Dark and bright exciton formation, thermalization, and photoluminescence in monolayer transition metal dichalcogenides

The remarkably strong Coulomb interaction in atomically thin transition metal dichalcogenides (TMDs) results in an extraordinarily rich many-particle physics including the formation of tightly bound excitons. Besides optically accessible bright excitonic states, these materials also exhibit a variety of dark excitons. Since they can even lie below the bright states, they have a strong influence on the exciton dynamics, lifetimes, and photoluminescence. While very recently, the presence of dark excitonic states has been experimentally demonstrated, the origin of these states, their formation, and dynamics have not been revealed yet. Here, we present a microscopic study shedding light on time- and energy-resolved formation and thermalization of bright and dark intra- and intervalley excitons as well as their impact on the photoluminescence in different TMD materials. We demonstrate that intervalley dark excitons, so far widely overlooked in current literature, play a crucial role in tungsten-based TMDs giving rise to an enhanced photoluminescence and reduced exciton lifetimes at elevated temperatures

Assignment of the NV0 575 nm zero-phonon line in diamond to a 2E-2A2 transition

The time-averaged emission spectrum of single nitrogen-vacancy defects in diamond gives zero-phonon lines of both the negative charge state at 637 nm (1.945 eV) and the neutral charge state at 575 nm (2.156 eV). This occurs through photo-conversion between the two charge states. Due to strain in the diamond the zero-phonon lines are split and it is found that the splitting and polarization of the two zero-phonon lines are the same. From this observation and consideration of the electronic structure of the nitrogen-vacancy center it is concluded that the excited state of the neutral center has A2 orbital symmetry. The assignment of the 575 nm transition to a 2E - 2A2 transition has not been established previously.Comment: 5 pages, 5 figure

Enhanced Visibility of MoS2, MoSe2, WSe2 and Black Phosphorus: Making Optical Identification of 2D Semiconductors Easier

We explore the use of Si3N4/Si substrates as a substitute of the standard SiO2/Si substrates employed nowadays to fabricate nanodevices based on 2D materials. We systematically study the visibility of several 2D semiconducting materials that are attracting a great deal of interest in nanoelectronics and optoelectronics: MoS2, MoSe2, WSe2 and black phosphorus. We find that the use of Si3N4/Si substrates provides an increase of the optical contrast up to a 50%-100% and also the maximum contrast shifts towards wavelength values optimal for human eye detection, making optical identification of 2D semiconductors easier.Comment: 4 figures + 3 supp.info. figure

Phonon Sidebands in Transition Metal Dichalcogenides

Excitons dominate the optical properties of monolayer transition metal dichalcogenides (TMDs). Besides optically accessible bright exciton states, TMDs exhibit also a multitude of optically forbidden dark excitons. Here, we show that efficient exciton-phonon scattering couples bright and dark states and gives rise to an asymmetric excitonic line shape. The observed asymmetry can be traced back to phonon-induced sidebands that are accompanied by a polaron redshift. We present a joint theory-experiment study investigating the microscopic origin of these sidebands in different TMD materials taking into account intra- and intervalley scattering channels opened by optical and acoustic phonons. The gained insights contribute to a better understanding of the optical fingerprint of these technologically promising nanomaterials

Temperature dependence of the electron spin g factor in GaAs

The temperature dependence of the electron spin $g$ factor in GaAs is investigated experimentally and theoretically. Experimentally, the $g$ factor was measured using time-resolved Faraday rotation due to Larmor precession of electron spins in the temperature range between 4.5 K and 190 K. The experiment shows an almost linear increase of the $g$ value with the temperature. This result is in good agreement with other measurements based on photoluminescence quantum beats and time-resolved Kerr rotation up to room temperature. The experimental data are described theoretically taking into account a diminishing fundamental energy gap in GaAs due to lattice thermal dilatation and nonparabolicity of the conduction band calculated using a five-level kp model. At higher temperatures electrons populate higher Landau levels and the average $g$ factor is obtained from a summation over many levels. A very good description of the experimental data is obtained indicating that the observed increase of the spin $g$ factor with the temperature is predominantly due to band's nonparabolicity.Comment: 6 pages 4 figure

Ultrafast dynamics in monolayer TMDCs: the interplay of dark excitons, phonons and intervalley Coulomb exchange

Understanding the ultrafast coupling and relaxation mechanisms between valleys in transition metal dichalcogenide semiconductors is of crucial interest for future valleytronic devices. Recent ultrafast pump-probe experiments showed an unintuitive significant bleaching at the excitonic $B$ transition after optical excitation of the energetically lower excitonic $A$ transition. Here, we present a possible microscopic explanation for this surprising effect. It is based on the joint action of exchange coupling and phonon-mediated thermalization into dark exciton states and does not involve a population of the B exciton. Our work demonstrates how intra- and intervalley coupling on a femtosecond timescale governs the optical valley response of 2D semiconductors