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At least 19 records

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.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Stoner versus Heisenberg: Ultrafast exchange reduction and magnon generation during laser-induced demagnetization

Understanding how the electronic band structure of a ferromagnetic material is modified during laser-induced demagnetization on femtosecond timescales has been a long-standing question in condensed matter physics. Here, we use ultrafast high harmonics to measure time-, energy-, and angle-resolved M-edge magnetic asymmetry spectra for Co lms after optical pumping to induce ultrafast demagnetization. This provides a complete data set that we can compare with advanced ab initio magneto-optical calculations. Here, tur analysis identifies that the dominant mechanisms contributing to ultrafast demagnetization on timescales up to several picoseconds are a transient reduction in the exchange splitting and the excitation of ultrafast magnons. Surprisingly, we nd that the magnon contribution to ultrafast demagnetization is already strong on sub-picosecond timescales, while the reduction in exchange splitting persists to several picoseconds.

36 MATERIALS SCIENCE↗

Laser-induced ultrafast transport and demagnetization at the earliest time: first-principles and real-time investigation

It is generally believed that there are at least two ways to use an ultrafast laser pulse to demagnetize a magnetic sample. One is to directly photo-demagnetize the system through spin-orbit coupling (SOC), and the other is to utilize ultrafast hot electron transport without SOC. The challenge is that these two processes are entangled on the same time scale. While the experimental results have been inconclusive, theoretical investigations are even scarcer, beyond those earlier studies based on spin superdiffusion. For instance, we even do not know how fast electrons move under laser excitation and how far they move. Here we carry out a first-principles time-dependent calculation to investigate how fast electrons actually move under laser excitation and how large the electron transport affects demagnetization on the shortest time scale. To take into account the transport effect, we implement the intraband transition in our theory. In the bulk fcc Ni, we find the effect of the spin transport on the demagnetization is extremely small, no more than 1%. The collective electron velocity in Ni is 0.4 Å/fs, much smaller than the Fermi velocity, and the collective displacement is no more than 0.1 Å. But this does not mean that electrons do not travel fast; instead we find that electron velocities at two opposite crystal momenta cancel each other. We follow the Γ-X line and find a huge dispersion in the velocities in the crystal momentum space. In the Fe/W(110) thin film, the overall demagnetization is larger than Ni, and the Fermi velocity is higher than Ni. However, the effect of the spin transport is still small in the Fe/W(110) thin film. Based on our numerical results and existing experimental findings, we propose a different mechanism that can explain two latest experimental results. Our finding sheds new light on the effect of ballistic transport on demagnetization.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Laser-induced forces on atoms during ultrafast demagnetization

Laser-induced femtosecond demagnetization has attracted a broad attention as a possible candidate for information storage technology. However, whether or not lattice vibration directly participates in demagnetization has been highly controversial over a decade. A recent electron diffraction experiment attributed the demagnetization to the polarized phonon effect, but a similar x-ray diffraction experiment attributed it to the Einstein–de Haas effect. Common to both experiments is that neither the angular momentum of the lattice nor the rotation of the sample was directly probed. Here, we report our first first-principles calculation of forces on atoms induced by an ultrafast laser during ultrafast demagnetization. We employ two complementary methods: (i) the frozen lattice with electronic excitation and (ii) frozen excitation but moving the lattice. We find that the forces on atoms start at –50 fs and peak around 30 fs. The magnitude of the force is far smaller than the empirical estimates. Within the limit of our theory, our results suggest that the polarized phonon effect and the Einstein–de Haas effect are unlikely to be the main course of demagnetization. As a result, we expect that our finding has a profound impact on the future direction of laser-induced dynamics in magnetic and quantum materials.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Spin-orbit coupling induced demagnetization in Ni: Ab initio nonadiabatic molecular dynamics perspective

