycle excitation pulses that provide sub-10\,fs temporal resolution. The capabilities of the technique are demonstrated in studies of ultrafast photorefractive changes in the semiconductors Ge and GaAs, where the …
The emission times of laser-triggered electrons from a sharp tungsten tip are directly characterized under ultrafast, near-infrared laser excitation at Keldysh parameters $6.6< γ< 19.1$. Emission delays up to 10 fs are observed, which are inferred from the energy gain of photoelectrons emitted into a synchronously driven microwave cavity. ~ fs timing resolution is achieved in a configuration capable of measuring timing shifts up to 55 ps. The technique can also be used to measure the microwave phase inside the cavity with a precision below 70 fs upon the energy resolved detection of a single e…
We present a novel setup to measure the transverse magneto-optical Kerr effect in the extreme ultraviolet spectral range at exceptionally high repetition rates based on a fiber laser amplifier system. This affords a very high and stable flux of extreme ultraviolet light, which we use to measure element-resolved demagnetization dynamics with unprecedented depth of information. Furthermore, the setup is equipped with a strong electromagnet and a cryostat, allowing measurements between 10 and 420 K using magnetic fields up to 0.86 T. The performance of our setup is demonstrated by a set of temper…
Metal-corroles are macrocycle organic molecules with numerous practical applications. In particular, copper corroles exhibit an interesting saddled geometry, which has attracted significant attention from theoreticians and experimentalists over the years. The present work is dedicated to understand the effect of structural saddling in a copper corrole on potential probe signals via imaging ultrafast coherent electron dynamics. A linearly polarized pulse is used to trigger the electron dynamics and time-resolved x-ray diffraction is employed to image the triggered dynamics. It is found that the…
Ultrafast internal dynamics of chiral domain walls probed by time-resolved XRMS
Universität Siegen（锡根大学）；Elettra Sincrotrone Trieste（的里雅斯特 Elettra 同步辐射中心）；Ca' Foscari University of Venice（威尼斯卡福斯卡里大学）；Synchrotron SOLEIL（索莱尔同步辐射中心）；Johannes Gutenberg-Universität Mainz（美因茨约翰内斯·古腾堡大学）；Laboratoire Albert Fert, CNRS, Thales, Université Paris-Saclay（阿尔贝·费尔特实验室，法国国家科学研究中心，泰雷兹集团，巴黎萨克雷大学）
Watching the motion of electrons on their natural nanometre length- and femtosecond time scales is a fundamental goal and an open challenge of contemporary ultrafast science. Optical techniques and electron microscopy currently mostly provide either ultrahigh temporal or spatial resolution, yet, microscopy techniques with combined space-time resolution need further development. Here we create an ultrafast electron source by plasmon nanofocusing on a sharp gold taper and implement this source in an ultrafast point-projection electron microscope. This source is used, in an optical pump - electro…
We present a table-top extreme ultraviolet (XUV) beamline for measuring time- and frequency-resolved XUV excited optical luminescence (XEOL) with additional femtosecond-resolution XUV transient absorption spectroscopy functionality. XUV pulses are generated via high-harmonic generation using a near-infrared pulse in a noble gas medium, and focused to excite luminescence from a solid sample. The luminescence is collimated and guided into a streak camera, where its spectral components are temporally resolved with picosecond temporal resolution. We time-resolve XUV excited luminescence and compar…
Ultrafast science and technology have brought in burgeoning opportunities to optical metrology, strong-field physics, non-equilibrium physics, etc., through light-matter interaction due to ever-advancing temporal resolution and peak power of ultrafast laser. The superior temporal and spectral resolution, has brought forth pump-probe spectroscopy for ultrafast dynamic study of transient states in various intriguing materials, such as quantum materials, metamaterials, and plasmonic materials, by directly reporting spectroscopic complex response function, using either time- or frequency-domain- b…
Ultrafast scattering using X-rays or electrons is an emerging method to obtain structure dynamics at the atomic length and time scales. However, directly resolving in real-space atomic motions is inherently limited by the finite detector range and the probe energy. As a result, the time-resolved signal interpretation is mostly done in reciprocal space and relies on modeling and simulations of specific structures and processes. Here, we introduce a model-free approach to directly resolve scattering signals in real space, surpassing the diffraction limit, using scattering kernels and signal prio…
Copper (Cu), gold (Au) (111) crystals were illuminated with 120 fs pulses and probed by 600 fs X-ray pulses. Rocking curves were measured versus 267 nm (UV) pump- 0.154 nm probe delay time. Curve width broadening, peak diffracted intensity and angular shift were recorded for the range of UV excitation intensities of 2-8 mJ/cm2 . Observed oscillations in time delay dependences of shift, width and of peak intensity of rocking curves are correlated, as described by acoustic pulse bouncing between crystal surfaces. In (111) Au, acoustic pulse originates from pump absorption layer, and peak intensi…
