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Title: High Quality, Low Cost Ammonothermal Bulk GaN Substrates

Abstract

Ammonothermal GaN growth using a novel apparatus has been performed on c-plane, m-plane, and semipolar seed crystals with diameters between 5 mm and 2 in. to thicknesses of 0.5-3 mm. The highest growth rates are greater than 40 mu m/h and rates in the 10-30 mu m/h range are routinely observed for all orientations. These values are 5-100x larger than those achieved by conventional ammonothermal GaN growth. The crystals have been characterized by X-ray diffraction rocking-curve (XRC) analysis, optical and scanning electron microscopy (SEM), cathodoluminescence (CL), optical spectroscopy, and capacitance-voltage measurements. The crystallinity of the grown crystals is similar to or better than that of the seed crystals, with FWHM values of about 20-100 arcsec and dislocation densities of 1 x 10(5)-5 x 10(6) cm(-2). Dislocation densities below 10(4) cm(-2) are observed in laterally-grown crystals. Epitaxial InGaN quantum well structures have been successfully grown on ammonothermal wafers. (C) 2013 The Japan Society of Applied Physics

Authors:
; ; ; ; ; ; ;
Publication Date:
Sponsoring Org.:
USDOE Advanced Research Projects Agency - Energy (ARPA-E)
OSTI Identifier:
1211521
DOE Contract Number:
DE-AR0000020
Resource Type:
Journal Article
Resource Relation:
Journal Name: Japanese Journal of Applied Physics; Journal Volume: 52; Journal Issue: 8
Country of Publication:
United States
Language:
English

