arXiv subjects

Pablo Maldonado

Publications and source records attributed to Pablo Maldonado.

16 recordsLinked to original sources

arXiv2023

Real-time observation of phonon-electron energy and angular momentum flow in laser-heated nickel

Identifying the microscopic nature of non-equilibrium energy transfer mechanisms among electronic, spin and lattice degrees of freedom is central for understanding ultrafast phenomena such as manipulating magnetism on the femtosecond timescale. Here we use time and angle-resolved photoemission spectroscopy to go beyond the often-employed ensemble-averaged view of non-equilibrium dynamics in terms of quasiparticle temperature evolutions. We show for ferromagnetic Ni that the non-equilibrium electron and spin dynamics display pronounced variations with electron momentum whereas the magnetic exchange interaction remains isotropic. This highlights the influence of lattice-mediated scattering processes and opens a pathway towards unraveling the still elusive microscopic mechanism of spin-lattice angular momentum transfer.

cond-mat.mtrl-sci↗

arXiv2022

Theory of superdiffusive spin transport in noncollinear magnetic multilayers

Ultrafast demagnetization induced by femtosecond laser pulses in thin metallic layers is caused by the outflow of spin-polarized hot electron currents describable by the superdiffusive transport model. These laser-generated spin currents can cross the interface into another magnetic layer and give rise to magnetization dynamics in magnetic spin valves with noncollinear magnetizations. To describe ultrafast transport and spin dynamics in such nanostructures we develop here the superdiffusive theory for general noncollinear magnetic multilayers. Specifically, we introduce an Al/Ni/Ru/Fe/Ru multilayer system with noncollinear Ni and Fe magnetic moments and analyze how the ultrafast demagnetization and spin-transfer torque depend on the noncollinearity. We employ ab initio calculations to compute the spin- and energy-dependent transmissions of hot electrons at the interfaces of the multilayer. Taking into account multiple electron scattering at interfaces and spin mixing in the spacer layer we find that the laser-induced demagnetization of the Ni layer and magnetization change of the Fe layer strongly depend on the angle between their magnetizations. Similarly, the spin-transfer torques on the Ni and Fe layers and the total spin momentum absorbed in the Ni and Fe layer are found to vary markedly with the amount of noncollinearity. These results suggest that changing the amount of noncollinearity in magnetic multilayers one can efficiently control the hot electron spin transport, which may open a way toward achieving fast, laser-driven spintronic devices.

cond-mat.mes-hall↗

arXiv2019

Theory of out-of-equilibrium electron and phonon dynamics in metals after ultrafast laser excitation

The out-of-equilibrium dynamics of electrons and phonons upon laser excitation are often described by the two-temperature model, which assumes that both subsystems are separately in thermal equilibrium. However, recent experiments show that this description is not sufficient to describe the out-of-equilibrium dynamics on ultrashort timescales. Here, we extend and apply a parameter-free microscopic out-of-equilibrium model to describe the ultrafast laser-induced system dynamics of archetypical metallic systems such as gold, aluminum, iron, nickel, and cobalt. We report strong deviations from the two-temperature model on the picosecond timescale for all the materials studied, even for those where the assumption of separate thermal equilibriums seemed less restrictive, like in gold. Furthermore, we demonstrate the importance of the phonon-mode dependent electron-phonon coupling for the relaxation process and reveal the significance of this channel in the lattice equilibration through an indirect coupling between phonons via the electronic system.

cond-mat.mtrl-sci↗

arXiv2019

High-frequency magnon excitation due to femtosecond spin-transfer torques

Femtosecond laser pulses can induce ultrafast demagnetization as well as generate bursts of hot electron spin currents. In trilayer spin valves consisting of two metallic ferromagnetic layers separated by a nonmagnetic one, hot electron spin currents excited by an ultrashort laser pulse propagate from the first ferromagnetic layer through the spacer reaching the second magnetic layer. When the magnetizations of the two magnetic layers are noncollinear, this spin current exerts a torque on magnetic moments in the second ferromagnet. Since this torque is acting only within the sub-ps timescale, it excites coherent high-frequency magnons as recently demonstrated in experiments. Here, we calculate the temporal shape of the hot electron spin currents using the superdiffusive transport model and simulate the response of the magnetic system to the resulting ultrashort spin-transfer torque pulse by means of atomistic spin-dynamics simulations. Our results confirm that the acting spin-current pulse is short enough to excite magnons with frequencies beyond 1 THz, a frequency range out of reach for current induced spin-transfer torques. We demonstrate the formation of thickness dependent standing spin waves during the first picoseconds after laser excitation. In addition, we vary the penetration depth of the spin-transfer torque to reveal its influence on the excited magnons. Our simulations clearly show a suppression effect of magnons with short wavelengths already for penetration depths in the range of 1 nm confirming experimental findings reporting penetration depths below $2\, {\rm nm}$.

