Simultaneous measurements of transient transmission and reflectivity were performed in the unintentionally doped InN film to reveal ultrafast optical bleaching and its recovery behavior under intense laser irradiation. The optical bleaching is attributed to Pauli blocking due to the occupation of photoexcited electrons at the probing energy level. The time constant for the transition from the excitation state to the conduction band edge is $\sim$260 fs. The interplay between band filling and band gap renormalization caused by electron-hole and electron-electron interactions gives rise to complex spectral characteristics of transient reflectivity, from which the time constants of photoexcited electron-hole direct recombination and band edge recombination are extracted as $\sim$60 fs and 250$\sim$400 fs, respectively. Our results also reveal that the electron-electron interaction suppresses band edge recombination, and mitigates the recovery process. Our experiments highlight the controllability of the band structure of semiconductors by intense laser irradiation.
We investigate the ultrafast electron dynamics triggered by terahertz and optical pulses in thin platinum and gold films by probing their transient optical reflectivity. The response of the platinum film to an intense terahertz pulse is similar to the optically-induced dynamics of both films and can be described by a two-temperature model. Surprisingly, gold can exhibit a much smaller terahertz pulse-induced reflectivity change and with opposite sign. For platinum, we estimate a 20% larger electron-phonon coupling for the terahertz-driven dynamics compared to the optically-induced one, which w…
Epsilon-near-zero (ENZ) materials have shown significant potential for nonlinear optical applications due to their ultrafast hot carriers and consequent optical nonlinearity enhancement. Modified poly(3,4-ethylenedioxythiophene) (PEDOT) films show metallic characteristics and a resultant ENZ wavelength near 1550nm through polar solvent treatment and annealing. The metallic PEDOT film exhibits an intrinsic optical nonlinear response that is comparable to gold and 100-fold higher than typical inorganic semiconductor ENZ materials due to π-conjugated delocalized electrons. Hot carriers generate a…
Irradiation with an ultrashort laser pulse can completely destroy the magnetic order of ferromagnetic thin films on the femtosecond timescale. This phenomenon holds great potential for ultrafast spintronics and information processing and is an active field of research. It is still an open question if the angular momentum of light can support this effect. While it has been shown that the spin of light only has a negligible influence, we experimentally demonstrate the influence of ultrashort laser pulses with orbital angular momentum (OAM) on the magnetization dynamics of a thin nickel film. Our…
We theoretically investigate ultrafast and nonlinear optical properties of graphite thin films based on first-principles time-dependent density functional theory. We first calculate electron dynamics in a unit cell of graphite under a strong pulsed electric field and explore the transient optical properties of graphite. It is shown that the optical response of graphite shows a sudden change from conducting to insulating phase at a certain intensity range of the applied electric field. It also appears as a saturable absorption, the saturation in the energy transfer from the electric field to el…
Transient Pauli blocking in a InN film as a mechanism for broadband ultrafast optical switching
Global Center for Science and Engineering (GCSE), Faculty of Science and Engineering, Waseda University（早稻田大学理工学部）；Graduate School of Advanced Science and Engineering, Waseda University（早稻田大学先进理工学研究科）；Graduate School of Science and Engineering, Aoyama Gakuin University（青山学院大学理工学府）；Institute for Molecular Science（分子科学研究所）；The Graduate University for Advanced Studies (SOKENDAI)（综合研究大学院大学）；National Metrology Institute of Japan (NMIJ), National Institute of Advanced Industrial Science and Technology (AIST)（产业技术综合研究所国家计量标准研究所）
As a high-order quantum transition, two-photon emission has an extremely low occurrence rate compared to one-photon emission, thus having been considered a forbidden process. Here, we propose a scheme that allows ultrafast two-photon emission, leveraging highly confined surface plasmon polariton modes in a degenerately-doped, light-emitting semiconductor thin film. The surface plasmon polariton modes are tailored to have simultaneous spectral and spatial overlap with the two-photon emission in the semiconductor. Using degenerately-doped InSb as the prototype material, we show that the two-phot…
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…
