arXiv subjects

Thomas F. George

Publications and source records attributed to Thomas F. George.

At least 19 recordsLinked to original sources

arXiv2025

Nonlinear optical quantum theory of demagnetization in L1$_0$ FePt and FePd

It is now well established that a laser pulse can demagnetize a ferromagnet. However, for a long time, it has not had an analytic theory because it falls into neither nonlinear optics (NLO) nor magnetism. Here we attempt to fill this gap by developing a nonlinear optical theory centered on the spin moment, instead of the more popular susceptibility. We first employ group theory to pin down the lowest order of the nonzero spin moment in a centrosymmetric system to be the second order, where the second-order density matrix contains four terms of sum frequency generation (SFG) and four terms of difference frequency generation (DFG). By tracing over the product of the density matrix and the spin matrix, we are now able to compute the light-induced spin moment. We apply our theory to FePt and FePd, two most popular magnetic recording materials with identical crystal and electronic structures. We find that the theory can clearly distinguish the difference between those two similar systems. Specifically, we show that FePt has a stronger light-induced spin moment than FePd, in agreement with our real-time ultrafast demagnetization simulation and the experimental results. Among all the possible NLO processes, DFGs produce the largest spin moment change, a manifestation of optical rectification. Our research lays a solid theoretical foundation for femtomagnetism, so the light-induced spin moment reduction can now be computed and compared among different systems, without time-consuming real-time calculations, representing a significant step forward.

cond-mat.mtrl-sci↗

arXiv2024

Gateway to all-optical spin switching in Heusler ferrimagnets: Pancharatnam-Berry tensor and magnetic moment ratio

All-optical spin switching (AOS) is a new phenomenon found in a small group of magnetic media, where a single laser pulse can switch spins from one direction to another, without assistance of a magnetic field, on a time scale much shorter than existing magnetic technology. However, despite intensive efforts over a decade, its underlying working principle remains elusive. Here through manganese-based Heusler ferrimagnets, we show that a group of flat bands around the Fermi level act as gateway states to form efficient channels or spin switching, where their noncentrosymmetry allows us to correlate the spin dynamics to the second-order optical response. To quantify their efficacy, we introduce the third-rank Pancharatnam-Berry tensor (PB tensor), $\boldsymbolη^{(3)}=\langle i |{\bf p} |m\rangle \langle m|{\bf p} |f\rangle \langle f|{\bf p} |i\rangle,$ where $|i\rangle$, $|m\rangle$ and $|f\rangle$ are initial, intermediate and final band states, respectively, and ${\bf p}$ is the momentum operator. A picture emerges: Those which show AOS, such as the recently discovered Mn$_2$RuGa, always have a large PB tensor element} but have a small sublattice spin moment ratio, consistent with the prior experimental small remanence criterion. This does not only reveal that the delicate balance between the large PB tensor element and the small sublattice spin ratio plays a decisive role in AOS, but also, conceptually, connects the $n$th-order nonlinear optics to $(n+1)$th-rank PB tensors in general.

cond-mat.mtrl-sci↗

arXiv2022

Spin-phonon dispersion in magnetic materials

Microscopic coupling between the electron spin and the lattice vibration is responsible for an array of exotic properties from morphic effects in simple magnets to magnetodielectric coupling in multiferroic spinels and hematites. Traditionally, a single spin-phonon coupling constant is used to characterize how effectively the lattice can affect the spin, but it is hardly enough to capture novel electromagnetic behaviors to the full extent. Here, we introduce a concept of spin-phonon dispersion to project the spin moment change along the phonon crystal momentum direction, so the entire spin change can be mapped out. Different from the phonon dispersion, the spin-phonon dispersion has both positive and negative frequency branches {even in the equilibrium ground state}, which correspond to the spin enhancement and spin reduction, respectively. Our study of bcc Fe and hcp Co reveals that the spin force matrix, that is, the second-order spatial derivative of spin moment, is similar to the vibrational force matrix, but its diagonal elements are smaller than the off-diagonal ones. This leads to the distinctive spin-phonon dispersion. The concept of spin-phonon dispersion expands the traditional Elliott-Yafet theory in nonmagnetic materials to the entire Brillouin zone in magnetic materials, thus opening the door to excited states in systems such as CoF$_2$ and NiO, where a strong spin-lattice coupling is detected in the THz regime.

cond-mat.mtrl-sci↗

arXiv2022

First-principles insights into all-optical spin switching in the half-metallic Heusler ferrimagnet Mn$_2$RuGa

