Spin Flips versus Spin Transport in Nonthermal Electrons Excited by Ultrashort Optical Pulses in Transition Metals.

A joint theoretical and experimental investigation is performed to understand the underlying physics of laser-induced demagnetization in Ni and Co films with varying thicknesses excited by 10 fs optical pulses. Experimentally, the dynamics of spins is studied by determining the time-dependent amplitude of the Voigt vector, retrieved from a full set of magnetic and nonmagnetic quantities performed on both sides of films, with absolute time reference. Theoretically, ab initio calculations are performed using time-dependent density functional theory. Overall, we demonstrate that spin-orbit induced spin flips are the most significant contributors with superdiffusive spin transport, which assumes only that the transport of majority spins without spin flips induced by scattering does not apply in Ni. In Co it plays a significant role during the first ∼20 fs only. Our study highlights the material dependent nature of the demagnetization during the process of thermalization of nonequilibrium spins.

Directly probing spin dynamics in a molecular magnet with femtosecond time-resolution.

We show that a vanadium-chromium Prussian blue analogue, which is a room-temperature molecule-based magnet, displays a fast magnetic response on a femtosecond timescale that is attributed to the super-exchange interaction between the metal ions. These dynamics are obtained from femtosecond Faraday magneto-optical (MO) measurements, performed at 50 and 300 K. Exciting at the ligand-to-metal charge-transfer (LMCT) band results in the formation of the 2E excited state on the Cr ion via intersystem crossing (ISC) from the 4LMCT state in less than 250 fs. Subsequent vibrational relaxation in the 2E state occurs on a 0.78 ± 0.05 ps timescale at 50 K and 1.1 ± 0.1 ps at 300 K. The MO measurements can detect the formation of the 2E state on the Cr ion from the change in the super-exchange interaction taking place as a result of the corresponding spin flip associated with the formation of the 2E state. These results open up a new avenue to study molecular magnets using a powerful method that is capable of directly probing spin dynamics on a sub-picosecond timescale in thin film environments.

Ultrafast Optical Properties of Dense Electron Gas in Silicon Nanostructures.

We investigate the ultrafast dynamics of carriers in a silicon nanostructure by performing spectrally resolved femtosecond spectroscopy measurements with a supercontinuum probe. The nanostructure consists of a 158-nm-thick crystalline Si layer on top of which a SiO2 passivation layer leads to a very high quality of the Si surface. In addition, a dielectric function approach, including contributions from a Drude part and interband transitions, combined with the Transition Matrix Approximation is used to model the photogenerated carrier dynamics. The spectrotemporal reflectivity reveals two mechanisms. First, an electron-hole plasma is created by the pump pulse and lasts for a few picoseconds. Importantly, its spectral signature is either a positive or a negative change of reflectivity, depending on the probe wavelength. This is complementary to the already reported results obtained with degenerate frequency measurements. The second mechanism is a thermal diffusion of carriers which occurs during several hundreds of picoseconds. The overall dynamics at short and long delays in the whole visible spectrum is well explained with our model which shows that the main contribution to the reflectivity dynamics is due to the Drude dielectric function. The observation of this predominance of free carriers requires both a long lived high density of carriers as well as a little influence of surface scattering as provided by our thin crystalline Si layer with passivated Si/SiO2 interface.

Exciton diffusion in near-infrared absorbing solution-processed organic thin films.

We report on singlet-singlet annihilation and exciton diffusion in as-prepared p-type and annealed n-type thin films of the low-bandgap quinoidal quaterthiophene [QQT(CN)4] using ultrafast transient absorption measurements. The decay dynamics of exciton populations are well described by a one-dimensional diffusion-limited bimolecular recombination, indicating that the singlet excitons migrate preferentially along the stacking direction. Our results show that the exciton diffusion constants in QQT(CN)4 films do not vary significantly upon thermal annealing. Exciton diffusion lengths are measured to be as high as 4 and 5 nm in as-prepared and annealed QQT(CN)4 films, respectively. We also observe an influence of the excitation densities on the singlet exciton diffusion, which is attributed to phonon scattering. Because of the possibility of patterning p-n regions in QQT(CN)4 films by thermal nanolithography techniques, this study provides important insight not only into the photophysical properties of quinoidal oligothiophene derivatives but also for their future integration into high-performance p-n nanostructured near infrared light-sensing devices.

