We describe an ultrafast time resolved pump-probe spectroscopy setup aimed at studying the switching of nanophotonic structures. Both fs pump and probe pulses can be independently tuned over broad frequency range between 3850 and 21050 cm$^{-1}$. A broad pump scan range allows a large optical penetration depth, while a broad probe scan range is crucial to study strongly photonic crystals. A new data acquisition method allows for sensitive pump-probe measurements, and corrects for fluctuations in probe intensity and pump stray light. We observe a tenfold improvement of the precision of the setup compared to laser fluctuations, allowing a measurement accuracy of better than $Δ$R= 0.07% in a 1 s measurement time. Demonstrations of the improved technique are presented for a bulk Si wafer, a 3D Si inverse opal photonic bandgap crystal, and z-scan measurements of the two-photon absorption coefficient of Si, GaAs, and the three-photon absorption coefficient of GaP in the infrared wavelength range.
The theory of energy transfer dynamics of a pair of donor and acceptor molecules located in the plasmonic hot spots is developed by means of the master equation approach and the electromagnetic Green's tensor technique. A nonlocal effect has been considered by using a hydrodynamic model. The coherent interaction between the two molecules in plasmonic nanostructures is investigated under some strong coupling conditions. It is shown that the energy transfer efficiency of a pair of molecules can be improved largely and the transfer time decreases to dozens of femtoseconds when the contribution of…
The inclusion of atomic inversion in Raman scattering can significantly alter field dynamics in plasmonic settings. Our calculations show that large local fields and femtosecond pulses combine to yield: (i) population inversion within hot spots; (ii) gain saturation; and (iii) conversion efficiencies characterized by a switch-like transition to the stimulated regime that spans twelve orders of magnitude. While in Raman scattering atomic inversion is usually neglected, we demonstrate that in some circumstances full accounting of the dynamics of the Bloch vector is required.
We performed non-degenerate pump-probe experiments on a GaAs/AlAs photonic structure. We switched the photonic properties using the optical Kerr effect and free carriers excited by three photon absorption. From these measurements we extracted the non-degenerate Kerr coefficients over a broad wavelength range and we extracted the three photon absorption coefficient for GaAs at three wavelengths in the near infrared. We show that the optical Kerr effect is large enough to switch a cavity resonance with a high \emph{Q} ($Q>1000$) photonic cavity.
The functionalities of a wide range of optical and opto-electronic devices are based on resonance effects and active tuning of the amplitude and wavelength response is often essential. Plasmonic nanostructures are an efficient way to create optical resonances, a prominent example is the extraordinary optical transmission (EOT) through arrays of nanoholes patterned in a metallic film. Tuning of resonances by heating, applying electrical or optical signals has proven to be more elusive, due to the lack of materials that can induce modulation over a broad spectral range and/or at high speeds. Her…
Optical quadratic nonlinearity is ultrafast in nature, while parametric interaction usually manifests only the broadband characteristic. Enormous progress has been made toward broadband phase-matching for parametric amplification and wide applications. In existing devices of broadband parametric amplification, the power efficiency of conversion is restricted to approximately the energy efficiency, and the desire for the signal power enhancement necessitates additional pulse compression after amplification. Here, we demonstrate ultrafast parametric amplification having an extraordinary power ef…
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.
