Due to critical environmental and technological issues, there is a pressing need to switch from current refrigeration methods based on compression of gases to novel solid-state cooling technologies. Solid-state cooling is based on the thermal response of materials to external magnetic, electric, or mechanic fields, the so-called caloric effect. The electrocaloric (EC) effect, which is caused by electric fields and typically occurs in polar materials, is particularly promising from a technological point of view owing to its good scalability and natural implementation in circuitry. Simulation of EC effects represents an efficient and physically insightful strategy for advancing the field of solid-state cooling by complementing, and in some cases guiding, experiments. Theoretical estimation of EC effects can be achieved with different approaches ranging from computationally inexpensive but physically insightful phenomenological free-energy models to computationally very demanding and quantitatively accurate first-principles methods. In this Chapter, we review EC simulation approaches that rely on first-principles methods. In this category, we include ab initio quasi-harmonic methods, bond-valence and classical interatomic potentials and effective Hamiltonians. In analogy to the experiments, these simulation approaches can be used to estimate EC effects either directly or indirectly and we review here well-established protocols that can be followed for each case. The Chapter finalises with a collection of representative examples in which first-principles based approaches have been used to predict and understand original EC effects.
We address the question of how the electrocaloric effect in epitaxial thin films of the prototypical ferroelectric BaTiO$_3$ is affected by the clamping to the substrate and by substrate-induced misfit strain. We use molecular dynamics simulations and a first-principles-based effective Hamiltonian to calculate the adiabatic temperature change $ΔT$ under different epitaxial constraints. Our results demonstrate that, consistent with phenomenological theory, clamping by the substrate reduces the maximum $ΔT$ compared to bulk BaTiO$_3$. On the other hand, compressive misfit-strain leads to a stron…
We use molecular dynamics simulations for a first principles-based effective Hamiltonian to calculate two important quantities characterizing the electrocaloric effect in BaTiO$_3$, the adiabatic temperature change $ΔT$ and the isothermal entropy change $ΔS$, for different electric field strengths. We compare direct and indirect methods to obtain $ΔT$ and $ΔS$, and we confirm that both methods indeed lead to identical result provided that the system does not actually undergo a first order phase transition. We also show that a large electrocaloric response is obtained for electric fields beyond…
Molecular dynamics simulations predict a giant electrocaloric effect at the ferroelectric-antiferroelectric phase boundary in PZT (PbTiO$_3$-PbZrO$_3$). These large-scale simulations also give insights into the atomistic mechanisms of the electrocaloric effect in PZT materials. Studying a range of ferroelectric (FE) and antiferroelectric (AFE) PZT materials we found positive electrocaloric effect in FE composites, but AFE ones exhibit a positive-to-negative crossover. At the AFE-FE phase boundary we find complex domain patterns. We demonstrate that the origin of giant electrocaloric change of …
The perovskite crystal BaTiO3 is modeled using a first-principles based effective Hamiltonian and molecular dynamics simulations are performed to estimate the pyroelectric response. The electrocaloric temperature change, \DeltaT, is calculated for different temperatures and externally applied electric fields. It is found that it is possible to achieve a large \DeltaT, around 5-6 K, for a relatively small electric field gradient, less than 100 kV/cm, if the applied fields have a small absolute magnitude.