Spin-orbit coupling (SOC), which can induce spin flip during the relaxation of photoexcited charge carrier, plays a crucial role in spin dynamics. Here in this work, we have used time-domain ab initio nonadiabatic molecular dynamics (NAMD) method to study the SOC induced ultrafast demagnetization in Ni at 300K. The spin-diabatic representation using spin-polarized Kohn-Sham (KS) basis sets and spin-adiabatic representation using spinor basis sets have been applied, and both of them achieve demagnetization in Ni with a timescale around 100fs. The spin-diabatic representation suggests a picture that the electron-phonon coupling (EPC) provides direct energy relaxation channel among the same-spin states, while the SOC can induce spin flip. After photoexcitation, it is found the spin-minority electrons relax to the same-spin states rather than the opposite-spin states, since EPC is larger than SOC by one order of magnitude. By contrast, for the spin-majority electrons, spin flip occurs since there are no empty same-spin states as electron acceptor above the Fermi level. The different relaxation pathways for spin-majority and spin-minority electrons induce the demagnetization. The spin-adiabatic representation provides an Elliott-Yafet spin-phonon scattering picture. The SOC induced reduction of magnetic moment in Ni may induce magnon to drive further demagnetization. The ab initio NAMD simulation provides a critical angle to understand how the SOC and EPC affect demagnetization process in Ni.

36 MATERIALS SCIENCE↗

Demagnetization of Nd 2 Fe 14 B, Pr 2 Fe 14 B, and Sm 2 Co 17 Permanent Magnets in Spallation Irradiation Fields

Prompted by the need for radiation-resistant permanent magnets for insertion devices (IDs) of high-brilliance next-generation synchrotrons such as the National Synchrotron Light Source II, the demagnetization of Nd 2 Fe 14 B and Pr 2 Fe 14 B was studied after exposure to a mixed irradiating field. Degradation and damage of the permanent magnetic material by components of electromagnetic showers induced in magnets by intense high-energy electron beams will alter the magnetic field structure of the IDs. Plate-like Nd 2 Fe 14 B magnets were irradiated to 1.8 Grad dose and were evaluated against Pr 2 Fe 14 B magnets irradiated to a lower dose of 20 Mrad. In addition, annular Sm 2 Co 17 and Nd 2 Fe 14 B magnets integrated within a ferrofluidic feedthrough (FFFT) rotary seal were also irradiated to dose levels of 2 Grad for Sm 2 Co 17 and 20 Mrad for Nd 2 Fe 14 B. Post-irradiation measurements of the magnetic intensity revealed that severe demagnetization exceeding 85% occurs in Nd 2 Fe 14 B magnets after only 50 Mrad dose and over 87% for Pr 2 Fe 14 B after 10 Mrad dose. The annular-shaped Sm 2 Co 17 magnets of the FFFTs were almost insensitive to irradiation up to a dose of 2 Grad. Annular-shaped Nd 2 Fe 14 B magnets also showed resistance to demagnetization, a direct consequence of the annular shape which is characterized by the removal of the stronger demagnetizing field present at the center of a disk-like magnet. As a result, the sensitivity of boron-based permanent magnets to neutron energy (thermal versus fast) was also assessed via specifically designed experiments and discussed.

43 PARTICLE ACCELERATORS↗

Tomography based numerical simulation of the demagnetizing field in soft magnetic composites

The magneto-static behaviour of soft magnetic composites (SMCs) is investigated using tomography based direct numerical simulation. The microgeometry crucially affects the magnetic properties of the composite since a geometry dependent demagnetizing field is established inside the composite, which lowers the magnetic permeability. We determine the magnetic field information inside the SMC using direct numerical simulation of the magnetic field based on high resolution micro-computed tomography data of the SMC's microstructure as well as artificially generated data made of statistically homogeneous systems of identical fully penetrable spheres and prolate spheroids. Quasi-static electromagnetic behaviour and linear material response are assumed. The 3D magnetostatic Maxwell equations are solved using Whitney finite elements. Simulations show that clustering and percolation behaviour determine the demagnetizing factor of SMCs rather than the particle shape. The demagnetizing factor correlates with the slope of a 2-point probability function at its origin, which is related to the specific surface area of the SMC. Comparison with experimental results indicates that the relatively low permeability of SMCs cannot be explained by demagnetizing effects alone and suggests that the permeability of SMC particles has to be orders of magnitude smaller than the bulk permeability of the particle material.