cond-mat.mtrl-sci↗

arXiv2019

Domain wall dynamics due to femtosecond laser-induced superdiffusive spin transport

Manipulation of magnetic domain walls via a helicity-independent laser pulse has recently been experimentally demonstrated and various physical mechanisms leading to domain wall dynamics have been discussed. Spin-dependent superdiffusive transport of hot electrons has been identified as one of the possible ways how to affect a magnetic domain wall. Here, we develop a model based on superdiffusive spin-dependent transport to study the laser-induced transport of hot electrons through a smooth magnetic domain wall. We show that the spin transfer between neighboring domains can enhance ultrafast demagnetization in the domain wall. More importantly, our calculations reveal that when the laser pulse is properly focused on to the vicinity of the domain wall, it can excite sufficiently strong spin currents to generate a spin-transfer torque that can rapidly move the magnetic domain wall by several nanometers in several hundreds of femtoseconds, leading to a huge nonequilibrium domain wall velocity.

cond-mat.mes-hall↗

arXiv2019

Coherent modulation of the electron temperature and electron-phonon couplings in a 2D material

Ultrashort light pulses can selectively excite charges, spins and phonons in materials, providing a powerful approach for manipulating their properties. Here we use femtosecond laser pulses to coherently manipulate the electron and phonon distributions, and their couplings, in the charge density wave (CDW) material 1T-TaSe$_2$. After exciting the material with a short light pulse, spatial smearing of the electrons launches a coherent lattice breathing mode, which in turn modulates the electron temperature. This indicates a bi-directional energy exchange between the electrons and the strongly-coupled phonons. By tuning the laser excitation fluence, we can control the magnitude of the electron temperature modulation, from ~ 200 K in the case of weak excitation, to ~ 1000 K for strong laser excitation. This is accompanied by a switching of the dominant mechanism from anharmonic phonon-phonon coupling to coherent electron-phonon coupling, as manifested by a phase change of $π$ in the electron temperature modulation. Our approach thus opens up possibilities for coherently manipulating the interactions and properties of quasi-2D and other quantum materials using light.

cond-mat.mtrl-sci↗

arXiv2018

Microscopic Theory of Ultrafast Out-of-Equilibrium Dynamics in Magnetic Insulators. Unraveling the Magnon-Phonon Coupling

The interaction between lattice and spins is at the heart of an extremely intriguing ultrafast dynamics in magnetic materials. In this work we formulate a general non-equilibrium theory that disentangles the complex interplay between them in a THz laser-excited antiferromagnetic insulator. The theory provides a quantitative description of the transient energy flow between the spin and lattice sub-systems, subject to magnon-phonon and phonon-phonon scatterings, giving rise to finite life-times of the quasiparticles and to the equilibration time of the system. We predict a novel kind of scattering process where two magnons of opposite polarizations decay into a phonon, previously omitted in the literature. The theory is combined with first-principle calculations and then applied to simulate a realistic dynamics of NiO. The main relaxation channels and hot spots in the reciprocal space, giving the strongest contribution to the energy transfer between phonons and magnons are identified. The diverse interaction strengths lead to distinct coupled dynamics of the lattice and spin systems and subsequently to different equilibration timescales.

cond-mat.mtrl-sci↗

arXiv2018

Dissecting spin-phonon equilibration in ferrimagnetic insulators by ultrafast lattice excitation

To gain control over magnetic order on ultrafast time scales, a fundamental understanding of the way electron spins interact with the surrounding crystal lattice is required. However, measurement and analysis even of basic collective processes such as spin-phonon equilibration have remained challenging. Here, we directly probe the flow of energy and angular momentum in the model insulating ferrimagnet yttrium iron garnet. Following ultrafast resonant lattice excitation, we observe that magnetic order reduces on distinct time scales of 1 ps and 100 ns. Temperature-dependent measurements, a spin-coupling analysis and simulations show that the two dynamics directly reflect two stages of spin-lattice equilibration. On the 1-ps scale, spins and phonons reach quasi-equilibrium in terms of energy through phonon-induced modulation of the exchange interaction. This mechanism leads to identical demagnetization of the ferrimagnet's two spin-sublattices and a novel ferrimagnetic state of increased temperature yet unchanged total magnetization. Finally, on the much slower, 100-ns scale, the excess of spin angular momentum is released to the crystal lattice, resulting in full equilibrium. Our findings are relevant for all insulating ferrimagnets and indicate that spin manipulation by phonons, including the spin Seebeck effect, can be extended to antiferromagnets and into the terahertz frequency range.

