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

Phonon-mediated negative differential conductance in molecular quantum dots

Transport through a single molecular conductor is considered, showing negative differential conductance behavior associated with phonon-mediated electron tunneling processes. This theoretical work is motivated by a recent experiment by Leroy et al. using a carbon nanotube contacted by an STM tip [Nature {\bf 432}, 371 (2004)], where negative differential conductance of the breathing mode phonon side peaks could be observed. A peculiarity of this system is that the tunneling couplings which inject electrons and those which collect them on the substrate are highly asymmetrical. A quantum dot model is used, coupling a single electronic level to a local phonon, forming polaron levels. A "half-shuttle" mechanism is also introduced. A quantum kinetic formulation allows to derive rate equations. Assuming asymmetric tunneling rates, and in the absence of the half-shuttle coupling, negative differential conductance is obtained for a wide range of parameters. A detailed explanation of this phenomenon is provided, showing that NDC is maximal for intermediate electron-phonon coupling. In addition, in absence of a gate, the "floating" level results in two distinct lengths for the current plateaus, related to the capacitive couplings at the two junctions. It is shown that the "half-shuttle" mechanism tends to reinforce the negative differential regions, but it cannot trigger this behavior on its own

Intersublevel Polaron Dephasing in Self-Assembled Quantum Dots

Polaron dephasing processes are investigated in InAs/GaAs dots using far-infrared transient four wave mixing (FWM) spectroscopy. We observe an oscillatory behaviour in the FWM signal shortly (< 5 ps) after resonant excitation of the lowest energy conduction band transition due to coherent acoustic phonon generation. The subsequent single exponential decay yields long intraband dephasing times of 90 ps. We find excellent agreement between our measured and calculated FWM dynamics, and show that both real and virtual acoustic phonon processes are necessary to explain the temperature dependence of the polarization decay.Comment: 10 pages, 4 figures, submitted to Phys Rev Let

Phonon Coherence and New Set of Sidebands in Phonon-Assisted Photoluminescence

We investigate excitonic polaron states comprising a local exciton and phonons in the longitudinal optical (LO) mode by solving the Schr\"{o}dinger equation. We derive an exact expression for the ground state (GS), which includes multi-phonon components with coefficients satisfying the Huang-Rhys factors. The recombination of GS and excited polaron states gives one set of sidebands in photoluminescence (PL): the multi-phonon components in the GS produce the Stokes lines and the zero-phonon components in the excited states produce the anti-Stokes lines. By introducing the mixing of the LO mode and environal phonon modes, the exciton will also couple with the latter, and the resultant polaron states result in another set of phonon sidebands. This set has a zero-phonon line higher and wider than that of the first set due to the tremendous number of the environal modes. The energy spacing between the zero-phonon lines of the first and second sets is proved to be the binding energy of the GS state. The common exciton origin of these two sets can be further verified by a characteristic Fano lineshape induced by the coherence in the mixing of the LO and the environal modes.Comment: 5 pages, 3 figures 1 figure (fig. 1) replaced 1 figure (fig. 2) remove

Chirality Dependence of the KK-Momentum Dark Excitons in Carbon Nanotubes

Using a collection of twelve semiconducting carbon nanotube samples, each highly enriched in a single chirality, we study the chirality dependence of the $K$-momentum dark singlet exciton using phonon sideband optical spectroscopy. Measurements of bright absorptive and emissive sidebands of this finite momentum exciton identify its energy as 20 - 38 meV above the bright singlet exciton, a separation that exhibits systematic dependencies on tube diameter, $2n+m$ family, and semiconducting type. We present calculations that explain how chiral angle dependence in this energy separation relates to the Coulomb exchange interaction, and elaborate the dominance of the $K_{A_1'}$ phonon sidebands over the zone-center phonon sidebands over a wide range of chiralities. The Kataura plot arising from these data is qualitatively well described by theory, but the energy separation between the sidebands shows a larger chiral dependence than predicted. This latter observation may indicate a larger dispersion for the associated phonon near the $K$ point than expected from finite distance force modeling.Comment: 24 pages, 12 figures, 1 table; slight title change, Figures 1 and 11 added, reference added, presentation improved throughout documen

Local density of states on a vibrational quantum dot out of equilibrium

We calculate the nonequilibrium local density of states on a vibrational quantum dot coupled to two electrodes at T=0 using a numerically exact diagrammatic Monte Carlo method. Our focus is on the interplay between the electron-phonon interaction strength and the bias voltage. We find that the spectral density exhibits a significant voltage dependence if the voltage window includes one or more phonon sidebands. A comparison with well-established approximate approaches indicates that this effect could be attributed to the nonequilibrium distribution of the phonons. Moreover, we discuss the long transient dynamics caused by the electron-phonon coupling.Comment: 9 pages, 11 figure