Kinetics and wavelength dependence of thermal and excited-state population on lens effect induced in a Nd:YAG rod amplifier.

Using a wavefront sensor, we have measured the temporal evolution of the lens induced in a Nd:YAG rod amplifier under side pumping by laser diode bars centered around 808 nm in a quasi-continuous wave regime. The evolution of the induced lens is drastically different when measured with a probe pulse centered at 532 nm or 1064.5 nm. To explain this evolution, we developed a model that accounts for both the excited state population of the Nd3+ ions and the thermal contribution to the refractive index of the amplifier. This model, which takes into account amplification and wavelength shift of the probe pulse at 1064.5 nm, makes it possible to quantitatively describe the spectral and temporal evolution of the amplifier focal length. It also shows that the excited state population contribution is more important around 1064.5 nm and can partly compensate for the thermal lens induced in the amplifier.

Enhancement in optically induced ultrafast THz response of MoSe2MoS2 heterobilayer.

THz conductivity of large area MoS2 and MoSe2 monolayers as well as their vertical heterostructure, MoSe2MoS2 is measured in the 0.3-5 THz frequency range. Compared to the monolayers, the ultrafast THz reflectivity of the MoSe2MoS2 heterobilayer is enhanced many folds when optically excited above the direct band gap energies of the constituting monolayers. The free carriers generated in the heterobilayer evolve with the characteristic times found in each of the two monolayers. Surprisingly, the same enhancement is recorded in the ultrafst THz reflectivity of the heterobilayer when excited below the MoS2 bandgap energy. A mechanism accounting for these observations is proposed.

Conical versus Gaussian terahertz emission from two-color laser-induced air plasma filaments.

In this Letter, we demonstrate that the far-field terahertz (THz) beam generated from a Ti:Sapphire two-color laser-induced filament can exhibit a conical or Gaussian distribution, depending on the filtering experimental conditions. Using both an incoherent Golay cell detector and a two-dimensional coherent electro-optic detection covering the 0.2-2.6 THz spectral range, in our experimental conditions, we provide evidence that the conical emission is due to photo-induced carriers in the silicon filter, typically used to block the remaining pump laser light. Moreover, the low-frequency THz beam retrieves an almost $ {{\rm TEM}_{00}} $TEM00 Gaussian spatial distribution when the silicon filter is preceded by a large bandgap ceramic filter, which stops the pump beam, thus preventing the carrier generation in the silicon filter.

Ultrafast dynamics of metal complexes of tetrasulphonated phthalocyanines.

A promising material in medicine, electronics, optoelectronics, electrochemistry, catalysis, and photophysics, tetrasulphonated aluminum phthalocyanine (AlPcS(4)), is investigated by means of steady-state and time-resolved pump-probe spectroscopies. Absorption and steady-state fluorescence spectroscopy indicate that AlPcS(4) is essentially monomeric. Spectrally resolved pump-probe data are recorded on time scales ranging from femtoseconds to nanoseconds. The nature of these fast processes and pathways of the competing relaxation processes from the initially excited electronic states in aqueous and organic (dimethyl sulfoxide) solutions are discussed. The decays and bleaching recovery have been fitted in the ultrafast window (0-10 ps) and later time window extending to nanoseconds (0-1 ns). While the excited-state dynamics have been found to be sensitive to the solvent environment, we were able to show that the fast dynamics is described by three time constants in the ranges of 115-500 fs, 2-25 ps, and 150-500 ps. We were able to ascribe these three time constants to different processes. The shortest time constants have been assigned to vibrational wavepacket dynamics. The few picosecond components have been assigned to vibrational relaxation in the excited electronic states. Finally, the 150-500 ps components represent the decay from S(1) to the ground state. The experimental and theoretical treatment proposed in this paper provides a basis for a substantial revision of the commonly accepted interpretation of the Soret transition (B transition) that exists in the literature.

Three-dimensional terahertz computed tomography of human bones.

Three-dimensional terahertz computed tomography has been used to investigate dried human bones such as a lumbar vertebra, a coxal bone, and a skull, with a direct comparison with standard radiography. In spite of lower spatial resolution compared with x-ray, terahertz imaging clearly discerns a compact bone from a spongy one, with strong terahertz absorption as shown by additional terahertz time-domain transmission spectroscopy.

Optical damage limit of efficient spintronic THz emitters.

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.

Tuning and focusing THz pulses by shaping the pump laser beam profile in a nonlinear crystal.

Spatially shaped femtosecond laser pulses are used to generate and to focus tunable terahertz (THz) pulses by Optical Rectification in a Zinc Telluride (ZnTe) crystal. It is shown analytically and experimentally that the focusing position and spectrum of the emitted THz pulse can be changed, in the intermediate field zone, by controlling the spatial shape of the near-infrared (NIR) femtosecond (fs) laser pump. In particular, if the pump consists of concentric circles, the emitted THz radiation is confined around the propagation axis, producing a THz pulse train, and focusing position and spectrum can be controlled by changing the number of circles and their diameter.

Study of the Photoswitching of a Fe(II) Chiral Complex through Linear and Nonlinear Ultrafast Spectroscopy.

Photoswitching the physical properties of molecular systems opens large possibilities for driving materials far from equilibrium toward new states. Moreover, ultrashort pulses of light make it possible to induce and to record photoswitching on a very short time scale, opening the way to fascinating new functionalities. Among molecular materials, Fe(II) complexes exhibit an ultrafast spin-state transition during which the spin state of the complex switches from a low spin state (LS, S = 0) to a high spin state (HS, S = 2). The latter process is remarkable: It takes place within ∼100 fs with a quantum efficiency of ∼100%. Moreover, the spin-state switching induces an important shift of the broad metal-to-ligand absorption band of the complex, and it results in large modifications of the physical and chemical properties of the compounds. But because most of the Fe(II) complexes crystallize in centrosymmetric space groups, this prevents them from exhibiting piezoelectric, ferroelectric, as well as second-order nonlinear optical properties such as second-harmonic generation (SHG). This considerably limits their potential applications. We have recently synthesized [Fe(phen)3] [Δ-As2(tartrate)2] chiral complexes that crystallize in a noncentrosymmetric 32 space group. Hereafter, upon the excitation of a thin film of these complexes by a femtosecond laser pulse and performing simultaneously transient absorption (TRA) and time-resolved SHG (TRSH) measurements, we have recorded the ultrafast LS to HS switching. Whereas a single TRA measurement gives only partial information, we demonstrate that TRSH readily reveals the different mechanisms in play during the HS-to-LS state relaxation. Moreover, a simple model makes it possible to evaluate the relaxation times as well as the hyperpolarizabilities of the different excited states through which the system travels during the spin-state transition.