Pump-terahertz Probe Spectroscopy Research Articles

Ultrafast insulator–metal phase transition in vanadium dioxide studied using optical pump–terahertz probe spectroscopy

We studied the ultrafast dynamic behavior of the photoinduced insulator–metal phase transition in VO2 thin film using optical pump–terahertz probe spectroscopy with different excitation fluences and at different temperatures. We observed two processes in the insulator–metal phase transition in VO2: a fast process and a slow process. The fast process is a nonthermal process, which is ascribed to the nucleation of the metal phase, while the slow process is strongly affected by temperature and is ascribed to the thermally driven growth and coalescence of metal domains in VO2. The transient complex conductivity spectra at different delay times are also investigated.

Photocarriers dynamics in silicon wafer studied with optical-pump terahertz-probe spectroscopy

Optical pump-terahertz probe spectroscopy is employed to investigate the optical characteristics of silicon wafer. The wafer surface undergoes a phase transition from insulator to metal for terahertz wave with increasing pump fluence. The real part of the pump-induced conductivity shows strong frequency dependence, which can be well described with Drude–Smith model. Our results also demonstrate that the photoexcited Si layer acts as a broadband terahertz pulse antireflection coating with proper pump fluence. In addition, it is observed that the terahertz pulse apparently arrives at the detector earlier when silicon is optically excited.

Transient optical modulation properties in the terahertz metamaterial of split ring resonators

The ultrafast optical modulation properties of split ring resonators are characterized by utilizing optical pump-terahertz probe spectroscopy. The experimental results show that when the terahertz electric vector is perpendicular to the gap of the split ring resonator, resonant absorption can be quenched significantly under high pump excitation. However, when the terahertz electric vector is parallel to the gap, the resonant absorption is less sensitive to pump excitation due to the structural properties of the metamaterial. Our numerical simulations also demonstrate that the pump pulse significantly influences the split ring resonator current by generating carriers in the substrate.

Ultrafast optical modulation of terahertz metamaterials

We have characterized the ultrafast dynamical properties of split ring resonators byutilizing optical pump–terahertz probe spectroscopy on a subpicosecond timescale. Theexperimental results show that the pump-induced relative changes in terahertz peaktransmission, as well as the dynamical transmission spectra, are different when theterahertz electric vector is perpendicular and parallel to the gap of the split ring resonator.It is found that the pump-induced photogenerated carriers play two opposite roles in SRRs,showing one is to absorb terahertz to reduce the transmission in the substrate and theother is to weaken the resonant absorption to enhance the transmission. Our numericalsimulations also prove that the pump pulse significantly influences the split ringresonator currents. We also show that the blue-shifts of the resonances are due tothe change of optical constants in the photoexcited semiconductor substrate.

Ultrafast (but Many-Body) Relaxation in a Low-Density Electron Glass

We present a study of the relaxation dynamics of the photoexcited conductivity of the impurity states in the low-density electronic glass, phosphorous-doped silicon Si:P. Using subband gap optical pump-terahertz probe spectroscopy we find strongly temperature- and fluence-dependent glassy power-law relaxation occurring over subnanosecond time scales. Such behavior is in contrast to the much longer time scales found in higher electron density glassy systems. We also find evidence for both multiparticle relaxation mechanisms and/or coupling to electronic collective modes and a low temperature quantum relaxational regime.

Ultrafast carrier capture in InGaAs quantum posts

To explore the capture dynamics of photoexcited carriers in semiconductor quantum posts, optical pump terahertz (THz) probe and time-resolved photoluminescence spectroscopy were performed. The results of the THz experiment show that after ultrafast excitation, electrons relax within a few picoseconds into the quantum posts, which act as efficient traps. The saturation of the quantum post states, probed by photoluminescence, was reached at approximately ten times the quantum post density in the samples. The results imply that quantum posts are highly attractive nanostructures for future device applications.

