B. Urbaszek

Giant enhancement of the optical second-harmonic emission of WSe(2) monolayers by laser excitation at exciton resonances.

Monolayers (MLs) of MoS2 and WSe2 are 2D semiconductors with strong, direct optical transitions that are governed by tightly Coulomb bound eletron-hole pairs (excitons). The optoelectronic properties of these transition metal dichalcogenides are directly related to the inherent crystal inversion symmetry breaking. It allows for efficient second harmonic generation (SHG) and is at the origin of chiral optical selections rules, which enable efficient optical initialization of electrons in specific K-valleys in momentum space. Here we demonstrate how these unique non-linear and linear optical properties can be combined to efficiently prepare exciton valley coherence and polarization through resonant pumping of an excited exciton state. In particular a new approach to coherent alignment of excitons following two-photon excitation is demonstrated. We observe a clear deviation of the excited exciton spectrum from the standard Rydberg series via resonances in SHG spectroscopy and two- and one-photon absorption. The clear identification of the 2s and 2p exciton excited states combined with first principle calculations including strong anti-screening effects allows us to determine an exciton binding energy of the order of 600 meV in ML WSe2.

Valley dynamics probed through charged and neutral exciton emission in monolayer WSe 2

Optical interband transitions in monolayer transition metal dichalcogenides such as WSe2 and MoS2 are governed by chiral selection rules. This allows efficient optical initialization of an electron in a specific K valley in momentum space. Here we probe the valley dynamics in monolayer WSe2 by monitoring the emission and polarization dynamics of the well-separated neutral excitons (bound electron-hole pairs) and charged excitons (trions) in photoluminescence. The neutral exciton photoluminescence intensity decay time is about 4 ps, whereas the trion emission occurs over several tens of ps. The trion polarization dynamics shows a partial, fast initial decay within tens of ps before reaching a stable polarization of ≈20%, for which a typical valley polarization decay time of the order of 1 ns can be inferred.

Robust quantum dot exciton generation via adiabatic passage with frequency-swept optical pulses.

The energy states in semiconductor quantum dots are discrete as in atoms, and quantum states can be coherently controlled with resonant laser pulses. Long coherence times allow the observation of Rabi flopping of a single dipole transition in a solid state device, for which occupancy of the upper state depends sensitively on the dipole moment and the excitation laser power. We report on the robust population inversion in a single quantum dot using an optical technique that exploits rapid adiabatic passage from the ground to an excited state through excitation with laser pulses whose frequency is swept through the resonance. This observation in photoluminescence experiments is made possible by introducing a novel optical detection scheme for the resonant electron hole pair (exciton) generation.

Double resonant Raman scattering and valley coherence generation in monolayer WSe_{2}.

The electronic states at the direct band gap of monolayer transition metal dichalcogenides such as WSe_{2} at the K^{+} and K^{-} valleys are related by time reversal and may be viewed as pseudospins. The corresponding optical interband transitions are governed by robust excitons. Excitation with linearly polarized light yields the coherent superposition of exciton pseudospin states, referred to as coherent valley states. Here, we uncover how and why valley coherence can be generated efficiently. In double resonant Raman spectroscopy, we show that the optically generated 2s exciton state differs from the 1s state by exactly the energy of the combination of several prominent phonons. Superimposed on the exciton photoluminescence (PL), we observe the double resonant Raman signal. This spectrally narrow peak shifts with the excitation laser energy as incoming photons match the 2s and outgoing photons the 1s exciton transition. The multiphonon resonance has important consequences: following linearly polarized excitation of the 2s exciton, a superposition of valley states is efficiently transferred from the 2s to 1s state. This explains the high degree of valley coherence measured for the 1s exciton PL.

In-Plane Propagation of Light in Transition Metal Dichalcogenide Monolayers: Optical Selection Rules

The optical selection rules for interband transitions in WSe_{2}, WS_{2}, and MoSe_{2} transition metal dichalcogenide monolayers are investigated by polarization-resolved photoluminescence experiments with a signal collection from the sample edge. These measurements reveal a strong polarization dependence of the emission lines. We see clear signatures of the emitted light with the electric field oriented perpendicular to the monolayer plane, corresponding to an interband optical transition forbidden at normal incidence used in standard optical spectroscopy measurements. The experimental results are in agreement with the optical selection rules deduced from group theory analysis, highlighting the key role played by the different symmetries of the conduction and valence bands split by the spin-orbit interaction. These studies yield a direct determination of the bright-dark exciton splitting, for which we measure 40±1  meV and 55±2  meV in WSe_{2} and WS_{2} monolayer, respectively.

Gate-Controlled Spin-Valley Locking of Resident Carriers in WSe2 Monolayers

Using time-resolved Kerr rotation, we measure the spin-valley dynamics of resident electrons and holes in single charge-tunable monolayers of the archetypal transition-metal dichalcogenide (TMD) semiconductor WSe_{2}. In the n-type regime, we observe long (∼130  ns) polarization relaxation of electrons that is sensitive to in-plane magnetic fields B_{y}, indicating spin relaxation. In marked contrast, extraordinarily long (∼2  μs) polarization relaxation of holes is revealed in the p-type regime, which is unaffected by B_{y}, directly confirming long-standing expectations of strong spin-valley locking of holes in the valence band of monolayer TMDs. Supported by continuous-wave Kerr spectroscopy and Hanle measurements, these studies provide a unified picture of carrier polarization dynamics in monolayer TMDs, which can guide design principles for future valleytronic devices.

Intrinsic exciton-state mixing and nonlinear optical properties in transition metal dichalcogenide monolayers

© 2017 American Physical Society. Optical properties of transition metal dichalcogenides monolayers are controlled by Wannier-Mott excitons forming a series of 1s,2s,2p,... hydrogen-like states. We develop the theory of the excited excitonic states energy spectrum fine structure. We predict that p- and s-shell excitons are mixed due to the specific D3h point symmetry of the transition metal dichalcogenide monolayers. Hence, both s- and p-shell excitons are active in both single- and two-photon processes, providing an efficient mechanism of second harmonic generation. The corresponding contribution to the nonlinear susceptibility is calculated.

Electron and hole spin cooling efficiency in InAs quantum dots: The role of nuclear field

The spin dynamics of a resident carrier, hole or electron, in singly charged InAs/GaAs quantum dots has been measured by pump-probe experiments. The relative strength of the hole to the electron hyperfine couplings with nuclei is obtained by studying the magnetic-field dependence of the resident-carrier spin polarization. We find, in good agreement with recent theoretical studies, that the hole hyperfine coupling is ten times smaller than the electron one.

Exciton diffusion in WSe2 monolayers embedded in a van der Waals heterostructure

We have combined spatially-resolved steady-state micro-photoluminescence (

Observation of exciton-phonon coupling in MoSe 2 monolayers

\mu