We show that the electrocaloric (EC) effect -- e.g., the temperature change experienced by an insulator upon application of an electric bias -- lends itself to a straightforward interpretation when expressed as a Taylor series in the external field. Our formalism explains in a unified and simple way the most notable small-field effects reported the literature -- e.g., the so-called {\em normal} (increase of temperature under bias, as usually found in ferroelectrics) and {\em inverse} (decrease of temperature, as e.g. in antiferroelectrics) EC responses -- and clarifies their physical interpret…
Anomalous electrocaloric effect (ECE) with decreasing temperature upon application of an electric field is known to occur in antiferroelectrics (AFEs), and previous understanding refers to the field-induced canting of electric dipoles if there is no phase transitions. Here, we use a first-principle-based method to study the ECE in Nd-substituted BiFeO3 (BNFO) perovskite solid solutions, which has the Pnma-type AFE ground state. We demonstrate another scenario to achieve and explain anomalous ECE, emphasizing that explicit consideration of octahedral tiltings is indispensable for a correct unde…
We study the impact of thermal hysteresis at the first-order structural/ferroelectric phase transitions on the electrocaloric response in bulk BaTiO$_3$ by performing molecular dynamics simulations for a first-principles-based effective Hamiltonian. We demonstrate that the electrocaloric response can conceptually be separated in two contributions: a transitional part, stemming from the discontinuous jump in entropy at the first order phase transition, and a configurational part, due to the continuous change of polarization and entropy within each phase. This latter part increases with the stre…
Atomistic effective Hamiltonian simulations are used to investigate electrocaloric (EC) effects in the lead-free Ba(Zr$_{0.5}$Ti$_{0.5}$)O$_{3}$ (BZT) relaxor ferroelectric. We find that the EC coefficient varies non-monotonically with the field at any temperature, presenting a maximum that can be traced back to the behavior of BZT's polar nanoregions. We also introduce a simple Landau-based model that reproduces the EC behavior of BZT as a function of field and temperature, and which is directly applicable to other compounds. Finally, we confirm that, for low temperatures (i.e., in non-ergodi…
The electrocaloric effect (ECE) in BaTiO3 is simulated using two different first-principles based effective Hamiltonian molecular dynamics methods. The calculations are performed for a wide range of temperatures (30--900 K) and external electric fields (0--500 kV/cm). As expected, a large adiabatic temperature change, Delta-T, at the Curie temperature, T_C, is observed. It is found that for single crystals of pure BaTiO3, the temperature range where a large Delta-T is observed is narrow for small external electric fields (<50 kV/cm). Large fields (>100 kV/cm) may be required to broaden the eff…
We use molecular dynamics with a first-principles-based shell model potential to study the electrocaloric effect (ECE) in lithium niobate, LiNbO$_3$, and find a giant electrocaloric effect along a line passing through the ferroelectric transition. With applied electric field, a line of maximum ECE passes through the zero field ferroelectric transition, continuing along a Widom line at high temperatures with increasing field, and along the instability that leads to homogeneous ferroelectric switching below $T_c$ with an applied field antiparallel to the spontaneous polarization. This line is de…
An improved thermodynamic cycle is proposed, where the cooling effect of an electrocaloric refrigerant is enhanced by applying a reversed electric field. In contrast to conventional adiabatic heating or cooling by on-off cycles of the external electric field, applying a reversed field is significantly improving the cooling efficiency, since the variation in configurational entropy is increased. By comparing results from computer simulations using Monte-Carlo algorithms and experiments using direct electrocaloric measurements, we show that the electrocaloric cooling efficiency can be enhanced b…
We analyse the effects of applying an electric field on the critical temperature, Ts, at which superionicity appears in archetypal fast ion conductor CaF2 by means of molecular dynamics simulations. We find that the onset of superionicity can be reduced by about 100K when relatively small electric fields of ~50KV/cm are employed. Under large enough electric fields, however, ionic conductivity is depleted. The normal to superionic phase transition is characterised by a large increase of entropy, thereby sizeable electrocaloric effects can be realised in fast ion conductors that are promising fo…
An atomistic effective Hamiltonian is used to investigate electrocaloric (EC) effects of Pb(Mg$_{1/3}$Nb$_{2/3}$)O$_{3}$ (PMN) relaxor ferroelectrics in its ergodic regime, and subject to electric fields applied along the pseudocubic [111] direction. Such Hamiltonian qualitatively reproduces (i) the electric field-versus-temperature phase diagram, including the existence of a critical point where first-order and second-order transitions meet each other; and (ii) a giant EC response near such critical point. It also reveals that such giant response around this critical point is microscopically …