All-optical spin switching (AOS) represents a new frontier in magnetic storage technology -- spin manipulation without a magnetic field, -- but its underlying working principle is not well understood. Many AOS ferrimagnets such as GdFeCo are amorphous and renders the high-level first-principles study unfeasible. The crystalline half-metallic Heusler Mn$_2$RuGa presents an opportunity. Here we carry out hitherto the comprehensive density functional investigation into the material properties of Mn$_2$RuGa, and introduce two concepts - the spin anchor site and the optical active site - as two pillars for AOS in ferrimagnets. In Mn$_2$RuGa, Mn$(4a)$ serves as the spin anchor site, whose band structure is below the Fermi level and has a strong spin moment, while Mn$(4c)$ is the optical active site whose band crosses the Fermi level. Our magneto-optical Kerr spectrum and band structure calculation jointly reveal that the delicate competition between the Ru-$4d$ and Ga-$4p$ states is responsible for the creation of these two sites. These two sites found here not only present a unified picture for both Mn$_2$RuGa and GdFeCo, but also open the door for the future applications. Specifically, we propose a Mn$_2$Ru$_x$Ga-based magnetic tunnel junction where a single laser pulse can control magnetoresistance.

cond-mat.mtrl-sci↗

arXiv2021

Optically- and thermally-driven huge lattice orbital and spin angular momenta from spinning fullerenes

Lattice vibration in solids may carry angular momentum. But unlike the intrinsic spin of electrons, the lattice vibration is rarely rotational. To induce angular momentum, one needs to find a material that can accommodate a twisted normal mode, two orthogonal modes or excitation of magnons. If excitation is too strong, one may exceed the Lindemann limit, so the material melts. Therefore these methods are not ideal. Here, we theoretically propose a new route to phonon angular momentum in a molecular crystal $\rm C_{60}$. We find that a single laser pulse is able to inject a significant amount of angular momentum to $\rm C_{60}$, and the momentum transfer is helicity-dependent. Changing from right-circularly polarized light to left-circularly polarized light switches the direction of phonon angular momentum. On the ultrafast time scale, the orbital angular momentum change closely resembles the displacive excitation of coherent phonons, with a cosine-function dependence on time, different from the spin counterpart. Atomic displacements, even under strong laser excitation, remain far below the Lindemann criterion. Under thermal excitation, spinning $\rm C_{60}$ even at room temperature generates a huge angular momentum close to several hundred $\hbar$. Our finding opens the door to a large group of fullerenes, from $\rm C_{60}$, C$_{70}$ to their endohedral derivatives, where angular momentum can be generated through light or temperature. This paves the way to the phononic control electronic spin and harvesting thermal energy through phonon angular momentum.

cond-mat.mtrl-sci↗

arXiv2021

Correlation Between Spin and Orbital Dynamics During Laser-Induced Femtosecond Demagnetization

Spin and orbital angular momenta are two intrinsic properties of an electron and are responsible for the physics of a solid. How the spin and orbital evolve with respect to each other on several hundred femtoseconds is largely unknown, but it is at the center of laser-induced ultrafast demagnetization. In this paper, we introduce a concept of the spin-orbital correlation diagram, where spin angular momentum is plotted against orbital angular momentum, much like the position-velocity phase diagram in classical mechanics. We use four sets of highly accurate time-resolved x-ray magnetic circular dichroism (TR-XMCD) data to construct four correlation diagrams for iron and cobalt. To our surprise, a pattern emerges. The trace on the correlation diagram for iron is an arc, and at the end of demagnetization, it has a pronounced cusp. The correlation diagram for cobalt is different and appears more linear, but with kinks. We carry out first-principles calculations with two different methods: time-dependent density functional theory (TDDFT) and time-dependent Liouville density functional theory (TDLDFT). These two methods agree that the experimental findings for both Fe and Co are not due t experimental errors. It is the spin-orbit coupling that correlates the spin dynamics to the orbital dynamics.Microscopically, Fe and Co have different orbital occupations, which leads to distinctive correlation diagrams. We believe that this correlation diagram presents a useful tool to better understand spin and orbital dynamics on an ultrafast time scale. A brief discussion on the magnetic anisotropy energy is also provided.