We describe a two-color pump-probe scanning magneto-optical Kerr effect (MOKE) microscope which we have developed to investigate electron spin phenomena in semiconductors at cryogenic temperatures with picosecond time and micrometer spatial resolution. The key innovation of our microscope is the usage of an ultrafast `white light' supercontinuum fiber-laser source which provides access to the whole visible and near-infrared spectral range. Our Kerr microscope allows for the independent selection of the excitation and detection energy while avoiding the necessity to synchronize the pulse trains…
We present the controllability capabilities for the limit cycles of an extremely tunable photonic oscillator, consisting of two coupled semiconductor lasers. We show that this system supports stable limit cycles with frequencies ranging from a few to more than a hundred GHz that are characterized by a widely varying degree of asymmetry between the oscillations of the two lasers. These dynamical features are directly controllable via differential pumping as well as optical frequency detuning of the two lasers, suggesting a multi-functional oscillator for chip-scale radio-frequency photonics app…
We demonstrate, by theory and experiment, the ultrafast tilting of the dispersion curve of a photonic-crystal waveguide following the absorption of a femtosecond pump pulse. By shaping the pump-beam cross section with a nanometric shadow mask, different waveguide eigenmodes acquire different spatial overlap with the perturbing pump, leading to a local flattening of the dispersion by up to 11 %. We find that such partial mode perturbation can be used to adiabatically compress the spectrum of a light pulse traveling through the waveguide.
Optically generated electron-hole plasma in high-index dielectric nanostructures was demonstrated as a means of tuning of their optical properties. However, until now an ultrafast operation regime of such plasma driven nanostructures has not been attained. Here, we perform pump-probe experiments with resonant silicon nanoparticles and report on dense optical plasma generation near the magnetic dipole resonance with ultrafast (about 2.5 ps) relaxation rate. Basing on experimental results, we develop an analytical model describing transient response of a nanocrystalline silicon nanoparticle to a…
This paper demonstrates an arbitrary tunable spaser based on double-Fano resonance of a plasmonic nanostructure consisting of two sets of disk-ring (TSDR) nanostructure. TSDR nanostructure supports two Fano resonances, which can be served as the lasing mode and the pumping mode of a spaser. These two mode can be tuned in a very wide wavelength range because of the good tunability of the two nanorings. The tuning range of the lasing mode and the pumping mode can be reached to 710 nm and 620 nm. These results represent a significant step in the pursuit of ultimate spasers and propose a approach …
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…
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…
An experimental pump-probe study of the photoassociative creation of translationally ultracold rubidium molecules is presented together with numerical simulations of the process. The formation of loosely bound excited-state dimers is observed as a first step towards a fully coherent pump-dump approach to the stabilization of Rb$_2$ into its lowest ground vibrational states. The population that contributes to the pump-probe process is characterized and found to be distinct from a background population of pre-associated molecules.
Optical pump-probe spectroscopy is a powerful tool to directly probe the carrier dynamics in materials down to sub-femtosecond resolution. To perform such measurement, while keeping the pump induced perturbation to the sample as small as possible, it is essential to have a detection scheme with high signal to noise ratio. Achieving such high signal to noise ratio is easy with phase sensitive detection based on lock-in-amplifier when a high repetition rate laser is used as the optical pulse source. However such a lock-in-amplifier based method does not work well when a low repetition rate laser…
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…
Controlling Ultrafast Excitations in Germanium:The Role of Pump-Pulse Parameters and Multi-Photon Resonances
Università degli Studi di Salerno（萨莱诺大学）；CNR-SPIN, Unità di Salerno（意大利国家研究委员会自旋物理研究所萨莱诺分部）；CNISM, Unità di Salerno, Università degli Studi di Salerno（意大利凝聚态物质创新科学中心萨莱诺分部，萨莱诺大学）
