arXiv subjects

P. Elliott

Publications and source records attributed to P. Elliott.

At least 19 recordsLinked to original sources

arXiv2022

Electronic origin of x-ray absorption peak shifts

Encoded in the transient x-ray absorption (XAS) and magnetic circular (MCD) response functions resides a wealth of information of the microscopic processes of ultrafast demagnetisation. Employing state of the art first principles dynamical simulations we show that the experimentally observed energy shift of the L3 XAS peak in Ni, and the absence of a corresponding shift in the dichroic MCD response, can be explained in terms of laser induced changes in band occupation. Strikingly, we predict that for the same ultrashort pump pulse applied to Co the opposite effect will occur: a substantial shift upwards in energy of the MCD peaks will be accompanied by very small change in the position of XAS peaks, a fact we relate to the reduced $d$-band filling of Co that allows a greater energetic range above the Fermi energy into which charge can be excited. We also carefully elucidate the dependence of this effect on pump pulse parameters. These findings (i) establish a electronic origin for early time peak shifts in transient XAS and MCD spectroscopy and (ii) illustrate the rich information that may be extracted from transient response functions of the underlying dynamical system.

cond-mat.mtrl-sci↗

arXiv2022

Transient spin injection efficiencies at ferromagnet/metal interfaces

Spin injection across interfaces driven by ultrashort optical pulses on femtosecond timescales constitutes a new way to design spintronics applications. Targeted utilization of this phenomenon requires knowledge of the efficiency of non-equilibrium spin injection. From a quantitative comparison of ab-initio time-dependent density functional theory and interface-sensitive, time-resolved non-linear optical experiment, we determine the spin injection efficiencies (SIE) across ferromagnetic/metal interfaces and discuss their microscopic origin, i.e. the influence of spin-orbit coupling and the interface electronic structure. Moreover, we find that the SIE can be optimized through laser pulse and materials parameters, namely the fluence, pulse duration, and substrate material.

cond-mat.mtrl-sci↗

arXiv2022

The Giant Spin Hall Effect at Optical Frequencies

We generalize the spin Hall angle to laser pulses of finite frequencies in the linear response regime and predict a giant optical spin Hall effect. Namely, for certain transition metal elements, at particular frequencies, the spin current can be a significant fraction of the charge current, and even exceed it for XUV frequencies. By maximizing spin current while minimizing the charge current, we thus minimize a major source of heating in spintronic devices. We employ {\it ab-initio} time-dependent density functional theory (TDDFT), and with real-time simulations calculate the conductivity and transverse spin conductivity for all $3$d, $4$d, and $5$d transition metals for frequencies up to $50$ eV. In the XUV frequency range we find values greater than $1$ for the spin Hall angle, indicating spin currents larger than the charge current can be generated.

cond-mat.mes-hall↗

arXiv2022

Making a case for femto- phono- magnetism with FePt

In the field of femtomagnetism magnetic matter is controlled by ultrafast laser pulses; here we show that coupling phonon excitations of the nuclei to spin and charge leads to femto-phono-magnetism, a powerful route to control magnetic order at ultrafast times. With state-of-the-art theoretical simulations of coupled spin-, charge-, and lattice-dynamics we identify strong non-adiabatic spin-phonon coupled modes that dominate early time spin dynamics. Activating these phonon modes we show leads to an additional (up to 40\% extra) loss of moment in FePt occurring within 40 femtoseconds of the pump laser pulse. Underpinning this enhanced ultrafast loss of spin moment we identify a physical mechanism in which minority spin-current drives an enhanced inter-site minority charge transfer, in turn promoting increased on-site spin flips. Our finding demonstrates that the nuclear system, often assumed to play only the role of an energy sink aiding long time re-magnetisation of the spin system, can play a profound role in controlling femtosecond spin-dynamics in materials.

cond-mat.mtrl-sci↗

arXiv2022

Valley control by linearly polarized laser pulses

Underpinning the field of "valleytronics" is the coupling of the helicity of circularly polarized light to the valley degree of freedom, and this remains the only known lightform to exhibit this remarkable effect. Here we show that on femtosecond time scales valley coupling is a much more general effect. We find that two time separated linearly polarized pulses allow almost complete control over valley excitation, with the pulse time difference and polarization vectors emerging as key parameters for valley control. In contrast to the Berry curvature that underpins the effect for circularly polarized light, we demonstrate that a different phase structure drives this effect, with excitations during each linear pulse acquiring a valley discriminating phase involving the polarisation angle of linear light. Unimportant in a single linear pulse, for pairs of pulses these can constructively and destructively interfere. Employing state-of-the-art time dependent density function theory, we show that the effect is robust to the complexities of charge dynamics in a real material with the example of a transitional metal dichalcogenide.