cond-mat.mtrl-sci↗

arXiv2021

Spin Berry points as crucial for ultrafast demagnetization

Laser-induced ultrafast demagnetization has puzzled researchers around the world for over two decades. Intrinsic complexity in electronic, magnetic, and phononic subsystems is difficult to understand microscopically. So far it is not possible to explain demagnetization using a single mechanism, which suggests a crucial piece of information still missing. In this paper, we return to a fundamental aspect of physics: spin and its change within each band in the entire Brillouin zone. We employ fcc Ni as an example and use an extremely dense {\bf k} mesh to map out spin changes for every band close to the Fermi level along all the high symmetry lines. To our surprise, spin angular momentum at some special {\bf k} points abruptly changes from $\pm \hbar/2$ to $\mp \hbar/2$ simply by moving from one crystal momentum point to the next. This explains why intraband transitions, which the spin superdiffusion model is based upon, can induce a sharp spin moment reduction, and why electric current can change spin orientation in spintronics. These special {\bf k} points, which are called spin Berry points, are not random and appear when several bands are close to each other, so the Berry potential of spin majority states is different from that of spin minority states. Although within a single band, spin Berry points jump, when we group several neighboring bands together, they form distinctive smooth spin Berry lines. It is the band structure that disrupts those lines. Spin Berry points are crucial to laser-induced ultrafast demagnetization and spintronics.

cond-mat.mtrl-sci↗

arXiv2021

External light control of three-dimensional ultrashort far-infrared pulses in an inhomogeneous array of carbon nanotubes

We present a study of the propagation of three-dimensional (3D) bipolar electromagnetic ultrashort pulses in an inhomogeneous array of semiconductor carbon nanotubes (CNTs) in the presence of a control high-frequency (HF) electric field. The inhomogeneity is present in the form of a layer with an increased concentration of conduction electrons, which acts as a barrier for the propagation of ultrashort electromagnetic pulses through the CNT array. The dynamics of the pulse is described by a nonlinear equation for the vector potential of the electromagnetic field (it takes the form of a 3D generalization of the sine-Gordon equation), derived from the Maxwell's equations and averaged over the period of the HF control field. By means of systematic simulations, we demonstrate that, depending on the amplitude and frequency of the HF control, the ultrashort pulse approaching the barrier layer either passes it or bounces back. The layer's transmissivity for the incident pulse is significantly affected by the amplitude and frequency of the HF control field, with the reflection coefficient nearly vanishing in intervals that make up a discrete set of transparency windows, which resembles the effect of the electromagnetically-induced transparency. Having passed the barrier, the ultrashort pulse continues to propagate, keeping its spatiotemporal integrity. The results may be used for the design of soliton valves, with the transmissivity of the soliton stream accurately controlled by the HF field.

physics.optics↗

arXiv2020

An attempt to simulate laser-induced all-optical spin switching in a crystalline ferrimagnet

Interest in all-optical spin switching (AOS) is growing rapidly. The recent discovery of AOS in Mn$_2$RuGa provides a much needed clean case of crystalline ferrimagnets for theoretical simulations. Here, we attempt to simulate it using the state-of-the-art first-principles method combined with the Heisenberg exchange model. We first compute the spin moments at two inequivalent manganese sites and then feed them into our model Hamiltonian. We employ an ultrafast laser pulse to switch the spins. We find that there is a similar optimal laser field amplitude to switch spins. However, we find that the exchange interaction has a significant effect on the system switchability. Weakening the exchange interaction could make the system unswitchable. This provides a crucial insight into the switching mechanism in ferrimagnets.

cond-mat.mtrl-sci↗

arXiv2019

Spin-orbit torque-mediated spin-wave excitation as an alternative paradigm for femtomagnetism

Laser-induced femtosecond demagnetization, femtomagnetism, offers a potential route to develop faster magnetic storage devices. It is generally believed that the traditional spin-wave theory, which is developed for thermally driven slow demagnetization, can not explain this rapid demagnetization by design. Here we show that this traditional spin-wave theory, once augmented by laser-induced spin-orbit torque, provides a highly efficient paradigm for demagnetization, by capturing low-energy spin-wave excitation that is absent in existing mechanisms. Our paradigm is different from existing ones, but does not exclude them. Microscopically, we find that optical spin-orbit torque generates massive spin waves across several hundred lattice sites, collapsing the long-range spin-spin correlation within 20 fs. Our finding does not only explain new experiments, but also establishes an alternative paradigm for femtomagnetism. It is expected to have far-reaching impacts on future research.

cond-mat.mtrl-sci↗

arXiv2019

Asymptotic dynamics of three-dimensional bipolar ultrashort electromagnetic pulses in an array of semiconductor carbon nanotubes

