Gerd Plechinger

Raman spectroscopy of the interlayer shear mode in few-layer MoS2 flakes

Single- and few-layer MoS2 has recently gained attention as an interesting material system for opto-electronics. Here, we report on scanning Raman measurements on few-layer MoS2 flakes prepared by exfoliation. We observe a Raman mode corresponding to a rigid shearing oscillation of adjacent layers. This mode appears at very low Raman shifts between 20 and 30 cm−1. Its position strongly depends on the number of layers, which we independently determine using atomic force microscopy and investigation of the other characteristic Raman modes. Raman spectroscopy of the shear mode, therefore, is a useful tool to determine the number of layers for few-layer MoS2 flakes.

Resonant internal quantum transitions and femtosecond radiative decay of excitons in monolayer WSe2

Atomically thin two-dimensional crystals have revolutionized materials science. In particular, monolayer transition metal dichalcogenides promise novel optoelectronic applications, owing to their direct energy gaps in the optical range. Their electronic and optical properties are dominated by Coulomb-bound electron-hole pairs called excitons, whose unusual internal structure, symmetry, many-body effects and dynamics have been vividly discussed. Here we report the first direct experimental access to all 1s A excitons, regardless of momentum--inside and outside the radiative cone--in single-layer WSe2. Phase-locked mid-infrared pulses reveal the internal orbital 1s-2p resonance, which is highly sensitive to the shape of the excitonic envelope functions and provides accurate transition energies, oscillator strengths, densities and linewidths. Remarkably, the observed decay dynamics indicates an ultrafast radiative annihilation of small-momentum excitons within 150 fs, whereas Auger recombination prevails for optically dark states. The results provide a comprehensive view of excitons and introduce a new degree of freedom for quantum control, optoelectronics and valleytronics of dichalcogenide monolayers.

Identification of excitons, trions and biexcitons in single-layer WS2

Single-layer WS

Low-temperature photoluminescence of oxide-covered single-layer MoS2

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Trion fine structure and coupled spin–valley dynamics in monolayer tungsten disulfide

is a direct-gap semiconductor showing strong excitonic photoluminescence features in the visible spectral range. Here, we present temperature-dependent photoluminescence measurements on mechanically exfoliated single-layer WS

A direct comparison of CVD-grown and exfoliated MoS2 using optical spectroscopy

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Control of biaxial strain in single-layer molybdenite using local thermal expansion of the substrate

, revealing the existence of neutral and charged excitons at low temperatures as well as at room temperature. By applying a gate voltage, we can electrically control the ratio of excitons and trions and assert a residual n-type doping of our samples. At high excitation densities and low temperatures, an additional peak at energies below the trion dominates the photoluminescence, which we identify as biexciton emission.

Excitonic Valley Effects in Monolayer WS2 under High Magnetic Fields

We present a photoluminescence study of single-layer MoS2 flakes on SiO2 surfaces. We demonstrate that the luminescence peak position of flakes prepared from natural MoS2, which varies by up to 25 meV between individual flakes, can be homogenized by annealing in vacuum. We use HfO2 and Al2O3 layers prepared by atomic layer deposition to cover some of our flakes. In these flakes, we observe a suppression of the low-energy luminescence peak which appears in asprepared flakes at low temperatures. We infer that this peak originates from excitons bound to surface adsorbates. We also observe different temperature-induced shifts of the luminescence peaks for the oxide-covered flakes. This effect stems from the different thermal expansion coefficients of the oxide layers and the MoS2 flakes. It indicates that the single-layer MoS2 flakes strongly adhere to the oxide layers and are therefore strained. (© 2012 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim)

Observation of anisotropic interlayer Raman modes in few-layer ReS2

Monolayer transition-metal dichalcogenides have recently emerged as possible candidates for valleytronic applications, as the spin and valley pseudospin are directly coupled and stabilized by a large spin splitting. The optical properties of these two-dimensional crystals are dominated by tightly bound electron–hole pairs (excitons) and more complex quasiparticles such as charged excitons (trions). Here we investigate monolayer WS2 samples via photoluminescence and time-resolved Kerr rotation. In photoluminescence and in energy-dependent Kerr rotation measurements, we are able to resolve two different trion states, which we interpret as intravalley and intervalley trions. Using time-resolved Kerr rotation, we observe a rapid initial valley polarization decay for the A exciton and the trion states. Subsequently, we observe a crossover towards exciton–exciton interaction-related dynamics, consistent with the formation and decay of optically dark A excitons. By contrast, resonant excitation of the B exciton transition leads to a very slow decay of the Kerr signal.

Interlayer exciton dynamics in a dichalcogenide monolayer heterostructure

MoS2 is a highly interesting material, which exhibits a crossover from an indirect band gap in the bulk crystal to a direct gap for single layers. Here, we perform a direct comparison between large-area MoS2 films grown by chemical vapor deposition (CVD) and MoS2 flakes prepared by mechanical exfoliation from mineral bulk crystal. Raman spectroscopy measurements show differences between the in-plane and out-of-plane phonon mode positions in CVD-grown and exfoliated MoS2. Photoluminescence (PL) mapping reveals large regions in the CVD-grown films that emit strong PL at room-temperature, and low-temperature PL scans demonstrate a large spectral shift of the A exciton emission as a function of position. Polarization-resolved PL measurements under near-resonant excitation conditions show a strong circular polarization of the PL, corresponding to a valley polarization.