physics.optics↗

arXiv2021

Ab-initio study of ultrafast spin dynamics in Gdx(FeCo){1-x} alloys

Using an ultrashort laser pulse we explore {\it ab-initio} the spin dynamics of Gd$_x$(FeCo)$_{1-x}$ at femtosecond time scales. Optical excitations are found to drive charge from Fe majority $d$-states to the unoccupied Gd $f$-minority states, with $f$-electron character excited occupation lagging behind that of the $d$-electron character, leading to substantial demagnetisation of both species while leaving the global moment almost unchanged. For $x > 0.33$ this results in the creation of an ultrafast ferromagnetic (FM) transient by the end of the laser pulse, with the Gd demagnetization rate slower than that of Fe. For all concentrations the Gd moments begin to rotate from their ground state orientations developing in-plane moments of between 0.2-0.5~$\mu_B$. Thus, the ultrafast spin dynamics of the material captures three important ingredients of the all optical switching that occurs at much later (picosecond) times: (i) the development of a FM transient, (ii) the different rates of demagnetisation of Fe and Gd and, (iii), the breaking of the colinear symmetry of the ground state. Furthermore, several predictions are made about the behaviour of Fe-Gd alloys that can be experimentally tested and can lead to a spin-filtering device.

cond-mat.mtrl-sci↗

arXiv2021

Probing the energy conversion pathways between light, carriers and lattice in real time with attosecond core-level spectroscopy

Detection of the energy conversion pathways, between photons, charge carriers, and the lattice is of fundamental importance to understand fundamental physics and to advance materials and devices. Yet, such insight remains incomplete due to experimental challenges in disentangling the various signatures on overlapping time scales. Here, we show that attosecond core-level X-ray spectroscopy can identify these interactions with attosecond precision and across a picosecond range. We demonstrate this methodology on graphite since its investigation is complicated by a variety of mechanisms occurring across a wide range of temporal scales. Our methodology reveals, through the simultaneous real-time detection of electrons and holes, the different dephasing mechanisms for each carrier type dependent on excitation with few-cycle-duration light fields. These results demonstrate the general ability of our methodology to detect and distinguish the various dynamic contributions to the flow of energy inside materials on their native time scales.

cond-mat.mtrl-sci↗

arXiv2021

Numerical analysis of XMCD sum rules at the $L$-edge: when do they fail?

In the highly non-equilibrium conditions of laser induced spin dynamics magnetic moments can only be obtained from the spectral information, most commonly from the spectroscopy of semi-core states using the so-called x-ray magnetic circular dichroism (XMCD) sum rules. The validity of the these sum rules in tracking femtosecond spin dynamics remains, however, an open question. Employing the time dependent extension of density functional theory (TD-DFT) we compare spectroscopically obtained moments with those directly calculated from the TD-DFT densities. We find that for experimentally typical pump pulses these two very distinct routes to the spin moment are, for Co and Ni, in excellent agreement, validating the experimental approach. However, for short and intense pulses or high fluence pulses of long duration the XMCD sum rules fail, with errors exceeding 50\%. This failure persists only during the pulse and occurs when the pump pulse excites charge out of the $d$-band and into $sp$-character bands, invalidating the semi-core to $d$-state transitions assumed by the XMCD sum rules.

cond-mat.mtrl-sci↗

arXiv2020

Where does the spin angular momentum go in laser induced demagnetisation?

The dynamics of ultrafast demagnetisation in 3$d$ magnets is complicated by the presence of both spin ${\v S}$ and orbital ${\v L}$ angular momentum, with the microscopic mechanism by which the magnetic moment is redistributed to the lattice, and at what time scales, yet to be resolved. Employing state-of-the-art time dependent density function theory we disentangle the dynamics of these two momenta. Utilising ultra short (5~fs) pulses that separate spin-orbit (SO) and direct optical excitation time scales, we demonstrate a two-step microscopic mechanism: (i) an initial loss of ${\v L}$ due to laser excitation, followed post pulse by (ii) an increase of ${\v L}$ as ${\v S}$ transfers to ${\v L}$ during subsequent ($> 15$~fs) SO induced spin-flip demagnetisation. We also show that to see an unambiguous transfer of ${\v S}$ to ${\v L}$ a short pulse is required.

