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Register a new userAll-Optical Control of Magnetization in Quantum-Confined Ultrathin Magnetic Metals
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Saeedeh Mokarian Zanjani
Publication date
2021
fields
Physics
and research's language is
English
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All-optical control dynamics of magnetization in sub-10 nm metallic thin films are investigated, as these films with quantum confinement undergo unique interactions with femtosecond laser pulses. Our theoretical derivations based on the free electron model show that the density of states at Fermi level (DOS_F) and electron-phonon coupling coefficients (G_ep) in ultrathin metals have very high sensitivity to film thickness within a few Angstroms. As DOS_F and G_ep depend on thickness, we show that completely different magnetization dynamics characteristics emerge compared with bulk metals. Our model suggests highly-efficient energy transfer from fs laser photons to spin waves due to minimal energy absorption by phonon. This sensitivity to thickness and efficient energy transfer offers an opportunity to obtain ultrafast on-chip magnetization dynamics.
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We resolve a significant controversy about how to understand and engineer single-shot all-optical switching of magnetization in ferrimagnets using femto- or picosecond-long heat pulses. By realistically modelling a generic ferrimagnet as two coupled macrospins, we comprehensively show that the net magnetization can be reversed via different pathways, using a heat pulse with duration spanning all relevant timescales within the non-adiabatic limit. This conceptual understanding is fully validated by experiments studying the material and optical limits at which the switching process in GdFeCo alloys loses its reliability. Our interpretation and results constitute a blueprint for understanding how deterministic all-optical switching can be achieved in alternative ferrimagnets using short thermal pulses.
Spatially indirect Type-II band alignment in magnetically-doped quantum dot (QD) structures provides unexplored opportunities to control the magnetic interaction between carrier wavefunction in the QD and magnetic impurities. Unlike the extensively studied, spatially direct, QDs with Type-I band alignment where both electrons and holes are confined in the QD, in ZnTe QDs embedded in a (Zn,Mn)Se matrix only the holes are confined in the QDs. Photoexcitation with photon energy 3.06 eV (2.54 eV) generates electron-hole pairs predominantly in the (Zn,Mn)Se matrix (ZnTe QDs). The photoluminescence (PL) at 7 K in the presence of an external magnetic field exhibits an up to three-fold increase in the saturation red shift with the 2.54 eV excitation compared to the shift observed with 3.06 eV excitation. This unexpected result is attributed to multiple hole occupancy of the QD and the resulting increased penetration of the hole wavefunction tail further into the (Zn,Mn)Se matrix. The proposed model is supported by microscopic calculations which accurately include the role of hole-hole Coulomb interactions as well as the hole-Mn spin exchange interactions.
Efficient control of a magnetization without an application of the external magnetic fields is the ultimate goal of spintronics. We demonstrate, that in monolayers of $text{CrI}_3$, magnetization can be switched all optically, by application of the resonant pulses of circularly polarized light. This happens because of the efficient coupling of the lattice magnetization with bright excitonic transition. $text{CrI}_3$ is thus perspective functional material with high potential for applications in the domains of spintronics and ultra-fast magnetic memory.
We propose an orbital magnetothermal effect wherein a temperature gradient generates an orbital magnetization (OM) for Bloch electrons, and we present a unified theory for electrically and thermally induced OM, valid for both metals and insulators. We reveal that there exists an intrinsic response of OM, for which the susceptibilities are completely determined by the band geometric quantities such as interband Berry connections, interband orbital moments, and the quantum metric. The theory can be readily combined with first-principles calculations to study real materials. As an example, we calculate the OM response in CrI$_{3}$ bilayers, where the intrinsic contribution dominates. The temperature scaling of intrinsic and extrinsic responses, the effect of phonon drag, and the phonon angular momentum contribution to OM are discussed.
Photoluminescence (PL) intermittency is a ubiquitous phenomenon detrimentally reducing the temporal emission intensity stability of single colloidal quantum dots (CQDs) and the emission quantum yield of their ensembles. Despite efforts for blinking reduction via chemical engineering of the QD architecture and its environment, blinking still poses barriers to the application of QDs, particularly in single-particle tracking in biology or in single-photon sources. Here, we demonstrate the first deterministic all-optical suppression of quantum dot blinking using a compound technique of visible and mid-infrared (MIR) excitation. We show that moderate-field ultrafast MIR pulses (5.5 $mu$m, 150 fs) can switch the emission from a charged, low quantum yield grey trion state to the bright exciton state in CdSe/CdS core-shell quantum dots resulting in a significant reduction of the QD intensity flicker. Quantum-tunneling simulations suggest that the MIR fields remove the excess charge from trions with reduced emission quantum yield to restore higher brightness exciton emission. Our approach can be integrated with existing single-particle tracking or super-resolution microscopy techniques without any modification to the sample and translates to other emitters presenting charging-induced PL intermittencies, such as single-photon emissive defects in diamond and two-dimensional materials.
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