36 MATERIALS SCIENCE↗

Demagnetization analysis of an 18 GHz electron cyclotron resonance ion source permanent magnet hexapole

An upgrade of ECR2 at the Argonne Tandem Linac Accelerator System is under way, focusing on increasing the intensity capabilities of the facility. ECR2 is a room temperature electron cyclotron resonance ion source, and the upgrade has strict requirements to retain radial access to the plasma chamber and keep the ion source operating without the use of superconducting magnets. The upgrade design with respect to the magnet arrangement and magnetization vectors has recently been presented [R. C. Vondrasek, J. McLain, and R. H. Scott, J. Phys.: Conf. Ser. 2743 , 012044 (2024)] using the same magnetic material as the current ECR2 hexapole. A thorough exploration of the demagnetization potential of this hexapole was carried out, and the risk of demagnetization was deemed too high, despite the magnetic performance meeting the requirements for the upgrade. Additional permanent magnet materials are considered with their respective performance evaluated. Magnet strength and demagnetization resistance are investigated and optimized with the final room temperature design demonstrating a high temperature transient demagnetization resistance and a radial magnetic field of 1.18 T at the plasma chamber wall. Finally, the simulations of this hexapole suggest that it will be sufficient to optimize intensity with a 14.5 GHz driving frequency and will allow 18 GHz operation, while keeping a high safety margin for maintaining magnet performance.

Argonne Tandem Linac Accelerator System↗

Strong ultrafast demagnetization due to the intraband transitions

Abstract Demagnetization in ferromagnetic transition metals driven by a femtosecond laser pulse is a fundamental problem in solid state physics, and its understanding is essential to the development of spintronic devices.Ab initiocalculation of time-dependent magnetic moment in the velocity gauge so far has not been successful in reproducing the large amount of demagnetization observed in experiments. In this work, we propose a method to incorporate intraband transitions within the velocity gauge through a convective derivative in the crystal momentum space. Our results for transition-element bulk crystals (bcc Fe, hcp Co and fcc Ni) based on the time-dependent quantum Liouville equation show a dramatic enhancement in the amount of demagnetization after the inclusion of an intraband term, in agreement with experiments. We also find that the effect of intraband transitions on each ferromagnetic material is distinctly different because of their band structure and spin property differences. Our finding has a far-reaching impact on understanding of ultrafast demagnetization.

Physics↗

Effects of the Third Harmonic Demagnetization Field on the ac Losses of a Granular FeSeTe Superconductor in ac Field

The first harmonics of the magnetic response, of inter- and intragranular volume fractions of a FeSe{sub 0.5}Te{sub 0.5} granular superconducting sample in an alternate magnetic field, have been numerically extracted from the measured magnetization of the whole system by using a model which considers the effects of the fundamental demagnetization fields generated by the magnetization itself. This allowed us to obtain the temperature and field behaviors of the inter- and intragranular ac losses during an ac cycle. These parameters have been found sensitive to the existence of the third harmonic components of the demagnetization field produced by the corresponding magnetization harmonics of the sample. This confirms that the effects of the magnetic response third harmonic components on the sample magnetization, through the demagnetization field, should be taken into account for a more detailed analysis of the measured ac magnetic curves.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Frozen flux violation, electron demagnetization and magnetic reconnection

