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Bárbara Rosa

Publications and source records attributed to Bárbara Rosa.

3 recordsLinked to original sources

Resolving High-Energy States of Interlayer Excitons in MoSe$_2$/WSe$_2$ Heterostructures

High-energy states of interlayer excitons (IXs) in van der Waals heterostructures remain largely unexplored despite their importance for understanding many-body interactions and nonlinear optical phenomena. Here, we use photoluminescence excitation (PLE) spectroscopy to resolve a Rydberg-like series of excited IX states in MoSe$_2$/WSe$_2$ heterostructures. We observe multiple PLE resonances below the intralayer exciton energies, which we assign to the 2s-, 3s-, and 4s-like states of the IXs. These resonances are consistently observed across heterostructures with different twist angles, indicating that the high-energy state spectrum is only weakly affected by the twist angle. Wannier-exciton calculations incorporating screened Coulomb interactions reproduce the overall energy scale and qualitative trends of the measured Rydberg-like series, supporting the assignment of the observed resonances. Our findings demonstrate that PLE provides direct experimental access to the previously unexplored high-energy IX states in van der Waals heterostructures.

cond-mat.mes-hall↗

Probing Noncentrosymmetric 2D Materials by Fourier Space Second Harmonic Imaging

The controlled assembly of twisted 2D structures requires precise determination of the crystal orientation of their component layers. In the established procedure, the second-harmonic generation (SHG) intensity of a noncentrosymmetric layer is recorded while rotating the polarization of both the incident laser field and detected SHG, which can be time-consuming and tedious. Here, we demonstrate that the crystal orientation of transition metal dichalcogenides and hexagonal boron nitride can be directly determined by recording SHG images generated by tightly focused laser beams in Fourier space. Using an azimuthally polarized laser beam, the SHG image distinctly reflects the hexagonal structure of the crystal lattice, revealing its orientation quickly and accurately. This technique could significantly impact the field of twistronics, which studies the effects of the relative angle between the layers of a stacked 2D structure, as well as advances the nanofabrication of 2D materials.

physics.optics↗

In-situ spontaneous emission control of MoSe$_2$-WSe$_2$ interlayer excitons with near-unity quantum yield

Optical resonators are a powerful platform to control the spontaneous emission dynamics of excitons in solid-state nanostructures. Here, we study a MoSe$_2$-WSe$_2$ van-der-Waals heterostructure that is integrated in a widely tunable open optical microcavity to gain insights into fundamental optical properties of the emergent interlayer charge-transfer excitons. First, we utilize an ultra-low quality factor open planar vertical cavity and investigate the modification of the excitonic lifetime as on- and off-resonant conditions are met with consecutive longitudinal modes. Time-resolved photoluminescence measurements reveal that the interlayer exciton lifetime can thus be periodically tuned with an amplitude of 110 ps. The resulting oscillations of the interlayer exciton lifetime allows us to extract a 0.5 ns free-space radiative lifetime and a quantum efficiency as high as 81 \%. We subsequently engineer the local density of optical states by introducing a spatially confined and fully spectrally tunable Tamm-plasmon resonance. The dramatic redistribution of the local optical modes in this setting allows us to encounter a profound inhibition of spontaneous emission of the interlayer excitons by a factor of 3.2. We expect that specifically engineering the inhibition of radiation from moiré excitons is a powerful tool to steer their thermalization, and eventually their condensation into coherent condensate phases.

cond-mat.mtrl-sci↗