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Y. H. Bai

Publications and source records attributed to Y. H. Bai.

27 records · Page 2Linked to original sources

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↗

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↗

Superintermolecular orbitals in the C$_{60}$/pentacene complex

We report a group of unusually big molecular orbitals in the C60/pentacene complex. Our first-principles density functional calculation shows that these orbitals are very delocalized and cover both C60 and pentacene, which we call superintermolecular orbitals or SIMOs. Their spatial extension can reach 1 nm or larger. Optically, SIMOs are dark. Different from ordinary unoccupied molecular orbitals, SIMOs have a very weak Coulomb and exchange interaction. Their energy levels are very similar to the native superatomic molecular orbitals in C60, and can be approximately characterized by orbital angular momentum quantum numbers. They have a distinctive spatial preference. These features fit the key characters of charge-generation states that channel initially-bound electrons and holes into free charge carriers. Thus, our finding is important for C60/pentacene photovoltaics.

cond-mat.mtrl-sci↗

Presence of Exotic Electronic Surface States in LaBi and LaSb

Extremely high magnetoresistance (XMR) in the lanthanum monopnictides La$X$ ($X$ = Sb, Bi) has recently attracted interest in these compounds as candidate topological materials. However, their perfect electron-hole compensation provides an alternative explanation, so the possible role of topological surface states requires verification through direct observation. Our angle-resolved photoemission spectroscopy (ARPES) data reveal multiple Dirac-like surface states near the Fermi level in both materials. Intriguingly, we have observed circular dichroism in both surface and near-surface bulk bands. Thus the spin-orbit coupling-induced orbital and spin angular momentum textures may provide a mechanism to forbid backscattering in zero field, suggesting that surface and near-surface bulk bands may contribute strongly to XMR in La$X$. The extremely simple rock salt structure of these materials and the ease with which high-quality crystals can be prepared suggests that they may be an ideal platform for further investigation of topological matter.

cond-mat.str-el↗

All-optical spin switching: A new frontier in femtomagnetism -- A short review and a simple theory

Using an ultrafast laser pulse to manipulate the spin degree of freedom has broad technological appeal. It allows one to control the spin dynamics on a femtosecond time scale. The discipline, commonly called femtomagnetism, started with the pioneering experiment by Beaurepaire and coworkers in 1996, who showed subpicosecond demagnetization occurs in magnetic Ni thin films. This finding has motivated extensive research worldwide. All-optical helicity-dependent spin switching (AOS) represents a new frontier in femtomagnetism, where a single ultrafast laser pulse can permanently switch spin without any assistance from a magnetic field. This review summarizes some of the crucial aspects of this new discipline: key experimental findings, leading mechanisms, controversial issues, and possible future directions. The emphasis is on our latest investigation. We first develop the all-optical spin switching rule that determines how the switchability depends on the light helicity. This rule allows one to understand microscopically how the spin is reversed and why the circularly polarized light appears more powerful than the linearly polarized light. Then we invoke our latest spin-orbit coupled harmonic oscillator model to simulate single spin reversal. We consider both cw excitation and pulsed laser excitation. The results are in a good agreement with the experimental result. We then extend the code to include the exchange interaction among different spin sites. We show where the "inverse Faraday field" comes from and how the laser affects the spin reversal nonlinearly. Our hope is that this review will motivate new experimental and theoretical investigations and discussions.

cond-mat.mtrl-sci↗

Switching ferromagnetic spins by an ultrafast laser pulse: Emergence of giant optical spin-orbit torque

Faster magnetic recording technology is indispensable to massive data storage and big data sciences. {All-optical spin switching offers a possible solution}, but at present it is limited to a handful of expensive and complex rare-earth ferrimagnets. The spin switching in more abundant ferromagnets may significantly expand the scope of all-optical spin switching. Here by studying 40,000 ferromagnetic spins, we show that it is the optical spin-orbit torque that determines the course of spin switching in both ferromagnets and ferrimagnets. Spin switching occurs only if the effective spin angular momentum of each constituent in an alloy exceeds a critical value. Because of the strong exchange coupling, the spin switches much faster in ferromagnets than weakly-coupled ferrimagnets. This establishes a paradigm for all-optical spin switching. The resultant magnetic field (65 T) is so big that it will significantly reduce high current in spintronics, thus representing the beginning of photospintronics.

cond-mat.mtrl-sci↗

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↗

Magnetic spin moment reduction in photoexcited ferromagnets through exchange interaction quenching: Beyond the rigid band approximation

The exchange interaction among electrons is one of the most fundamental quantum mechanical interactions in nature and underlies any magnetic phenomena from ferromagnetic ordering to magnetic storage. The current technology is built upon a thermal or magnetic field, but a frontier is emerging to directly control magnetism using ultrashort laser pulses. However, little is known about the fate of the exchange interaction. Here we report unambiguously that photoexcitation is capable of quenching the exchange interaction in all three $3d$ ferromagnetic metals. The entire process starts with a small number of photoexcited electrons which build up a new and self-destructive potential that collapses the system into a new state with a reduced exchange splitting. The spin moment reduction follows a Bloch-like law as $M_z(ΔE)=M_z(0)(1-{ΔE}/{ΔE_0})^{\frac{1}β}$, where $ΔE$ is the absorbed photon energy and $β$ is a scaling exponent. A good agreement is found between the experimental and our theoretical results. Our findings may have a broader implication for dynamic electron correlation effects in laser-excited iron-based superconductors, iron borate, rare-earth orthoferrites, hematites and rare-earth transition metal alloys.

cond-mat.mtrl-sci↗

Imaging superatomic molecular orbitals in a ${\bf C_{60}}$ molecule through four 800-nm photons

Superatomic molecular orbitals (SAMO) in C60 are ideal building blocks for functional nanostructures. However, imaging them spatially in the gas phase has been unsuccessful. It is found experimentally that if C60 is excited by an 800-nm laser, the photoelectron casts an anisotropic velocity image, but the image becomes isotropic if excited at a 400-nm wavelength. This diffuse image difference has been attributed to electron thermal ionization, but more recent experiments (800 nm) reveal a clear non-diffuse image superimposed on the diffuse image, whose origin remains a mystery. Here we show that the non-diffuse anisotropic image is the precursor of the $f$ SAMO. We predict that four 800-nm photons can directly access the $1f$ SAMO, and with one more photon, can image the orbital, with the photoelectron angular distribution having two maxima at 0$^\circ$ and 180$^\circ$ and two humps separated by 56.5$^\circ$. Since two 400-nm photons only resonantly excite the spherical $1s$ SAMO and four 800-nm photon excite the anisotropic $1f$ SAMO, our finding gives a natural explanation of the non-diffuse image difference, complementing the thermal scenario.

cond-mat.mtrl-sci↗