We study the propagation of three-dimensional bipolar ultrashort electromagnetic pulses in an array of semiconductor carbon nanotubes at times much longer than the pulse duration, yet still shorter than the relaxation time in the system. The interaction of the electromagnetic field with the electronic subsystem of the medium is described by means of Maxwell's equations, taking into account the field inhomogeneity along the nanotube axis beyond the approximation of slowly varying amplitudes and phases. A model is proposed for the analysis of the dynamics of an electromagnetic pulse in the form of an effective equation for the vector potential of the field. Our numerical analysis demonstrates the possibility of a satisfactory description of the evolution of the pulse field at large times by means of a three-dimensional generalization of the sine-Gordon and double sine-Gordon equations.

physics.optics↗

arXiv2018

Understanding all-optical spin switching: Comparison between experiment and theory

Information technology depends on how one can control and manipulate signals accurately and quickly. Transistors are at the core of modern technology and are based on electron charges. But as the device dimension shrinks, heating becomes a major problem. The spintronics explores the spin degree of electrons and thus bypasses the heat, at least in principle. For this reason, spin-based technology offers a possible solution. In this review, we survey some of latest developments in all-optical switching (AOS), where ultrafast laser pulses are able to reverse spins from one direction to the other deterministically. But AOS only occurs in a special group of magnetic samples and within a narrow window of laser parameters. Some samples need multiple pulses to switch spins, while others need a single-shot pulse. To this end, there are several models available, but the underlying mechanism is still under debate. This review is different from other prior reviews in two aspects. First, we sacrifice the completeness of reviewing existing studies, while focusing on a limited set of experimental results that are highly reproducible in different labs and provide actual switched magnetic domain images. Second, we extract the common features from existing experiments that are critical to AOS, without favoring a particular switching mechanism. We emphasize that given the limited experimental data, it is really premature to identify a unified mechanism. We compare these features with our own model prediction, without resorting to a phenomenological scheme. We hope that this review serves the broad readership well.

cond-mat.mtrl-sci↗

arXiv2018

Generating high-order optical and spin harmonics from ferromagnetic monolayers

High-order harmonic generation (HHG) in solids has entered a new phase of intensive research, with envisioned band-structure mapping on an ultrashort time scale. This partly benefits from a flurry of new HHG materials discovered, but so far has missed an important group. HHG in magnetic materials should have profound impact on future magnetic storage technology advances. Here we introduce and demonstrate HHG in ferromagnetic monolayers. We find that HHG carries spin information and sensitively depends on the relativistic spin-orbit coupling; and if they are dispersed into the crystal momentum ${\bf k}$ space, harmonics originating from real transitions can be ${\bf k}$-resolved and carry the band structure information. Geometrically, the HHG signal is sensitive to spatial orientations of monolayers. Different from the optical counterpart, the spin HHG, though probably weak, only appears at even orders, a consequence of SU(2) symmetry. Our findings open an unexplored frontier -- magneto-high-order harmonic generation.

cond-mat.mtrl-sci↗

arXiv2017

First-principles and model simulation of all-optical spin reversal

All-optical spin switching is a potential trailblazer for information storage and communication at an unprecedented fast rate and free of magnetic fields. However, the current wisdom is largely based on semiempirical models of effective magnetic fields and heat pulses, so it is difficult to provide high-speed design protocols for actual devices. Here, we carry out a massively parallel first-principles and model calculation for thirteen spin systems and magnetic layers, free of any effective field, to establish a simpler and alternative paradigm of laser-induced ultrafast spin reversal and to point out a path to a full-integrated photospintronic device. It is the interplay of the optical selection rule and sublattice spin orderings that underlines seemingly irreconcilable helicity-dependent/independent switchings. Using realistic experimental parameters, we predict that strong ferrimagnets, in particular, Laves phase C15 rare-earth alloys, meet the telecommunication energy requirement of 10 fJ, thus allowing a cost-effective subpicosecond laser to switch spin in the GHz region.

cond-mat.mtrl-sci↗

arXiv2017

Is perpendicular magnetic anisotropy essential to all-optical ultrafast spin reversal in ferromagnets?

