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Title: Interaction of Black Phosphorus with Oxygen and Water

Abstract

Black phosphorus (BP) has attracted significant interest as a monolayer or few-layer material with extraordinary electrical and optoelectronic properties. Chemical reactions with different ambient species, notably oxygen and water, are important as they govern key properties such as stability in air, electronic structure and charge transport, wetting by aqueous solutions, etc. Here, we report experiments combined with ab-initio calculations that address the effects of oxygen and water in contact with BP. Our results show that the reaction with oxygen is primarily responsible for changing properties of BP. Oxidation involving the dissociative chemisorption of O2 causes the decomposition of BP and continuously lowers the conductance of BP field-effect transistors (FETs). In contrast, BP is stable in contact with deaerated (i.e., O2 depleted) water and the carrier mobility in BP FETs gated by H2O increases significantly due to efficient dielectric screening of scattering centers by the high-k dielectric. Isotope labeling experiments, contact angle measurements and calculations show that the pristine BP surface is hydrophobic, but is turned progressively hydrophilic by oxidation. Lastly, our results open new avenues for exploring applications that require contact of BP with aqueous solutions including solution gating, electrochemistry, and solution-phase approaches for exfoliation, dispersion, and delivery of BP.

Authors:
 [1];  [2];  [3];  [3];  [4];  [5];  [5];  [3];  [3];  [5];  [2];  [6];  [4]
  1. Institute for Basic Science (IBS), Ulsan (Republic of Korea); Brookhaven National Lab. (BNL), Upton, NY (United States)
  2. Renmin Univ. of China, Beijing (China)
  3. Brookhaven National Lab. (BNL), Upton, NY (United States)
  4. Univ. of Nebraska-Lincoln, Lincoln, NE (United States)
  5. Institute for Basic Science (IBS), Ulsan (Republic of Korea)
  6. Institute for Basic Science (IBS), Ulsan (Republic of Korea); Ulsan National Institute of Science and Technology, Ulsan (Republic of Korea)
Publication Date:
Research Org.:
Brookhaven National Lab. (BNL), Upton, NY (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1433967
Report Number(s):
BNL-203500-2018-JAAM
Journal ID: ISSN 0897-4756; TRN: US1803027
Grant/Contract Number:  
SC0012704
Resource Type:
Accepted Manuscript
Journal Name:
Chemistry of Materials
Additional Journal Information:
Journal Volume: 28; Journal Issue: 22; Journal ID: ISSN 0897-4756
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
29 ENERGY PLANNING, POLICY AND ECONOMY; black phosphorus; field-effect transistors

Citation Formats

Huang, Yuan, Qiao, Jingsi, He, Kai, Bliznakov, Stoyan, Sutter, Eli, Chen, Xianjue, Luo, Da, Meng, Fanke, Su, Dong, Decker, Jeremy, Ji, Wei, Ruoff, Rodney S., and Sutter, Peter. Interaction of Black Phosphorus with Oxygen and Water. United States: N. p., 2016. Web. doi:10.1021/acs.chemmater.6b03592.
Huang, Yuan, Qiao, Jingsi, He, Kai, Bliznakov, Stoyan, Sutter, Eli, Chen, Xianjue, Luo, Da, Meng, Fanke, Su, Dong, Decker, Jeremy, Ji, Wei, Ruoff, Rodney S., & Sutter, Peter. Interaction of Black Phosphorus with Oxygen and Water. United States. doi:10.1021/acs.chemmater.6b03592.
Huang, Yuan, Qiao, Jingsi, He, Kai, Bliznakov, Stoyan, Sutter, Eli, Chen, Xianjue, Luo, Da, Meng, Fanke, Su, Dong, Decker, Jeremy, Ji, Wei, Ruoff, Rodney S., and Sutter, Peter. Mon . "Interaction of Black Phosphorus with Oxygen and Water". United States. doi:10.1021/acs.chemmater.6b03592. https://www.osti.gov/servlets/purl/1433967.
@article{osti_1433967,
title = {Interaction of Black Phosphorus with Oxygen and Water},
author = {Huang, Yuan and Qiao, Jingsi and He, Kai and Bliznakov, Stoyan and Sutter, Eli and Chen, Xianjue and Luo, Da and Meng, Fanke and Su, Dong and Decker, Jeremy and Ji, Wei and Ruoff, Rodney S. and Sutter, Peter},
abstractNote = {Black phosphorus (BP) has attracted significant interest as a monolayer or few-layer material with extraordinary electrical and optoelectronic properties. Chemical reactions with different ambient species, notably oxygen and water, are important as they govern key properties such as stability in air, electronic structure and charge transport, wetting by aqueous solutions, etc. Here, we report experiments combined with ab-initio calculations that address the effects of oxygen and water in contact with BP. Our results show that the reaction with oxygen is primarily responsible for changing properties of BP. Oxidation involving the dissociative chemisorption of O2 causes the decomposition of BP and continuously lowers the conductance of BP field-effect transistors (FETs). In contrast, BP is stable in contact with deaerated (i.e., O2 depleted) water and the carrier mobility in BP FETs gated by H2O increases significantly due to efficient dielectric screening of scattering centers by the high-k dielectric. Isotope labeling experiments, contact angle measurements and calculations show that the pristine BP surface is hydrophobic, but is turned progressively hydrophilic by oxidation. Lastly, our results open new avenues for exploring applications that require contact of BP with aqueous solutions including solution gating, electrochemistry, and solution-phase approaches for exfoliation, dispersion, and delivery of BP.},
doi = {10.1021/acs.chemmater.6b03592},
journal = {Chemistry of Materials},
number = 22,
volume = 28,
place = {United States},
year = {2016},
month = {10}
}

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