Ferroelectrics are attractive candidate materials for environmentally friendly solid state refrigeration free of greenhouse gases. Their thermal response upon variations of external electric fields is largest in the vicinity of their phase transitions, which may occur near room temperature. The magnitude of the effect, however, is too small for useful cooling applications even when they are driven close to dielectric breakdown. Insight from microscopic theory is therefore needed to characterize materials and provide guiding principles to search for new ones with enhanced electrocaloric perform…
We study the electrocaloric (EC) effect in bulk BaTiO$_3$ (BTO) using molecular dynamics simulations of a first principles-based effective Hamiltonian, combined with direct measurements of the adiabatic EC temperature change in BTO single crystals. We examine in particular the dependence of the EC effect on the direction of the applied electric field at all three ferroelectric transitions, and we show that the EC response is strongly anisotropic. Most strikingly, an inverse caloric effect, i.e., a temperature increase under field removal, can be observed at both ferroelectric-ferroelectric tra…
The electrocaloric effect (ECE) of BaZr$_{x}$Ti$_{1-x}$O$_3$ (BZT) is closely related to the relaxor state transition of the materials. This work presents a systematic study on the ECE and the state transition of the BZT, using a combined canonical and microcanonical Monte Carlo simulations based a lattice-based on a Ginzburg-Landau-type Hamiltonian. For comparison and verification, experimental measurements have been carried on BTO and BZT ($x=0.12$ and $0.2$) samples, including the ECE at various temperatures, domain patterns by Piezoresponse Force Microscopy at room temperature, and the P-E…
In acceptor doped ferroelectrics and in ferroelectric films and nanocomposites, defect dipoles, strain gradients, and the electric boundary conditions at interfaces and surfaces often impose internal bias fields. In this work we delicately study the impact of internal bias fields on the electrocaloric effect (ECE), utilizing an analytical model and \emph{ab initio}-based molecular dynamics simulations. We reveal the complex dependency of the ECE on field protocol and relative strength of internal and external fields. The internal fields may even reverse the sign of the response (inverse or neg…
The influence of defect dipoles on the electrocaloric effect (ECE) in acceptor doped BaTiO$_3$ is studied by means of lattice-based Monte-Carlo simulations. A Ginzburg-Landau type effective Hamiltonian is used. Oxygen vacancy-acceptor associates are described by fixed defect dipoles with orientation parallel or anti-parallel to the external field. By a combination of canonical and microcanoncial simulations the ECE is directly evaluated. Our results show that in the case of anti-parallel defect dipoles the ECE can be positive or negative depending on the density of defect dipoles. Moreover, a …
There is a surge of interest in developing environmentally friendly cooling technology based on the solid--state electrocaloric effect (ECE). Here, we point out that negative ECE with a fast cooling rate ($\approx$10$^{11}$ K/s) can be achieved by driving solid crystals to a high--temperature phase with a properly designed electric field pulse. Specifically, we predict that an ultrafast electric field pulse can cause a negative ECE up to 35 K in PbTiO$_3$ occurring on few picosecond time scales. We acquire and analyze these results by clarifying the mechanism of ECE during an adiabatic irrever…
We study the magnetoelectric and electrocaloric response of strain-engineered, multiferroic SrMnO$_3$, using a phenomenological Landau theory with all parameters obtained from \emph{first-principles}-based calculations. This allows to make realistic and materials-specific predictions about the magnitude of the corresponding effects. We find that in the vicinity of a tetracritical point, where magnetic and ferroelectric phase boundaries intersect, an electric field has a huge effect on the antiferromagnetic order, corresponding to a magnetoelectric response several orders of magnitude larger th…
A material with reversible temperature change capability under an external electric field, known as the electrocaloric effect (ECE), has long been considered as a promising solid-state cooling solution. However, electrocaloric (EC) performance of EC materials generally is not sufficiently high for real cooling applications. As a result, exploring EC materials with high performance is of great interest and importance. Here, we report on the ECE of ferroelectric materials with van der Waals layered structure (CuInP2S6 or CIPS in this work in particular). Over 60% polarization charge change is ob…
Organic-inorganic hybrid perovskite architecture could serve as a robust platform for materials design to realize functionalities beyond photovoltaic applications. We explore caloric effects in organometal halide perovskites, taking methylammonium lead iodide (MAPbI$_3$) as an example, using all-atom molecular dynamics simulations with a first-principles based interatomic potential. The adiabatic thermal change is estimated directly by introducing different driving fields in the simulations. We find that MAPbI$_3$ exhibits both electrocaloric and mechanocaloric effects at room temperature. Loc…
