On the chemical homogeneity of InxGa1−xN alloys – Electron microscopy at the edge of technical limits

Specht, Petra; Kisielowski, Christian

doi:10.1016/j.mssp.2016.07.011

Title: On the chemical homogeneity of InxGa1−xN alloys – Electron microscopy at the edge of technical limits

Abstract

Ternary In_xGa_1–xN alloys became technologically attractive when p-doping was achieved to produce blue and green light emitting diodes (LED)s. Starting in the mid 1990th, investigations of their chemical homogeneity were driven by the need to understand carrier recombination mechanisms in optical device structures to optimize their performance. Transmission electron microscopy (TEM) is the technique of choice to complement optical data evaluations, which suggests the coexistence of local carrier recombination mechanisms based on piezoelectric field effects and on indium clustering in the quantum wells of LEDs. We summarize the historic context of homogeneity investigations using electron microscopy techniques that can principally resolve the question of indium segregation and clustering in In_xGa_1–xN alloys if optimal sample preparation and electron dose-controlled imaging techniques are employed together with advanced data evaluation.

Authors:: Specht, Petra; Kisielowski, Christian

Publication Date:: Sat Jul 01 00:00:00 EDT 2017

Research Org.:: Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)

Sponsoring Org.:: USDOE Office of Science (SC), Basic Energy Sciences (BES); USDOE National Nuclear Security Administration (NNSA), Office of Defense Nuclear Nonproliferation

OSTI Identifier:: 1875609

Alternate Identifier(s):: OSTI ID: 1419434

Grant/Contract Number:: AC02-05CH11231; 00002844

Resource Type:: Published Article

Journal Name:: Materials Science in Semiconductor Processing

Additional Journal Information:: Journal Name: Materials Science in Semiconductor Processing Journal Volume: 65 Journal Issue: C; Journal ID: ISSN 1369-8001

Publisher:: Elsevier

Country of Publication:: Netherlands

Language:: English

Subject:: 36 MATERIALS SCIENCE; Transmission electron microscopy; InxGa1−xN alloys; Homogeneity; Spinodal decomposition; Band gap

Citation Formats


                    Specht, Petra, and Kisielowski, Christian. On the chemical homogeneity of InxGa1−xN alloys – Electron microscopy at the edge of technical limits.  Netherlands: N. p., 2017. 
Web.  doi:10.1016/j.mssp.2016.07.011.

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                    Specht, Petra, & Kisielowski, Christian. On the chemical homogeneity of InxGa1−xN alloys – Electron microscopy at the edge of technical limits.  Netherlands.  https://doi.org/10.1016/j.mssp.2016.07.011

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                    Specht, Petra, and Kisielowski, Christian. Sat .  
"On the chemical homogeneity of InxGa1−xN alloys – Electron microscopy at the edge of technical limits".  Netherlands.  https://doi.org/10.1016/j.mssp.2016.07.011.

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@article{osti_1875609,

  title        = {On the chemical homogeneity of InxGa1−xN alloys – Electron microscopy at the edge of technical limits},

  author       = {Specht, Petra and Kisielowski, Christian},

  abstractNote = {Ternary InxGa1–xN alloys became technologically attractive when p-doping was achieved to produce blue and green light emitting diodes (LED)s. Starting in the mid 1990th, investigations of their chemical homogeneity were driven by the need to understand carrier recombination mechanisms in optical device structures to optimize their performance. Transmission electron microscopy (TEM) is the technique of choice to complement optical data evaluations, which suggests the coexistence of local carrier recombination mechanisms based on piezoelectric field effects and on indium clustering in the quantum wells of LEDs. We summarize the historic context of homogeneity investigations using electron microscopy techniques that can principally resolve the question of indium segregation and clustering in InxGa1–xN alloys if optimal sample preparation and electron dose-controlled imaging techniques are employed together with advanced data evaluation.},

  doi          = {10.1016/j.mssp.2016.07.011},

  journal      = {Materials Science in Semiconductor Processing},

  number       = C,

  volume       = 65,

  place        = {Netherlands},

  year         = {Sat Jul 01 00:00:00 EDT 2017},

  month        = {Sat Jul 01 00:00:00 EDT 2017}

}

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Journal Article Johnson, M C ; Bourret-Courchesne, E D ; Wu, J ; ... - Journal of Applied Physics

