The emerging field of valleytronics aims to coherently manipulate an electron and/or hole’s valley pseudospin as an information bearing degree of freedom (DOF). Monolayer transition metal dichalcogenides, due to their strongly bound excitons, their degenerate valleys and their seamless interfacing with photons are a promising candidate for room temperature valleytronics. Although the exciton binding energy suggests room temperature valley coherence should be possible, it has been elusive to-date. A potential solution involves the formation of half-light, half-matter cavity polaritons based on 2D material excitons. It has recently been discovered that cavity polaritons can inherit the valley DOF. Here, we demonstrate the room temperature valley coherence of valley-polaritons by embedding a monolayer of tungsten diselenide in a monolithic dielectric cavity. The extra decay path introduced by the exciton-cavity coupling, which is free from decoherence, is the key to room temperature valley coherence preservation. These observations paves the way for practical valleytronic devices.
Monolayer transition metal dichalcogenides (TMDCs) have recently emerged as a host material for localized optically active quantum emitters that generate single photons. (1-5) Here, we investigate fully localized excitons and trions from such TMDC quantum emitters embedded in a van der Waals heterostructure. We use direct electrostatic doping through the vertical heterostructure device assembly to generate quantum confined trions. Distinct spectral jumps as a function of applied voltage bias, and excitation power-dependent charging, demonstrate the observation of the two different excitonic complexes. We also observe a reduction of the intervalley electron-hole exchange interaction in the confined trion due to the addition of an extra electron, which is manifested by a decrease in its fine structure splitting. We further confirm this decrease of exchange interaction for the case of the charged states by a comparative study of the circular polarization resolved photoluminescence from individual excitonic states. The valley polarization selection rules inherited by the localized trions will provide a pathway toward realizing a localized spin-valley-photon interface.
We demonstrate the formation of CdSe nanoplatelet (NPL) exciton-polaritons in a distributed bragg reflector (DBR) cavity. The molecule-cavity hybrid system is in the strong coupling regime with an 83 meV Rabi splitting, characterized from angle-resolved reflectance and photoluminescence measurements. Mixed quantum-classical dynamics simulations are used to investigate the polariton photophysics of the hybrid system by treating the electronic and photonic degrees of freedom (DOF) quantum mechanically, and the nuclear phononic DOF classically. Our numerical simulations of the angle-resolved photoluminescence (PL) agree extremely well with the experimental data, providing a fundamental explanation of the asymmetric intensity distribution of the upper and lower polariton branches. Our results also provide mechanistic insights into the importance of phonon-assisted non-adiabatic transitions among polariton states which are reflected in the various features of the PL spectra. This work proves the feasibility of coupling nanoplatelet electronic states with the photon states of a dielectric cavity to form a hybrid system and provides a new platform for investigating cavity-mediated physical and chemical processes.
Generation of spectrally tunable single photon sources at predetermined spatial locations is a key enabling step toward scalable optical quantum technologies. In this regard, semiconducting two dimensional materials, like tungsten diselenide (WSe2), have recently been shown to host optically active quantum emitters that can be strain induced using nanostructured substrates and also be spectrally tuned with electric and magnetic fields. In this work, we employ a van der Waals heterostructure of WSe2, hexagonal boron nitride, and few layer graphene on a nanopillar array to yield electric field tunable single photon emission at locations with induced strain. The quantum emission lines, which have linewidths of hundreds of μeV, can be tuned by several times their linewidths. In contrast to previous reports of decrease in energy of randomly occurring quantum emitters in WSe2, we interestingly find an increase in energies (blueshift) in these strain-induced emitters.
Strain engineering is a natural route to control the electronic and
optical properties of two-dimensional (2D) materials. Recently, 2D
semiconductors have also been demonstrated as an intriguing host of
strain-induced quantum-confined emitters with unique valley properties
inherited from the host semiconductor. Here, we study the continuous
and reversible tuning of the light emitted by such localized emitters
in a monolayer tungsten diselenide embedded in a van der Waals
heterostructure. Biaxial strain is applied on the emitters via strain
transfer from a lead magnesium niobate–lead titanate (PMN-PT)
piezoelectric substrate. Efficient modulation of the emission energy
of several localized emitters up to 10 meV has been demonstrated on
application of a voltage on the piezoelectric substrate. Further, we
also find that the emission axis rotates by
∼
40
∘
as the magnitude of the biaxial
strain is varied on these emitters. These results elevate the prospect
of using all electrically controlled devices where the property of the
localized emitters in a 2D host can be engineered with elastic fields
for an integrated opto-electronics and nano-photonics platform.
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