Distinguishing the ultrafast dynamics of spin and orbital moments in solids.

For an isolated quantum particle, such as an electron, the orbital (L) and spin (S) magnetic moments can change provided that the total angular momentum of the particle is conserved. In condensed matter, an efficient transfer between L and S can occur owing to the spin-orbit interaction, which originates in the relativistic motion of electrons. Disentangling the absolute contributions of the orbital and spin angular momenta is challenging, however, as any transfer between the two occurs on femtosecond timescales. Here we investigate such phenomena by using ultrashort optical laser pulses to change the magnetization of a ferromagnetic film and then probe its dynamics with circularly polarized femtosecond X-ray pulses. Our measurements enable us to disentangle the spin and orbital components of the magnetic moment, revealing different dynamics for L and S. We highlight the important role played by the spin-orbit interaction in the ultrafast laser-induced demagnetization of ferromagnetic films, and show also that the magneto-crystalline anisotropy energy is an important quantity to consider in such processes. Our study provides insights into the dynamics in magnetic systems as well as perspectives for the ultrafast control of information in magnetic recording media.

Surface plasmon dynamics in arrays of subwavelength holes: the role of optical interband transitions.

Using femtosecond optical spectroscopy, we study the ultrafast dynamics of the surface plasmon polaritons in gold arrays of subwavelength holes. A large time dependent spectral broadening and shift of the surface plasmon resonances are reported. The experimental results are modeled by the diffraction of a transverse electromagnetic field through the nanostructure, taking into account both the electron dynamics near the interband transitions and the Drude-like conductivity of the metal. Our analysis, using either a theoretical or an experimentally determined dielectric function of gold, suggests that the losses propagation in plasmonic devices is strongly influenced by intrinsic and extrinsic electron scattering mechanisms.

Femtosecond spectroscopy probes the folding quality of antibody fragments expressed as GFP fusions in the cytoplasm.

Time-resolved femtosecond spectroscopy can improve the application of green fluorescent proteins (GFPs) as protein-folding reporters. The study of ultrafast excited-state dynamics (ESD) of GFP fused to single chain variable fragment (scFv) antibody fragments, allowed us to define and measure an empirical parameter that only depends on the folding quality (FQ) of the fusion. This method has been applied to the analysis of genetic fusions expressed in the bacterial cytoplasm and allowed us to distinguish folded and thus functional antibody fragments (high FQ) with respect to misfolded antibody fragments. Moreover, these findings were strongly correlated to the behavior of the same scFvs expressed in animal cells. This method is based on the sensitivity of the ESD to the modifications in the tertiary structure of the GFP induced by the aggregation state of the fusion partner. This approach may be applicable to the study of the FQ of polypeptides over-expressed under reducing conditions.

Femtosecond magneto-optical Kerr microscopy.

We have developed a magneto-optical Kerr microscope that allows us to measure the ultrafast magnetization dynamics of ferromagnetic nanostructures. The magneto-optical signal can be recorded in a confocal reflection geometry with an accurate selection of the polarization. The magnetization dynamics is obtained from pump-probe measurements using frequency nondegenerate collinear pump and probe beams with a temporal resolution of 180 fs. Both probe and pump beams are focused to their diffraction limit, leading to an overall spatial resolution of 600 nm. The efficiency of the apparatus is tested by investigating the magnetization dynamics of individual CoPt(3) disks with a submicrometer diameter and a thickness of 15 nm.