GaN template layer strain effects were investigated on the growth of InGaN/GaN LED devices. Seven period InGaN/GaN multiple quantum well structures were deposited on 5{micro}m and 15{micro}m GaN template layers. It was found that the electroluminescence emission of the 15{micro}m device was red-shifted by approximately 132meV. Triple-axis X-Ray Diffraction and Cross-Sectional Transmission Electron Microscopy show that the 15{micro}m templay layer device was virtually unstrained while the 5{micro}m layer experienced tensile strain. Dynamic Secondary Ion Mass Spectrometry depth profiles show that the 15{micro}m template layer device had an average indium concentration of 11% higher than that of the 5{micro}m template layermore »« less
https://doi.org/10.1063/1.1766407

Full Text Available
Effect of Gallium Nitride Template Layer Strain on the Growth of InxGa1-xN/GaN Multiple Quantum Well Light Emitting Diodes

Journal Article Johnson, Michael C ; Bourret-Courchesne, Edith D ; Wu, J ; ... - Journal of Applied Physics

GaN template layer strain effects on the growth of InGaN/GaN light emitting diodes (LED) devices were investigated. Seven-period InGaN/GaN multiple quantum well structures (MQW) were deposited on 5?m and 15?m GaN template layers. It was found that the electroluminescence (EL) emission of the 15?m device was red-shifted by approximately 132meV. Triple-axis X-Ray Diffraction (TAXRD) and Cross-Sectional Transmission Electron Microscopy (XTEM) show that the 15?m template layer device was virtually unstrained while the 5?m layer experienced tensile strain. Dynamic Secondary Ion Mass Spectrometry (SIMS) depth profiles show that the 15?m template layer device had an average indium concentration of 11% highermore »« less
https://doi.org/10.1063/1.1766407

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Title: On the chemical homogeneity of InxGa1−xN alloys – Electron microscopy at the edge of technical limits

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Citation Formats

Phase separation and ordering in InGaN alloys grown by molecular beam epitaxy journal, August 1998

The electron-beam-induced reduction of transition metal oxide surfaces to metallic lower oxides journal, January 1987

Temperature and compositional dependence of the energy band gap of AlGaN alloys journal, December 2005

From extended defects and interfaces to point defects in three dimensions—The case of InxGa1−xN journal, December 2007

The influence of the group V/III molar precursor ratio on the structural properties of InGaN layers grown by HPCVD journal, May 2010

Incomplete Solubility in Nitride Alloys journal, January 1996

Electron-beam-induced segregation in InGaN/GaN multiple-quantum wells journal, September 2003

Revisiting the “In-clustering” question in InGaN through the use of aberration-corrected electron microscopy below the knock-on threshold journal, May 2013

Surface segregation effects of In in GaAs journal, August 1993

Probing the Onset of Functional Behavior by Exciting Reversible Atom Displacements Using Variable Voltages and Dose Rates journal, August 2013

Indium redistribution in an InGaN quantum well induced by electron-beam irradiation in a transmission electron microscope journal, June 2005

Phase separation in In x Ga 1− x N journal, May 2007

MOVPE growth of InN films and quantum dots journal, August 2004

Radiation hardness of gallium nitride journal, December 2002

Atomic Scale Indium Distribution in a G a N / I n 0.43 G a 0.57 N / A l 0.1 G a 0.9 N Quantum Well Structure journal, November 1997

Time, energy, and spatially resolved TEM investigations of defects in InGaN journal, April 2006

Interface segregation and clustering in strained-layer InGaAs/GaAs heterostructures studied by cross-sectional scanning tunneling microscopy journal, April 1994

Resolution extension and exit wave reconstruction in complex HREM journal, January 2004

Local Strain Measurements in Hexagonal Systems journal, July 1998

Growth and applications of Group III-nitrides journal, October 1998

Observing Atoms at Work by Controlling Beam-Sample Interactions journal, June 2015

High-Brightness InGaN Blue, Green and Yellow Light-Emitting Diodes with Quantum Well Structures journal, July 1995

Optical band gap of indium nitride journal, May 1986

Electron microscopy image enhanced journal, April 1998

Recombination dynamics of localized excitons in In 0.20 Ga 0.80 N- In 0.05 Ga 0.95 N multiple quantum wells journal, January 1997

Ge segregation in SiGe/Si heterostructures and its dependence on deposition technique and growth atmosphere journal, November 1993

Complete composition tunability of InGaN nanowires using a combinatorial approach journal, October 2007

