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Amos, Stephanie

Publications and source records attributed to Amos, Stephanie.

Modulation of Electrostatic Potential in 2D Crystal Engineered by an Array of Alternating Polar Molecules

The moiré potential in rotationally misfit two-dimensional (2D) heterostructures has been used to build artificial exciton and electron lattices, which have become platforms for realizing exotic electronic phases. Here, we demonstrate a different approach to create a superlattice potential in 2D crystals by using the near field of an array of polar molecules. Here, a bilayer of titanyl phthalocyanine (TiOPc), consisting of alternating out-of-plane dipoles, is deposited on monolayer MoS 2 . Time-resolved two-photon photoemission spectroscopy reveals a pair of interlayer exciton states with an energy difference of ~0.1 eV, which is consistent with the electrostatic potential modulation induced by the TiOPc bilayer as determined by density functional theory calculations. Because the symmetry and the period of this potential superlattice can be changed readily by using molecules of different shapes and sizes, molecule/2D heterostructures can be promising platforms for designing artificial exciton and electron lattices.

2D heterostructures↗

Energy-valley-dependent charge transfer in few-layer transition metal dichalcogenide heterostructures

The effect of the energy valley on interlayer charge transfer in transition metal dichalcogenide (TMD) heterostructures is studied by transient absorption spectroscopy and density functional theory. First-principles calculations confirm that the Λ min valley in the conduction band of few-layer WSe 2 evolves from above its K valley in the monolayer (1L) to below it in 4L. Heterostructure samples of nL–WSe 2 /1L–MoS 2 , where n = 1,2,3, and 4, are obtained by mechanical exfoliation and dry transfer. Photoluminescence spectroscopy reveals a thickness-dependent WSe 2 band structure and efficient interlayer charge transfer. Transient absorption measurements show that the electron transfer time from the Λ min valley of 4L WSe 2 to the K valley of MoS 2 is on the order of 30 ps. This process is much slower than the K-K charge transfer in 1L/1L TMD heterostructures. Furthermore, the momentum-indirect interlayer excitons formed after charge transfer have lifetimes >1 ns.

77 NANOSCIENCE AND NANOTECHNOLOGY↗

Nanoscale Periodic Trapping Sites for Interlayer Excitons Built by Deformable Molecular Crystal on 2D Crystal

The nanoscale moiré pattern formed at 2D transition-metal dichalcogenide crystal (TMDC) heterostructures provides periodic trapping sites for excitons, which is essential for realizing various exotic phases such as artificial exciton lattices, Bose–Einstein condensates, and exciton insulators. At organic molecule/TMDC heterostructures, similar periodic potentials can be formed via other degrees of freedom. Here, we utilize the structure deformability of a 2D molecular crystal as a degree of freedom to create a periodic nanoscale potential that can trap interlayer excitons (IXs). Specifically, two semiconducting molecules, PTCDI and PTCDA, which possess similar band gaps and ionization potentials but form different lattice structures on MoS 2 , are investigated. The PTCDI lattice on MoS 2 is distorted geometrically, which lifts the degeneracy of the two molecules within the crystal’s unit cell. The degeneracy lifting results in a spatial variation of the molecular orbital energy, with an amplitude and periodicity of ~0.2 eV and ~2 nm, respectively. On the other hand, no such energy variation is observed in PTCDA/MoS 2 , where the PTCDA lattice is much less distorted. Furthermore, the periodic variation in molecular orbital energies provides effective trapping sites for IXs. For IXs formed at PTCDI/MoS 2 , rapid spatial localization of the electron in the organic layer toward the interface is observed, which demonstrates the effectiveness of these interfacial IX traps.

77 NANOSCIENCE AND NANOTECHNOLOGY↗