Search Results (10)

Diamond is a promising material for terahertz applications. In this work, we use a non-invasive optical pump–terahertz probe method to experimentally study the photoinduced carrier dynamics in doped diamond monocrystals and a new diamond-silicon composite. The chemical vapor deposited diamond substrate with embedded silicon microparticles showed two photoinduced carrier lifetimes (short lifetime on the order of 4 ps and long lifetime on the order of 200 ps). The short lifetime is several times less than in boron-doped diamonds and nitrogen-doped diamonds which were grown using a high temperature–high pressure technique. The observed phenomenon is explained by the transport of photoexcited carriers across the silicon–diamond interface, resulting in dual relaxation dynamics. The observed phenomenon could be used for ultrafast flexible terahertz modulation. Full article

Optical absorption spectra of 9 MeV electron-irradiated GaSe crystals were studied. Two absorption bands with the low-photon-energy threshold at 1.35 and 1.73 eV (T = 300 K) appeared in the transparency region of GaSe after the high-energy-electron irradiation. The observed absorption bands were attributed to the defect states induced by Ga vacancies in two charge states, having the energy positions at 0.23 and 0.61 eV above the valence band maximum at T = 300 K. The optical pump-terahertz probe technique (OPTP) was employed to study the dark and photoexcited terahertz conductivity and charge carrier recombination dynamics at two-photon excitation of as-grown and 9 MeV electron-irradiated GaSe crystals. The measured values of the differential terahertz transmission at a specified photoexcitation condition were used to extract the terahertz charge carrier mobilities. The determined terahertz charge carrier mobility values were ~46 cm²/V·s and ~14 cm²/V·s for as-grown and heavily electron-irradiated GaSe crystals, respectively. These are quite close to the values determined from the Lorentz–Drude–Smith fitting of the measured dielectric constant spectra. The photo-injection-level-dependent charge carrier lifetimes were determined from the measured OPTP data, bearing in mind the model injection-level dependencies of the recombination rates governed by interband and trap-assisted Auger recombination, bulk and surface Shockley–Read–Hall (SRH) recombination and interband radiative transitions in the limit of a high injection level. It was found that GaSe possesses a long charge carrier lifetime (a~1.9 × 10⁻⁶ ps⁻¹, b~2.7 × 10⁻²¹ cm³ps⁻¹ and c~1.3 × 10⁻³⁷ cm⁶ps⁻¹), i.e., τ~0.53 μs in the limit of a relatively low injection, when the contribution from SRH recombination is dominant. The electron irradiation of as-grown GaSe crystals reduced the charge carrier lifetime at a high injection level due to Auger recombination through radiation-induced defects. It was found that the terahertz spectra of the dielectric constants of as-grown and electron-irradiated GaSe crystals can be fitted with acceptable accuracy using the Lorentz model with the Drude–Smith term accounting for the free-carrier conductivity. Full article

Terahertz photoconductivity and charge carrier recombination dynamics at two-photon (ZnGeP₂) and three-photon (4H-SiC) excitation were studied. Thermally annealed, high-energy electron-irradiated and Sc-doped ZnGeP₂ crystals were tested. The terahertz charge carrier mobilities were extracted from both the differential terahertz transmission at a specified photoexcitation condition and the Drude–Smith fitting of the photoconductivity spectra. The determined terahertz charge carrier mobility values are ~453 cm²/V·s for 4H-SiC and ~37 cm²/V·s for ZnGeP₂ crystals. The charge carrier lifetimes and the contributions from various recombination mechanisms were determined at different injection levels using the model, which takes into account the influence of bulk and surface Shockley–Read–Hall (SRH) recombination, interband radiative transitions and interband and trap-assisted Auger recombination. It was found that ZnGeP₂ possesses short charge carrier lifetimes (a~0.01 ps⁻¹, b~6 × 10⁻¹⁹ cm³·ps⁻¹ and c~7 × 10⁻⁴⁰ cm⁶·ps⁻¹) compared with 4H-SiC (a~0.001 ps⁻¹, b~3 × 10⁻¹⁸ cm³·ps⁻¹ and c~2 × 10⁻³⁶ cm⁶·ps⁻¹), i.e., τ~100 ps and τ~1 ns at the limit of relatively low injection, when the contribution from Auger and interband radiative recombination is small. The thermal annealing of as-grown ZnGeP₂ crystals and the electron irradiation reduced the charge carrier lifetime, while their doping with 0.01 mass % of Sc increased the charger carrier lifetime and reduced mobility. It was found that the dark terahertz complex conductivity of the measured crystals is not fitted by the Drude–Smith model with reasonable parameters, while their terahertz photoconductivity can be fitted with acceptable accuracy. Full article