cond-mat.mtrl-sci↗

arXiv2020

Ultrafast optical control over spin and momentum in solids

The coupling of laser light to matter can exert sub-cycle coherent control over material properties, with optically induced currents and magnetism shown to be controllable on ultrafast femtosecond time scales. Here, by employing laser light consisting of both linear and circular pulses, we show that charge of specified spin and crystal momentum can be created with precision throughout the first Brillouin zone. Our hybrid pulses induce in a controlled way both adiabatic intraband motion as well as vertical interband excitation between valence and conduction bands, and require only a gapped spin split valley structure for their implementation. This scenario is commonly found in the 2d semi-conductors, and we demonstrate our approach with monolayer WSe$_2$. We thus establish a route from laser light to local control over excitations in reciprocal space, opening the way to the preparation of momenta specified excited states at ultrafast time scales.

physics.optics↗

arXiv2020

Ab-intio study of ultrafast charge dynamics in graphene

Monolayer graphene provides an ideal material to explore one of the fundamental light-field driven interference effects: Landau-Zener-St\"uckelberg interference. However, direct observation of the resulting interference patterns in momentum space has not proven possible, with Landau-Zener-St\"uckelberg interference observed only indirectly through optically induced residual currents. Here we show that the transient electron momentum density (EMD), an object that can easily be obtained in experiment, provides an excellent description of momentum resolved charge excitation. We employ state-of-the-art time-dependent density function theory calculations, demonstrating by direct comparison of EMD with conduction band occupancy, obtained from projecting the time propagated wavefunction onto the ground state, that the two quantities are in excellent agreement. For even the most intense laser pulses we find that the electron dynamics to be almost completely dominated by the $\pi$-band, with transitions to other bands strongly suppressed. Simple model based tight-binding approaches can thus be expected to provide an excellent description for the laser induced electron dynamics in graphene.

cond-mat.mes-hall↗

arXiv2020

Search for associations containing young stars (SACY) VIII. An updated census of spectroscopic binary systems showing hints of non-universal multiplicity among these associations

We seek to update the spectroscopy binary fraction of the SACY (Search for Associations Containing Young stars) sample taking in consideration all possible biases in our identification of binary candidates, such as activity and rotation. Using high-resolution spectroscopic observations we have produced $\sim$1300 cross-correlation functions (CCFs) to disentangle the previously mentioned sources of contamination. The radial velocity values obtained were cross-matched with the literature and were used to revise and update the spectroscopic binary (SB) fraction in each of the SACY association. In order to better describe the CCF profile, we calculated a set of high-order cross-correlation features to determine the origin of the variations in radial velocities. We identified 68 SB candidates from our sample of 410 objects. Our results hint that the youngest associations have a higher SB fraction. Specifically, we found sensitivity-corrected SB fractions of $22 \substack{+15 \\ -11} \%$ for $\epsilon$~Cha , $31 \substack{+16 \\ -14} \%$ for TW Hya and $32 \substack{+9 \\ -8} \%$ for $\beta$~Pictoris, in contrast with the five oldest ($\sim 35-125$ Myr) associations we have sampled which are $\sim 10\%$ or lower. This result seems independent of the methodology used to asses membership to the associations. The new CCF analysis, radial velocity estimates and SB candidates are particularly relevant for membership revision of targets in young stellar associations. These targets would be ideal candidates for follow-up campaigns using high-resolution techniques in order to confirm binarity, resolve the orbits, and ideally calculate dynamical masses. Additionally, if the results on SB fraction in the youngest associations are confirmed, it could hint of non-universal multiplicity among SACY associations.

astro-ph.SR↗

arXiv2019

Element specificity of transient extreme ultra-violet magnetic dichroism

In this work we combine theory and experiment to study transient magnetic circular dichroism (tr-MCD) in the extreme ultraviolet spectral range (XUV) in bulk Co and CoPt. We use the \emph{ab-initio} method of real-time time-dependent density functional theory (RT-TDDFT) to simulate the magnetization dynamics in the presence of ultrafast laser pulses. From this we demonstrate how tr-MCD may be calculated using an approximation to the excited-state linear-response. We apply this approximation to Co and CoPt and show computationally that element-specific dynamics of the local spin moments can be extracted from the tr-MCD in XUV energy range, as is commonly assumed. We then compare our theoretical prediction for the tr-MCD for CoPt with experimental measurement and find excellent agreement at many different frequencies including the $M_{2 3}$-edge of Co and $N_{6 7}$- and $O_{2 3}$- edges of Pt.