Using first-principles calculations, we predict a lightweight room-temperature ferroelectric carbon-boron framework in a host/guest clathrate structure. This ferroelectric clathrate, with composition ScB$_3$C$_3$, exhibits high polarization density and low mass density compared with widely used commercial ferroelectrics. Molecular dynamics simulations show spontaneous polarization with a moderate above-room-temperature T$_c$ of $\sim$370 K, which implies large susceptibility and possibly large electrocaloric and piezoelectric constants at room temperature. Our findings open the possibility for…
We investigate the effect of epitaxial strain on the electrocaloric effect (ECE) in BaTiO$_3$ by means of ab initio based molecular dynamics simulations. We show that tensile strain can be used to optimize the operation range for ferroic cooling. Strain in the range of $\leq 1$ % can be used to shift the operation temperature by several hundreds of Kelvin both to higher and lower temperatures, depending on the direction of the external field. In addition, the transformation between multi-domain and mono-domain states, induced by an in-plane electric field, results in an additional peak of the …
Due to critical environmental issues there is a pressing need to switch from current refrigeration methods based on compression of greenhouse gases to novel solid-state cooling technologies. Solid-state cooling capitalizes on the thermal response of materials to external fields named "caloric effect". The barocaloric (BC) effect driven by hydrostatic pressure is particularly promising from a technological point of view since typically presents larger cooling potential than other caloric variants (e.g., magnetocaloric and electrocaloric effects driven by magnetic and electric fields, respective…
Based on first principles calculations, we predict and characterize the flexibility of two aluminium-based Metal-Organic Frameworks (MOFs), CAU-13 and NOTT-300. Both materials have a wine rack topology similar to that of MIL-53(Al), the archetypal breathing MOF, yet their flexibility has not been demonstrated so far.
First principles calculations based on density functional theory, with generalised gradient corrections and ultrasoft pseudopotentials, have been used to simulate solid and liquid aluminium in direct coexistence at zero pressure. Simulations have been carried out on systems containing up to 1000 atoms for 15 ps. The points on the melting curve extracted from these simulations are in very good agreement with previous calculations, which employed the same electronic structure method but used an approach based on the explicit calculation of free energies [L. Vočadlo and D. Alfè, Phys. Rev. B, {\b…
The properties of perfect screw dislocations have been investigated for several zinc-blende materials such as diamond, Si, $β$-SiC, Ge and GaAs, by performing first principles calculations. For almost all elements, a core configuration belonging to shuffle set planes is favored, in agreement with low temperature experiments. Only for diamond, a glide configuration has the lowest defect energy, thanks to an sp$^2$ hybridization in the core.
Hybrid quantum/classical techniques can flexibly couple ab initio simulations to an empirical or elastic medium to model materials systems that cannot be contained in small periodic supercells. However, due to electronic non-locality a total energy cannot be defined, meaning energy barriers cannot be calculated. We provide a general solution using the principle of virtual work in a modified nudged elastic band algorithm. Our method enables the first ab initio calculations of the kink formation energy for <100> edge dislocations in molybdenum and lattice trapping barriers to brittle fracture in…
First-principles molecular dynamics simulations have been employed to analyze the proton diffusion in cubic BaZrO3 perovskite at 1300K, and a non-linear effect of an applied isometric strain of 2% on the lattice parameter has been observed. The structural and electronic properties of BaZrO3 are analyzed, based on Density Functional Theory calculations, and after an analysis of the electronic structure, we provide a possible explanation for an enhanced ionic conductivity, that can be caused by the formation of a preferential path for proton diffusion under compressive strain conditions.
The dynamic structures of the cubic and tetragonal phase in BaTiO3 and its dielectric response above the cubic-to-tetragonal phase transition temperature (Tp) are studied by first-principles molecular dynamics (MD) simulation. It's shown that the phase transition is due to the condensation of one of the transverse correlations. Calculation of the phonon properties for both the cubic and tetragonal phase shows a saturation of the soft mode frequency near 60 cm-1 near Tp and advocates its order-disorder nature. Our first-principles calculation leads directly to a two modes feature of the dielect…
Using the catalytic CO oxidation at RuO2(110) as a showcase, we employ first-principles kinetic Monte Carlo simulations to illustrate the intricate effects on temperature programmed reaction spectroscopy data brought about by the mere correlations between the locations of the active sites at a nanostructured surface. Even in the absence of lateral interactions, this nanostructure alone can cause inhomogeneities that cannot be grasped by prevalent mean-field data analysis procedures, which thus lead to wrong conclusions on the reactivity of the different surface species.
