Femtosecond Optical Excitation Research Articles

Pulsed THz radiation under ultrafast optical discharge of vacuum photodiode

In this paper, we first present an experimental demonstration of terahertz radiation pulse generation with energy up to 5 pJ under the electron emission during ultrafast optical discharge of a vacuum photodiode. We use a femtosecond optical excitation of metallic copper photocathode for the generation of ultrashort electron bunch and up to 45 kV/cm external electric field for the photo-emitted electron acceleration. Measurements of terahertz pulses energy as a function of emitted charge density, incidence angle of optical radiation and applied electric field have been provided. Spectral and polarization characteristics of generated terahertz pulses have also been studied. The proposed semi-analytical model and simulations in COMSOL Multiphysics prove the experimental data and allow for the optimization of experimental conditions aimed at flexible control of radiation parameters.Graphical

Large area Terahertz digitated photoconductive antennas based on a single high resistivity metal and nanoplasmonic electrode

Optical excited photoconductive antennas are a central technology for the Terahertz (THz) domain, crucial for both emitting and detecting THz radiation. This work proposes and experimentally realises a new approach in digitated photoconductive antennas (d-PCAs) based on a single digitated high resistivity metal contact with integrated resistances as voltage dividers. This permits a uniform applied electric field over a large surface area and a single step device processing procedure, simplifying the device realisation. This concept is further combined with digitated plasmonic nano-antennas that permits to enhance the light-matter interaction. Through femtosecond optical excitation of such structures, THz pulses can be generated efficiently through this device. Further, for the plasmonic d-PCA, the detected THz electric field of the device shows the effect of polarisation of the incident IR beam, highlighting the role of the nanostructured digitated contacts. This work is supported by electromagnetic simulations showing the optical and THz response of this new type of photoconductive antenna with integrated resistances.

Optical control of ultrafast structural dynamics in a fluorescent protein

The photoisomerization reaction of a fluorescent protein chromophore occurs on the ultrafast timescale. The structural dynamics that result from femtosecond optical excitation have contributions from vibrational and electronic processes and from reaction dynamics that involve the crossing through a conical intersection. The creation and progression of the ultrafast structural dynamics strongly depends on optical and molecular parameters. When using X-ray crystallography as a probe of ultrafast dynamics, the origin of the observed nuclear motions is not known. Now, high-resolution pump–probe X-ray crystallography reveals complex sub-ångström, ultrafast motions and hydrogen-bonding rearrangements in the active site of a fluorescent protein. However, we demonstrate that the measured motions are not part of the photoisomerization reaction but instead arise from impulsively driven coherent vibrational processes in the electronic ground state. A coherent-control experiment using a two-colour and two-pulse optical excitation strongly amplifies the X-ray crystallographic difference density, while it fully depletes the photoisomerization process. A coherent control mechanism was tested and confirmed the wave packets assignment.

Ultrafast Thermalization Pathways of Excited Bulk and Surface States in the Ferroelectric Rashba Semiconductor GeTe.

A large Rashba effect is essential for future applications in spintronics. Particularly attractive is understanding and controlling nonequilibrium properties of ferroelectric Rashba semiconductors. Here, time- and angle-resolved photoemission is utilized to access the ultrafast dynamics of bulk and surface transient Rashba states after femtosecond optical excitation of GeTe. A complex thermalization pathway is observed, wherein three different timescales can be clearly distinguished: intraband thermalization, interband equilibration, and electronic cooling. These dynamics exhibit an unconventional temperature dependence: while the cooling phase speeds up with increasing sample temperature, the opposite happens for interband thermalization. It is demonstrated how, due to the Rashba effect, an interdependence of these timescales on the relative strength of both electron-electron and electron-phonon interactions is responsible for the counterintuitive temperature dependence, with spin-selection constrained interband electron-electron scatterings found both to dominate dynamics away from the Fermi level, and to weaken with increasing temperature. These findings are supported by theoretical calculations within the Boltzmann approach explicitly showing the opposite behavior of all relevant electron-electron and electron-phonon scattering channels with temperature, thus confirming the microscopic mechanism of the experimental findings. The present results are important for future applications of ferroelectric Rashba semiconductors and their excitations in ultrafast spintronics.

