Kavli Affiliate: David A. Muller
| First 5 Authors: Tomojit Chowdhury, Fauzia Mujid, Zehra Naqvi, Ariana Ray, Ce Liang
| Summary:
Controlling the spectral and polarization responses of two-dimensional (2D)
crystals is vital for developing ultra-thin platforms for compact
optoelectronic devices. However, independently tuning optical anisotropy and
spectral response remains challenging in conventional semiconductors due to the
intertwined nature of their lattice and electronic structures. Here, we report
spectra-orthogonal optical anisotropy, where polarization anisotropy is tuned
independently of spectral response, in wafer-scale, one-atom-thick 2D molecular
crystal (2DMC) monolayers synthesized on monolayer transition metal
dichalcogenide (TMD) crystals. Utilizing the concomitant spectral consistency
and structural tunability of perylene derivatives, we demonstrate tunable
optical polarization anisotropy in 2DMCs with similar spectral profiles, as
confirmed by room-temperature scanning tunneling microscopy and cross-polarized
reflectance microscopy. Additional angle-dependent analysis of the single- and
polycrystalline molecular domains reveals an epitaxial relationship between the
2DMC and the TMD. Our results establish a scalable, molecule-based 2D
crystalline platform for unique and tunable functionalities unattainable in
covalent 2D solids.
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