Damped precession of the magnetization vector of superparamagnetic nanoparticles excited by femtosecond optical pulses.

The ultrafast magnetization and electron dynamics of superparamagnetic cobalt nanoparticles, embedded in a dielectric matrix, have been investigated using femtosecond optical pulses. Our experimental approach allows us to bypass the superparamagnetic thermal fluctuations and to observe the trajectory of the magnetization vector which exhibits a strongly damped precession motion. The magnetization precession is damped faster in the superparamagnetic particles than in cobalt films or when the particle size decreases, suggesting that the damping is enhanced at the metal dielectric interface. Our observations question the gyroscopic nature of the magnetization pathway when superparamagnetic fluctuations take place as we discuss in the context of Brown's model.

Optical response of periodically modulated nanostructures near the interband transition threshold of noble metals.

We investigate the influence of the core d-electrons on the spectral optical response of arrays of sub-wavelength holes near the transition from the d-band to the Fermi level of noble metals (d?E(F)). Our model shows that, due to the dispersion of the metal dielectric function near d?E(F), the first order peaks in the enhanced spectral transmission shift nonlinearly as a function of the period of the nanostructure. In addition, we outline in that spectral region an apparent large resonance which does not depend on the geometrical parameters of the nanostructure. It is shown to correspond to the transparency window resulting from the spectral superposition of the large absorption associated to the core d-electrons and high reflectivity due to the conduction electrons. The analysis is performed for gold, copper and silver nanostructures.

Real space trajectory of the ultrafast magnetization dynamics in ferromagnetic metals.

We have measured the real space trajectory of the ultrafast magnetization dynamics in ferromagnetic metals induced by femtosecond optical pulses. Our approach allows the observation of the initial change of the modulus and orientation of the magnetization, occurring within a few hundreds of femtoseconds, as well as its subsequent precession and damping around the effective field. The role of the magnetocrystalline anisotropy shows up in the magnetization reorientation occurring during the electron-lattice relaxation. In addition, we propose a model which takes into account the initial demagnetization in the Bloch formalism describing the magnetization dynamics.

Analytical model of the optical response of periodically structured metallic films.

In this paper we investigate the optical response of periodically structured metallic films constituted of sub-wavelength apertures. Our approach consists in studying the diffraction of transverse magnetic polarized electromagnetic waves by a one-dimensional grating. The method that we use is the Rigorous Coupled Waves Analysis allowing us to obtain an analytical model to calculate the diffraction efficiencies. The zero and first order terms allow determining the transmission, reflectivity and absorption of symmetric or asymmetric nanostructures surrounded either by identical or different dielectric media. For both type of nanostructures the spectral shape of the enhanced resonant transmission associated to surface plasmons displays a Fano profile. In the case of symmetric nanostructures, we study the conditions of formation of coupled surface plasmon-polaritons as well as their effect on the optical response of the modulated structure. For asymmetric nanostructures, we discuss the non-reciprocity of the reflectivity and we investigate the spectral dependency of the enhanced resonant transmission on the refractive index of the dielectric surrounding the metal film.

Femtosecond spectrotemporal magneto-optics.

A new method to measure and analyze the time and spectrally resolved polarimetric response of magnetic materials is presented. It allows us to study the ultrafast magnetization dynamics of a CoPt3 ferromagnetic film. The analysis of the pump-induced rotation and ellipticity detected by a broad spectrum probe beam shows that magneto-optical signals predominantly reflect the spin dynamics in ferromagnets.

Surface plasmon dynamics of simple metal clusters excited with femtosecond optical pulses.

We report a new mechanism on the dynamics of correlated electrons in simple metal clusters which manifests by a strong electron temperature dependence of the surface plasmon resonance spectral profile. This effect is revealed thanks to a theoretical approach based on the time-dependent local-density approximation at finite electronic temperature, and it should be experimentally observable using pump-probe femtosecond spectroscopy techniques.