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M. Battiato

Publications and source records attributed to M. Battiato.

13 recordsLinked to original sources

Comparing scattering rates from Boltzmann and dynamical mean-field theory

We compute scattering rates for electrons in the two-dimensional Hubbard model for a one-orbital metal and a two-orbital band insulator by means of the Boltzmann scattering equation (BSE) and dynamical mean-field theory (DMFT). As an intermediate method between both, we also consider the BSE without momentum conservation. In the weak interaction regime and for the band insulator, the last two agree to very good accuracy. The BSE with momentum conservation, on the other hand, shows slightly larger scattering rates, and a momentum differentiation of these on the Fermi surface. For the Mott insulator at strong interaction, the DMFT electron scattering rates are much larger and defy a BSE description. Noteworthy, the scattering rates for the band insulator are exceedingly small because -- in contrast to the Mott insulator -- there is virtually no impact ionization.

cond-mat.str-el

Impact of ultrafast transport on the high-energy states of a photoexcited topological insulator

Ultrafast dynamics in three-dimensional topological insulators (TIs) opens new routes for increasing the speed of information transport up to frequencies thousand times faster than in modern electronics. However, up to date, disentangling the exact contributions from bulk and surface transport to the subpicosecond dynamics of these materials remains a difficult challenge. Here, using time- and angle-resolved photoemission, we demonstrate that driving a TI from the bulk-conducting into the bulk-insulating transport regime allows to selectively switch on and off the emergent channels of ultrafast transport between the surface and the bulk. We thus establish that ultrafast transport is one of the main driving mechanisms responsible for the decay of excited electrons in prototypical TIs following laser excitation. We further show how ultrafast transport strongly affects the thermalization and scattering dynamics of the excited states up to high energies above the Fermi level. In particular, we observe how inhibiting the transport channels leads to a thermalization bottleneck that substantially slows down electron-hole recombination via electron-electron scatterings. Our results pave the way for exploiting ultrafast transport to control thermalization time scales in TI-based optoelectronic applications, and expand the capabilities of TIs as intrinsic solar cells.

cond-mat.mes-hall

Distinctive Picosecond Spin Polarization Dynamics in Bulk Half-Metals

Femtosecond laser excitations in half-metal (HM) compounds are theoretically predicted to induce an exotic picosecond spin dynamics. In particular, conversely to what is observed in conventional metals and semiconductors, the thermalization process in HMs leads to a long living partially thermalized configuration characterized by three Fermi--Dirac distributions for the minority, majority conduction and majority valence electrons respectively. Remarkably, these distributions have the same temperature but different chemical potentials. This unusual thermodynamics state causes a persistent non-equilibrium spin polarization only well above the Fermi energy. Femtosecond spin dynamics experiments performed on Fe$_3$O$_4$ by time-, spin-, and angle-resolved photoelectron spectroscopy confirm our model. Furthermore, the spin polarization response proves to be very robust and it can be adopted to selectively test the bulk HM character in a wide range of compounds.

cond-mat.mtrl-sci

Boltzmann approach to high-order transport: the non-linear and non-local responses

The phenomenological textbook equations for the charge and heat transport are extensively used in a number of fields ranging from semiconductor devices to thermoelectricity. We provide a rigorous derivation of transport equations by solving the Boltzmann equation in the relaxation time approximation and show that the currents can be rigorously represented by an expansion in terms of the 'driving forces'. Besides the linear and non-linear response to the electric field, the gradient of the chemical potential and temperature, there are also terms that give the response to the higher-order derivatives of the potentials. These new, non-local responses, which have not been discussed before, might play an important role for some materials and/or in certain conditions, like extreme miniaturization. Our solution provides the general solution of the Boltzmann equation in the relaxation time approximation (or equivalently the particular solution for the specific boundary conditions). It differs from the Hilbert expansion which provides only one of infinitely many solutions which may or may not satisfy the required boundary conditions.

cond-mat.mtrl-sci

Laser-induced persistent photovoltage on the surface of a ternary topological insulator at room temperature

