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Register a new userMagneto-optics in transition metal diselenide monolayers
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We perform photoluminescence experiments at 4K on two different transition metal diselenide monolayers, namely MoSe2 and WSe2 in magnetic fields $B_z$ up to 9T applied perpendicular to the sample plane. In MoSe2 monolayers the valley polarization of the neutral and the charged exciton (trion) can be tuned by the magnetic field, independent of the excitation laser polarization. In the investigated WSe2 monolayer sample the evolution of the trion valley polarization depends both on the applied magnetic field and the excitation laser helicity, while the neutral exciton valley polarization depends only on the latter. Remarkably we observe a reversal of the sign of the trion polarization between WSe2 and MoSe2. For both systems we observe a clear Zeeman splitting for the neutral exciton and the trion of about $pm2$meV at $B_zmp9$T. The extracted Land{e}-factors for both exciton complexes in both materials are $gapprox -4$.
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We have investigated the exciton dynamics in transition metal dichalcogenide mono-layers using time-resolved photoluminescence experiments performed with optimized time-resolution. For MoSe2 monolayers, we measure $tau_{rad}=1.8pm0.2$ ps that we interpret as the intrinsic radiative recombination time. Similar values are found for WSe2 mono-layers. Our detailed analysis suggests the following scenario: at low temperature (T $leq$ 50 K), the exciton oscillator strength is so large that the entire light can be emitted before the time required for the establishment of a thermalized exciton distribution. For higher lattice temperatures, the photoluminescence dynamics is characterized by two regimes with very different characteristic times. First the PL intensity drops drastically with a decay time in the range of the picosecond driven by the escape of excitons from the radiative window due to exciton- phonon interactions. Following this first non-thermal regime, a thermalized exciton population is established gradually yielding longer photoluminescence decay times in the nanosecond range. Both the exciton effective radiative recombination and non-radiative recombination channels including exciton-exciton annihilation control the latter. Finally the temperature dependence of the measured exciton and trion dynamics indicates that the two populations are not in thermodynamical equilibrium.
Transition metal dichalcogenide (TMDC) monolayers are newly discovered semiconductors for a wide range of applications in electronics and optoelectronics. Most studies have focused on binary monolayers that share common properties: direct optical bandgap, spin-orbit (SO) splittings of hundreds of meV, light-matter interaction dominated by robust excitons and coupled spin-valley states of electrons. Studies on alloy-based monolayers are more recent, yet they may not only extend the possibilities for TMDC applications through specific engineering but also help understanding the differences between each binary material. Here, we synthesized highly crystalline Mo$_{(1-x)}$W$_{x}$Se$_2$ to show engineering of the direct optical bandgap and the SO coupling in ternary alloy monolayers. We investigate the impact of the tuning of the SO spin splitting on the optical and polarization properties. We show a non-linear increase of the optically generated valley polarization as a function of tungsten concentration, where 40% tungsten incorporation is sufficient to achieve valley polarization as high as in binary WSe2. We also probe the impact of the tuning of the conduction band SO spin splitting on the bright versus dark state population i.e. PL emission intensity. We show that the MoSe2 PL intensity decreases as a function of temperature by an order of magnitude, whereas for WSe2 we measure surprisingly an order of magnitude increase over the same temperature range (T=4-300K). The ternary material shows a trend between these two extreme behaviors. These results show the strong potential of SO engineering in ternary TMDC alloys for optoelectronics and applications based on electron spin- and valley-control.
Layered transition metal trichalcogenides with the chemical formula $ABX_3$ have attracted recent interest as potential candidates for two-dimensional magnets. Using first-principles calculations within density functional theory, we investigate the magnetic ground states of monolayers of Mn- and Cr-based semiconducting trichalcogenides. We show that the second and third nearest-neighbor exchange interactions ($J_2$ and $J_3$) between magnetic ions, which have been largely overlooked in previous theoretical studies, are crucial in determining the magnetic ground state. Specifically, we find that monolayer $text{CrSiTe}_3$ is an antiferromagnet with a zigzag spin texture due to significant contribution from $J_3$, whereas $text{CrGeTe}_3$ is a ferromagnet with a Curie temperature of 106 K. Monolayers of Mn-compounds ($text{MnPS}_3$ and $text{MnPSe}_3$) always show antiferromagnetic Neel order. We identify the physical origin of various exchange interactions, and demonstrate that strain can be an effective knob for tuning the magnetic properties. Possible magnetic ordering in the bulk is also discussed. Our study suggests that $text{ABX}_3$ can be a promising platform to explore 2D magnetic phenomena.
Atomically thin transition metal dichalcogenide (TMD) semiconductors hold enormous potential for modern optoelectronic devices and quantum computing applications. By inducing long-range ferromagnetism (FM) in these semiconductors through the introduction of small amounts of a magnetic dopant, it is possible to extend their potential in emerging spintronic applications. Here, we demonstrate light-mediated, room temperature (RT) FM, in V-doped WS2 (V-WS2) monolayers. We probe this effect using the principle of magnetic LC resonance, which employs a soft ferromagnetic Co-based microwire coil driven near its resonance in the radio frequency (RF) regime. The combination of LC resonance with an extraordinary giant magneto-impedance effect, renders the coil highly sensitive to changes in the magnetic flux through its core. We then place the V-WS2 monolayer at the core of the coil where it is excited with a laser while its change in magnetic permeability is measured. Notably, the magnetic permeability of the monolayer is found to depend on the laser intensity, thus confirming light control of RT magnetism in this two-dimensional (2D) material. Guided by density functional calculations, we attribute this phenomenon to the presence of excess holes in the conduction and valence bands, as well as carriers trapped in the magnetic doping states, which in turn mediates the magnetization of the V-WS2 monolayer. These findings provide a unique route to exploit light-controlled ferromagnetism in low powered 2D spintronic devices capable of operating at RT.
Using first-principles calculations, we demonstrate that an Fe monolayer can assume very different magnetic phases on hexagonal hcp (0001) and fcc (111) surfaces of 4d- and 5d-transition metals. Due to the substrates d-band filling, the nearest-neighbor exchange coupling of Fe changes gradually from antiferromagnetic (AFM) for Fe films on Tc, Re, Ru and Os to ferromagnetic on Rh, Ir, Pd, and Pt. In combination with the topological frustration on the triangular lattice of these surfaces the AFM coupling results in a 120-degree Neel structure for Fe on Re and Ru and an unexpected double-row-wise AFM structure on Rh, which is a superposition of a left- and right-rotating 90-degree spin spiral.
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