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Register a new userFlipping exciton angular momentum with chiral phonons in MoSe$_2$/WSe$_2$ heterobilayers
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Cl\\'ement Faugeras
Publication date
2020
fields
Physics
and research's language is
English
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Identifying quantum numbers to label elementary excitations is essential for the correct description of light-matter interaction in solids. In monolayer semiconducting transition metal dichalcogenides (TMDs) such as MoSe$_2$ or WSe$_2$, most optoelectronic phenomena are described well by labelling electron and hole states with the spin projection along the normal to the layer (S$_z$). In contrast, for WSe$_2$/MoSe$_2$ interfaces recent experiments show that taking S$_z$ as quantum number is not a good approximation, and spin mixing needs to be always considered. Here we argue that the correct quantum number for these systems is not S$_z$, but the $z$-component of the total angular momentum -- J$_z$ = L$_z$ + S$_z$ -- associated to the C$_3$ rotational lattice symmetry, which assumes half-integer values corresponding modulo 3 to distinct states. We validate this conclusion experimentally through the observation of strong intervalley scattering mediated by chiral optical phonons that -- despite carrying angular momentum 1 -- cause resonant intervalley transitions of excitons, with an angular momentum difference of 2.
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The optical spectra of vertically stacked MoSe$_2$/WSe$_2$ heterostructures contain additional interlayer excitonic peaks that are absent in the individual monolayer materials and exhibit a significant spatial charge separation in out-of-plane direction. Extending on a previous study, we used a many-body perturbation theory approach to simulate and analyse the excitonic spectra of MoSe$_2$/WSe$_2$ heterobilayers with three stacking orders, considering both momentum-direct and momentum-indirect excitons. We find that the small oscillator strengths and corresponding optical responses of the interlayer excitons are significantly stacking-dependent and give rise to high radiative lifetimes in the range of 5-200,ns (at T=4,K) for the bright interlayer excitons. Solving the finite-momentum Bethe-Salpeter Equation, we predict that the lowest-energy excitation should be an indirect exciton over the fundamental indirect band gap (K$rightarrow$Q), with a binding energy of 220,meV. However, in agreement with recent magneto-optics experiments and previous theoretical studies, our simulations of the effective excitonic Lande g-factors suggest that the low-energy momentum-indirect excitons are not experimentally observed for MoSe$_2$/WSe$_2$ heterostructures. We further reveal the existence of interlayer C excitons with significant exciton binding energies and optical oscillator strengths, which are analogous to the prominent band nesting excitons in mono- and few-layer transition-metal dichalcogenides.
The availability of accessible fabrication methods based on deterministic transfer of atomically thin crystals has been essential for the rapid expansion of research into van der Waals heterostructures. An inherent issue of these techniques is the deformation of the polymer carrier film during the transfer, which can lead to highly non-uniform strain induced in the transferred two-dimensional material. Here, using a combination of optical spectroscopy, atomic force and Kelvin probe force microscopy, we show that the presence of nanometer scale wrinkles formed due to transfer-induced stress relaxation can lead to strong changes in the optical properties of MoSe$_2$/WSe$_2$ heterostructures and the emergence of the linearly polarized interlayer exciton photoluminescence. We attribute these changes to the local breaking of crystal symmetry in the nanowrinkles, which act as efficient accumulation centers for the interlayer excitons due to the strain-induced interlayer band gap reduction. The surface potential images of the rippled heterobilayer samples acquired using Kelvin probe force microscopy reveal the variation of the local work function consistent with the strain-induced band gap modulation, while the potential offset observed at the ridges of the wrinkles shows a clear correlation with the value of the tensile strain estimated from the wrinkle geometry. Our findings highlight the important role of the residual strain in defining optical properties of van der Waals heterostructures and suggest novel approaches for interlayer exciton manipulation by local strain engineering.
The creation of moire patterns in crystalline solids is a powerful approach to manipulate their electronic properties, which are fundamentally influenced by periodic potential landscapes. In 2D materials, a moire pattern with a superlattice potential can form by vertically stacking two layered materials with a twist and/or finite lattice constant difference. This unique approach has led to emergent electronic phenomena, including the fractal quantum Hall effect, tunable Mott insulators, and unconventional superconductivity. Furthermore, theory predicts intriguing effects on optical excitations by a moire potential in 2D valley semiconductors, but these signatures have yet to be experimentally detected. Here, we report experimental evidence of interlayer valley excitons trapped in a moire potential in MoSe$_2$/WSe$_2$ heterobilayers. At low temperatures, we observe photoluminescence near the free interlayer exciton energy but with over 100 times narrower linewidths. The emitter g-factors are homogeneous across the same sample and only take two values, -15.9 and 6.7, in samples with twisting angles near 60{deg} and 0deg, respectively. The g-factors match those of the free interlayer exciton, which is determined by one of two possible valley pairing configurations. At a twist angle near 20deg, the emitters become two orders of magnitude dimmer, but remarkably, they possess the same g-factor as the heterobilayer near 60deg. This is consistent with the Umklapp recombination of interlayer excitons near the commensurate 21.8{deg} twist angle. The emitters exhibit strong circular polarization, which implies the preservation of three-fold rotation symmetry by the trapping potential. Together with the power and excitation energy dependence, all evidence points to their origin as interlayer excitons trapped in a smooth moire potential with inherited valley-contrasting physics.
We investigate WSe$_2$-MoSe$_2$ heterobilayers with different twist angles $theta pm delta$ between the two layers, by low-frequency Raman scattering. In sufficiently aligned samples with $theta=0^circ$, or $theta=60^circ$, and $delta lesssim 3^circ$, we observe an interlayer shear mode (ISM), which is a clear sign of a commensurate bilayer structure, i.e., the layers must undergo an atomic reconstruction to form R-type or H-type stacking orders. We find slightly different ISM energies of about 18~cm$^{-1}$ and 17~cm$^{-1}$ for H-type and R-type reconstructions, respectively, independent of the exact value of $thetapm delta$. Our findings are corroborated by the fact that the ISM is not observed in samples with twist angles, which deviate by $delta > 3^circ$ from $0^circ$ or $60^circ$. This is expected, since in such incommensurate structures, with the possibility of Moir$acute{text{e}}$-lattice formation, there is no restoring force for an ISM. Furthermore, we observe the ISM even in sufficiently aligned heterobilayers, which are encapsulated in hexagonal Boron nitride. This is particularly relevant for the characterization of high-quality heterostructure devices.
Moire heterobilayer transition metal dichalcogenides (TMDs) emerge as an ideal system for simulating the single-band Hubbard model and interesting correlated phases have been observed in these systems. Nevertheless, the moire bands in heterobilayer TMDs were believed to be topologically trivial. Recently, it was reported that both a quantum valley Hall insulating state at filling $ u=2$ (two holes per moire unit cell) and a valley polarized quantum anomalous Hall state at filling $ u=1$ were observed in AB stacked moire MoTe$_2$/WSe$_2$ heterobilayers. However, how the topologically nontrivial states emerge is not known. In this work, we propose that the pseudo-magnetic fields induced by lattice relaxation in moire MoTe$_2$/WSe$_2$ heterobilayers could naturally give rise to moire bands with finite Chern numbers. We show that a time-reversal invariant quantum valley Hall insulator is formed at full-filing $ u=2$, when two moire bands with opposite Chern numbers are filled. At half-filling $ u=1$, Coulomb interaction lifts the valley degeneracy and results in a valley polarized quantum anomalous Hall state, as observed in the experiment. Our theory identifies a new way to achieve topologically non-trivial states in heterobilayer TMD materials.
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