cond-mat.mtrl-sci↗

arXiv2018

Transport theory for femtosecond laser-induced spin-transfer torques

Ultrafast demagnetization of magnetic layers pumped by a femtosecond laser pulse is accompanied by a nonthermal spin-polarized current of hot electrons. These spin currents are studied here theoretically in a spin valve with noncollinear magnetizations. To this end, we introduce an extended model of superdiffusive spin transport that enables to treat noncollinear magnetic configurations, and apply it to the perpendicular spin valve geometry. We show how spin-transfer torques arise due to this mechanism and calculate their action on the magnetization present, as well as how the latter depends on the thicknesses of the layers and other transport parameters. We demonstrate that there exists a certain optimum thickness of the out-of-plane magnetized spin-current polarizer such that the torque acting on the second magnetic layer is maximal. Moreover, we study the magnetization dynamics excited by the superdiffusive spin-transfer torque due to the flow of hot electrons employing the Landau-Lifshitz-Gilbert equation. Thereby we show that a femtosecond laser pulse applied to one magnetic layer can excite small-angle precessions of the magnetization in the second magnetic layer. We compare our calculations with recent experimental results.

cond-mat.mes-hall↗

arXiv2017

Observation of Gapless Dirac Surface States in ZrGeTe

The experimental discovery of the topological Dirac semimetal establishes a platform to search for various exotic quantum phases in real materials. ZrSiS-type materials have recently emerged as topological nodal-line semimetals where gapped Dirac-like surface states are observed. Here, we present a systematic angle-resolved photoemission spectroscopy (ARPES) study of ZrGeTe, a nonsymmorphic symmetry protected Dirac semimetal. We observe two Dirac-like gapless surface states at the same $\bar X$ point of the Brillouin zone. Our theoretical analysis and first-principles calculations reveal that these are protected by crystalline symmetry. Hence, ZrGeTe appears as a rare example of a naturally fine tuned system where the interplay between symmorphic and non-symmorphic symmetry leads to rich phenomenology, and thus opens for opportunities to investigate the physics of Dirac semimetallic and topological insulating phases realized in a single material.

cond-mat.mes-hall↗

arXiv2017

Distinct multiple fermionic states in a single topological metal

Among the quantum materials that gained interest recently are the topological Dirac/Weyl semimetals, where conduction and valence bands touch at points in reciprocal (k)-space, and the Dirac nodal-line semimetals, where these bands touch along a line or a loop in k-space. However, the coexistence of multiple fermion phases in one and the same material has not been verified yet. Using angle-resolved photoemission spectroscopy (ARPES) and first-principles electronic structure calculations, we systematically study the metallic topological quantum material, Hf2Te2P. Our investigations discover various properties that are rare and never observed in a single Dirac material. We observe the coexistence of both weak and strong topological surface states in the same material and interestingly, at the same momentum position. An one-dimensional Dirac crossing{the Dirac-node arc-along a high-symmetry direction is revealed by our first-principles calculations and confirmed by our ARPES measurements. This novel state is associated with the surface bands of a weak topological insulator protected by in-plane time-reversal invariance. Ternary compound Hf2Te2P thus emerges as an intriguing platform to study the coexistence and competition of multi-fermionic states in one material.

cond-mat.mes-hall↗

arXiv2017

Theory of Out-of-Equilibrium Ultrafast Relaxation Dynamics in Metals

Ultrafast laser excitation of a metal causes correlated, highly nonequilibrium dynamics of electronic and ionic degrees of freedom, which are however only poorly captured by the widely-used two-temperature model. Here we develop an out-of-equilibrium theory that captures the full dynamic evolution of the electronic and phononic populations and provides a microscopic description of the transfer of energy delivered optically into electrons to the lattice. All essential nonequilibrium energy processes, such as electron-phonon and phonon-phonon interactions are taken into account. Moreover, as all required quantities are obtained from first-principles calculations, the model gives an exact description of the relaxation dynamics without the need for fitted parameters. We apply the model to FePt and show that the detailed relaxation is out-of-equilibrium for picoseconds.