Herein we describe a novel spinning pump-probe photoacoustic technique developed to study nonlinear absorption in thin films. As a test case, an organic polycrystalline thin film of quinacridone, a well-known pigment, with a thickness in the tens of nanometers range, is excited by a femtosecond laser pulse which generates a time-domain Brillouin scattering signal. This signal is directly related to the strain wave launched from the film into the substrate and can be used to quantitatively extract the nonlinear optical absorption properties of the film itself. Quinacridone exhibits both quadrat…
The ultrafast response of metals to light is governed by intriguing non-equilibrium dynamics involving the interplay of excited electrons and phonons. The coupling between them gives rise to nonlinear diffusion behavior on ultrashort timescales. Here, we use scanning ultrafast thermo-modulation microscopy to image the spatio-temporal hot-electron diffusion in a thin gold film. By tracking local transient reflectivity with 20 nm and 0.25 ps resolution, we reveal two distinct diffusion regimes, consisting of an initial rapid diffusion during the first few picoseconds after optical excitation, fo…
Next-generation communication networks require > Tbit/s single-channel data transfer and processing with sub-picosecond switches and routers at network nodes. Materials enabling ultrafast all-optical switching have high potential to solve the speed limitations of current optoelectronic circuits. Chromoproteins have been shown to exhibit a fast light-controlled refractive index change much larger than that induced by the optical Kerr effect due to a purely electronic nonlinearity, alleviating the driving energy requirements for optical switching. Here, we report femtosecond transient grating ex…
For terahertz (THz) wave applications, tunable and rapid modulation is highly required. When studied by means of optical pump-terahertz probe spectroscopy, single-walled carbon nanotubes (SWCNTs) thin films demonstrated ultrafast carrier recombination lifetimes with a high relative change in the signal under optical excitation, making them promising candidates for high-speed modulators. Here, combination of SWCNTthin films and stretchable substrates facilitated studies of the SWCNT mechanical properties under strain,and enabled the development of a new type of an opto-mechanical modulator. By …
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 quest to improve density, speed and energy efficiency of magnetic memory storage has led to exploration of new ways of optically manipulating magnetism at the ultrafast time scale, in particular in ferrimagnetic alloys. While all-optical magnetization switching is well-established on the femtosecond timescale, lateral nanoscale confinement and thus potential significant reduction of the size of the magnetic element remains an outstanding challenge. Here we employ resonant electromagnetic energy-funneling plasmon nanoantennas to influence the demagnetization dynamics of a ferrimagnetic TbCo…
Probing the formation of femtosecond laser-induced periodic surface structures on silica films by ultrafast small-angle X-ray scattering
University of Duisburg-Essen（杜伊斯堡-埃森大学）；Bentley Systems, Incorporated（宾利系统公司）；European XFEL（欧洲自由电子激光实验室）；Bundesanstalt für Materialforschung und -prüfung (BAM)（联邦材料研究与测试研究所）；Warsaw University of Technology（华沙理工大学）；Institute of Physics, Polish Academy of Sciences（波兰科学院物理研究所）；SLAC National Accelerator Laboratory（斯坦福直线加速器中心）
An epsilon-near-zero-based nonlinear platform for ultrafast re-writable holography
University of Ottawa（渥太华大学）；Tampere University（坦佩雷大学）；University of Rochester（罗切斯特大学）；Yale University（耶鲁大学）；Technische Universität Darmstadt（达姆施塔特工业大学）
Using long-range surface plasmon polaritons light can propagate in metal nano-scale waveguides for ultracompact opto-electronic devices. Gold is an important material for plasmonic waveguides, but although its linear optical properties are fairly well understood, the nonlinear response is still under investigation. We consider propagation of pulses in ultrathin gold strip waveguides, modeled by the nonlinear Schrödinger equation. The nonlinear response of gold is accounted for by the two-temperature model, revealing it as a delayed nonlinearity intrinsic in gold. The consequence is that the me…
Ultrafast and long-term stability Integrated Pockels laser with thin-film PZT
State Key Laboratory for Extreme Photonics and Instrumentation, Zhejiang Key Laboratory of Optoelectronic Information Technology, College of Optical Science and Engineering, International Research Center for Advanced Photonics, Zhejiang University（浙江大学极端光子学与仪器教育部重点实验室、光电信息技术浙江省重点实验室、光学与光学工程学院、先进光子学国际研究中心）；China Jiliang University（中国计量大学）；Hangzhou Institute for Advanced Study, University of Chinese Academy of Sciences（中国科学院大学杭州高等研究院）
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…
