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Register a new userTrion Valley Coherence in Monolayer Semiconductors
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The emerging field of valleytronics aims to exploit the valley pseudospin of electrons residing near Bloch band extrema as an information carrier. Recent experiments demonstrating optical generation and manipulation of exciton valley coherence (the superposition of electron-hole pairs at opposite valleys) in monolayer transition metal dichalcogenides (TMDs) provide a critical step towards control of this quantum degree of freedom. The charged exciton (trion) in TMDs is an intriguing alternative to the neutral exciton for control of valley pseudospin because of its long spontaneous recombination lifetime, its robust valley polarization, and its coupling to residual electronic spin. Trion valley coherence has however been unexplored due to experimental challenges in accessing it spectroscopically. In this work, we employ ultrafast two-dimensional coherent spectroscopy to resonantly generate and detect trion valley coherence in monolayer MoSe$_2$ demonstrating that it persists for a few-hundred femtoseconds. We conclude that the underlying mechanisms limiting trion valley coherence are fundamentally different from those applicable to exciton valley coherence. Based on these observations, we suggest possible strategies for extending valley coherence times in two-dimensional materials.
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Due to degeneracies arising from crystal symmetries, it is possible for electron states at band edges (valleys) to have additional spin-like quantum numbers. An important question is whether coherent manipulation can be performed on such valley pseudospins, analogous to that routinely implemented using true spin, in the quest for quantum technologies. Here we show for the first time that SU(2) valley coherence can indeed be generated and detected. Using monolayer semiconductor WSe2 devices, we first establish the circularly polarized optical selection rules for addressing individual valley excitons and trions. We then reveal coherence between valley excitons through the observation of linearly polarized luminescence, whose orientation always coincides with that of any linearly polarized excitation. Since excitons in a single valley emit circularly polarized photons, linear polarization can only be generated through recombination of an exciton in a coherent superposition of the two valleys. In contrast, the corresponding photoluminescence from trions is not linearly polarized, consistent with the expectation that the emitted photon polarization is entangled with valley pseudospin. The ability to address coherence, in addition to valley polarization, adds a critical dimension to the quantum manipulation of valley index necessary for coherent valleytronics.
Optical excitation typically enhances electrical conduction and low-frequency radiation absorption in semiconductors. We have, however, observed a pronounced transient decrease of conductivity in doped monolayer molybdenum disulfide (MoS2), a two-dimensional (2D) semiconductor, under femtosecond laser excitation. In particular, the conductivity is reduced dramatically down to only 30% of its equilibrium value with high pump fluence. This anomalous phenomenon arises from the strong many-body interactions in the system, where photoexcited electron-hole pairs join the doping-induced charges to form trions, bound states of two electrons and one hole. The resultant increase of the carrier effective mass substantially diminishes the carrier conductivity.
Transition metal dichalcogenides represent an ideal testbed to study excitonic effects, spin-related phenomena and fundamental light-matter coupling in nanoscopic condensed matter systems. In particular, the valley degree of freedom, which is unique to such direct band gap monolayers with broken inversion symmetry, adds fundamental interest in these materials. Here, we implement a Tamm-plasmon structure with an embedded MoSe2 monolayer and study the formation of polaritonic quasi-particles. Strong coupling conditions between the Tamm-mode and the trion resonance of MoSe2 are established, yielding bright luminescence from the polaritonic ground state under non-resonant optical excitation. We demonstrate, that tailoring the electrodynamic environment of the monolayer results in a significantly increased valley polarization. This enhancement can be related to change in recombination dynamics shown in time-resolved photoluminescence measurements. We furthermore observe strong upconversion luminescence from resonantly excited polariton states in the lower polariton branch. This upconverted polariton luminescence is shown to preserve the valley polarization of the trion-polariton, which paves the way towards combining spin-valley physics and exciton scattering experiments.
Monolayers of semiconducting transition metal dichalcogenides are two-dimensional direct-gap systems which host tightly-bound excitons with an internal degree of freedom corresponding to the valley of the constituting carriers. Strong spin-orbit interaction and the resulting ordering of the spin-split subbands in the valence and conduction bands makes the lowest-lying excitons in WX$_2$ (X~being S or Se) spin-forbidden and optically dark. With polarization-resolved photoluminescence experiments performed on a WSe$_2$ monolayer encapsulated in a hexagonal boron nitride, we show how the intrinsic exchange interaction in combination with the applied in-plane and/or out-of-plane magnetic fields enables one to probe and manipulate the valley degree of freedom of the dark excitons.
Highly nonlinear optical materials with strong effective photon-photon interactions (Kerr-like nonlinearity) are required in the development of novel quantum sources of light as well as for ultrafast and quantum optical signal processing circuitry. Here we report very large Kerr-like nonlinearities by employing strong optical transitions of charged excitons (trions) observed in semiconducting transition metal dichalcogenides (TMDCs). By hybridising trions in monolayer MoSe$_2$ at low electron densities with a microcavity mode, we realise trion-polaritons exhibiting significant energy shifts at very small photon fluxes due to phase space filling. Most notably, the strong trion-polariton nonlinearity is found to be 10 to 1000 larger than in other polariton systems, including neutral exciton-polaritons in TMDCs. Furthermore it exceeds by factors of $sim 10^3-10^5$ the magnitude of Kerr nonlinearity in bare TMDCs, graphene and other widely used optical materials (e.g. Si, AlGaAs etc) in weak light-matter coupling regimes. The results are in good agreement with a theory which accounts for the composite nature of excitons and trions and deviation of their statistics from that of ideal bosons and fermions. This work opens a new highly nonlinear system for quantum optics applications enabling in principle scalability and control through nano-engineering of van der Waals heterostructures.
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