Optically Induced Picosecond Lattice Compression in the Dielectric Component of a Strongly Coupled Ferroelectric/Dielectric Superlattice

AbstractAbove‐bandgap femtosecond optical excitation of a ferroelectric/dielectric BaTiO3/CaTiO3 superlattice leads to structural responses that are a consequence of the screening of the strong electrostatic coupling between the component layers. Time‐resolved X‐ray free‐electron laser diffraction shows that the structural response to optical excitation includes a net lattice expansion of the superlattice consistent with depolarization‐field screening driven by the photoexcited charge carriers. The depolarization‐field‐screening‐driven expansion is separate from a photoacoustic pulse launched from the bottom electrode on which the superlattice is epitaxially grown. The distribution of diffracted intensity of superlattice X‐ray reflections indicates that the depolarization‐field‐screening‐induced strain includes a photoinduced expansion in the ferroelectric BaTiO3 and a contraction in CaTiO3. The magnitude of expansion in BaTiO3 layers is larger than the contraction in CaTiO3. The difference in the magnitude of depolarization‐field‐screening‐driven strain in the BaTiO3 and CaTiO3 components can arise from the contribution of the oxygen octahedral rotation patterns at the BaTiO3/CaTiO3 interfaces to the polarization of CaTiO3. The depolarization‐field‐screening‐driven polarization reduction in the CaTiO3 layers points to a new direction for the manipulation of polarization in the component layers of a strongly coupled ferroelectric/dielectric superlattice.

Photocurrent-driven transient symmetry breaking in the Weyl semimetal TaAs.

Symmetry plays a central role in conventional and topological phases of matter, making the ability to optically drive symmetry changes a critical step in developing future technologies that rely on such control. Topological materials, like topological semimetals, are particularly sensitive to a breaking or restoring of time-reversal and crystalline symmetries, which affect both bulk and surface electronic states. While previous studies have focused on controlling symmetry via coupling to the crystal lattice, we demonstrate here an all-electronic mechanism based on photocurrent generation. Using second harmonic generation spectroscopy as a sensitive probe of symmetry changes, we observe an ultrafast breaking of time-reversal and spatial symmetries following femtosecond optical excitation in the prototypical type-I Weyl semimetal TaAs. Our results show that optically driven photocurrents can be tailored to explicitly break electronic symmetry in a generic fashion, opening up the possibility of driving phase transitions between symmetry-protected states on ultrafast timescales.

Devitrification of thin film Cu–Zr metallic glass via ultrashort pulsed laser annealing

In this work we report on an ultrashort pulsed laser annealing-driven devitrification of thin film Cu67Zr33 metallic glass characterized by micro-beam X-ray diffraction and electron microscopy techniques. The essential feature of ultrashort pulsed laser annealing is ultrafast heating (1014 K/s) by femtosecond optical excitation followed by extremely rapid cooling (1010–12 K/s) due to heat dissipation into the film substrate. During repetitive optical excitation, we take X-ray diffraction snapshots of the intermediate, frozen-in stages of the glass-crystal transformation to study its kinetics. A quantitative analysis of the diffraction patterns supported by electron microscopy result shows that the glass-crystal transformation proceeds by a rapid formation of an energetically favourable layer of crystalline ZrO2 on the free surface of the glassy film accompanied by nucleation and growth of fcc-Cu in the residual amorphous matrix. We demonstrate that at low effective annealing temperatures the devitrification kinetics of both products is correlated, while at high temperatures they decouple and ZrO2 forms an order of magnitude faster than Cu.

Toward ultrafast magnetic depth profiling using time-resolved x-ray resonant magnetic reflectivity.

During the last two decades, a variety of models have been developed to explain the ultrafast quenching of magnetization following femtosecond optical excitation. These models can be classified into two broad categories, relying either on a local or a non-local transfer of angular momentum. The acquisition of the magnetic depth profiles with femtosecond resolution, using time-resolved x-ray resonant magnetic reflectivity, can distinguish local and non-local effects. Here, we demonstrate the feasibility of this technique in a pump–probe geometry using a custom-built reflectometer at the FLASH2 free-electron laser (FEL). Although FLASH2 is limited to the production of photons with a fundamental wavelength of 4 nm (), we were able to probe close to the Fe L3 edge () of a magnetic thin film employing the third harmonic of the FEL. Our approach allows us to extract structural and magnetic asymmetry signals revealing two dynamics on different time scales which underpin a non-homogeneous loss of magnetization and a significant dilation of 2 Å of the layer thickness followed by oscillations. Future analysis of the data will pave the way to a full quantitative description of the transient magnetic depth profile combining femtosecond with nanometer resolution, which will provide further insight into the microscopic mechanisms underlying ultrafast demagnetization.

