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Register a new userExciton-exciton interaction in transition metal dichalcogenide monolayers and van der Waals heterostructures
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Due to a strong Coulomb interaction, excitons dominate the excitation kinetics in 2D materials. While Coulomb-scattering between electrons has been well studied, the interaction of excitons is more challenging and remains to be explored. As neutral composite bosons consisting of electrons and holes, excitons show a non-trivial scattering dynamics. Here, we study on microscopic footing exciton-exciton interaction in transition-metal dichalcogenides and related van der Waals heterostructures. We demonstrate that the crucial criterion for efficient scattering is a large electron/hole mass asymmetry giving rise to internal charge inhomogeneities of excitons and emphasizing their cobosonic substructure. Furthermore, both exchange and direct exciton-exciton interactions are boosted by enhanced exciton Bohr radii. We also predict an unexpected temperature dependence that is usually associated to phonon-driven scattering and we reveal an orders of magnitude stronger interaction of interlayer excitons due to their permanent dipole moment. The developed approach can be generalized to arbitrary material systems and will help to study strongly correlated exciton systems, such as moire super lattices.
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Heterostructures of atomically thin van der Waals bonded monolayers have opened a unique platform to engineer Coulomb correlations, shaping excitonic, Mott insulating, or superconducting phases. In transition metal dichalcogenide heterostructures, electrons and holes residing in different monolayers can bind into spatially indirect excitons with a strong potential for optoelectronics, valleytronics, Bose condensation, superfluidity, and moire-induced nanodot lattices. Yet these ideas require a microscopic understanding of the formation, dissociation, and thermalization dynamics of correlations including ultrafast phase transitions. Here we introduce a direct ultrafast access to Coulomb correlations between monolayers; phase-locked mid-infrared pulses allow us to measure the binding energy of interlayer excitons in WSe2/WS2 hetero-bilayers by revealing a novel 1s-2p resonance, explained by a fully quantum mechanical model. Furthermore, we trace, with subcycle time resolution, the transformation of an exciton gas photogenerated in the WSe2 layer directly into interlayer excitons. Depending on the stacking angle, intra- and interlayer species coexist on picosecond scales and the 1s-2p resonance becomes renormalized. Our work provides a direct measurement of the binding energy of interlayer excitons and opens the possibility to trace and control correlations in novel artificial materials.
The optical properties of MoS2 monolayers are dominated by excitons, but for spectrally broad optical transitions in monolayers exfoliated directly onto SiO2 substrates detailed information on excited exciton states is inaccessible. Encapsulation in hexagonal boron nitride (hBN) allows approaching the homogenous exciton linewidth, but interferences in the van der Waals heterostructures make direct comparison between transitions in optical spectra with different oscillator strength more challenging. Here we reveal in reflectivity and in photoluminescence excitation spectroscopy the presence of excited states of the A-exciton in MoS2 monolayers encapsulated in hBN layers of calibrated thickness, allowing to extrapolate an exciton binding energy of about 220 meV. We theoretically reproduce the energy separations and oscillator strengths measured in reflectivity by combining the exciton resonances calculated for a screened two-dimensional Coulomb potential with transfer matrix calculations of the reflectivity for the van der Waals structure. Our analysis shows a very different evolution of the exciton oscillator strength with principal quantum number for the screened Coulomb potential as compared to the ideal two-dimensional hydrogen model.
We study theoretically the Coulomb interaction between excitons in transition metal dichalcogenide (TMD) monolayers. We calculate direct and exchange interaction for both ground and excited states of excitons. The screening of the Coulomb interaction, specific to monolayer structures, leads to the unique behavior of the exciton-exciton scattering for excited states, characterized by the non-monotonic dependence of the interaction as function of the transferred momentum. We find that the nontrivial screening enables the description of TMD exciton interaction strength by approximate formula which includes exciton binding parameters. The influence of screening and dielectric environment on the exciton-exciton interaction was studied, showing qualitatively different behavior for ground state and excited states of excitons. Furthermore, we consider exciton-electron interaction, which for the excited states is governed by the dominant attractive contribution of the exchange component, which increases with the excitation number. The results provide a quantitative description of the exciton-exciton and exciton-electron scattering in transition metal dichalcogenides, and are of interest for the design of perspective nonlinear optical devices based on TMD monolayers.
We have investigated the exciton dynamics in transition metal dichalcogenide mono-layers using time-resolved photoluminescence experiments performed with optimized time-resolution. For MoSe2 monolayers, we measure $tau_{rad}=1.8pm0.2$ ps that we interpret as the intrinsic radiative recombination time. Similar values are found for WSe2 mono-layers. Our detailed analysis suggests the following scenario: at low temperature (T $leq$ 50 K), the exciton oscillator strength is so large that the entire light can be emitted before the time required for the establishment of a thermalized exciton distribution. For higher lattice temperatures, the photoluminescence dynamics is characterized by two regimes with very different characteristic times. First the PL intensity drops drastically with a decay time in the range of the picosecond driven by the escape of excitons from the radiative window due to exciton- phonon interactions. Following this first non-thermal regime, a thermalized exciton population is established gradually yielding longer photoluminescence decay times in the nanosecond range. Both the exciton effective radiative recombination and non-radiative recombination channels including exciton-exciton annihilation control the latter. Finally the temperature dependence of the measured exciton and trion dynamics indicates that the two populations are not in thermodynamical equilibrium.
Raman scattering is a ubiquitous phenomenon in light-matter interactions which reveals a materials electronic, structural and thermal properties. Controlling this process would enable new ways of studying and manipulating fundamental material properties. Here, we report a novel Raman scattering process at the interface between different van der Waals (vdW) materials as well as between a monolayer semiconductor and 3D crystalline substrates. We find that interfacing a WSe2 monolayer with materials such as SiO2, sapphire, and hexagonal boron nitride (hBN) enables Raman transitions with phonons which are either traditionally inactive or weak. This Raman scattering can be amplified by nearly two orders of magnitude when a foreign phonon mode is resonantly coupled to the A exciton in WSe2 directly, or via an A1 optical phonon from WSe2. We further showed that the interfacial Raman scattering is distinct between hBN-encapsulated and hBN-sandwiched WSe2 sample geometries. This cross-platform electron-phonon coupling, as well as the sensitivity of 2D excitons to their phononic environments, will prove important in the understanding and engineering of optoelectronic devices based on vdW heterostructures.
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