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Title: In situ laser reflectivity to monitor and control the nucleation and growth of atomically thin 2D materials*

Abstract

The growth of atomically thin two-dimensional (2D) layered and other quantum materials is typically performed without in situ monitoring or control. Here, a simple laser reflectivity approach is demonstrated to provide in situ control over sub-monolayer thickness and growth kinetics during pulsed laser deposition (PLD) of MoSe2 layers. First, the general technique is presented with emphasis on designing the maximum sensitivity of the optical contrast through consideration of Fresnel's equations with proper choice of layer thickness, substrate, and laser monitoring wavelength, incidence angle, and laser polarization. Then the 632.8 nm optical reflectivity of MoSe2 layers on SiO2/Si substrates was predicted and compared with in situ monitoring of MoSe2 growth by PLD under actual growth conditions using a probe HeNe laser beam. The measurements showed high sensitivity and excellent agreement with MoSe2 surface coverages calculated from atomic resolution STEM analysis of 2D layers deposited in arrested growth experiments. Finally, growth kinetics revealed by these measurements showed sigmoidal nucleation and growth stages in the formation of the 2D MoSe2 layers that are described by a simple model, indicating the promise of the laser reflectivity technique for in situ monitoring and control of 2D materials deposition.

Authors:
ORCiD logo [1]; ORCiD logo [1];  [2];  [3]; ORCiD logo [1]; ORCiD logo [4]; ORCiD logo [1]; ORCiD logo [1];  [5]; ORCiD logo [1]
  1. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
  2. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Univ. of Tennessee, Knoxville, TN (United States)
  3. Texas A & M Univ., College Station, TX (United States)
  4. Technical Inst. of Denmark, Lyngby (Denmark)
  5. Univ. of Tennessee, Knoxville, TN (United States)
Publication Date:
Research Org.:
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Materials Sciences & Engineering Division
OSTI Identifier:
1608207
Grant/Contract Number:  
AC05-00OR22725
Resource Type:
Accepted Manuscript
Journal Name:
2D Materials
Additional Journal Information:
Journal Volume: 7; Journal Issue: 2; Journal ID: ISSN 2053-1583
Publisher:
IOP Publishing
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; in situ reflectivity; pulsed laser deposition (PLD); 2D materials; MoSe2; kinetic modeling

Citation Formats

Puretzky, Alexander, Lin, Yu-Chuan, Liu, Chenze, Strasser, Alexander M., Yu, Yiling, Canulescu, Stela, Rouleau, Christopher, Xiao, Kai, Duscher, Gerd, and Geohegan, David. In situ laser reflectivity to monitor and control the nucleation and growth of atomically thin 2D materials*. United States: N. p., 2020. Web. doi:10.1088/2053-1583/ab7a72.
Puretzky, Alexander, Lin, Yu-Chuan, Liu, Chenze, Strasser, Alexander M., Yu, Yiling, Canulescu, Stela, Rouleau, Christopher, Xiao, Kai, Duscher, Gerd, & Geohegan, David. In situ laser reflectivity to monitor and control the nucleation and growth of atomically thin 2D materials*. United States. doi:https://doi.org/10.1088/2053-1583/ab7a72
Puretzky, Alexander, Lin, Yu-Chuan, Liu, Chenze, Strasser, Alexander M., Yu, Yiling, Canulescu, Stela, Rouleau, Christopher, Xiao, Kai, Duscher, Gerd, and Geohegan, David. Thu . "In situ laser reflectivity to monitor and control the nucleation and growth of atomically thin 2D materials*". United States. doi:https://doi.org/10.1088/2053-1583/ab7a72. https://www.osti.gov/servlets/purl/1608207.
@article{osti_1608207,
title = {In situ laser reflectivity to monitor and control the nucleation and growth of atomically thin 2D materials*},
author = {Puretzky, Alexander and Lin, Yu-Chuan and Liu, Chenze and Strasser, Alexander M. and Yu, Yiling and Canulescu, Stela and Rouleau, Christopher and Xiao, Kai and Duscher, Gerd and Geohegan, David},
abstractNote = {The growth of atomically thin two-dimensional (2D) layered and other quantum materials is typically performed without in situ monitoring or control. Here, a simple laser reflectivity approach is demonstrated to provide in situ control over sub-monolayer thickness and growth kinetics during pulsed laser deposition (PLD) of MoSe2 layers. First, the general technique is presented with emphasis on designing the maximum sensitivity of the optical contrast through consideration of Fresnel's equations with proper choice of layer thickness, substrate, and laser monitoring wavelength, incidence angle, and laser polarization. Then the 632.8 nm optical reflectivity of MoSe2 layers on SiO2/Si substrates was predicted and compared with in situ monitoring of MoSe2 growth by PLD under actual growth conditions using a probe HeNe laser beam. The measurements showed high sensitivity and excellent agreement with MoSe2 surface coverages calculated from atomic resolution STEM analysis of 2D layers deposited in arrested growth experiments. Finally, growth kinetics revealed by these measurements showed sigmoidal nucleation and growth stages in the formation of the 2D MoSe2 layers that are described by a simple model, indicating the promise of the laser reflectivity technique for in situ monitoring and control of 2D materials deposition.},
doi = {10.1088/2053-1583/ab7a72},
journal = {2D Materials},
number = 2,
volume = 7,
place = {United States},
year = {2020},
month = {3}
}

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