Role of gross well-width fluctuations in bright, green-emitting single InGaN∕GaN quantum well structures journal, March 2007

Local indium segregation and bang gap variations in high efficiency green light emitting InGaN/GaN diodes journal, January 2006

Vacancy defects in epitaxial InN: identification and electrical properties journal, August 2004

Subangstrom Resolution by Underfocused Incoherent Transmission Electron Microscopy journal, November 1998

Band transitions in wurtzite GaN and InN determined by valence electron energy loss spectroscopy journal, August 2005

Zincblende and wurtzite phases in InN epilayers and their respective band transitions journal, March 2006

Spontaneous emission of localized excitons in InGaN single and multiquantum well structures journal, December 1996

Strain state analysis of InGaN/GaN - sources of error and optimized imaging conditions journal, January 2006

Low-temperature growth of InGaN films over the entire composition range by MBE journal, September 2015

P-Type Conduction in Mg-Doped GaN Treated with Low-Energy Electron Beam Irradiation (LEEBI) journal, December 1989

High resolution transmission electron microscopy of InN journal, September 2007

On the dose-rate threshold of beam damage in TEM journal, February 2012

The effects of indium concentration and well-thickness on the mechanisms of radiative recombination in In x Ga 1−x N quantum wells journal, January 2000

Maximum-likelihood method for focus-variation image reconstruction in high resolution transmission electron microscopy journal, August 1996

Observation and control of the surface kinetics of InGaN for the elimination of phase separation journal, July 2012

Aberration Corrected Lattice Imaging With Sub Ångstrom Resolution journal, August 2000

Instrumental requirements for the detection of electron beam-induced object excitations at the single atom level in high-resolution transmission electron microscopy journal, January 2015

Strain-related phenomena in GaN thin films journal, December 1996

Native defects and impurities in InN: First-principles studies using the local-density approximation and self-interaction and relaxation-corrected pseudopotentials journal, March 2000

Atomic Resolution Phase Contrast Imaging and In-Line Holography Using Variable Voltage and Dose Rate journal, October 2012

Impact of low-temperature buffer layers on nitride-based optoelectronics journal, June 2002

Phase separation in InGaN grown by metalorganic chemical vapor deposition journal, January 1998

Growth and characterization of bulk InGaN films and quantum wells journal, May 1996

Proton Radiation-Induced Void Formation in Ni/Au-Gated AlGaN/GaN HEMTs journal, December 2014

Mie Resonances, Infrared Emission, and the Band Gap of InN journal, March 2004

Background, status and future of the Transmission Electron Aberration-corrected Microscope project journal, August 2009

Absorption and Emission of Hexagonal InN. Evidence of Narrow Fundamental Band Gap journal, February 2002

Band-gap evolution, hybridization, and thermal stability of In x Ga 1 − x N alloys measured by soft X-ray emission and absorption journal, April 2002

Optical assessment of the main electron trap in bulk semi‐insulating GaAs journal, November 1981

Real-time sub- Å ngstrom imaging of reversible and irreversible conformations in rhodium catalysts and graphene journal, July 2013

Approaches for high internal quantum efficiency green InGaN light-emitting diodes with large overlap quantum wells journal, January 2011

Investigation of inhomogeneities in (Al, Ga, In)N heterostructures by STEM and cathodoluminescence journal, February 1998

Imaging columns of the light elements carbon, nitrogen and oxygen with sub Ångstrom resolution journal, November 2001

Degradation mechanisms of 2 MeV proton irradiated AlGaN/GaN HEMTs journal, August 2015

Physical properties of InN with the band gap energy of 1.1eV journal, July 2001

The Coulomb Scattering of Relativistic Electrons by Nuclei journal, December 1948

An approach to quantitative high-resolution transmission electron microscopy of crystalline materials journal, May 1995

Radiation damage in the TEM and SEM journal, August 2004

Phase separation in confined geometries: Solving the Cahn–Hilliard equation with generic boundary conditions journal, January 2001

Are the Materials Properties of Indiumnitride Dominated by Defects? journal, January 2007

Atomic Scale Aluminum and Strain Distribution in a Gan/Al x Ga 1−X N Heterostructure journal, January 1997