We argue that the analogue in collisionless plasma of the collisional diffusion region of magnetic reconnection is properly defined in terms of the demagnetization of the plasma electrons that enable “frozen flux” slippage to occur. This condition differs from the violation of the “frozen-in” condition, which only implies that two fluid effects are involved, rather than the necessary slippage of magnetic flux as viewed in the electron frame. Using 2D Particle In Cell (PIC) simulations, this approach properly finds the saddle point region of the flux function. Our demagnetization conditions are the dimensionless guiding center approximation expansion parameters for electrons which we show are observable and determined locally by the ratio of non-ideal electric to magnetic field strengths. Proxies for frozen flux slippage are developed that (a) are measurable on a single spacecraft, (b) are dimensionless with theoretically justified threshold values of significance, and (c) are shown in 2D simulations to recover distinctions theoretically possible with the (unmeasurable) flux function. A new potentially observable dimensionless frozen flux rate, Λ{sub Φ}, differentiates significant from anecdotal frozen flux slippage. A single spacecraft observable, ϒ, is shown with PIC simulations to be essentially proportional to the unobservable local Maxwell frozen flux rate. This relationship theoretically establishes electron demagnetization in 3D as the general cause of frozen flux slippage. In simple 2D cases with an isolated central diffusion region surrounded by separatrices, these diagnostics uniquely identify the traditional diffusion region (without confusing it with the two fluid “ion-diffusion” region) and clarify the role of the separatrices where frozen flux violations do occur but are not substantial. In the more complicated guide and asymmetric 2D cases, substantial flux slippage regions extend out along, but inside of, the preferred separatrices, demonstrating that Λ{sub Φ} ≠ 0 violations are present over significant distances (in ion inertial units) from the separator identified by the 2D flux function; these violations are, however, generally weaker than seen at known separators in 2D simulations.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Analysis of thermal demagnetization behavior of Nd–Fe–B sintered magnets using magnetic domain observation

We used magnetic domain observation to statistically observe the thermal demagnetization behavior of Nd–Fe–B sintered magnets at elevated temperatures up to 150 °C. Simultaneous magnetization reversal in a hundred adjacent grains occurred at 90 °C because of the magnetic interaction among the grains beyond grain boundaries in the Dysprosium (Dy)-free low-coercivity magnet. Conversely, simultaneous magnetization reversal in a hundred grains did not occur in the Dy-added high-coercivity magnets, and the demagnetizing ratio steadily increased with temperature. Furthermore, the addition of Dy induced high thermal stability by eliminating the simultaneous thermal demagnetization, which was caused by the magnetic interaction among the grains.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Revealing angular momentum transfer channels and timescales in the ultrafast demagnetization process of ferromagnetic semiconductors

Ultrafast control of magnetic order by light provides a promising realization for spintronic devices beyond Moore’s Law and has stimulated intense research interest in recent years. Yet, despite 2 decades of debates, the key question of how the spin angular momentum flows on the femtosecond timescale remains open. The lack of direct first-principle methods and pictures for such process exacerbates the issue. Here, we unravel the laser-induced demagnetization mechanism of ferromagnetic semiconductor GaMnAs, using an efficient time-dependent density functional theory approach that enables the direct real-time snapshot of the demagnetization process. Our results show a clear spin-transfer trajectory from the localized Mn-d electrons to itinerant carriers within 20 fs, illustrating the dominant role of $\textit{sp–d}$ interaction. We find that the total spin of localized electrons and itinerant carriers is not conserved in the presence of spin-orbit coupling (SOC). Immediately after laser excitation, a growing percentage of spin-angular momentum is quickly transferred to the electron orbital via SOC in about 1 ps, then slowly to the lattice via electron–phonon coupling in a few picoseconds, responsible for the 2-stage process observed experimentally. The spin-relaxation time via SOC is about 300 fs for itinerant carriers and about 700 fs for Mn-d electrons. These results provide a quantum-mechanical microscopic picture for the long-standing questions regarding the channels and timescales of spin transfer, as well as the roles of different interactions underlying the GaMnAs demagnetization process.

36 MATERIALS SCIENCE↗

Ultrafast Electron Correlations and Memory Effects at Work: Femtosecond Demagnetization in Ni

Experimental observations of the ultrafast (less than 50 fs) demagnetization of Ni have so far defied theoretical explanations particularly since its spin-flipping time is much less than that resulting from spin-orbit and electron-lattice interactions. Through the application of an approach that benefits from spin-flip time-dependent density-functional theory and dynamical mean-field theory, we show that proper inclusion of electron correlations and memory (time dependence of electron-electron interaction) effects leads to demagnetization at the femtosecond scale, in good agreement with experimental observations. Furthermore, our calculations reveal that this ultrafast demagnetization results mainly from spin-flip transitions from occupied to unoccupied orbitals implying a dynamical reduction of exchange splitting. In this work, these conclusions are found to be valid for a wide range of laser pulse amplitudes. They also pave the way for ab initio investigations of ultrafast charge and spin dynamics in a variety of quantum materials in which electron correlations may play a definitive role.

