Second order resonant Raman scattering in single layer tungsten disulfide (WS2_{2})

Resonant Raman spectra of single layer WS$_{2}$ flakes are presented. A second order Raman peak (2LA) appears under resonant excitation with a separation from the E$^{1}_{2g}$ mode of only $4$cm$^{-1}$. Depending on the intensity ratio and the respective line widths of these two peaks, any analysis which neglects the presence of the 2LA mode can lead to an inaccurate estimation of the position of the E$^{1}_{2g}$ mode, leading to a potentially incorrect assignment for the number of layers. Our results show that the intensity of the 2LA mode strongly depends on the angle between the linear polarization of the excitation and detection, a parameter which is neglected in many Raman studies.Comment: 6 pages, 4 figure

Site-selective measurement of coupled spin pairs in an organic semiconductor

From organic electronics to biological systems, understanding the role of intermolecular interactions between spin pairs is a key challenge. Here we show how such pairs can be selectively addressed with combined spin and optical sensitivity. We demonstrate this for bound pairs of spin-triplet excitations formed by singlet fission, with direct applicability across a wide range of synthetic and biological systems. We show that the site sensitivity of exchange coupling allows distinct triplet pairs to be resonantly addressed at different magnetic fields, tuning them between optically bright singlet (S=0) and dark triplet quintet (S=1,2) configurations: This induces narrow holes in a broad optical emission spectrum, uncovering exchange-specific luminescence. Using fields up to 60 T, we identify three distinct triplet-pair sites, with exchange couplings varying over an order of magnitude (0.3–5 meV), each with its own luminescence spectrum, coexisting in a single material. Our results reveal how site selectivity can be achieved for organic spin pairs in a broad range of systems

Electron and hole g-factors and spin dynamics of negatively charged excitons in CdSe/CdS colloidal nanoplatelets with thick shells

We address spin properties and spin dynamics of carriers and charged excitons in CdSe/CdS colloidal nanoplatelets with thick shells. Magneto-optical studies are performed by time-resolved and polarization-resolved photoluminescence, spin-flip Raman scattering and picosecond pump-probe Faraday rotation in magnetic fields up to 30 T. We show that at low temperatures the nanoplatelets are negatively charged so that their photoluminescence is dominated by radiative recombination of negatively charged excitons (trions). Electron g-factor of 1.68 is measured and heavy-hole g-factor varying with increasing magnetic field from -0.4 to -0.7 is evaluated. Hole g-factors for two-dimensional structures are calculated for various hole confining potentials for cubic- and wurtzite lattice in CdSe core. These calculations are extended for various quantum dots and nanoplatelets based on II-VI semiconductors. We developed a magneto-optical technique for the quantitative evaluation of the nanoplatelets orientation in ensemble

Addressing the exciton fine structure in colloidal nanocrystals: the case of CdSe nanoplatelets

We study the band-edge exciton fine structure and in particular its bright-dark splitting in colloidal semiconductor nanocrystals by four different optical methods based on fluorescence line narrowing and time-resolved measurements at various temperatures down to 2 K. We demonstrate that all these methods provide consistent splitting values and discuss their advances and limitations. Colloidal CdSe nanoplatelets with thicknesses of 3, 4 and 5 monolayers are chosen for experimental demonstrations. The bright-dark splitting of excitons varies from 3.2 to 6.0 meV and is inversely proportional to the nanoplatelet thickness. Good agreement between experimental and theoretically calculated size dependence of the bright-dark exciton slitting is achieved. The recombination rates of the bright and dark excitons and the bright to dark relaxation rate are measured by time-resolved techniques

Magnetoexcitons in large area CVD-grown monolayer MoS2 and MoSe2 on sapphire

Magnetotransmission spectroscopy was employed to study the valley Zeeman effect in large area monolayer MoS2 and MoSe2. The extracted values of the valley g factors for both A and B excitons were found to be similar with g(v) similar or equal to -4.5. The samples are expected to be strained due to the CVD growth on sapphire at high temperature (700 degrees C). However, the estimated strain, which is maximum at low temperature, is only similar or equal to 0.2%. Theoretical considerations suggest that the strain is too small to significantly influence the electronic properties. This is confirmed by the measured value of the valley g factor, and the measured temperature dependence of the band gap, which are almost identical for CVD and mechanically exfoliated MoS2