We study ultrafast magnetization quenching of ferromagnetic iron following excitation by an optical vs a terahertz pump pulse. While the optical pump (photon energy of 3.1 eV) induces a strongly nonthermal electron distribution, terahertz excitation (~4 meV) results in a quasi-thermal perturbation of the electron population. The pump-induced spin and electron dynamics are interrogated by the magneto-optic Kerr effect (MOKE). A deconvolution procedure allows us to push the time resolution down to 130 fs, even though the driving terahertz pulse is more than 0.5 ps long. Remarkably, the MOKE sign…
We present a systematic study of ultrafast all-optical switching of Si photonic band gap woodpile crystals using broadband tunable nondegenerate pump-probe spectroscopy. At pump-probe coincidence, we investigate the behavior the differential reflectivity at the blue edge of the stopband for a wide range of pump- and probe frequencies. Both dispersive and absorptive features are observed from the probe spectra at coincidence. As the pump frequency is tuned through half the electronic bandgap of Si, the magnitude of both these features increases. For the first time we unambiguously identify this…
Femtosecond pump-probe spectroscopy is applied to identify transient optical signatures of phase transitions in optimally doped YBa2Cu3O7-δ films. To elucidate the dynamics of superconducting and pseudogap phases, the slow thermal component is removed from the time-domain traces of photo-induced reflectivity in a high-flux regime with low frequency pulse rate. The rescaled data exhibit distinct signatures of the phase separation with abrupt changes at the onsets of TSC and TPG in excellent agreement with transport data. Compared to the superconducting phase, the response of the pseudogap phase…
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…
Realizing remarkable tunability in optical properties without sacrificing speed is critical to obtain all optical ultrafast devices. In this work, we investigate the ultrafast temporal behavior of optically tunable epsilon-near-zero (ENZ) metamaterials, operating in the visible spectral range. To perform this the ultrafast dynamics of the hot electrons is acquired by femtosecond pump-probe spectroscopy and studied based on two-temperature model (2TM). We show that pumping with femtosecond pulses changes the effective permittivity of the metamaterial more than 400 %. This significant modulation…
Ultrafast nanophotonics is an emerging research field aimed at the development of nanodevices capable of light modulation with unprecedented speed. A promising approach exploits the optical nonlinearity of nanostructured materials (either metallic or dielectric) to modulate their effective permittivity via interaction with intense ultrashort laser pulses. While the ultrafast temporal dynamics of such nanostructures following photoexcitation has been studied in depth, sub-ps transient spatial inhomogeneities taking place at the nanoscale have been so far almost ignored. Here we theoretically pr…
Ultrafast pump-probe spectroscopy is a powerful tool to study the nonequilibrium dynamics in high-Tc cuprate superconductors. The photo-induced quasiparticle (QP) dynamics revealed by pump-probe spectroscopy are sensitive to the near-Fermi level electronic structures. Here we review several selected examples to illustrate the enduring challenges including pairing glue, phase separation, and phase transitions in cuprate superconductors. We also present the data obtained on thin films of YBa2Cu3O7-δ in connection to these issues.
Ultrafast imaging is essential in physics and chemistry to investigate the femtosecond dynamics of nonuniform samples or of phenomena with strong spatial variations. It relies on observing the phenomena induced by an ultrashort laser pump pulse using an ultrashort probe pulse at a later time. Recent years have seen the emergence of very successful ultrafast imaging techniques of single non-reproducible events with extremely high frame rate, based on wavelength or spatial frequency encoding. However, further progress in ultrafast imaging towards high spatial resolution is hampered by the lack o…
The Free-Electron Laser (FEL) FLASH offers the worldwide still unique capability to study ultrafast processes with high-flux, high-repetition rate XUV and soft X-ray pulses. The vast majority of experiments at FLASH are of pump-probe type. Many of them rely on optical ultrafast lasers. Here, a novel FEL facility laser is reported which combines high average power output from Yb:YAG amplifiers with spectral broadening in a Herriott-type multi-pass cell and subsequent pulse compression to sub-100 fs durations. Compared to other facility lasers employing optical parametric amplification, the new …
