RESUMEN
Quasiparticles consisting of correlated electron(s) and hole(s), such as excitons and trions, play important roles in the optical phenomena of van der Waals semiconductors and serve as unique platforms for studies of many-body physics. Herein, we report a gate-tunable exciton-to-trion transition in pressurized monolayer MoSe2, in which the electronic band structures are modulated continuously within a diamond anvil cell. The emission energies of both the exciton and trion undergo large blueshifts over 90 meV with increasing pressure. Surprisingly, the trion binding energy remains constant at 30 meV, regardless of the applied pressure. Combining ab initio density functional theory calculations and quantum Monte Carlo simulations, we find that the remarkable robustness of the trion binding energy originates from the spatially diffused nature of the trion wave function and the weak correlation between its constituent electron-hole pairs. Our findings shed light on the optical properties of correlated excitonic quasiparticles in low-dimensional materials.
RESUMEN
Complex correlated states emerging from many-body interactions between quasiparticles (electrons, excitons and phonons) are at the core of condensed matter physics and material science. In low-dimensional materials, quantum confinement affects the electronic, and subsequently, optical properties for these correlated states. Here, by combining photoluminescence, optical reflection measurements and ab initio theoretical calculations, we demonstrate an unconventional excitonic state and its bound phonon sideband in layered silicon diphosphide (SiP2), where the bound electron-hole pair is composed of electrons confined within one-dimensional phosphorus-phosphorus chains and holes extended in two-dimensional SiP2 layers. The excitonic state and emergent phonon sideband show linear dichroism and large energy redshifts with increasing temperature. Our ab initio many-body calculations confirm that the observed phonon sideband results from the correlated interaction between excitons and optical phonons. With these results, we propose layered SiP2 as a platform for the study of excitonic physics and many-particle effects.
RESUMEN
The technological appeal of van der Waals ferromagnetic materials is the ability to control magnetism under external fields with desired thickness toward novel spintronic applications. For practically useful devices, ferromagnetism above room temperature or tunable magnetic anisotropy is highly demanded but remains challenging. To date, only a few layered materials exhibit unambiguous ferromagnetic ordering at room temperature via gating techniques or interface engineering. Here, it is demonstrated that the magnetic anisotropy control and dramatic modulation of Curie temperature (Tc ) up to 400 K are realized in layered Fe5 GeTe2 via the high-pressure diamond-anvil-cell technique. Magnetic phases manifesting with in-plane anisotropic, out-of-plane anisotropic and nearly isotropic magnetic states can be tuned in a controllable way, depicted by the phase diagram with a maximum Tc up to 360 K. Remarkably, the Tc can be gradually enhanced to above 400 K owing to the Fermi surface evolution during a pressure loading-deloading process. Such an observation sheds light on the understanding and control of emergent magnetic states in practical spintronic applications.
RESUMEN
Valence fluctuation of interacting electrons plays a crucial role in emergent quantum phenomena in correlated electron systems. The theoretical rationale is that this effect can drive a band insulator into a superconductor through charge redistribution around the Fermi level. However, the root cause of such a fluctuating leap in the ionic valency remains elusive. Here, we demonstrate a valence-skipping-driven insulator-to-superconductor transition and realize quasi-two-dimensional superconductivity in a van der Waals insulator GeP under pressure. This is shown to result from valence skipping of the Ge cation, altering its average valency from 3+ to 4+, turning GeP from a layered compound to a three-dimensional covalent system with superconducting critical temperature reaching its maximum of 10 K. Such a valence-skipping-induced superconductivity with a quasi-two-dimensional nature in thin samples, showing a Berezinskii-Kosterlitz-Thouless-like character, is further confirmed by angle-dependent upper-critical-field measurements. These findings provide a model system to examine competing order parameters in valence-skipping systems.
RESUMEN
Interlayer coupling in two-dimensional (2D) layered materials plays an important role in controlling their properties. 2H- and 3R-MoS2 with different stacking orders and the resulting interlayer coupling have been recently discovered to have different band structures and a contrast behavior in valley physics. However, the role of carrier doping in interlayer coupling in 2D materials remains elusive. Here, based on the electric double layer interface, we demonstrated the experimental observation of carrier doping-enhanced interlayer coupling in 3R-MoS2. A remarkable tuning of interlayer Raman modes can be observed by changing the stacking sequence and carrier doping near their monolayer limit. The modulated interlayer vibration modes originated from the interlayer coupling show a doping-induced blue shift and are supposed to be associated with the interlayer coupling enhancement, which is further verified using our first-principles calculations. Such an electrical control of interlayer coupling of layered materials in an electrical gating geometry provides a new degree of freedom to modify the physical properties in 2D materials.