Nonlinear optical properties and carrier relaxation dynamics in graphene, suspended in three different solvents, are investigated using femtosecond (80 fs pulses) Z-scan and degenerate pumpprobe spectroscopy at 790 nm. The results demonstrate saturable absorption property of graphene with a nonlinear absorption coefficient, β, of ~2 to 9x10 -8 cm/W. Two distinct time scales associated with the relaxation of photoexcited carriers, a fast one in the range of 130-330 fs (related to carriercarrier scattering) followed by a slower one in 3.5-4.9 ps range (associated with carrier-phonon scattering) are observed.Graphene is a two-dimensional carbon nanomaterial which has received tremendous interest in recent years owing to its various remarkable properties and applications in modern electronics and photonics [1,2]. Ultrafast degenerate and nondegenerate pump-probe measurements on single and multilayer epitaxial [3,4] or exfoliated [5] graphenes deposited on a substrate have shown two types of dynamics of the carriers: a fast component of the order of ~100 fs attributed to the intraband carrier-carrier scattering and a slower component ~2 ps associated with carrierphonon scattering. In the degenerate pump-probe studies on single and multilayer graphene films grown on a SiC substrate using 85 fs laser pulses centered at 790 nm, a positive change in the transient differential transmission of the probe was observed with two relaxation times, the faster one in the range of 70-120 fs and a slower one between 0.4-1.7 ps [3]. Similar carrier relaxation dynamics was obtained in the nondegenerate pump-probe experiments on exfoliated graphene films on SiO 2 /Si substrate [5]. On a few layer thick graphene film on SiC, nondegenerate pump-probe experiments [4] using 800 nm pump showed that the sign of the differential transmission signal is positive over the entire probe spectral range of 1.1 to 2.6 µm but becomes negative after 2 ps if the probe wavelength falls between 1.78 and 2.35 µm. The initial positive part of the signal within 150 fs has been described in terms of thermalization and emission of high energy-phonons followed by a slow decay of the order of a few ps determined by electron-acoustic phonon scattering. Nonlinear optical properties of graphene have been reported recently in the nanosecond (ns) and picosecond (ps) regimes [6,7]. Using 35 ps laser pulses centered at 532 nm, it has been shown that the nonlinear response of graphene oxide suspensions changes from saturable absorption at low intensity (2.1 GW/cm 2 ) to reverse saturable absorption or optical limiting at higher intensities (>4.5 GW/cm 2 ) [6]. In comparison, in the ns regime suspensions of graphene oxide and functionalized graphene in dimethylformamide showed optical limiting property at all values of intensities above 0.6 GW/cm 2 [6,7].We have carried out femtosecond (80 fs) Z-scan and degenerate pump-probe experiments at 790 nm to study the nonlinear optical response and carrier dynamics in colloidal suspensions of graphene which have not been invest...

Degenerate pump-probe reflectivity experiments have been performed on a single crystal of bismuth telluride (Bi 2 Te 3 ) as a function of sample temperature (3K to 296K) and pump intensity using ∼ 50 femtosecond laser pulses with central photon energy of 1.57 eV. The time resolved reflectivity data show two coherently generated totally symmetric A 1g modes at 1.85 THz and 3.6THz at 296K which blue shift to 1.9 THz and 4.02 THz, respectively at 3K. At high photoexcited carrier density of ∼ 1.7 × 10 21 cm −3 , the phonon mode at 4.02 THz is two orders of magnitude higher positively chirped (i.e the phonon time period decreases with increasing delay time between the pump and the probe pulses) than the lower frequency mode at 1.9 THz. The chirp parameter, β is shown to be inversely varying with temperature. The time evolution of these modes is studied using continuous wavelet transform of the time-resolved reflectivity data.

We demonstrate the ultrafast formation of terahertz (THz) metasurfaces through all-optical creation of spatially modulated carrier density profiles in a deep-subwavelength GaAs film. The switch-on of the transient plasmon mode, governed by the GaAs effective electron mass and electron–phonon interactions, is revealed by structured-optical pump THz probe spectroscopy, on a time scale of 500 fs. By modulating the carrier density using different pump fluences, we observe a wide tuning of the electric dipole resonance of the transient GaAs metasurface from 0.5 THz to 1.7 THz. Furthermore, we numerically demonstrate that the metasurface presented here can be generalized to more complex architectures for realizing functionalities such as perfect absorption, leading to a 30 dB modulation depth. The platform also provides a pathway to achieve ultrafast manipulation of infrared beams in the linear and, potentially, nonlinear regime.

Coherent radiation with frequencies ranging from 0.3 to 30 THz has recently become accessible using femtosecond laser technology. These terahertz (THz) waves have already been applied in spectroscopy and imaging and can be manipulated using static optical elements such as lenses, polarizers and filters. However, ultrafast modulation of THz radiation is required as well, for instance, in short-range wireless communication or for preparing shaped THz transients for the coherent control of numerous material excitations. Here, we demonstrate an all-optically created transient metamaterial that allows us to manipulate the polarization of THz waveforms with subcycle switch-on times. The polarization-modulated pulses are potentially interesting for controlling elementary motions such as the vibration of crystal lattices, the rotation of molecules and the precession of spins.