Carrier dynamics and terahertz photoconductivity of doped silicon measured by femtosecond pump-terahertz probe spectroscopy

The carrier dynamics and terahertz photoconductivity in the n-type silicon (n-Si) as well as in the p-type Silicon (p-Si) have been investigated by using femtosecond pump-terahertz probe technique. The measurements show that the relative change of terahertz transmission of p-Si at low pump power is slightly smaller than that of n-Si, due to the lower carrier density induced by the recombination of original holes in the p-type material and the photogenerated electrons. At high pump power, the bigger change of terahertz transmission of p-Si originates from the greater mobility of the carriers compared to n-Si. The transient photoconductivities are calculated and fit well with the Drude-Smith model, showing that the mobility of the photogenerated carriers decreases with the increasing pump power. The obtained results indicate that femtosecond pump-terahertz probe technique is a promising method to investigate the carrier dynamics of semiconductors.

Study of photo-induced phenomena in VO 2 by terahertz pump-probe spectroscopy

The ultrafast terahertz response to the photoexcitation in vanadium dioxide was investigated using the optical-pump terahertz-probe technique at room temperature. The optical excitation at 790 nm induced an ultrafast decrease of the transmittance of the terahertz pulses corresponding to the increase of the electronic conductivity within 0.7 ps, and then the transmittance decreases gradually up to 100 ps. This two-step behavior is very similar to the previous reports of the time resolved X-ray and electron diffractions. This fact indicates that the increase of the electronic conductivity and the change of the lattice structure proceed in parallel, and the photo-induced insulator–metal phase transition is of the Peierls type.

Photoionization of atmospheric gases studied by time-resolved terahertz spectroscopy

We investigate the laser induced ionization and plasma formation in pure oxygen and nitrogen by means of optical pump–terahertz probe spectroscopy. Focused amplified femtosecond pulses at 405 and 810 nm are used to ionize the gas molecules by nonlinear processes. The ionized gas is probed by picosecond terahertz pulses in the frequency range of 0.2–2 THz to obtain the free electron density (10 13–10 17 cm −3) and the electron scattering time (0.2 ps for N 2 and 0.4 ps for O 2 ). We demonstrate the importance of the centrifugal barrier for the photoionization process using circularly polarized light.

Ultrafast high-field carrier transport in GaAs measured by femtosecond pump-terahertz probe spectroscopy

Femtosecond pump-terahertz probe studies of carrier dynamics in semi-insulating GaAs have been investigated in detail for various pump powers and at electric fields up to 15kV∕cm. The pump-induced attenuation of terahertz transmission reduces obviously at high field, and the carrier relaxation time is also found to be correlated with photoinjected carrier density and electric field. These effects can be fully explained in terms of the carrier intervalley scattering and the surface states filling in GaAs, which may influence the carrier recombination process. Moreover, the carrier screening effect at high pump powers is also discussed.

Photoconductive response correction for detectors of terahertz radiation

Photoconductive detectors are convenient devices for detecting pulsed terahertz radiation. We have optimized Fe+ ion-damaged InP materials for photoconductive detector signal to noise performance using dual-energy doses in the range from 2.5×1012 to 1.0×1016 cm−2. Ion implantation allowed the production of semiconducting materials with free-carrier lifetimes between 0.5 and 2.1 ps, which were measured by optical pump terahertz probe spectroscopy. The time resolved photoconductivity of the detector substrates was acquired as a function of time after excitation by 2 nJ pulses from a laser oscillator. These data, when combined with a deconvolution algorithm, provide an excellent spectral response correction to the raw photocurrent signal recorded by the photoconductive detectors.