A newly developed fast molecular-dynamics method is applied to BaTiO3 ferroelectric thin-film capacitors with short-circuited electrodes or under applied voltage. The molecular-dynamics simulations based on a first-principles effective Hamiltonian clarify that dead layers (or passive layers) between ferroelectrics and electrodes markedly affect the properties of capacitors, and predict that the system is unable to hop between a uniformly polarized ferroelectric structure and a striped ferroelectric domain structure at low temperatures. Simulations of hysteresis loops of thin-film capacitors ar…
First principles calculations based on density functional theory are performed to investigate the structural, electronic and magnetic properties of wurtzite ZnO/NiO (0001) interface. By using DFT+U method we discover that the half-metallic behavior of wurtzite NiO (w-NiO) retains in the ZnO/NiO (0001) interface. Through analyses of density of state, charge population and magnetic moments, we find the half-metallicity is weakened around the interface but interface effect is quite localized. More over the interface system keeps a ferromagnetic ground state as bulk w-NiO does. Based on the simula…
The properties of hot dense helium at megabar pressures were studied with two first-principles computer simulation techniques, path integral Monte Carlo and density functional molecular dynamics. The simulations predicted that the compressibility of helium is substantially increased by electronic excitations that are present in the hot fluid at thermodynamic equilibrium. A maximum compression ratio of 5.24(4)-fold the initial density was predicted for 360 GPa and 150000 K. This result distinguishes helium from deuterium, for which simulations predicted a maximum compression ratio of 4.3(1). Hu…
We have implemented non-collinear GGA and a generalized Bloch's theorem to simulate unconmensurate spiral arrangements of spins in a Density Functional Theory code based on localized wave functions. We have subsequently performed a thorough study of the different states of bulk Iron. We determine the minimal basis set required to obtain reliable orderings of ground and excited states. We find that the most stable fcc phase is a spiral with an equilibrium lattice constant 3.56 A.
We report first-principles calculations, within the density functional theory, on the structural and energetic properties of 180$^\circ$ stripe domains in (PbTiO$_{3}$)$_{n}$/(SrTiO$_{3}$)$_{n}$ superlattices. For the explored periodicities ($n$=3 and 6) we find that the polydomain structures compete in energy with the monodomain phases. Our results suggest the progressive transition, as a function of $n$, from a strong to a weak electrostatic coupling regime between the SrTiO$_{3}$ and PbTiO$_{3}$ layers. Structurally, they display continuous rotation of polarization connecting 180$^\circ$ do…
The mean-free-paths (MFPs) of energy carriers are of critical importance to the nano-engineering of better thermoelectric materials. Despite significant progress in the first-principles-based understanding of the spectral distribution of phonon MFPs in recent years, the spectral distribution of electron MFPs remains unclear. In this work, we compute the energy dependent electron scatterings and MFPs in silicon from first-principles. The electrical conductivity accumulation with respect to electron MFPs is compared to that of the phonon thermal conductivity accumulation to illustrate the quanti…
Transition metal carbides include a wide variety of materials with attractive properties that are suitable for numerous and diverse applications. Most recent experimental advance could provide a path toward successful synthesis of large-area and high-quality ultrathin Mo2C membranes with superconducting properties. In the present study, we used first-principles density functional theory calculations to explore the mechanical and optical response of single-layer and free-standing Mo2C. Uniaxial tensile simulations along the armchair and zigzag directions were conducted and we found that while t…
We present a density-functional theory based kinetic Monte Carlo study of CO oxidation at the (111) facet of RuO$_2$. We compare the detailed insight into elementary processes, steady-state surface coverages and catalytic activity to equivalent published simulation data for the frequently studied RuO$_2$(110) facet. Qualitative differences are identified in virtually every aspect ranging from binding energetics over lateral interactions to the interplay of elementary processes at the different active sites. Nevertheless, particularly at technologically relevant elevated temperatures, near-ambi…
Electron microscopy is a powerful tool for studying the properties of materials down to their atomic structure. In many cases, the quantitative interpretation of images requires simulations based on atomistic structure models. These typically use the independent atom approximation that neglects bonding effects, which may, however, be measurable and of physical interest. Since all electrons and the nuclear cores contribute to the scattering potential, simulations that go beyond this approximation have relied on computationally highly demanding all-electron calculations. Here, we describe a new …
Quantum molecular dynamic simulations have been employed to study the equation of state (EOS) of fluid helium under shock compressions. The principal Hugoniot is determined from EOS, where corrections from atomic ionization are added onto the calculated data. Our simulation results indicate that principal Hugoniot shows good agreement with gas gun and laser driven experiments, and maximum compression ratio of 5.16 is reached at 106 GPa.