Optical metasurfaces have come into the spotlight as a promising platform for light manipulation at the nanoscale, including ultrafast all-optical control via excitation with femtosecond laser pulses. Recently, dichroic metasurfaces have been exploited to modulate the polarization state of light with unprecedented speed. Here, we theoretically predict and experimentally demonstrate by pump-probe spectroscopy the capability to reconfigure the ultrafast dichroic signal of a gold metasurface by simply acting on the polarization of the pump pulse, which is shown to reshape the spatio-temporal dist…
Triple sum-frequency (TSF) spectroscopy measures multidimensional spectra by resonantly exciting multiple quantum coherences of vibrational and electronic states. In this work we demonstrate pump-TSF-probe spectroscopy in which a pump excites a sample and some time later three additional electric fields generate a probe field which is measured. We demonstrate pump-TSF-probe spectroscopy on polycrystalline, smooth, thin films and spiral nanostructures of both MoS2 and WS2. The pump-TSF-probe spectra are qualitatively similar to the more conventional transient-reflectance spectra. While transien…
A novel polarization-modulation transient method has been developed for studying fast anisotropic relaxation in electronic excited states of polyatomic and biologically relevant molecules under excitation with femtosecond laser pulses. The method is based on the modulation of pump beam polarization with a photo-elastic modulator and detection of an anisotropic contribution to the transient signal by a highly-sensitive demodulation balanced scheme. The method was tested on aqueous solution of coenzyme NADH (nicotin-amideadenine-dinucleotide) pumped at 360 nm and probed at 720 nm. Anisotropic vi…
We demonstrate a two-crystal mid-infrared dual-wavelength optical parametric oscillator, synchronously pumped by a high power femtosecond Yb:fiber laser. The singly-resonant ring cavity, containing two periodically poled lithium niobate crystals, is capable of generating two synchronized idler wavelengths, independently tunable over 30 THz in the 2.9 - 4.2 μm wavelength region, due to the cascaded quadratic nonlinear effect. The independent tunability of the two idlers makes the optical parametric oscillator a promising source for ultrafast pulse generation towards the THz wavelength region, b…
We demonstrate that ultrafast nonlinear dynamics gives rise to reciprocity breaking in a random photonic medium. Reciprocity breaking is observed via the suppression of coherent backscattering, a manifestation of weak localization of light. The effect is observed in a pump-probe configuration where the pump induces an ultrafast step-change of the refractive index during the dwell time of the probe light in the material. The dynamical suppression of coherent backscattering is reproduced well by a multiple scattering Monte Carlo simulation. Ultrafast reciprocity breaking provides a distinct mech…
Cascaded nonlinearities have attracted much interest, but ultrafast applications have been seriously hampered by the simultaneous requirements of being near phase-matching and having ultrafast femtosecond response times. Here we show that in strongly phase-mismatched nonlinear frequency conversion crystals the pump pulse can experience a large and extremely broadband self-defocusing cascaded Kerr-like nonlinearity. The large cascaded nonlinearity is ensured through interaction with the largest quadratic tensor element in the crystal, and the strong phase-mismatch ensures an ultrafast nonlinear…
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…
Increasing any degree of freedom of light beam may open a wide application area of this special light beam. Vortex beam with a dimension of orbital angular momentum (OAM) as a useful light source has been widely applied in many fields. Here, unique multicolor concentric ultrafast vortex beams (MUCU-VBs), which are also named ultrafast photonic rainbow, with controllable orbital angular momentum are firstly generated using cascaded four-wave mixing (CFWM) in an yttrium aluminum garnet (YAG) plate. Up to 9 multicolor concentric annular ultrafast vortex sidebands are generated simultaneously. The…
We report an ultrafast optical tuning of the reflectivity of AlGaAs/InAlGaAs multiple quantum well photonic crystal waveguides using a reflection geometry, pump-probe technique.