In this paper, we propose an optically controlling broadband terahertz modulator of a layer-dependent PtSe₂ nanofilm based on a high-resistance silicon substrate. Through optical pump and terahertz probe system, the results show that compared with 6-, 10-, and 20-layer films, a 3-layer PtSe₂ nanofilm has better surface photoconductivity in the terahertz band and has a higher plasma frequency ω_p of 0.23 THz and a lower scattering time τ_s of 70 fs by Drude–Smith fitting. By the terahertz time-domain spectroscopy system, the broadband amplitude modulation of a 3-layer PtSe₂ film in the range of 0.1–1.6 THz was obtained, and the modulation depth reached 50.9% at a pump density of 2.5 W/cm². This work proves that PtSe₂ nanofilm devices are suitable for terahertz modulators. Full article

By employing optical pump Terahertz (THz) probe spectroscopy, ultrafast photocarrier dynamics of a two-dimensional (2D) semiconductor, SnS₂ nanoflake film, has been investigated systematically at room temperature. The dynamics of photoexcitation is strongly related to the density of edge sites and defects in the SnS₂ nanoflakes, which is controllable by adjusting the height of vertically aligned SnS₂ during chemical vapor deposition growth. After photoexcitation at 400 nm, the transient THz photoconductivity response of the films can be well fitted with bi-exponential decay function. The fast and slow processes are shorter in the thinner film than in the thicker sample, and both components are independent on the pump fluence. Hereby, we propose that edge-site trapping as well as defect-assisted electron-hole recombination are responsible for the fast and slow decay progress, respectively. Our experimental results demonstrate that the edge sites and defects in SnS₂ nanoflakes play a dominant role in photocarrier relaxation, which is crucial in understanding the photoelectrochemical performance of SnS₂ nanoflakes. Full article

In recent years, two-dimensional (2D) halide perovskites have been widely used in solar cells and photoelectric devices due to their excellent photoelectric properties and high environmental stability. However, the terahertz (THz) and ultrafast responses of the 2D halide perovskites are seldom studied, limiting the developments and applications of tunable terahertz devices based on 2D perovskites. Here, 2D R-P type (PEA)₂(MA)₂Pb₃I₁₀ perovskite films are fabricated on quartz substrates by a one-step spin-coating process to study their THz and ultrafast characteristics. Based on our homemade ultrafast optical pump–THz probe (OPTP) system, the 2D perovskite film shows an intensity modulation depth of about 10% and an ultrafast relaxation time of about 3 ps at a pump power of 100 mW due to the quantum confinement effect. To further analyze the recombination mechanisms of the photogenerated carriers, a three-exponential function is used to fit the carrier decay processes, obtaining three different decay channels, originating from free carrier recombination, exciton recombination, and trap-assisted recombination, respectively. In addition, the photoconductor changes (∆σ) at different pump–probe delay times are also investigated using the Drude-Smith model, and a maximum difference of 600 S/m is obtained at τ_p = 0 ps for a pump power of 100 mW. Therefore, these results show that the 2D (PEA)₂(MA)₂Pb₃I₁₀ film has potential applications in high-performance tunable and ultrafast THz devices. Full article

