Nonlinear Photoluminescence in Atomically Thin Layered WSe2 Arising from Diffusion-Assisted Exciton-Exciton Annihilation

We studied multi-exciton dynamics in monolayer WSe2 using nonlinear photoluminescence (PL) spectroscopy and Monte Carlo simulations. We observed strong nonlinear saturation behavior of exciton PL with increasing excitation power density, and long-distance exciton diffusion reaching several micrometers. We demonstrated that the diffusion-assisted exciton-exciton annihilation model accounts for the observed nonlinear PL behavior. The long-distance exciton diffusion and subsequent efficient exciton-exciton annihilation process determined the unusual multi-exciton dynamics in atomically thin layered transition metal dichalcogenides

Nonlinear magnetotransport shaped by Fermi surface topology and convexity in WTe2

The nature of Fermi surface defines the physical properties of conductors and many physical phenomena can be traced to its shape. Although the recent discovery of a current-dependent nonlinear magnetoresistance in spin-polarized non-magnetic materials has attracted considerable attention in spintronics, correlations between this phenomenon and the underlying fermiology remain unexplored. Here, we report the observation of nonlinear magnetoresistance at room temperature in a semimetal WTe2, with an interesting temperature-driven inversion. Theoretical calculations reproduce the nonlinear transport measurements and allow us to attribute the inversion to temperature-induced changes in Fermi surface convexity. We also report a large anisotropy of nonlinear magnetoresistance in WTe2, due to its low symmetry of Fermi surfaces. The good agreement between experiments and theoretical modeling reveals the critical role of Fermi surface topology and convexity on the nonlinear magneto-response. These results lay a new path to explore ramifications of distinct fermiology for nonlinear transport in condensed-matter

Measuring valley polarization in two-dimensional materials with second-harmonic spectroscopy

A population imbalance at different valleys of an electronic system lowers its effective rotational symmetry. We introduce a technique to measure such imbalance - a valley polarization - that exploits the unique fingerprints of this symmetry reduction in the polarization-dependent second-harmonic generation (SHG). We present the principle and detection scheme in the context of hexagonal two-dimensional crystals, which include graphene-based systems and the family of transition metal dichalcogenides, and provide a direct experimental demonstration using a 2H-MoSe$_{2}$ monolayer at room temperature. We deliberately use the simplest possible setup, where a single pulsed laser beam simultaneously controls the valley imbalance and tracks the SHG process. We further developed a model of the transient population dynamics which analytically describes the valley-induced SHG rotation in very good agreement with the experiment. In addition to providing the first experimental demonstration of the effect, this work establishes a conceptually simple, com-pact and transferable way of measuring instantaneous valley polarization, with direct applicability in the nascent field of valleytronics

Transient magneto-optical spectrum of photoexcited electrons in the van der Waals ferromagnet Cr2Ge2Te6

Femtosecond optical control of magnetic materials shows promise for future ultrafast data storage devices. To date, most studies in this area have relied on quasimonochromatic light in magneto-optical pump-probe experiments, which limited their ability to probe semiconducting and molecule-based materials with structured optical spectra. Here, we demonstrate the possibility of extracting the magneto-optical spectrum of the electrons in the conduction band in the two-dimensional van der Waals ferromagnet Cr2Ge2Te6 (CGT), which is made possible due to broadband probing in the visible spectrum. The magneto-optical signal is a sum of contributions from electrons in the conduction and valence bands, which are of opposite sign for CGT. Depending on the probe wavelength used, this difference could lead to an erroneous interpretation that the magnetization direction is reversed after excitation, which has important consequences for understanding spin toggle switching phenomena