Gentle STEM: ADF imaging and EELS at low primary energies journal, July 2010

Small band gap bowing in In1−xGaxN alloys journal, June 2002

Origin of Luminescence from InGaN Diodes journal, January 1999

Atomic-resolution imaging of lithium in Al 3 Li precipitates journal, July 2009

Phase imaging and the evolution of a gold-vacuum interface at atomic resolution journal, November 2006

A quantitative procedure to probe for compositional inhomogeneities in InxGa1−xN alloys journal, October 2008

Reliability of GaN HEMTs: Electrical and Radiation-Induced Failure Mechanism journal, August 2013

Quantitative measurement of displacement and strain fields from HREM micrographs journal, August 1998

Focal-series reconstruction in HRTEM: simulation studies on non-periodic objects journal, August 1996

Phase separation and ordering in InGaN alloys grown by molecular beam epitaxy
journal, August 1998

The electron-beam-induced reduction of transition metal oxide surfaces to metallic lower oxides
journal, January 1987

Temperature and compositional dependence of the energy band gap of AlGaN alloys
journal, December 2005

From extended defects and interfaces to point defects in three dimensions—The case of InxGa1−xN
journal, December 2007

The influence of the group V/III molar precursor ratio on the structural properties of InGaN layers grown by HPCVD
journal, May 2010

Incomplete Solubility in Nitride Alloys
journal, January 1996

Electron-beam-induced segregation in InGaN/GaN multiple-quantum wells
journal, September 2003

Revisiting the “In-clustering” question in InGaN through the use of aberration-corrected electron microscopy below the knock-on threshold
journal, May 2013

Surface segregation effects of In in GaAs
journal, August 1993

Probing the Onset of Functional Behavior by Exciting Reversible Atom Displacements Using Variable Voltages and Dose Rates
journal, August 2013

Indium redistribution in an InGaN quantum well induced by electron-beam irradiation in a transmission electron microscope
journal, June 2005

Phase separation in In _x Ga ₁₋ _x N
journal, May 2007

MOVPE growth of InN films and quantum dots
journal, August 2004

Radiation hardness of gallium nitride
journal, December 2002

Atomic Scale Indium Distribution in a G a N / I n _0.43 G a _0.57 N / A l _0.1 G a _0.9 N Quantum Well Structure
journal, November 1997

Time, energy, and spatially resolved TEM investigations of defects in InGaN
journal, April 2006

Interface segregation and clustering in strained-layer InGaAs/GaAs heterostructures studied by cross-sectional scanning tunneling microscopy
journal, April 1994

Resolution extension and exit wave reconstruction in complex HREM
journal, January 2004

Local Strain Measurements in Hexagonal Systems
journal, July 1998

Growth and applications of Group III-nitrides
journal, October 1998

Observing Atoms at Work by Controlling Beam-Sample Interactions
journal, June 2015

High-Brightness InGaN Blue, Green and Yellow Light-Emitting Diodes with Quantum Well Structures
journal, July 1995

Optical band gap of indium nitride
journal, May 1986

Electron microscopy image enhanced
journal, April 1998

Recombination dynamics of localized excitons in ${In}_{0.20}$ ${Ga}_{0.80}$ N- ${In}_{0.05}$ ${Ga}_{0.95}$ N multiple quantum wells
journal, January 1997

Ge segregation in SiGe/Si heterostructures and its dependence on deposition technique and growth atmosphere
journal, November 1993

Complete composition tunability of InGaN nanowires using a combinatorial approach
journal, October 2007

Role of gross well-width fluctuations in bright, green-emitting single InGaN∕GaN quantum well structures
journal, March 2007

Local indium segregation and bang gap variations in high efficiency green light emitting InGaN/GaN diodes
journal, January 2006

Vacancy defects in epitaxial InN: identification and electrical properties
journal, August 2004

Subangstrom Resolution by Underfocused Incoherent Transmission Electron Microscopy
journal, November 1998

Band transitions in wurtzite GaN and InN determined by valence electron energy loss spectroscopy
journal, August 2005

Zincblende and wurtzite phases in InN epilayers and their respective band transitions
journal, March 2006

Spontaneous emission of localized excitons in InGaN single and multiquantum well structures
journal, December 1996

Strain state analysis of InGaN/GaN - sources of error and optimized imaging conditions
journal, January 2006

Low-temperature growth of InGaN films over the entire composition range by MBE
journal, September 2015

P-Type Conduction in Mg-Doped GaN Treated with Low-Energy Electron Beam Irradiation (LEEBI)
journal, December 1989

