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Title: Direct Nanoscale Characterization of Deep Levels in AgCuInGaSe2 Using Electron Energy–Loss Spectroscopy in the Scanning Transmission Electron Microscope

Abstract

A new experimental framework for the characterization of defects in semiconductors is demonstrated. Through the direct, energy-resolved correlation of three analytical techniques spanning six orders of magnitude in spatial resolution, a critical mid-bandgap electronic trap level (EV + 0.56 eV) within Ag0.2Cu0.8In1–xGaxSe2 is traced to its nanoscale physical location and chemical source. This is achieved through a stepwise, site-specific correlated characterization workflow consisting of device-scale (≈1 mm2) deep level transient spectroscopy (DLTS) to survey the traps present, scanning probe–based DLTS (scanning-DLTS) for mesoscale-resolved (hundreds of nanometers) mapping of the target trap state’s spatial distribution, and scanning transmission electron microscope based electron energy-loss spectroscopy (STEM-EELS) and X-ray energy-dispersive spectroscopy for nanoscale energy-, structure, and chemical-resolved investigation of the defect source. Furthermore, this first demonstration of the direct observation of sub-bandgap defect levels via STEM-EELS, combined with the DLTS methods, provides strong evidence that the longsuspected CuIn/Ga substitutional defects are indeed the most likely source of the EV + 0.56 eV trap state and serves as a key example of this approach for the fundamental identification of defects within semiconductors, in general.

Authors:
ORCiD logo [1];  [1];  [2];  [2];  [2];  [1];  [1]; ORCiD logo [1]
  1. The Ohio State Univ., Columbus, OH (United States)
  2. MiaSolé Hi‐Tech Corp., Santa Clara, CA (United States)
Publication Date:
Research Org.:
Colorado School of Mines, Golden, CO (United States)
Sponsoring Org.:
USDOE Office of Energy Efficiency and Renewable Energy (EERE)
OSTI Identifier:
1766327
Alternate Identifier(s):
OSTI ID: 1547553
Grant/Contract Number:  
EE0007141
Resource Type:
Accepted Manuscript
Journal Name:
Advanced Energy Materials
Additional Journal Information:
Journal Volume: 9; Journal Issue: 35; Journal ID: ISSN 1614-6832
Publisher:
Wiley
Country of Publication:
United States
Language:
English
Subject:
14 SOLAR ENERGY; Defect characterization; semiconductors; chalcopyrites; DLTS; electron energy-loss spectroscopy; electron microscopy; photovoltaics

Citation Formats

Deitz, Julia I., Paul, Pran K., Farshchi, Rouin, Poplavskyy, Dmitry, Bailey, Jeff, Arehart, Aaron R., McComb, David W., and Grassman, Tyler J. Direct Nanoscale Characterization of Deep Levels in AgCuInGaSe2 Using Electron Energy–Loss Spectroscopy in the Scanning Transmission Electron Microscope. United States: N. p., 2019. Web. doi:10.1002/aenm.201901612.
Deitz, Julia I., Paul, Pran K., Farshchi, Rouin, Poplavskyy, Dmitry, Bailey, Jeff, Arehart, Aaron R., McComb, David W., & Grassman, Tyler J. Direct Nanoscale Characterization of Deep Levels in AgCuInGaSe2 Using Electron Energy–Loss Spectroscopy in the Scanning Transmission Electron Microscope. United States. https://doi.org/10.1002/aenm.201901612
Deitz, Julia I., Paul, Pran K., Farshchi, Rouin, Poplavskyy, Dmitry, Bailey, Jeff, Arehart, Aaron R., McComb, David W., and Grassman, Tyler J. Mon . "Direct Nanoscale Characterization of Deep Levels in AgCuInGaSe2 Using Electron Energy–Loss Spectroscopy in the Scanning Transmission Electron Microscope". United States. https://doi.org/10.1002/aenm.201901612. https://www.osti.gov/servlets/purl/1766327.
@article{osti_1766327,
title = {Direct Nanoscale Characterization of Deep Levels in AgCuInGaSe2 Using Electron Energy–Loss Spectroscopy in the Scanning Transmission Electron Microscope},
author = {Deitz, Julia I. and Paul, Pran K. and Farshchi, Rouin and Poplavskyy, Dmitry and Bailey, Jeff and Arehart, Aaron R. and McComb, David W. and Grassman, Tyler J.},
abstractNote = {A new experimental framework for the characterization of defects in semiconductors is demonstrated. Through the direct, energy-resolved correlation of three analytical techniques spanning six orders of magnitude in spatial resolution, a critical mid-bandgap electronic trap level (EV + 0.56 eV) within Ag0.2Cu0.8In1–xGaxSe2 is traced to its nanoscale physical location and chemical source. This is achieved through a stepwise, site-specific correlated characterization workflow consisting of device-scale (≈1 mm2) deep level transient spectroscopy (DLTS) to survey the traps present, scanning probe–based DLTS (scanning-DLTS) for mesoscale-resolved (hundreds of nanometers) mapping of the target trap state’s spatial distribution, and scanning transmission electron microscope based electron energy-loss spectroscopy (STEM-EELS) and X-ray energy-dispersive spectroscopy for nanoscale energy-, structure, and chemical-resolved investigation of the defect source. Furthermore, this first demonstration of the direct observation of sub-bandgap defect levels via STEM-EELS, combined with the DLTS methods, provides strong evidence that the longsuspected CuIn/Ga substitutional defects are indeed the most likely source of the EV + 0.56 eV trap state and serves as a key example of this approach for the fundamental identification of defects within semiconductors, in general.},
doi = {10.1002/aenm.201901612},
journal = {Advanced Energy Materials},
number = 35,
volume = 9,
place = {United States},
year = {Mon Aug 05 00:00:00 EDT 2019},
month = {Mon Aug 05 00:00:00 EDT 2019}
}

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