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 pump-probe spectroscopy at 790 nm. The results demonstrate saturable absorption property of graphene with a nonlinear absorption coefficient, β of (∼2–9)×10−8 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 carrier-carrier scattering) followed by a slower one in 3.5–4.9 ps range (associated with carrier-phonon scattering) are observed.
Nonlinear transmission of 80 and pulsed light with wavelength through single walled carbon nanotubes suspended in water containing sodium dodecyl sulfate is studied. Pulse-width independent saturation absorption and negative cubic nonlinearity are observed, respectively, in open and closed aperture -scan experiments. The theoretical expressions derived to analyze the -dependent transmission in the saturable limit require two photon absorption coefficient and a nonlinear index to fit the data.
THz generation from femtosecond photoexcited spintronic heterostructures has become a versatile tool for investigating ultrafast spin-transport and transient charge-current in a non-contact and non-invasive manner. The equivalent effect from the orbital degree of freedom is still in the primitive stage. Here, we experimentally demonstrate orbital-to-charge current conversion in metallic heterostructures, consisting of a ferromagnetic layer adjacent to either a light or a heavy metal layer, through detection of the emitted THz pulses. Our temperature-dependent experiments help to disentangle the orbital and spin components that are manifested in the respective Hall-conductivities, contributing to THz emission. NiFe/Nb shows the strongest inverse orbital Hall effect with an experimentally extracted value of effective intrinsic Hall-conductivity, $${({\sigma }_{{SOH}}^{{{{{\mathrm{int}}}}}})}^{{eff}} \sim 195{\varOmega }^{-1}{{cm}}^{-1}$$ , while CoFeB/Pt shows maximum contribution from the inverse spin Hall effect. In addition, we observe a nearly ten-fold enhancement in the THz emission due to pronounced orbital-transport in W-insertion heavy metal layer in CoFeB/W/Ta heterostructure as compared to CoFeB/Ta bilayer counterpart.
THz pulses are generated from femtosecond pulse-excited ferromagnetic/nonmagnetic spintronic heterostructures via inverse spin Hall effect. The highest possible THz signal strength from spintronic THz emitters is limited by the optical damage threshold of the corresponding heterostructures at the excitation wavelength. For the thickness-optimized spintronic heterostructure, the THz generation efficiency does not saturate with the excitation fluence even up till the damage threshold. Bilayer (Fe, CoFeB)/(Pt, Ta)-based ferromagnetic/nonmagnetic (FM/NM) spintronic heterostructures have been studied for an optimized performance for THz generation when pumped by sub-50 fs amplified laser pulses at 800 nm. Among them, CoFeB/Pt is the best combination for an efficient THz source. The optimized FM/NM spintronic heterostructure having α-phase Ta as the nonmagnetic layer shows the highest damage threshold as compared to those with Pt, irrespective of their generation efficiency. The damage threshold of the Fe/Ta heterostructure on a quartz substrate is ∼85 GW/cm2.
Degenerate pump-probe reflectivity experiments have been performed on a single crystal of bismuth telluride (Bi2Te3) as a function of sample temperature (3 K to 296 K) 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 A1g modes at 1.85 THz and 3.6 THz at 296 K which blue-shift to 1.9 THz and 4.02 THz, respectively, at 3 K. At high photoexcited carrier density of ~1.7×1021 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.