Optical spin pumping induced pseudo-magnetic field in two dimensional heterostructures

Two dimensional heterostructures are likely to provide new avenues for the manipulation of magnetization that is crucial for spintronics or magnetoelectronics. Here, we demonstrate that optical spin pumping can generate a large effective magnetic field in two dimensional MoSe2/WSe2 heterostructures. We determine the strength of the generated field by polarization-resolved measurement of the interlayer exciton photoluminescence spectrum: the measured splitting exceeding 10 milli-electron volts (meV) between the emission originating from the two valleys corresponds to an effective magnetic field of ~ 30 T. The strength of this optically induced field can be controlled by the excitation light polarization. Our finding opens up new possibilities for optically controlled spintronic devices based on van der Waals heterostructures

Stacking sequence determines Raman intensities of observed interlayer shear modes in 2D layered materials - A general bond polarizability model

2D layered materials have recently attracted tremendous interest due to their fascinating properties and potential applications. The interlayer interactions are much weaker than the intralayer bonds, allowing the as-synthesized materials to exhibit different stacking sequences (e.g. ABAB, ABCABC), leading to different physical properties. Here, we show that regardless of the space group of the 2D material, the Raman frequencies of the interlayer shear modes observed under the typical configuration blue shift for AB stacked materials, and red shift for ABC stacked materials, as the number of layers increases. Our predictions are made using an intuitive bond polarizability model which shows that stacking sequence plays a key role in determining which interlayer shear modes lead to the largest change in polarizability (Raman intensity); the modes with the largest Raman intensity determining the frequency trends. We present direct evidence for these conclusions by studying the Raman modes in few layer graphene, MoS2, MoSe2, WSe2 and Bi2Se3, using both first principles calculations and Raman spectroscopy. This study sheds light on the influence of stacking sequence on the Raman intensities of intrinsic interlayer modes in 2D layered materials in general, and leads to a practical way of identifying the stacking sequence in these materials.Comment: 30 pages, 8 figure

Top-Down Structure and Device Fabrication using \u3ci\u3eIn Situ\u3c/i\u3e Nanomachining

We demonstrate the potential of an alternative tool for the fabrication of nanoscale structures and devices. A nanoindenter integrated with an atomic force microscope is shown to be a powerful machine tool for cutting precise length nanowires or nanobelts and for manipulating the shortened wires. We also demonstrate its utility in cutting grooves and fabricating dents (or periodic arrays of dents) in ZnSnanobelts. This approach permits the direct mechanical machining of nanodevices that are supported on a substrate without the inherent complications of e beam or photolithography

Observation of forbidden phonons and dark excitons by resonance Raman scattering in few-layer WS2_2

The optical properties of the two-dimensional (2D) crystals are dominated by tightly bound electron-hole pairs (excitons) and lattice vibration modes (phonons). The exciton-phonon interaction is fundamentally important to understand the optical properties of 2D materials and thus help develop emerging 2D crystal based optoelectronic devices. Here, we presented the excitonic resonant Raman scattering (RRS) spectra of few-layer WS$_2$ excited by 11 lasers lines covered all of A, B and C exciton transition energies at different sample temperatures from 4 to 300 K. As a result, we are not only able to probe the forbidden phonon modes unobserved in ordinary Raman scattering, but also can determine the bright and dark state fine structures of 1s A exciton. In particular, we also observed the quantum interference between low-energy discrete phonon and exciton continuum under resonant excitation. Our works pave a way to understand the exciton-phonon coupling and many-body effects in 2D materials.Comment: 14 pages, 11 figure

Exciton polariton critical non-Hermitian skin effect with spin-momentum-locked gains

The critical skin effect, an intriguing phenomenon in non-Hermitian systems, displays sensitivity to system size and manifests distinct dynamical behaviors. In this work, we propose a novel scheme to achieve the critical non-Hermitian skin effect of exciton polaritons in an elongated microcavity system. We show that by utilising longitudinal-transverse spin splitting and spin-momentum-locked gain, a critical non-Hermitian skin effect can be achieved in a continuous system without the need of an underlying lattice. We find that a phase transition can be induced by changing the cavity detuning with respect to the exciton energy. We identify a measurable order parameter associated with this phase transition and demonstrate the corresponding critical behavior. Our work offers a flexible approach to manipulate non-Hermitian phases of exciton polaritons, thereby expanding the potential applications of polaritonic devices

Chiral plasmonics and enhanced chiral light-matter interactions

International audienceChirality, which describes the broken mirror symmetry in geometric structures, exists macroscopically in our daily life as well as microscopically down to molecular levels. Correspondingly, chiral molecules interact differently with circularly polarized light exhibiting opposite handedness (left-handed and right-handed). However, the interaction between chiral molecules and chiral light is very weak. In contrast, artificial chiral plasmonic structures can generate “super-chiral” plasmonic near-field, leading to enhanced chiral light-matter (or chiroptical) interactions. The “super-chiral” near-field presents different amplitude and phase under opposite handedness incidence, which can be utilized to engineer linear and nonlinear chiroptical interactions. Specifically, in the interaction between quantum emitters and chiral plasmonic structures, the chiral hot spots can favour the emission with a specific handedness. This article reviews the state-of-the-art research on the design, fabrication and chiroptical response of different chiral plasmonic nanostructures or metasurfaces. This review also discusses enhanced chiral light-matter interactions that are essential for applications like chirality sensing, chiral selective light emitting and harvesting. In the final part, the review ends with a perspective on future directions of chiral plasmonics

Impact of bright-dark exciton thermal population mixing on the brightness of CsPbBr3_3 nanocrystals

Understanding the interplay between bright and dark exciton states is crucial for deciphering the luminescence properties of low-dimensional materials. The origin of the outstanding brightness of lead halide perovskites remains elusive. Here, we analyse temperature-dependent time-resolved photoluminescence to investigate the population mixing between bright and dark exciton sublevels in individual CsPbBr$_3$ nanocrystals in the intermediate confinement regime. We extract bright and dark exciton decay rates, and show quantitatively that the decay dynamics can only be reproduced with second-order phonon transitions. Furthermore, we find that any exciton sublevel ordering is compatible with the most likely population transfer mechanism. The remarkable brightness of lead halide perovskite nanocrystals rather stems from a reduced asymmetry between bright-to-dark and dark-to-bright conversion originating from the peculiar second-order phonon-assisted transitions that freeze bright-dark conversion at low temperature together with the very fast radiative recombination and favourable degeneracy of the bright exciton state

Anomalous Frequency Trends in MoS2 Thin Films Attributed to Surface Effects

The layered dichalcogenide MoS2 has many unique physical properties in low dimensions. Recent experimental Raman spectroscopies report an anomalous blue shift of the in-plane E2g1 mode with decreasing thickness, a trend that is not understood. Here, we combine experimental Raman scattering and theoretical studies to clarify and explain this trend. Special attention is given to understanding the surface effect on Raman frequencies by using a force constants model based on first-principles calculations. Surface effects refer to the larger Mo-S force constants at the surface of thin film MoS2, which results from a loss of neighbours in adjacent MoS2 layers. Without surface effects, the frequencies of both out-of-plane A1g and in-plane E2g1 modes decrease with decreasing thickness. However, the E2g1 mode blue shifts while the A1g mode red shifts once the surface effect is included, in agreement with the experiment. Our results show that competition between the thickness effect and the surface effect determines the mechanical properties of two-dimensional MoS2, which we believe applies to other layered materials