Single‐Mode Lasing from a Single 7 nm Thick Monolayer of Colloidal Quantum Wells in a Monolithic Microcavity

AbstractIn this work, monolithically‐fabricated vertical cavity surface emitting lasers (VCSELs) of densely‐packed, orientation‐controlled, atomically flat colloidal quantum wells (CQWs) using a self‐assembly method is reported and single‐mode lasing from a record thin colloidal gain medium with a film thickness of 7 nm under femtosecond optical excitation is demonstrated. Specially engineered CQWs are used to demonstrate these hybrid CQW‐VCSELs consisting of only a few layers to a single monolayer of CQWs and are achieved the lasing from these thin gain media by thoroughly modeling and implementing a vertical cavity consisting of distributed Bragg reflectors with an additional dielectric layer for mode tuning. Accurate spectral and spatial alignment of the cavity mode with the CQW films is secured with the help of full electromagnetic computations. While overcoming the long‐pending problem of limited electrical conductivity in thicker colloidal films, such ultrathin colloidal gain media can be helpful to enable fully electrically‐driven colloidal lasers.

Reduced Thermal Conductivity in Ultrafast Laser Heated Silicon Measured by Time-Resolved X-ray Diffraction

We investigate the effect of free carrier dynamics on heat transport in bulk crystalline Silicon following femtosecond optical excitation of varying fluences. By taking advantage of the dense 500 MHz standard fill pattern in the PLS-II storage ring, we perform high angular-resolution X-ray diffraction measurements on nanosecond-to-microsecond time-scales with femtometer spatial sensitivity. We find noticeably slowed lattice recovery at increasingly high excitation intensities. Modeling the temporal evolution of lattice displacements due to the migration of the near surface generated heat into the bulk requires reduced thermal diffusion coefficients. We attribute this pump-fluence dependent thermal transport behavior to two separate effects: first, the enhanced nonradiative recombination of free carriers, and, second, reduced size of the effective heat source in the material. These results demonstrate the capability of time-resolved X-ray scattering as an effective means to explore the connection between charge carrier dynamics and macroscopic transport properties.

Compact ring resonator enhanced silicon metal-semiconductor-metal photodetector in SiN-on-SOI platform.

We present a compact on-chip resonator enhanced silicon metal-semiconductor-metal (MSM) photodetector in 850 nm wavelength band for communication and lab-on-chip bio-sensing applications. We report the highest responsivity of 0.81 A/W for a 5 µm long device. High responsivity is achieved by integrating the detector in a silicon nitride ring resonator. The resonance offers 100X responsivity improvement over a single-pass photodetector due to cavity enhancement. We also present a detailed study of the high-speed response of the cavity and single-pass detector. We report an electro-optic bandwidth of 7.5 GHz measured using a femtosecond optical excitation. To the best of our knowledge, we report for the first time silicon nitride resonator integrated Si-MSM detector in SiN-SOI platform.

Synthesis of Macroscopic Single Crystals of Ge2Sb2Te5 via Single-Shot Femtosecond Optical Excitation

Using in situ electron diffraction techniques, we demonstrate that femtosecond optical excitation above a threshold fluence of the amorphous, as-deposited, phase change material Ge2Sb2Te5 creates l...