cond-mat.mtrl-sci↗

arXiv2017

Observation of topological nodal-line fermionic phase in GdSbTe

Topological Dirac semimetals with accidental band touching between conduction and valence bands protected by time reversal and inversion symmetry are at the frontier of modern condensed matter research. Theoretically one can get Weyl and/or nodal-line semimetals by breaking either one of them. Most of the discovered topological semimetals are nonmagnetic i.e respect time reversal symmetry. Here we report the experimental observation of a topological nodal-line semi metallic state in GdSbTe using angle-resolved photoemission spectroscopy. Our systematic study reveals the detailed electronic structure of the paramagnetic state of GdSbTe. We observe the presence of multiple Fermi surface pockets including a diamond-shape, an elliptical shape, and small circular pockets around the zone center and high symmetry M and X points of the Brillouin zone (BZ), respectively. Furthermore, we observe the presence of a Dirac-like state at the X point of the BZ. Interestingly, our experimental data shows a robust Dirac like state both below and above the magnetic transition temperature (T_N ~ 13 K). Having relatively higher transition temperature, GdSbTe provides an archetype platform to study the interaction between magnetism and topological states of matter.

cond-mat.mes-hall↗

arXiv2016

Tunability of the topological nodal-line semimetal phase in ZrSiX-type materials

The discovery of a topological nodal-line (TNL) semimetal phase in ZrSiS has invigorated the study of other members of this family. Here, we present a comparative electronic structure study of ZrSiX (where X = S, Se, Te) using angle-resolved photoemission spectroscopy (ARPES) and first-principles calculations. Our ARPES studies show that the overall electronic structure of ZrSiX materials comprises of the diamond-shaped Fermi pocket, the nearly elliptical-shaped Fermi pocket, and a small electron pocket encircling the zone center ($Γ$) point, the M point, and the X point of the Brillouin zone, respectively. We also observe a small Fermi surface pocket along the M-$Γ$-M direction in ZrSiTe, which is absent in both ZrSiS and ZrSiSe. Furthermore, our theoretical studies show a transition from nodal-line to nodeless gapped phase by tuning the chalcogenide from S to Te in these material systems. Our findings provide direct evidence for the tunability of the TNL phase in ZrSiX material systems by adjusting the spin-orbit coupling (SOC) strength via the X anion.

cond-mat.mes-hall↗

arXiv2016

Observation of Topological Nodal Fermion Semimetal Phase in ZrSiS

Unveiling new topological phases of matter is one of the current objectives in condensed matter physics. Recent experimental discoveries of Dirac and Weyl semimetals prompt to search for other exotic phases of matter. Here we present a systematic angle-resolved photoemission spectroscopy (ARPES) study of ZrSiS, a prime topological nodal semimetal candidate. Our wider Brillouin zone (BZ) mapping shows multiple Fermi surface pockets such as the diamond-shaped Fermi surface, ellipsoidal-shaped Fermi surface, and a small electron pocket encircling at the zone center (G) point, the M point and the X point of the BZ, respectively. We experimentally establish the spinless nodal fermion semimetal phase in ZrSiS, which is supported by our first-principles calculations. Our findings evidence that the ZrSiS-type of material family is a new platform to explore exotic states of quantum matter, while these materials are expected to provide an avenue for engineering two-dimensional topological insulator systems.

cond-mat.mes-hall↗

arXiv2015

Magnetic-Field-Induced Odd-Frequency Superconductivity in MgB$_2$

In all known superconductors the pairing of fermions is not sensitive to the sign of their time-argument difference, leading to a Cooper pair wavefunction that is even in time/frequency. Four decades ago it was suggested that odd-frequency superconductivity should in principle be realizable. However, observation of odd-frequency superconductivity in bulk materials has remained elusive. Solving the field-dependent anisotropic Eliashberg equations, we present \textit{ab initio} evidence for the emergence of odd-frequency pairing under an applied magnetic field in the archetypal superconductor MgB$_2$. We provide the full momentum, frequency and spin resolved dependence and magnetic field-temperature phase diagrams of the even and odd-frequency superconducting pair amplitudes and predict fingerprints of the odd-frequency state in tunnelling experiments.

cond-mat.supr-con↗