74 ATOMIC AND MOLECULAR PHYSICS↗

Role of initial magnetic disorder: A time-dependent ab initio study of ultrafast demagnetization mechanisms

Despite more than 20 years of development, the underlying physics of the laser-induced demagnetization process is still debated. We present a fast, real-time time-dependent density functional theory (rt-TDDFT) algorithm together with the phenomenological atomic Landau-Lifshitz-Gilbert model to investigate this problem. Our Hamiltonian considers noncollinear magnetic moment, spin-orbit coupling (SOC), electron-electron, electron-phonon, and electron-light interactions. The algorithm for time evolution achieves hundreds of times of speedup enabling calculation of large systems. Our simulations yield a demagnetization rate similar to experiments. We found that (i) the angular momentum flow from light to the system is not essential and the spin Zeeman effect is negligible. (ii) The phonon can play a role but is not essential. (iii) The initial spin disorder and the self-consistent update of the electron-electron interaction play dominant roles and enhance the demagnetization to the experimentally observed rate. The spin disorder connects the electronic structure theory with the phenomenological three-temperature model.

36 MATERIALS SCIENCE↗

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 face-centered cubic (fcc) Ni as an example and use an extremely dense 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 k points abruptly changes from [Formula: see text] to [Formula: see text] 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 k points, which are called spin Berry points [M. V. Berry, Proc. R. Soc. Lond. A 393 (1984) 45], 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.

Physics↗

X-ray induced demagnetization of single-molecule magnets

Low-temperature x-ray magnetic circular dichroism measurements on the endohedral single-molecule magnet DySc{sub 2}N@C{sub 80} at the Dy M{sub 4,5} edges reveal a shrinking of the opening of the observed hysteresis with increasing x-ray flux. Time-dependent measurements show that the exposure of the molecules to x-rays resonant with the Dy M{sub 5} edge accelerates the relaxation of magnetization more than off-resonant x-rays. The results cannot be explained by a homogeneous temperature rise due to x-ray absorption. Moreover, the observed large demagnetization cross sections indicate that the resonant absorption of one x-ray photon induces the demagnetization of many molecules.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Super-heavy electron material as metallic refrigerant for adiabatic demagnetization cooling

Low-temperature refrigeration is of crucial importance in fundamental research of condensed matter physics, because the investigations of fascinating quantum phenomena, such as superconductivity, superfluidity, and quantum criticality, often require refrigeration down to very low temperatures. Currently, cryogenic refrigerators with 3 He gas are widely used for cooling below 1 Kelvin. However, usage of the gas has been increasingly difficult because of the current world-wide shortage. Therefore, it is important to consider alternative methods of refrigeration. We show that a new type of refrigerant, the super-heavy electron metal YbCo 2 Zn 20 , can be used for adiabatic demagnetization refrigeration, which does not require 3 He gas. This method has a number of advantages, including much better metallic thermal conductivity compared to the conventional insulating refrigerants. We also demonstrate that the cooling performance is optimized in Yb 1$-$x Sc x Co 2 Zn 20 by partial Sc substitution, with x ~ 0.19. The substitution induces chemical pressure that drives the materials to a zero-field quantum critical point. This leads to an additional enhancement of the magnetocaloric effect in low fields and low temperatures, enabling final temperatures well below 100 mK. This performance has, up to now, been restricted to insulators. For nearly a century, the same principle of using local magnetic moments has been applied for adiabatic demagnetization cooling. Lastly, this study opens new possibilities of using itinerant magnetic moments for cryogen-free refrigeration.

36 MATERIALS SCIENCE↗