The ultrafast optical Kerr effect (OKE) is widely used to investigate the structural dynamics and interactions of liquids, solutions and solids by observing their intrinsic nonlinear temporal responses through nearly-collinear four-wave mixing (FWM). Non-degenerate mixing schemes allow for background free detection and can provide information on the interplay between a material's internal degrees of freedom. Here we show a source of temporal dynamics in the OKE signal that is not reflective of the intrinsic nonlinear response but arises from group index and momentum mismatch. It is observed in…
We establish time-resolved high harmonic generation (tr-HHG) as a powerful spectroscopy for photoinduced dynamics in strongly correlated materials through a detailed investigation of the insulator-to-metal transitions in vanadium dioxide. We benchmark our technique by comparing our measurements to established momentum-resolved ultrafast electron diffraction, and theoretical density functional calculations. Tr-HHG allows distinguishing of individual dynamic channels, including a transition to a thermodynamically hidden phase. In addition, the HHG yield is shown to be modulated at a frequency ch…
Ultrafast electronic dynamics in solids lies at the core of modern condensed matter and materials physics. To build up a practical ab initio method for studying solids under photoexcitation, we develop a momentum-resolved real-time time dependent density functional theory (rt-TDDFT)algorithm using numerical atomic basis, together with the implementation of both the length and vector gauge of the electromagnetic field. When applied to simulate elementary excitations in two-dimensional materials such as graphene, different excitation modes, only distinguishable in momentum space, are observed. T…
An ultrafast all-optical shutter is presented, based on a simple two-color two-photon absorption technique. For time-resolved luminescence measurements this shutter is an interesting alternative to the optical Kerr gate. The rejection efficiency is 99%, the switching-off and switching-on speeds are limited by the pulse length only, the rejection time is determined by the crystal slab thickness, and the bandwidth spans the entire visible spectrum. We show that our shutter can also be used for accurate measurement of group velocity inside a transparent material.
Phase-locked ultrashort pulses in the rich terahertz (THz) spectral range have provided key insights into phenomena as diverse as quantum confinement, first-order phase transitions, high-temperature superconductivity, and carrier transport in nanomaterials. Ultrabroadband electro-optic sampling of few-cycle field transients can even reveal novel dynamics that occur faster than a single oscillation cycle of light. However, conventional THz spectroscopy is intrinsically restricted to ensemble measurements by the diffraction limit. As a result, it measures dielectric functions averaged over the s…
Excitation and propagation dynamics of spin waves in an iron-based garnet film under out-of-plane magnetic field were investigated by time-resolved magneto-optical imaging. The experimental results and the following data analysis by phase-resolved spin-wave tomography reveal the excitation of spin waves triggered by photo-induced demagnetization (PID) along the sample depth direction. Moreover, the fast relaxation of PID accompanied by the spin transfer due to spin-wave emission was observed. Possible scenarios of PID in the garnet film are discussed. Finally, we develop a model for the spin-w…
The ultrafast detection of single photons is currently restricted by the limited time resolution (a few picoseconds) of the available single-photon detectors. Optical gates offer a faster time resolution, but so far they have been mostly applied to ensembles of emitters. Here, we demonstrate through a semi-analytical model that the ultrafast time-resolved detection of single quantum emitters can be possible using an optical-Kerr-shutter (OKS) at GHz rates under focused illumination. This technique provides sub-picosecond time resolution, while keeping a gate efficiency at around 85 \%. These f…
We predict a strong-field ultrafast optical Faraday effect, where a circularly polarized ultrashort optical pulse induces transient chirality in an achiral transparent dielectric. This effect is attractive for time-resolved measurements because it gives access to the non-instantaneity of the nonlinear medium response, and also because it represents relaxation of time-reversal symmetry by all-optical means. We propose probing the induced transient chirality with a weak linearly polarized ultraviolet pulse that is shorter than the near-infrared pump pulse. The predicted effects are ultrafast: th…
Time- and Angle-resolved photoelectron spectroscopy from surfaces can be used to record the dynamics of electrons and holes in condensed matter on ultrafast time scales. However, ultrafast photoemission experiments using extreme-ultraviolet (XUV) light have previously been limited by either space-charge effects, low photon flux, or limited tuning range. In this article, we describe space-charge-free XUV photoelectron spectroscopy experiments with up to 5 nA of average sample current using a tunable cavity-enhanced high-harmonic source operating at 88 MHz repetition rate. The source delivers $ …