cond-mat.mtrl-sci↗

arXiv2019

Control of magnons via ultrafast magnetization modulation

We demonstrate optical control of magnons using femtosecond laser pulses by performing ab-initio real-time time-dependent density functional theory (TDDFT) simulations. We predict that the spin-wave dynamics in Fe$_{50}$Ni$_{50}$ can be manipulated by tailoring the applied laser pulse via three distinct mechanisms: (1) element selective destruction of magnon modes depending on the laser intensity, (2) delay dependent freezing of the magnon mode into a transient non-collinear state (where delay is in the pulse peak with respect to the start of simulations), and (3) optically induced inter sublattice transfer (OISTR) driven renormalization of the optical magnon frequency. Harnessing such processes would significantly speed up magnonic devices.

cond-mat.mtrl-sci↗

arXiv2018

The generalized gradient approximation kernel in time-dependent density functional theory

A complete understanding of a material requires both knowledge of the excited states as well as of the ground state. In particular, the low energy excitations are of utmost importance while studying the electronic, magnetic, dynamical, and thermodynamical properties of the material. Time-Dependent Density Functional Theory (TDDFT), within the linear regime, is a successful \textit{ab-initio} method to access the electronic charge and spin excitations. However, it requires an approximation to the exchange-correlation (XC) kernel which encapsulates the effect of electron-electron interactions in the many-body system. In this work we derive and implement the spin-polarized XC kernel for semi-local approximations such as the adiabatic Generalized Gradient Approximation (AGGA). This kernel has a quadratic dependence on the wavevector, {\bf q}, of the perturbation, however the impact of this on the electron energy loss spectra (EELS) is small. Although the GGA functional is good in predicting structural properties, it generality overestimates the exchange spin-splitting. This leads to higher magnon energies, as compared to both ALDA and experiment. In addition, interaction with the Stoner spin-flip continuum is enhanced by AGGA, which strongly suppresses the intensity of spin-waves.

cond-mat.mtrl-sci↗

arXiv2018

Competing spin transfer and dissipation at Co/Cu(001) interfaces on femtosecond timescales

By combining interface-sensitive non-linear magneto-optical experiments with femtosecond time resolution and ab-initio time-dependent density functional theory, we show that optically excited spin dynamics at Co/Cu(001) interfaces proceeds via spin-dependent charge transfer and backtransfer between Co and Cu. This ultrafast spin transfer competes with dissipation of spin angular momentum mediated by spin-orbit coupling already on sub 100 fs timescales. We thereby identify the fundamental microscopic processes during laser-induced spin transfer at a model interface for technologically relevant ferromagnetic heterostructures.

cond-mat.mtrl-sci↗

arXiv2017

A deep staring campaign in the Sigma Orionis cluster. Variability in substellar members

Deep optical imaging is used to study time-domain properties of young brown dwarfs in sigma Orionis over typical rotational time-scales and to search for new substellar and planetary-mass cluster members. We used VIMOS at the VLT to monitor a 24 arcmin x 16 arcmin field in the I-band. Using the individual images from this run we investigated the photometric time series of nine substellar cluster members with masses from 10 to 60 Mj. The deep stacked image shows cluster members down to $\approx$ 5 Mj. We search for new planetary mass objects by combining our deep I-band photometry with public J-band magnitudes and by examining the nearby environment of known very low mass members for possible companions. We find two brown dwarfs, with significantly variable, aperiodic light curves, both with masses around 50 Mj, one of which was previously unknown to be variable. The physical mechanism responsible for the observed variability is likely different for the two objects. The variability of the first object, a single-lined spectroscopic binary, is most likely linked to its accretion disc, the second may be caused by variable extinction by large grains. We find five new candidate members from the colour-magnitude diagram and three from a search for companions within 2000 au. We rule all eight sources out as potential members based on non-stellar shape and/or infrared colours. The I-band photometry is made available as a public dataset. We present two variable brown dwarfs. One is consistent with ongoing accretion, the other, exhibiting apparent transient variability without presence of an accretion disc. Our analysis confirms the existing census of substellar cluster members down to $\approx$ 7 Mj. The zero result from our companion search agrees with the low occurrence rate of wide companions to brown dwarfs found in other works.

astro-ph.SR↗

arXiv2017

Role of Spin Flips versus Spin Transport in Non Thermal 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. Experimentally dynamics of spins is studied by determining the time-dependent amplitude of the Voigt vector and theoretically ab-initio calculations are performed using time-dependent density functional theory. We demonstrate that overall spin-orbit induced spin-flips are the most significant contributors with super-diffusive spin transport playing very limited to no role. Our study highlights the material dependent nature of the demagnetization during the process of thermalization of non-equilibrium spins.

cond-mat.mtrl-sci↗