Using an effective Hamiltonian parametrized from first principles, Monte Carlo simulations are performed in order to study the piezoelectric response of BaTiO3 in the ferroelectric tetragonal phase as a function of temperature. The effect of an electric field on the phase behavior is also illustrated by a simulation of the transformation of a rhombohedral domain into a tetragonal one under a strong field.
Second Harmonic Generation (SHG) of single-layer monochalcogenides, such as GaSe and InSe, has been recently reported [2D Mater. 5 (2018) 025019; J. Am. Chem. Soc. 2015, 137, 79947997] to be extremely strong with respect to bulk and multilayer forms. To clarify the origin of this strong SHG signal, we perform first-principles real-time simulations of linear and non-linear optical properties of these two-dimensional semiconducting materials. The simulations, based on ab-initio many-body theory, accurately treat the electron-hole correlation and capture excitonic effects that are deemed importan…
The extreme sensitivity of 2D materials to defects and nanostructure requires precise imaging techniques to verify presence of desirable and absence of undesirable features in the atomic geometry. Helium-ion beams have emerged as a promising materials imaging tool, achieving up to 20 times higher resolution and 10 times larger depth-of-field than conventional or environmental scanning electron microscopes. Here, we offer first-principles theoretical insights to advance ion-beam imaging of atomically thin materials by performing real-time time-dependent density functional theory simulations of …
The Earth's core consists of a solid ball with a radius of 1221 Km, surrounded by a liquid shell which extends up to 3480 Km from the centre of the planet, roughly half way towards the surface (the mean radius of the Earth is 6373 km). The main constituent of the core is iron, and therefore the melting temperature of iron at the pressure encountered at the boundary between the solid and the liquid (the ICB) provides an estimate of the temperature of the core. Here I report the melting temperature of Fe at pressures near that of the ICB, obtained with first principles techniques based on densit…
It is well established that it is possible to switch certain antiferromagnets electrically, yet the interplay of Néel-spin-orbit torques and thermal activation is only poorly understood. Combining ab initio calculations and atomistic spin dynamics simulations we develop a multiscale model to study the current induced switching in Mn2Au. We compute from first principles the strength and direction of the electrically induced magnetic moments, caused by the Rashba--Edelstein effect, and take these into account in atomistic spin dynamics simulations. Our simulations reveal the switching paths as w…
Surface doping of ZnO allows for tailoring the surface chemistry of the material while preserving the superb electronic structure of the bulk. Apart from obvious changes in adsorption energies and activation energies for catalysis, surface doping can alter the workfunction of the material and allow it to be tuned for specific photocatalytic and optoelectronic applications. We present first-principles electronic structure calculations for surface doping of Mn on the ZnO (0001) surface. Various dopant concentrations have been considered at the out-most (surface) layer of Zn atoms, while the inte…
We present the first-principles determination of electronic stopping power for protons and α particles in a semiconductor material of great technological interest: silicon carbide. The calculations are based on nonequilibrium simulations of the electronic response to swift ions using real-time, time-dependent density functional theory (RT-TDDFT). We compare the results from this first-principles approach to those of the widely used linear response formalism and determine the ion velocity regime within which linear response treatments are appropriate. We also use the nonequilibrium electron den…
We formulate and implement Cyclic Density Functional Theory (Cyclic DFT) -- a self-consistent first principles simulation method for nanostructures with cyclic symmetries. Using arguments based on Group Representation Theory, we rigorously demonstrate that the Kohn-Sham eigenvalue problem for such systems can be reduced to a fundamental domain (or cyclic unit cell) augmented with cyclic-Bloch boundary conditions. Analogously, the equations of electrostatics appearing in Kohn-Sham theory can be reduced to the fundamental domain augmented with cyclic boundary conditions. By making use of this sy…
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 p…