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 report on the demonstration of a femtosecond all-optical modulator providing, without nonlinearity and therefore at arbitrarily low intensity, ultrafast light-by-light control. The device engages the coherent interaction of optical waves on a metamaterial nanostructure only 30 nm thick to efficiently control absorption of near-infrared (750-1040 nm) femtosecond pulses, providing switching contrast ratios approaching 3:1 with a modulation bandwidth in excess of 2 THz. The functional paradigm illustrated here opens the path to a family of novel meta-devices for ultra-fast optical data process…
Future technologies underpinning high-performance optical communications, ultrafast computations and compact biosensing will rely on densely packed reconfigurable optical circuitry based on nanophotonics. For many years, plasmonics was considered as the only available platform for nanoscale optics, but the recently emerged novel field of Mie resonant metaphotonics provides more practical alternatives for nanoscale optics by employing resonances in high-index dielectric nanoparticles and structures. In this mini-review we highlight some recent trends in the physics of dielectric Mie-resonant na…
"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 ad…
We present the results of an experimental and numerical investigation into temporally non-local coherent interactions between ultrashort pulses, mediated by Raman coherence, in gas-filled kagomé-style hollow-core photonic crystal fiber. A pump pulse first set up the Raman coherence, creating a refractive index grating in the gas that travels at the group velocity of the pump pulse. Varying the arrival time of a second probe pulse allows high degree of control over its evolution as it propagates along the fiber, in particular soliton self-compression and dispersive wave (DW) emission. In the ex…
In experiment and theory, we resolve the mechanism of ultrafast optical magnon excitation in antiferromagnetic NiO. We employ time-resolved optical two-color pump-probe measurements to study the coherent non-thermal spin dynamics. Optical pumping and probing with linearly and circularly polarized light along the optic axis of the NiO crystal scrutinizes the mechanism behind the ultrafast optical magnon excitation. A phenomenological symmetry-based theory links these experimental results to expressions for the optically induced magnetization via the inverse Faraday effect and the inverse Cotton…
We demonstrate that the dispersion of surface plasmon polaritons in a periodically perforated gold film can be efficiently manipulated by femtosecond laser pulses with the wavelengths far from the intrinsic resonances of gold. Using a time- and frequency- resolved pump-probe technique we observe shifting of the plasmon polariton resonances with response times from 200 to 800 fs depending on the probe photon energy, through which we obtain comprehensive insight into the electron dynamics in gold. We show that Wood anomalies in the optical spectra provide pronounced resonances in differential tr…
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…
Here we describe an optical method to determine the dynamics of optically excited carriers in nanostructured composite samples. By combining pump-probe time-resolved reflectivity with scattering measurements, we extract the characteristic times for charge carrier evolution. We use the 3D Maxwell-Garnett formulae, modified to include the Drude optical response, to model the results. The method, applied to hydrogenated amorphous silicon containing crystalline silicon nanoparticles, showed that the recombination times in the nanocrystals and in the matrix were ~4.9 ps and ~22 ps, respectively. Th…
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 present a pump-probe technique for monitoring ultrafast polarizability changes. In particular, we use it to measure the plasma density created at the temporal focus of a self-compressing higher-order pump soliton in gas-filled hollow-core photonic crystal fiber. This is done by monitoring the wavelength of the dispersive wave emission from a counter-propagating probe soliton. By varying the relative delay between pump and probe, the plasma density distribution along the fiber can be mapped out. Compared to the recently introduced interferometric side-probing for monitoring the plasma densit…
Ultrafast spectroscopy is an important tool for studying photoinduced dynamical processes in atoms, molecules, and nanostructures. Typically, the time to perform these experiments ranges from several minutes to hours depending on the choice of spectroscopic method. It is desirable to reduce this time overhead to not only to shorten time and laboratory resources, but also to make it possible to examine fragile specimens which quickly degrade during long experiments. In this article, we motivate using compressive sensing to significantly shorten data acquisition time by reducing the total number…
Ultrafast pump-probe measurements of plasmonic nanostructures probe the non-equilibrium behavior of excited carriers, which involves several competing effects obscured in typical empirical analyses. Here we present pump-probe measurements of plasmonic nanoparticles along with a complete theoretical description based on first-principles calculations of carrier dynamics and optical response, free of any fitting parameters. We account for detailed electronic-structure effects in the density of states, excited carrier distributions, electron-phonon coupling, and dielectric functions which allow us…
