Revealing the preferred interlayer orientations and stackings of two-dimensional bilayer gallium selenide crystals

Li, Xufan; Basile Carrasco, Leonardo A.; Yoon, Mina; Ma, Cheng; Puretzky, Alexander A.; Lee, Jaekwang; Idrobo Tapia, Juan Carlos; Chi, Miaofang; Rouleau, Christopher M.; Geohegan, David B.; Xiao, Kai

doi:10.1002/anie.201409743

Title: Revealing the preferred interlayer orientations and stackings of two-dimensional bilayer gallium selenide crystals

Journal Article · Wed Jan 21 00:00:00 EST 2015 · Angewandte Chemie (International Edition)

DOI:https://doi.org/10.1002/anie.201409743· OSTI ID:1185701

Li, Xufan ^[1]; Basile Carrasco, Leonardo A. ^[2]; Yoon, Mina ^[1]; Ma, Cheng ^[1]; Puretzky, Alexander A. ^[1]; Lee, Jaekwang ^[1]; Idrobo Tapia, Juan Carlos ^[1]; Chi, Miaofang ^[1]; Rouleau, Christopher M. ^[1]; Geohegan, David B. ^[1]; Xiao, Kai ^[1]

Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Escuela Politecnica Nacional, Quito (Ecuador)

Characterizing and controlling the interlayer orientations and stacking order of bilayer two-dimensional (2D) crystals and van der Waals (vdW) heterostructure is crucial to optimize their electrical and optoelectronic properties. The four polymorphs of layered gallium selenide (GaSe) that result from different layer stacking provide an ideal platform to study the stacking configurations in bilayer 2D crystals. Here, through a controllable vapor-phase deposition method we selectively grow bilayer GaSe crystals and investigate their two preferred 0° or 60° interlayer rotations. The commensurate stacking configurations (AA' and AB-stacking) in as-grown 2D bilayer GaSe crystals are clearly observed at the atomic scale and the Ga-terminated edge structure are identified for the first time by using atomic-resolution scanning transmission electron microscopy (STEM). Theoretical analysis of the interlayer coupling energetics vs. interlayer rotation angle reveals that the experimentally-observed orientations are energetically preferred among the bilayer GaSe crystal polytypes. Here, the combined experimental and theoretical characterization of the GaSe bilayers afforded by these growth studies provide a pathway to reveal the atomistic relationships in interlayer orientations responsible for the electronic and optical properties of bilayer 2D crystals and vdW heterostructures.

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Research Organization:: Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Sciences (CNMS)

Sponsoring Organization:: USDOE Laboratory Directed Research and Development (LDRD) Program; USDOE Office of Science (SC)

Grant/Contract Number:: AC05-00OR22725

OSTI ID:: 1185701

Journal Information:: Angewandte Chemie (International Edition), Vol. 54, Issue 9; ISSN 1433-7851

Publisher:: WileyCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 39 works

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36 MATERIALS SCIENCE
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Title: Revealing the preferred interlayer orientations and stackings of two-dimensional bilayer gallium selenide crystals

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