Terahertz mobility measurements on poly-3-hexylthiophene films: Device comparison, molecular weight, and film processing effects

We directly compare relative carrier mobilities in semiconducting organic polymer films measured using noncontact optical pump terahertz (THz) probe spectroscopy to those reported in electrical device studies. Relative transient signal amplitude measurements of photoinjected carrier mobility as a function of poly-3-hexylthiophene (P3HT) molecular weight correlate directly with electrical device test values, indicating that the THz method shows promise as a rapid material screening approach. We also present measurements on P3HT conducting films as a function of structural regularity, dispersing solvent, addition of C60 electron traps, sample temperature, and other growth parameters relevant to device manufacture.

Photoinduced metallic state in VO2 proved by the terahertz pump-probe spectroscopy

We investigated the ultrafast terahertz response to the photoexcitation for vanadium dioxide single crystals and thin films using the optical-pump terahertz-probe technique at room temperature. The optical excitation induced an ultrafast decrease of the transmittance of the terahertz radiation within 0.7ps. Since we expect only the free carrier response in the terahertz range, the decrease of the transmittance is unambiguously assigned to the appearance of the high electronic conductivity due to free carriers. The conductivity increases more than ten times in the picosecond time range after photoexcitation and it is concluded that the electronic states are metallic.

Propagation of terahertz pulses in photoexcited media: Analytical theory for layered systems

Optical pump-terahertz probe spectroscopy has become a widely used experimental tool for the investigation of the ultrafast far-infrared response of polar systems. In this paper the authors present an analytical method of calculating the propagation of ultrashort terahertz pulses in photoexcited media. The transient terahertz wave form transmitted through the sample is equal to a product of the incident terahertz field (at a mixed frequency), transient susceptibility, and a so called transfer function which depends on the properties of the sample in equilibrium. The form of the transfer function is derived for general layered systems and for specific cases including one-dimensional photonic crystals, thin films, and bulk samples. Simplified expressions directly applicable to the analysis of the experimental results related to the most common sample geometries are shown and discussed.

Terahertz time-domain spectroscopy of photoinduced carriers in [formula omitted

We have performed an optical characterization of photoinduced carriers in the Mott insulator YTiO 3 by using the optical pump-terahertz probe spectroscopy. The complex conductivity, σ ( ω ) , of photoinduced carriers is deduced to be similar to that of bad metals. The energy relaxation time of the photoinduced carriers is longer than 13 ns. The anisotropic terahertz response of photoinduced state is confirmed.

Nonresonant ionization of oxygen molecules by femtosecond pulses: Plasma dynamics studied by time-resolved terahertz spectroscopy

We show that optical pump-terahertz probe spectroscopy is a direct experimental tool for exploring laser-induced ionization and plasma formation in gases. Plasma was produced in gaseous oxygen by focused amplified femtosecond pulses. The ionization mechanisms at 400- and 800-nm excitation wavelengths differ significantly being primarily of a multiphoton character in the former case and a strong-field process in the latter case. The generation of the plasma in the focal volume of the laser and its expansion on subnanosecond time scale is directly monitored through its density-dependent susceptibility. A Drude model used to evaluate the plasma densities and electron-scattering rates successfully captures the observations for a wide range of pump intensities. In addition, rotational fingerprints of molecular and ionic species were also observed in the spectra.

Optical pump-terahertz probe spectroscopy of dyes in solutions: probing the dynamics of liquid solvent or solid precipitate?

The optical pump-terahertz probe spectroscopy was used together with ab initio calculations and molecular dynamics simulations to investigate ultrafast dynamics following electronic excitation of Coumarin 153 and TBNC (2,11,20,29-tetra-tert-butyl-2,3-naphtalocyanine) dyes in polar solvents. By scanning the terahertz waveform for different pump-probe delays this experimental technique allows us to obtain two dimensional spectra directly reflecting the temporal response of the system. A distinct signal was obtained for TBNC in chloroform, 2-propanol, and n-butanol, while no signal was recorded for Coumarin 153 in either of these solvents. We explain the nonequilibrium signal detected in TBNC solutions by the presence of a solid, polycrystalline phase of the dye resulting from irradiating the solution by intense optical pulses.