Using time- and angle-resolved photoemission, we investigate the ultrafast response of excited electrons in the ternary topological insulator (Bi$_{1 x}$Sb$_{x}$)$_2$Te$_3$ to fs-infrared pulses. We demonstrate that at the critical concentration $x$=0.55, where the system becomes bulk insulating, a surface voltage can be driven at room temperature through the topological surface state solely by optical means. We further show that such a photovoltage persists over a time scale that exceeds $\sim$6 $μ$s, i.e, much longer than the characteristic relaxation times of bulk states. We attribute the origin of the photovoltage to a laser-induced band-bending effect which emerges near the surface region on ultrafast time scales. The photovoltage is also accompanied by a remarkable increase in the relaxation times of excited states as compared to undoped topological insulators. Our findings are relevant in the context of applications of topological surface states in future optical devices.

cond-mat.mes-hall

Sub-picosecond spin dynamics of excited states in the topological insulator Bi$_2$Te$_3$

Using time-, spin- and angle-resolved photoemission, we investigate the ultrafast spin dynamics of hot electrons on the surface of the topological insulator Bi$_2$Te$_3$ following optical excitation by fs-infrared pulses. We observe two surface-resonance states above the Fermi level coexisting with a transient population of Dirac fermions that relax in about $\sim$2 ps. One state is located below $\sim$0.4 eV just above the bulk continuum, the other one at $\sim$0.8 eV inside a projected bulk band gap. At the onset of the excitation, both states exhibit a reversed spin texture with respect to that of the transient Dirac bands, in agreement with our one-step photoemission calculations. Our data reveal that the high-energy state undergoes spin relaxation within $\sim$0.5 ps, a process that triggers the subsequent spin dynamics of both the Dirac cone and the low-energy state, which behave as two dynamically-locked electron populations. We discuss the origin of this behavior by comparing the relaxation times observed for electrons with opposite spins to the ones obtained from a microscopic Boltzmann model of ultrafast band cooling introduced into the photoemission calculations. Our results demonstrate that the nonequilibrium surface dynamics is governed by electron-electron rather than electron-phonon scattering, with a characteristic time scale unambiguously determined by the complex spin texture of excited states above the Fermi level. Our findings reveal the critical importance of detecting momentum and energy-resolved spin textures with fs resolution to fully understand the sub-ps dynamics of transient electrons on the surface of topological insulators.

cond-mat.mes-hall

Ultrafast and gigantic spin injection in semiconductors

The injection of spin currents in semiconductors is one of the big challenges of spintronics. Motivated by the ultrafast demagnetisation and spin injection into metals, we propose an alternative femtosecond route based on the laser excitation of superdiffusive spin currents in a ferromagnet such as Ni. Our calculations show that even though only a fraction of the current crosses the Ni-Si interface, the laser-induced creation of strong transient electrical fields at a ferromagnet-semiconductor interface allows for the injection of chargeless spin currents with a record spin polarisations of 80%. Beyond that they are pulsed on the time scale of 100 femtoseconds which opens the door for new experiments and ultrafast spintronics.

cond-mat.mtrl-sci

Unified picture for the colossal thermopower compound FeSb$_2$

We identify the driving mechanism of the gigantic Seebeck coefficient in FeSb$_2$ as the phonon-drag effect associated with an in-gap density of states that we demonstrate to derive from excess iron. We accurately model electronic and thermoelectric transport coefficients and explain the so far ill-understood correlation of maxima and inflection points in different response functions. Our scenario has far-reaching consequences for attempts to harvest the spectacular powerfactor of FeSb$_2$.

cond-mat.mtrl-sci

Microscopic electronic configurations after ultrafast magnetization dynamics

We provide a model for the prediction of the electronic and magnetic configurations of ferromagnetic Fe after an ultrafast decrease or increase of magnetization. The model is based on the well-grounded assumption that, after the ultrafast magnetization change, the system achieves a partial thermal equilibrium. With statistical arguments it is possible to show that the magnetic configurations are qualitatively different in the case of reduced or increased magnetization. The predicted magnetic configurations are then used to compute the dielectric response at the 3p (M) absorption edge, which can be related to the changes observed in the experimental T-MOKE data. The good qualitative agreement between theory and experiment offers a substantial support to the existence of an ultrafast increase of magnetisation, which has been fiercely debated in the last years.