Large non-thermal contribution to picosecond strain pulse generation using the photo-induced phase transition in VO2

Picosecond strain pulses are a versatile tool for investigation of mechanical properties of meso- and nano-scale objects with high temporal and spatial resolutions. Generation of such pulses is traditionally realized via ultrafast laser excitation of a light-to-strain transducer involving thermoelastic, deformation potential, or inverse piezoelectric effects. These approaches unavoidably lead to heat dissipation and a temperature rise, which can modify delicate specimens, like biological tissues, and ultimately destroy the transducer itself limiting the amplitude of generated picosecond strain. Here we propose a non-thermal mechanism for generating picosecond strain pulses via ultrafast photo-induced first-order phase transitions (PIPTs). We perform experiments on vanadium dioxide VO2 films, which exhibit a first-order PIPT accompanied by a lattice change. We demonstrate that during femtosecond optical excitation of VO2 the PIPT alone contributes to ultrafast expansion of this material as large as 0.45%, which is not accompanied by heat dissipation, and, for excitation density of 8 mJ cm−2, exceeds the contribution from thermoelastic effect by a factor of five.

Acoustic response of a laser-excited polycrystalline Au-film studied by ultrafast Debye–Scherrer diffraction at a table-top short-pulse x-ray source

The transient acoustic response of a free-standing, polycrystalline thin Au-film upon femtosecond optical excitation has been studied by time-resolved Debye–Scherrer x-ray diffraction using ultrashort Cu Kα x-ray pulses from a laser-driven plasma x-ray source. The temporal strain evolution has been determined from the transient shifts of multiple Bragg diffraction peaks. The experimental data are in good agreement with the results of calculations based on the two-temperature model and an acoustic model assuming uniaxial strain propagation in the laser-excited thin film.

Time-resolved observation of transient precursor state of CO on Ru(0001) using carbon K-edge spectroscopy.

The transient dynamics of carbon monoxide (CO) molecules on a Ru(0001) surface following femtosecond optical laser pump excitation has been studied by monitoring changes in the unoccupied electronic structure using an ultrafast X-ray free-electron laser (FEL) probe. The particular symmetry of perpendicularly chemisorbed CO on the surface is exploited to investigate how the molecular orientation changes with time by varying the polarization of the FEL pulses. The time evolution of spectral features corresponding to the desorption precursor state was well distinguished due to the narrow line-width of the C K-edge in the X-ray absorption (XA) spectrum, illustrating that CO molecules in the precursor state rotated freely and resided on the surface for several picoseconds. Most of the CO molecules trapped in the precursor state ultimately cooled back down to the chemisorbed state, while we estimate that ∼14.5 ± 4.9% of the molecules in the precursor state desorbed into the gas phase. It was also observed that chemisorbed CO molecules diffused over the metal surface from on-top sites toward highly coordinated sites. In addition, a new "vibrationally hot precursor" state was identified in the polarization-dependent XA spectra.

Generation and detection of coherent longitudinal acoustic waves in ultrathin 1T’-MoTe2

Layered transition metal dichalcogenides have attracted substantial attention owing to their versatile functionalities and compatibility with current nanofabrication technologies. Thus, noninvasive means to determine the mechanical properties of nanometer (nm) thick specimens are of increasing importance. Here, we report on the detection of coherent longitudinal acoustic phonon modes generated by impulsive femtosecond (fs) optical excitation. Broadband fs-transient absorption experiments in 1T’-MoTe2 flakes as a function of thickness (4–30 nm) yield a longitudinal sound speed of vL = (2990 ± 90) m s−1. In addition, temperature-dependent measurements unveil a linear decrease in the normalized Young's modulus EL/EL, 295 K with a slope of δ(EL/EL, 295 K)/δT = (–2.0 ± 0.1) 10−3 K−1 and no noticeable change caused by the Td – 1T’ structural phase transition or variations in film thickness.

Effect of Optical Excitation on the Band Structure and X-Ray Absorption Spectra of BaBiO3-Based High-Temperature Superconductors: Ab Initio Calculation

The band structure, densities of states, and O K-edge X-ray absorption spectra have been calculated by the density functional theory method for BaBiO3-based perovskite high-temperature superconductors at different potassium doping levels in the ground and optically excited states. It has been shown that this approach including local structural inhomogeneities caused by doping and optical irradiation allows the correct description of changes in the properties of the electron subsystem near the Fermi level. It has been shown that doping is accompanied by the appearance of hole carriers on the Bi6s−O2pσ*. hybridized orbital in agreement with the model of the electronic structure of bismuth-based high-temperature superconductors in terms of a spatially separated Fermi-Bose mixture. It has been found that the band structure for the excited state of the undoped compound is equivalent to the band structure of the tight binding model for a cubic lattice. The results are important for the preliminary analysis of time-resolved X-ray absorption spectra on an X-ray free electron laser at femtosecond optical excitation.