Citation Formats

Ehrentraut, D, Pakalapati, RT, Kamber, DS, Jiang, WK, Pocius, DW, Downey, BC, McLaurin, M, and D'Evelyn, MP. High Quality, Low Cost Ammonothermal Bulk GaN Substrates. United States: N. p., 2013. Web. doi:10.7567/JJAP.52.08JA01.
Ehrentraut, D, Pakalapati, RT, Kamber, DS, Jiang, WK, Pocius, DW, Downey, BC, McLaurin, M, & D'Evelyn, MP. High Quality, Low Cost Ammonothermal Bulk GaN Substrates. United States. doi:10.7567/JJAP.52.08JA01.
Ehrentraut, D, Pakalapati, RT, Kamber, DS, Jiang, WK, Pocius, DW, Downey, BC, McLaurin, M, and D'Evelyn, MP. 2013. "High Quality, Low Cost Ammonothermal Bulk GaN Substrates". United States. doi:10.7567/JJAP.52.08JA01.
@article{osti_1211521,
title = {High Quality, Low Cost Ammonothermal Bulk GaN Substrates},
author = {Ehrentraut, D and Pakalapati, RT and Kamber, DS and Jiang, WK and Pocius, DW and Downey, BC and McLaurin, M and D'Evelyn, MP},
abstractNote = {Ammonothermal GaN growth using a novel apparatus has been performed on c-plane, m-plane, and semipolar seed crystals with diameters between 5 mm and 2 in. to thicknesses of 0.5-3 mm. The highest growth rates are greater than 40 mu m/h and rates in the 10-30 mu m/h range are routinely observed for all orientations. These values are 5-100x larger than those achieved by conventional ammonothermal GaN growth. The crystals have been characterized by X-ray diffraction rocking-curve (XRC) analysis, optical and scanning electron microscopy (SEM), cathodoluminescence (CL), optical spectroscopy, and capacitance-voltage measurements. The crystallinity of the grown crystals is similar to or better than that of the seed crystals, with FWHM values of about 20-100 arcsec and dislocation densities of 1 x 10(5)-5 x 10(6) cm(-2). Dislocation densities below 10(4) cm(-2) are observed in laterally-grown crystals. Epitaxial InGaN quantum well structures have been successfully grown on ammonothermal wafers. (C) 2013 The Japan Society of Applied Physics},
doi = {10.7567/JJAP.52.08JA01},
journal = {Japanese Journal of Applied Physics},
number = 8,
volume = 52,
place = {United States},
year = 2013,
month =
}
  • A novel apparatus has been employed to grow ammonothermal (0001) gallium nitride (GaN) with diameters up to 2 in The crystals have been characterized by x-ray diffraction rocking-curve (XRC) analysis, optical and scanning electron microscopy (SEM), cathodoluminescence (CL), and optical spectroscopy. High crystallinity GaN with FWHM values about 20-50 arcsec and dislocation densities below 1 x 10(5) cm(-2) have been obtained. High optical transmission was achieved with an optical absorption coefficient below 1 cm(-1) at a wavelength of 450 nm. (C) 2014 Elsevier B.V. All rights reserved.
  • Broad Funding Opportunity Announcement Project: The new GaN crystal growth method is adapted from that used to grow quartz crystals, which are very inexpensive and represent the second-largest market for single crystals for electronic applications (after silicon). More extreme conditions are required to grow GaN crystals and therefore a new type of chemical growth chamber was invented that is suitable for large-scale manufacturing. A new process was developed that grows GaN crystals at a rate that is more than double that of current processes. The new technology will enable GaN substrates with best-in-world quality at lowest-in-world prices, which in turnmore » will enable new generations of white LEDs, lasers for full-color displays, and high-performance power electronics.« less
  • The objective of this project was to develop the Electrochemical Solution Growth (ESG) method conceived / patented at Sandia National Laboratory into a commercially viable bulk gallium nitride (GaN) growth process that can be scaled to low cost, high quality, and large area GaN wafer substrate manufacturing. The goal was to advance the ESG growth technology by demonstrating rotating seed growth at the lab scale and then transitioning process to prototype commercial system, while validating the GaN material and electronic / optical device quality. The desired outcome of the project is a prototype commercial process for US-based manufacturing of highmore » quality, large area, and lower cost GaN substrates that can drive widespread deployment of energy efficient GaN-based power electronic and optical devices. In year 1 of the project (Sept 2012 – Dec 2013) the overall objective was to demonstrate crystalline GaN growth > 100um on a GaN seed crystal. The development plan included tasks to demonstrate and implement a method for purifying reagent grade salts, develop the reactor 1 process for rotating seed Electrochemical Solution Growth (ESG) of GaN, grow and characterize ESG GaN films, develop a fluid flow and reaction chemistry model for GaN film growth, and design / build an improved growth reactor capable of scaling to 50mm seed diameter. The first year’s project objectives were met in some task areas including salt purification, film characterization, modeling, and reactor 2 design / fabrication. However, the key project objective of the growth of a crystalline GaN film on the seed template was not achieved. Amorphous film growth on the order of a few tenths of a micron has been detected with a film composition including Ga and N, plus several other impurities originating from the process solution and hardware. The presence of these impurities, particularly the oxygen, has inhibited the demonstration of crystalline GaN film growth on the seed template. However, the presence of both Ga and N at the growth surface indicates that the reactor hardware physics is all functioning properly; achieving film growth is a matter of controlling the chemistry at the interface. The impurities originating from the hardware are expected to be straightforward to eliminate. Activities were defined for an extension of budget period 1 to eliminate the undesired impurities originating from the reactor hardware and interfering with crystalline GaN film growth. The budget period 1 extension was negotiated during the 1st half of 2014. The budget period 1 extension spanned approximately from August 2014 to August 2015. The project objective for this extension period was to demonstrate at least 0.5um crystalline GaN film on a GaN seed in the lab scale reactor. The focus of the budget 1 extension period from August 2014 to August 2015 was to eliminate oxygen contamination interference with GaN film growth. The team procured the highest purity lowest oxygen salt for testing. Low oxygen crucible materials such as silicon carbide were installed and evaluated in the laboratory reactor. Growth experiments were performed with high purity salt, high purity hardware, and optimized oxide removal from the seed surface. Experiments were characterized with methods including UV inspection, profilometry, x-ray diffraction (XRD) to determine crystalline structure, optical and scanning electron microscopy, photoluminescence, x-ray photon spectroscopy (XPS), transmission electron microscopy (TEM), and secondary ion mass spectroscopy (SIMS). Despite successfully integrating the low oxygen materials in the laboratory reactor, the goal of depositing 0.5um of crystalline GaN on the MOCVD GaN seed was not met. Very thin (ca. 10nm) cubic phase GaN deposition was observed on the hexagonal MOCVD GaN seeds. But there was a competing etching reaction which was also observed and thought to be related to the presence of metallic lithium, a byproduct of the LiCl-KCl salt used as the process medium. The etching reaction could potentially be addressed by alternate salts not containing lithium, but would necessitate starting all over on the reactor and process design. Further, controlling the reaction of Ga and N in the bulk salt to favor deposition on the seed has proved to be very difficult and unlikely to be solved within the scope of this project in a manner consistent with the original objective for wafer or crystal scale thickness for GaN deposition on a GaN seed. Upon completion of the budget 1 extension period in August 2015 the project partners and DOE agreed to stop work on the project.« less
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