High resolution transmission electron microscopy of InN
journal, September 2007

On the dose-rate threshold of beam damage in TEM
journal, February 2012

The effects of indium concentration and well-thickness on the mechanisms of radiative recombination in In _x Ga _1−x N quantum wells
journal, January 2000

Maximum-likelihood method for focus-variation image reconstruction in high resolution transmission electron microscopy
journal, August 1996

Observation and control of the surface kinetics of InGaN for the elimination of phase separation
journal, July 2012

Aberration Corrected Lattice Imaging With Sub Ångstrom Resolution
journal, August 2000

Instrumental requirements for the detection of electron beam-induced object excitations at the single atom level in high-resolution transmission electron microscopy
journal, January 2015

Strain-related phenomena in GaN thin films
journal, December 1996

Native defects and impurities in InN: First-principles studies using the local-density approximation and self-interaction and relaxation-corrected pseudopotentials
journal, March 2000

Atomic Resolution Phase Contrast Imaging and In-Line Holography Using Variable Voltage and Dose Rate
journal, October 2012

Impact of low-temperature buffer layers on nitride-based optoelectronics
journal, June 2002

Phase separation in InGaN grown by metalorganic chemical vapor deposition
journal, January 1998

Growth and characterization of bulk InGaN films and quantum wells
journal, May 1996

Proton Radiation-Induced Void Formation in Ni/Au-Gated AlGaN/GaN HEMTs
journal, December 2014

Mie Resonances, Infrared Emission, and the Band Gap of InN
journal, March 2004

Background, status and future of the Transmission Electron Aberration-corrected Microscope project
journal, August 2009

Absorption and Emission of Hexagonal InN. Evidence of Narrow Fundamental Band Gap
journal, February 2002

Band-gap evolution, hybridization, and thermal stability of ${In}_{x} {Ga}_{1 - x} N$ alloys measured by soft X-ray emission and absorption
journal, April 2002

Optical assessment of the main electron trap in bulk semi‐insulating GaAs
journal, November 1981

Real-time sub- $Å$ ngstrom imaging of reversible and irreversible conformations in rhodium catalysts and graphene
journal, July 2013

Approaches for high internal quantum efficiency green InGaN light-emitting diodes with large overlap quantum wells
journal, January 2011

Investigation of inhomogeneities in (Al, Ga, In)N heterostructures by STEM and cathodoluminescence
journal, February 1998

Imaging columns of the light elements carbon, nitrogen and oxygen with sub Ångstrom resolution
journal, November 2001

Degradation mechanisms of 2 MeV proton irradiated AlGaN/GaN HEMTs
journal, August 2015

Physical properties of InN with the band gap energy of 1.1eV
journal, July 2001

The Coulomb Scattering of Relativistic Electrons by Nuclei
journal, December 1948

An approach to quantitative high-resolution transmission electron microscopy of crystalline materials
journal, May 1995

Radiation damage in the TEM and SEM
journal, August 2004

Phase separation in confined geometries: Solving the Cahn–Hilliard equation with generic boundary conditions
journal, January 2001

Are the Materials Properties of Indiumnitride Dominated by Defects?
journal, January 2007

Atomic Scale Aluminum and Strain Distribution in a Gan/Al _x Ga _1−X N Heterostructure
journal, January 1997

Gentle STEM: ADF imaging and EELS at low primary energies
journal, July 2010

Small band gap bowing in In1−xGaxN alloys
journal, June 2002

Origin of Luminescence from InGaN Diodes
journal, January 1999

Atomic-resolution imaging of lithium in ${Al}_{3} Li$ precipitates
journal, July 2009

Phase imaging and the evolution of a gold-vacuum interface at atomic resolution
journal, November 2006

A quantitative procedure to probe for compositional inhomogeneities in InxGa1−xN alloys
journal, October 2008

Reliability of GaN HEMTs: Electrical and Radiation-Induced Failure Mechanism
journal, August 2013

Quantitative measurement of displacement and strain fields from HREM micrographs
journal, August 1998

Focal-series reconstruction in HRTEM: simulation studies on non-periodic objects
journal, August 1996

Sub-ångstrom resolution using aberration corrected electron optics
journal, August 2002

The impact of gross well width fluctuations on the efficiency of GaN-based light emitting diodes
journal, September 2013

Comment on ‘‘Chemical mapping of semiconductor interfaces at near-atomic resolution’’
journal, October 1990