The time dynamics of nonequilibrium charge carrier relaxation processes in SI GaAs:EL2 (semi-insulating gallium arsenide compensated with EL2 centers) and HR GaAs:Cr (high-resistive gallium arsenide compensated with chromium) were studied by the optical pump–terahertz probe technique. Charge carrier lifetimes and contributions from various recombination mechanisms were determined at different injection levels using the model, which takes into account the influence of surface and volume Shockley–Read–Hall (SRH) recombination, interband radiative transitions and interband and trap-assisted Auger recombination. It was found that, in most cases for HR GaAs:Cr and SI GaAs:EL2, Auger recombination mechanisms make the largest contribution to the recombination rate of nonequilibrium charge carriers at injection levels above ~(0.5–3)·10¹⁸ cm⁻³, typical of pump–probe experiments. At a lower photogenerated charge carrier concentration, the SRH recombination prevails. The derived charge carrier lifetimes, due to the SRH recombination, are approximately 1.5 and 25 ns in HR GaAs:Cr and SI GaAs:EL2, respectively. These values are closer to but still lower than the values determined by photoluminescence decay or charge collection efficiency measurements at low injection levels. The obtained results indicate the importance of a proper experimental data analysis when applying terahertz time-resolved spectroscopy to the determination of charge carrier lifetimes in semiconductor crystals intended for the fabrication of devices working at lower injection levels than those at measurements by the optical pump–terahertz probe technique. It was found that the charge carrier lifetime in HR GaAs:Cr is lower than that in SI GaAs:EL2 at injection levels > 10¹⁶ cm⁻³. Full article

In past decades, ultrafast spin dynamics in magnetic systems have been associated with heat deposition from high energy laser pulses, limiting the selective access to spin order. Here, we use a long wavelength terahertz (THz) pump–optical probe setup to measure structural features in the ultrafast time scale. We find that complete demagnetization is possible with <6 THz pulses. This occurs concurrently with longitudinal acoustic phonons and an electronic response. Full article

A proposal for building a Free Electron Laser, EuPRAXIA@SPARC_LAB, at the Laboratori Nazionali di Frascati, is at present under consideration. This FEL facility will provide a unique combination of a high brightness GeV-range electron beam generated in a X-band RF linac, a 0.5 PW-class laser system and the first FEL source driven by a plasma accelerator. The FEL will produce ultra-bright pulses, with up to 10 ${}^{12}$ photons/pulse, femtosecond timescale and wavelength down to 3 nm, which lies in the so called “water window”. The experimental activity will be focused on the realization of a plasma driven short wavelength FEL able to provide high-quality photons for a user beamline. In this paper, we describe the main classes of experiments that will be performed at the facility, including coherent diffraction imaging, soft X-ray absorption spectroscopy, Raman spectroscopy, Resonant Inelastic X-ray Scattering and photofragmentation measurements. These techniques will allow studying a variety of samples, both biological and inorganic, providing information about their structure and dynamical behavior. In this context, the possibility of inducing changes in samples via pump pulses leading to the stimulation of chemical reactions or the generation of coherent excitations would tremendously benefit from pulses in the soft X-ray region. High power synchronized optical lasers and a TeraHertz radiation source will indeed be made available for THz and pump–probe experiments and a split-and-delay station will allow performing XUV-XUV pump–probe experiments. Full article

Photoinduced phase transitions in organic compounds with strong electron correlation ET [bis(ethylenedithio)-tetrathiafulvalene)-based salts α-(ET)₂I₃, θ-(ET)₂RbZn(SCN)₄, κ-(d-ET)₂Cu[N(CN)₂Br] were discussed based, on time resolved optical pump-probe spectroscopy using ~150 fs mid-infrared pulse, 12 fs near infrared pulse, and sub-picosecond terahertz pulse. (i) In charge-ordered insulators α-(ET)₂I₃ and θ-(ET)₂RbZn(SCN)₄, we captured ultrafast snapshots of charge dynamics i.e., immediate (ca. 15 fs) generation of a microscopic metallic state (or equivalently the microscopic melting of the charge order) which is driven by the coherent oscillation (period; 18 fs) of correlated electrons. Subsequently, condensation of the microscopic metallic state to the macroscopic scale occurs in α-(ET)₂I₃. However, in θ-(ET)₂RbZn(SCN)₄, such condensation is prevented by the large potential barrier reflecting the structural difference between the insulator and metal; (ii) In a Dimer–Mott insulator κ-(d-ET)₂Cu[N(CN)₂Br], photogeneration of the metallic state rises during ca. 1 ps that is much slower than the melting of charge order, because the photoinduced insulator to metal transition is driven by the intradimer molecular displacement in the dimer Mott insulator. The ultrafast dynamics of photoinduced insulator–metal transitions depend strongly on the molecular arrangement, reflecting various competing phases in the ET sheets. Full article