Strained Monolayer MoTe2 as a Photon Absorber in the Telecom Range.

To achieve the atomistic control of two-dimensional materials for emerging technological applications, such as valleytronics, spintronics, and single-photon emission, it is of paramount importance to gain an in-depth understanding of their structure-property relationships. In this work, we present a systematic analysis, carried out in the framework of density-functional theory, on the influence of uniaxial strain on the electronic and optical properties of monolayer MoTe2. By spanning a ±10% range of deformation along the armchair and zigzag direction of the two-dimensional sheet, we inspect how the fundamental gap, the dispersion of the bands, the frontier states, and the charge distribution are affected by strain. Under tensile strain, the system remains a semiconductor but a direct-to-indirect band gap transition occurs above 7%. Compressive strain, instead, is highly direction-selective. When it is applied along the armchair edge, the material remains a semiconductor, while along the zigzag direction a semiconductor-to-metal transition happens above 8%. The characteristics of the fundamental gap and wave function distribution are also largely dependent on the strain direction, as demonstrated by a thorough analysis of the band structure and of the charge density. Additional ab initio calculations based on many-body perturbation theory confirm the ability of strained MoTe2 to absorb radiation in the telecom range, thus suggesting the application of this material as a photon absorber upon suitable strain modulation.

Phonon-driven intra-exciton Rabi oscillations in CsPbBr3 halide perovskites.

Coupling electromagnetic radiation with matter, e.g., by resonant light fields in external optical cavities, is highly promising for tailoring the optoelectronic properties of functional materials on the nanoscale. Here, we demonstrate that even internal fields induced by coherent lattice motions can be used to control the transient excitonic optical response in CsPbBr3 halide perovskite crystals. Upon resonant photoexcitation, two-dimensional electronic spectroscopy reveals an excitonic peak structure oscillating persistently with a 100-fs period for up to ~2 ps which does not match the frequency of any phonon modes of the crystals. Only at later times, beyond 2 ps, two low-frequency phonons of the lead-bromide lattice dominate the dynamics. We rationalize these findings by an unusual exciton-phonon coupling inducing off-resonant 100-fs Rabi oscillations between 1s and 2p excitons driven by the low-frequency phonons. As such, prevailing models for the electron-phonon coupling in halide perovskites are insufficient to explain these results. We propose the coupling of characteristic low-frequency phonon fields to intra-excitonic transitions in halide perovskites as the key to control the anharmonic response of these materials in order to establish new routes for enhancing their optoelectronic properties.