Molecular tuning of excitons in four-atom-thick hybrid bilayer crystals

Fuente: arXiv
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Main Authors: Chowdhury, Tomojit, Champagne, Aurélie, Knüppel, Patrick, Naqvi, Zehra, Gao, Mengyu, Guisinger, Nathan, Mak, Kin Fai, Neaton, Jeffrey B., Park, Jiwoong
Format: Preprint
Published: 2024
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author Chowdhury, Tomojit
Champagne, Aurélie
Knüppel, Patrick
Naqvi, Zehra
Gao, Mengyu
Guisinger, Nathan
Mak, Kin Fai
Neaton, Jeffrey B.
Park, Jiwoong
author_facet Chowdhury, Tomojit
Champagne, Aurélie
Knüppel, Patrick
Naqvi, Zehra
Gao, Mengyu
Guisinger, Nathan
Mak, Kin Fai
Neaton, Jeffrey B.
Park, Jiwoong
contents Bilayer crystals, formed by stacking monolayers of two-dimensional (2D) crystals, create interlayer potentials that govern excitonic phenomena but are constrained by their fixed covalent lattices. Replacing one layer with an atomically thin molecular crystal overcomes this limitation, as precise control of functional groups enables tunable 2D molecular lattices and, consequently, electronic structures. Here, we report molecular tuning of lattices and excitons in four-atom-thick hybrid bilayer crystals (HBCs), synthesized as monolayers of perylene-based molecular and transition metal dichalcogenide (TMD) single crystals. In HBCs, we observe an anisotropic photoluminescence signal exhibiting characteristics of both molecular and TMD excitons, directly tuned by molecular geometry and HBC composition. Ab initio calculations reveal that this anisotropic emission arises from hybrid excitons, which inherit properties from both layers through a hybridized bilayer band structure. Our work establishes a synthetically derived, molecule-based 2D quantum materials platform with the potential for engineering interlayer potentials.
format Preprint
id arxiv_https___arxiv_org_abs_2412_12027
institution arXiv
publishDate 2024
record_format arxiv
spellingShingle Molecular tuning of excitons in four-atom-thick hybrid bilayer crystals
Chowdhury, Tomojit
Champagne, Aurélie
Knüppel, Patrick
Naqvi, Zehra
Gao, Mengyu
Guisinger, Nathan
Mak, Kin Fai
Neaton, Jeffrey B.
Park, Jiwoong
Materials Science
Computational Physics
Optics
Bilayer crystals, formed by stacking monolayers of two-dimensional (2D) crystals, create interlayer potentials that govern excitonic phenomena but are constrained by their fixed covalent lattices. Replacing one layer with an atomically thin molecular crystal overcomes this limitation, as precise control of functional groups enables tunable 2D molecular lattices and, consequently, electronic structures. Here, we report molecular tuning of lattices and excitons in four-atom-thick hybrid bilayer crystals (HBCs), synthesized as monolayers of perylene-based molecular and transition metal dichalcogenide (TMD) single crystals. In HBCs, we observe an anisotropic photoluminescence signal exhibiting characteristics of both molecular and TMD excitons, directly tuned by molecular geometry and HBC composition. Ab initio calculations reveal that this anisotropic emission arises from hybrid excitons, which inherit properties from both layers through a hybridized bilayer band structure. Our work establishes a synthetically derived, molecule-based 2D quantum materials platform with the potential for engineering interlayer potentials.
title Molecular tuning of excitons in four-atom-thick hybrid bilayer crystals
topic Materials Science
Computational Physics
Optics
url https://arxiv.org/abs/2412.12027