cond-mat.mtrl-sci

Momentum resolved spin dynamics of bulk and surface excited states in the topological insulator $\mathrm{Bi_{2}Se_{3}}$

The prospective of optically inducing a spin polarized current for spintronic devices has generated a vast interest in the out-of-equilibrium electronic and spin structure of topological insulators (TIs). In this Letter we prove that only by measuring the spin intensity signal over several order of magnitude in spin, time and angle resolved photoemission spectroscopy (STAR-PES) experiments is it possible to comprehensively describe the optically excited electronic states in TIs materials. The experiments performed on $\mathrm{Bi_{2}Se_{3}}$ reveal the existence of a Surface-Resonance-State in the 2nd bulk band gap interpreted on the basis of fully relativistic ab-initio spin resolved photoemission calculations. Remarkably, the spin dependent relaxation of the hot carriers is well reproduced by a spin dynamics model considering two non-interacting electronic systems, derived from the excited surface and bulk states, with different electronic temperatures.

cond-mat.mtrl-sci

Ab initio theory of electron-phonon mediated ultrafast spin relaxation of laser-excited hot electrons in transition-metal ferromagnets

We report a computational theoretical investigation of electron spin-flip scattering induced by the electron-phonon interaction in the transition-metal ferromagnets bcc Fe, fcc Co and fcc Ni. The Elliott-Yafet electron-phonon spin-flip scattering is computed from first-principles, employing a generalized spin-flip Eliashberg function as well as ab initio computed phonon dispersions. Aiming at investigating the amount of electron-phonon mediated demagnetization in femtosecond laser-excited ferromagnets, the formalism is extended to treat laser-created thermalized as well as nonequilibrium, nonthermal hot electron distributions. Using the developed formalism we compute the phonon-induced spin lifetimes of hot electrons in Fe, Co, and Ni. The electron-phonon mediated demagnetization rate is evaluated for laser-created thermalized and nonequilibrium electron distributions. Nonthermal distributions are found to lead to a stronger demagnetization rate than hot, thermalized distributions, yet their demagnetizing effect is not enough to explain the experimentally observed demagnetization occurring in the subpicosecond regime.

cond-mat.mes-hall

Engineering ultrafast spin currents and terahertz transients by magnetic heterostructures

In spin-based electronics, information is encoded by the spin state of electron bunches. Processing this information requires the controlled transport of spin angular momentum through a solid, preferably at frequencies reaching the so far unexplored terahertz (THz) regime. Here, we demonstrate, by experiment and theory, that the temporal shape of femtosecond spin-current bursts can be manipulated by using specifically designed magnetic heterostructures. A laser pulse is employed to drive spins from a ferromagnetic Fe thin film into a nonmagnetic cap layer that has either low (Ru) or high (Au) electron mobility. The resulting transient spin current is detected by means of an ultrafast, contactless amperemeter based on the inverse spin Hall effect that converts the spin flow into a THz electromagnetic pulse. We find that the Ru cap layer yields a considerably longer spin-current pulse because electrons are injected in Ru d states that have a much smaller mobility than Au sp states. Thus, spin current pulses and the resulting THz transients can be shaped by tailoring magnetic heterostructures, which opens the door for engineering high-speed spintronic devices as well as broadband THz emitters in particular covering the elusive range from 5 to 10THz.

cond-mat.mes-hall

Ab initio investigation of Elliott-Yafet electron-phonon mechanism in laser-induced ultrafast demagnetization

The spin-flip (SF) Eliashberg function is calculated from first-principles for ferromagnetic Ni to accurately establish the contribution of Elliott-Yafet electron-phonon SF scattering to Ni's femtosecond laser-driven demagnetization. This is used to compute the SF probability and demagnetization rate for laser-created thermalized as well as non-equilibrium electron distributions. Increased SF probabilities are found for thermalized electrons, but the induced demagnetization rate is extremely small. A larger demagnetization rate is obtained for {non-equilibrium} electron distributions, but its contribution is too small to account for femtosecond demagnetization.

cond-mat.mes-hall