Dynamics of Magnetization in Multilayer TbCo / FeCo Structures under the Influence of Femtosecond Optical Excitation

The need to study ultrafast processes in magnetism is due to the prospects for creating ultrafast magnetic recording and ultrafast spintronic devices. In order to excite the magnetic subsystem femtosecond optical pulses are used. The excitement is manifested as in spin precession. In metals, the material is heated first due to significant optical absorption, and significant Joule losses occur. The most important task is to search for materials in which spin processes are excited without heating. Obvious candidates are weakly absorbing materials, such as ferrite garnets. However, the range of such materials and the range of their functionality are limited.The purpose of this work is to study the dynamics of systems with nonthermal mechanisms of spin precession excitation. Such excitation is possible in ferromagnetic / antiferromagnetic heterostructures with exchange interaction, provided that the recombination time of photocarriers is shorter than the time of heat diffusion. Multilayer TbCo / FeCo structures of the near IR range were investigated for a femtosecond optical pulse. The spin dynamics are compared with the direction of the wave vector of the exciting pulse along and perpendicular to the axis of easy magnetization of the structures (“easy axis” and “hard axis” geometry, respectively). It is shown that in case of “easy axis” geometry the determinative mechanism is the thermal interaction. When the system is exposed to an excitation pulse, this mechanism leads to a decrease in the projection of magnetization on the direction of propagation of the test beam. In case of “hard axis” geometry, the magnetization turns to the magnetic field at the initial stage. Then it precesses and relaxes to an equilibrium angular orientation. Such dynamics indicate a rapid recovery of the uniaxial anisotropy field after laser irradiation. The presented results demonstrate an ultrafast change in the magnetic anisotropy induced during the fabrication of the heterostructure under study, which may be of interest for optical control of the orientation of the magnetization.

Random Lasing in ZnO Nanopowders Based on Multiphoton Absorption for Ultrafast Upconversion Application

This study reports ultraviolet picosecond random lasing (RL) based on multiphoton absorption in zinc oxide (ZnO) nanopowders with a mean size of ∼100 nm under femtosecond optical excitation. Upconversion random lasing is achieved with an excitation wavelength increasing from 600 to 1800 nm, corresponding to a five-photon excitation. The RL threshold has a slight positive relationship with excitation wavelength, except for a significant increase with four-photon excitation at 1200–1300 nm, demonstrating promising upconversion lasing properties of ZnO nanopowders. A remarkably lower RL threshold is observed at long excitation wavelengths ranging from 1500 to 1800 nm than that for four-photon pumping (1200–1300 nm) processes. Defect states in ZnO are suggested to be the reason that results in the excitation wavelength dependence of random lasing. Transient RL characteristics are investigated using time-resolved photoluminescence measurements, with the RL pulse delay time and pulse width observed to decrease ...

Colloidal CsPbX3 (X = Cl, Br, I) Nanocrystals 2.0: Zwitterionic Capping Ligands for Improved Durability and Stability.

Colloidal lead halide perovskite nanocrystals (NCs) have recently emerged as versatile photonic sources. Their processing and optoelectronic applications are hampered by the loss of colloidal stability and structural integrity due to the facile desorption of surface capping molecules during isolation and purification. To address this issue, herein, we propose a new ligand capping strategy utilizing common and inexpensive long-chain zwitterionic molecules such as 3-(N,N-dimethyloctadecylammonio)propanesulfonate, resulting in much improved chemical durability. In particular, this class of ligands allows for the isolation of clean NCs with high photoluminescence quantum yields (PL QYs) of above 90% after four rounds of precipitation/redispersion along with much higher overall reaction yields of uniform and colloidal dispersible NCs. Densely packed films of these NCs exhibit high PL QY values and effective charge transport. Consequently, they exhibit photoconductivity and low thresholds for amplified spontaneous emission of 2 μJ cm–2 under femtosecond optical excitation and are suited for efficient light-emitting diodes.