All-optical spin reversal presents a new opportunity for spin manipulations, free of a magnetic field. Most of all-optical-spin-reversal ferromagnets are found to have a perpendicular magnetic anisotropy (PMA), but it has been unknown whether PMA is necessary for the spin reversal. Here we theoretically investigate magnetic thin films with either PMA or in-plane magnetic anisotropy (IMA). Our results show that the spin reversal in IMA systems is possible, but only with a longer laser pulse and within a narrow laser parameter region. The spin reversal does not show a strong helicity dependence where the left- and right-circularly polarized light lead to the identical results. By contrast, the spin reversal in PMA systems is robust, provided both the spin angular momentum and laser field are strong enough while the magnetic anisotropy itself is not too strong. This explains why experimentally the majority of all-optical spin-reversal samples are found to have strong PMA and why spins in Fe nanoparticles only cant out of plane. It is the laser-induced spin-orbit torque that plays a key role in the spin reversal. Surprisingly, the same spin-orbit torque results in laser-induced spin rectification in spin-mixed configuration, a prediction that can be tested experimentally. Our results clearly point out that PMA is essential to the spin reversal, though there is an opportunity for in-plane spin reversal.

cond-mat.mtrl-sci↗

arXiv2016

Laser-induced ultrafast demagnetization time and spin moment in ferromagnets: First-principles calculation

When a laser pulse excites a ferromagnet, its spin undergoes a dramatic change. The initial demagnetization process is very fast. Experimentally, it is found that the demagnetization time is related to the spin moment in the sample. In this study, we employ the first-principles method to directly simulate such a process. We use the fixed spin moment method to change the spin moment in ferromagnetic nickel, and then we employ the Liouville equation to couple the laser pulse to the system. We find that in general the dependence of demagnetization time on the spin moment is nonlinear: It decreases with the spin moment up to a point, after which an increase with the spin moment is observed, followed by a second decrease. To understand this, we employ an extended Heisenberg model, which includes both the exchange interaction and spin-orbit coupling. The model directly links the demagnetization rate to the spin moment itself and demonstrates analytically that the spin relaxes more slowly with a small spin moment. A future experimental test of our predictions is needed.

cond-mat.mtrl-sci↗

arXiv2016

Ultrafast reduction of exchange splitting in ferromagnetic nickel

A decade ago Rhie \et (Phys. Rev. Lett. {\bf 90}, 247201 (2003)) reported that when ferromagnetic nickel is subject to an intense ultrashort laser pulse, its exchange splitting is reduced quickly. But to simulate such reduction remains a big challenge. The popular rigid band approximation (RBA), where both the band structure and the exchange splitting are held fixed before and after laser excitation, is unsuitable for this purpose, while the time-dependent density functional theory could be time-consuming. To overcome these difficulties, we propose a time-dependent Liouville and density functional theory (TDLDFT) that integrates the time-dependent Liouville equation into the density functional theory. As a result, the excited charge density is reiterated back into the Kohn-Sham equation, and the band structure is allowed to change dynamically. Even with the ground-state density functional, a larger demagnetization than RBA is found; after we expand Ortenzi's spin scaling method into an excited-state (laser) density functional, we find that the exchange splitting is indeed strongly reduced, as seen in the experiment. Both the majority and minority bands are shifted toward the Fermi level, but the majority shifts a lot more. The ultrafast reduction in exchange splitting occurs concomitantly with demagnetization. While our current theory is still unable to yield the same percentage loss in the spin moment as observed in the experiment, it predicts a correct trend that agrees with the experiments. With a better functional, we believe that our results can be further improved.

cond-mat.mtrl-sci↗

arXiv2016

A new and simple model for magneto-optics uncovers an unexpected spin switching

In magneto-optics the spin angular momentum $S_z$ of a sample is indirectly probed by the rotation angle and ellipticity, which are mainly determined by the off-diagonal susceptibility $χ^{(1)}_{xy}$. A direct and analytic relation between $S_z$ and $χ^{(1)}_{xy}$ is necessary and of paramount importance to the success of magneto-optics, but is often difficult to acquire since quantum mechanically the relation is hidden in the sum-over-states. Here we propose a new and simple model to establish such a much needed relation. Our model is based on the Hookean model, but includes spin-orbit coupling. Under cw excitation, we show that $χ^{(1)}_{xy}(ω)$ is indeed directly proportional to $S_z$ for a fixed photon frequency $ω$. Such an elegant relation is encouraging, and we wonder whether our model can describe spin dynamics as well. By allowing the spin to change dynamically, to our surprise, our model predicts that an ultrafast laser pulse can induce a spin precession; with appropriate parameters, the laser can even reverse spin from one direction to another. This works for both the circularly and linearly polarized light. The spin reversal window is narrow. These unexpected results closely resemble all-optical helicity-dependent magnetic switching found in much more complicated ferrimagnetic rare earth compounds. Therefore, we believe that our spin-orbit coupled model may find some important applications in spin switching processes, a hot topic in femtomagnetism.

cond-mat.mtrl-sci↗