No Arabic abstract
Transition metal dichalcogenide (TMD) materials have received enormous attention due to their extraodinary optical and electrical properties, among which MoS2 is the most typical one. As thickness increases from monolayer to multilayer, the photoluminescence (PL) of MoS2 is gradually quenched due to the direct-to-indirect band gap transition. How to enhance PL response and decrease the layer dependence in multilayer MoS2 is still a challenging task. In this work, we report, for the first time, simultaneous generation of three PL peaks at around 1.3, 1.4 and 1.8 eV on multilayer MoS2 bubbles. The temperature dependent PL measurements indicate that the two peaks at 1.3 and 1.4 eV are phonon-assisted indirect-gap transitions while the peak at 1.8 eV is the direct-gap transition. Using first-principles calculations, the band structure evolution of multilayer MoS2 under strain is studied, from which the origin of the three PL peaks of MoS2 bubbles is further confirmed. Moreover, PL standing waves are observed in MoS2 bubbles that creates Newton-Ring-like patterns. This work demonstrates that the bubble structure may provide new opportunities for engineering the electronic structure and optical properties of layered materials.
Three-dimensional topological Dirac semimetals have hitherto stimulated unprecedented research interests as a new class of quantum materials. Breaking certain types of symmetries has been proposed to enable the manipulation of Dirac fermions; and that was soon realized by external modulations such as magnetic fields. However, an intrinsic manipulation of Dirac states, which is more efficient and desirable, remains a significant challenge. Here, we report a systematic study of quasi-particle dynamics and band evolution in Cd3As2 thin films with controlled Chromium (Cr) doping by both magneto-infrared spectroscopy and electrical transport. For the first time, we observe square-root-B relation of inter-Landau-level resonance in undoped Cd3As2 Dirac semimetal, an important signature of ultra-relativistic Dirac state inaccessible in previous optical experiments. A crossover from quantum to quasi-classical behavior makes it possible to directly probe the mass of Dirac fermions. Importantly, Cr doping allows for a Dirac mass acquisition and topological phase transition enabling a desired dynamic control of Dirac fermions. Corroborating with the density-functional theory calculations, we show that the mass generation is essentially driven by explicit C4 rotation symmetry breaking and the resultant Dirac gap engineering through Cr substitution for Cd atoms. The manipulation of the system symmetry and Dirac mass in Cd3As2 thin films provides a tuning knob to explore the exotic states stemming from the parent phase of Dirac semimetals.
We show that the lack of inversion symmetry in monolayer MoS2 allows strong optical second harmonic generation. Second harmonic of an 810-nm pulse is generated in a mechanically exfoliated monolayer, with a nonlinear susceptibility on the order of 1E-7 m/V. The susceptibility reduces by a factor of seven in trilayers, and by about two orders of magnitude in even layers. A proof-of-principle second harmonic microscopy measurement is performed on samples grown by chemical vapor deposition, which illustrates potential applications of this effect in fast and non-invasive detection of crystalline orientation, thickness uniformity, layer stacking, and single-crystal domain size of atomically thin films of MoS2 and similar materials.
Competing interactions produce finite-size textures in myriad condensed matter systems, typically forming elongated stripe or round bubble domains. Transitions between stripe and bubble phases, driven by field or temperature, are expected to be reversible in nature. Here we report on the distinct character of the analogous transition for nanoscale spin textures in chiral Co/Pt-based multilayer films, known to host N{e}el skyrmions, using microscopy, magnetometry, and micromagnetic simulations. Upon increasing field, individual stripes fission into multiple skyrmions, and this transition exhibits a macroscopic signature of irreversibility. Crucially, upon field reversal, the skyrmions do not fuse back into stripes, with many skyrmions retaining their morphology down to zero field. Both the macroscopic irreversibility and the microscopic zero-field skyrmion density are governed by the thermodynamic material parameter determining chiral domain stability. These results establish the thermodynamic and microscopic framework underlying ambient skyrmion generation and stability in chiral multilayer films and provide immediate directions for their functionalization in devices.
Optoelectronic excitations in monolayer MoS2 manifest from a hierarchy of electrically tunable, Coulombic free-carrier and excitonic many-body phenomena. Investigating the fundamental interactions underpinning these phenomena - critical to both many-body physics exploration and device applications - presents challenges, however, due to a complex balance of competing optoelectronic effects and interdependent properties. Here, optical detection of bound- and free-carrier photoexcitations is used to directly quantify carrier-induced changes of the quasiparticle band gap and exciton binding energies. The results explicitly disentangle the competing effects and highlight longstanding theoretical predictions of large carrier-induced band gap and exciton renormalization in 2D semiconductors.
Spin orientation of photoexcited carriers and their energy relaxation is investigated in bulk Ge by studying spin-polarized recombination across the direct band gap. The control over parameters such as doping and lattice temperature is shown to yield high polarization degree, namely larger than 40%, as well as a fine-tuning of the angular momentum of the emitted light with a complete reversal between right- and left-handed circular polarization. By combining the measurement of the optical polarization state of band-edge luminescence and Monte Carlo simulations of carrier dynamics, we show that these very rich and complex phenomena are the result of the electron thermalization and cooling in the multi-valley conduction band of Ge. The circular polarization of the direct-gap radiative recombination is indeed affected by energy relaxation of hot electrons via the X valleys and the Coulomb interaction with extrinsic carriers. Finally, thermal activation of unpolarized L valley electrons accounts for the luminescence depolarization in the high temperature regime.