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Front. Mater. Sci.    2022, Vol. 16 Issue (1) : 220590    https://doi.org/10.1007/s11706-022-0590-z
REVIEW ARTICLE
Chemical vapor deposited diamond with versatile grades: from gemstone to quantum electronics
Yuting ZHENG1,2,3, Chengming LI1(), Jinlong LIU1(), Junjun WEI1,2, Xiaotong ZHANG2,3,4, Haitao YE5, Xiaoping OUYANG6
1. Institute for Advanced Materials and Technology (IAMT), State Key Laboratory for Advanced Metals and Materials, University of Science and Technology Beijing, Beijing 100083, China
2. Shunde Graduate School, University of Science and Technology Beijing, Foshan 528399, China
3. School of Computer and Communication Engineering, University of Science and Technology Beijing, Beijing 100083, China
4. Beijing Advanced Innovation Center for Materials Genome Engineering, University of Science and Technology Beijing, Beijing 100083, China
5. School of Engineering, University of Leicester, Leicester LE1 7RH, UK
6. School of Materials Science and Engineering, Xiangtan University, Xiangtan 411105, China
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Abstract

Chemical vapor deposited (CVD) diamond as a burgeoning multi-functional material with tailored quality and characteristics can be artificially synthesized and controlled for various applications. Correspondingly, the application-related “grade” concept associated with materials choice and design was gradually formulated, of which the availability and the performance are optimally suited. In this review, the explicit diversity of CVD diamond and the clarification of typical grades for applications, i.e., from resplendent gem-grade to promising quantum-grade, were systematically summarized and discussed, according to the crystal quality and main consideration of ubiquitous nitrogen impurity content as well as major applications. Realizations of those, from quantum-grade with near-ideal crystal to electronic-grade having extremely low imperfections and then to optical, thermal as well as mechanical-grade needing controlled flaws and allowable impurities, would competently fulfill the multi-field application prospects with appropriate choice in terms of cost and quality. Exceptionally, wide range defects and impurities in the gem-grade diamond (only indicating single crystal), which are detrimental for technology applications, endows CVD crystals with fancy colors to challenge their natural counterparts.
Keywords CVD diamond      synthesis and characterization      quality and impurity      grading      application     
Corresponding Author(s): Chengming LI,Jinlong LIU   
About author:

Miaojie Yang and Mahmood Brobbey Oppong contributed equally to this work.
Issue Date: 02 March 2022
 Cite this article:   
Yuting ZHENG,Chengming LI,Jinlong LIU, et al. Chemical vapor deposited diamond with versatile grades: from gemstone to quantum electronics[J]. Front. Mater. Sci., 2022, 16(1): 220590.
 URL:  
https://academic.hep.com.cn/foms/EN/10.1007/s11706-022-0590-z
https://academic.hep.com.cn/foms/EN/Y2022/V16/I1/220590
Fig.1  Versatile CVD diamonds with specific applicable grade for diverse practical applications.
Fig.2  Phase diagram of carbon associated with diamond synthesis.
Fig.3  (a) Schematic illustrations of dislocation propagation and proliferation behavior from a substrate to an epitaxial layer and (b) cross-sectional CL view of band-A mapping taken at different acceleration voltages of the electron beam. Reproduced with permission from Ref. [45] (Copyright 2019 Wiley-VCH). (c) SIMS fine element profile of impurities from grown layer to substrate. Reproduced with permission from Ref. [46] (Copyright 2015 Wiley-VCH).
Type Properties
Quantity Nitrogen content/ppm Dominant nitrogen form Color Stress, Δn Dislocation/cm–2
Natural type IIa (IIb) Rare (extremely rare) <10, or even<5 Aggregates or substitutional (additional boron) Colorless or weak brown (light blue or gray) 10–4–10–2 10–8–10–9
CVD type IIa (IIb) General (intentionally design) <1–2, or in ppb range Single substitutional (additional boron) Colorless or intentionally colored (light blue or gray) <5×10–5 ≤10–4
Natural type Ia (Ib) General (rare few) Hundreds even thousands Aggregates (isolated) Colorless to yellow to brown (wider range of color) 10–6–10–2 <10–6
CVD type Ia or Ib Extremely rare (unless intentionally design) >10 (even 5) to hundreds, even thousands Aggregates (isolated) Yellow >10–5 ~10–4–10–6
Tab.1  Comparison of general properties for natural and CVD synthetic single crystal diamonds [37,49–51]
Color Cause of color (defect or impurity as well as relative wavelengths)
Yellow N3/N2 “cape” (3NV, 415/478 nm); isolated nitrogen “C centers” (N); H3 absorption (2NV0, 503.5 nm); H4 (496 nm); hydrogen (unknown); 480 nm band (unknown); vacancy (595 nm)
Brown Vacancy clusters (multiple V) or deformation; isolated nitrogen “C centers” (N); H3 absorption (2NV0) + 550 nm; band (unknown); hydrogen (unknown)
Blue Boron (B); radiation damage — GR1 (V0,741 nm); hydrogen (unknown)
Pink (red) Plastic deformation — 550 nm; band (unknown); nitrogen vacancy (NV0, 575 nm; NV–, 637 nm)
Purple (violet) Hydrogen (unknown); plastic deformation — 550 nm; band (unknown)
Milky (white) deformation (536 nm); VN3H defects (490 nm); 3107 cm–1; 3085.4 cm–1 (accompanying)
Gray Deformation — related defects (<500 nm); carbon inclusions
Green Radiation damage — GR1 (V0, 741 nm); H3 fluorescence; H2 (986 nm); hydrogen (unknown); nickel (unknown); 595 nm (V)
Orange H3 absorption (2NV0) + 550 nm; band (unknown); 480 nm band (unknown); isolated nitrogen “C centers” (N)
Tab.2  A brief description of common causes of color in gem diamonds [2,59–71]
Fig.4  Evolution of an as-grown CVD synthetic diamond to a facetted gemstone. Reproduced with permission from Ref. [78] (Copyright 2014 Elsevier).
Fig.5  (a) Indentation patterns for as-grown and (b) annealed near colorless as well as (c) ultra-tough CVD SCD. (d) Vickers hardness and fracture toughness measurements on {1?0?0} faces of various SCDs in the {1?0?0} direction. Reproduced with permission from Ref. [102] (Copyright 2009 Elsevier).
Fig.6  (a) Close-up view of the SCD micro-tool fabricated by a FIB. Reproduced with permission from Ref. [105] (Copyright 2012 Elsevier). (b) Experimental diamond tool setup using ultraprecision cutting machine with shuttle unit together with the left inset of textured diamond cutting tools and the right inset of surface topographies of workpiece after machining by diamond tool. Reproduced with permission from Ref. [106] (Copyright 2019 Elsevier).
Diamond color Nitrogen concentration/ppm Hardness/GPa Abrasion resistance
Yellow 70 95 0.84
20 106 1.31
Pale green ~2 – 1.72
~0.1 131 3.11
Colorless ~0.3 110 3.05
Tab.3  Hardness and abrasion resistance of man-made diamond single crystals [29]
Fig.7  Hardness, fracture strength, fracture toughness and Young’s modulus of PCD as a function of grain size comparing with SCDs. Reproduced with permission from Ref. [109] (Copyright 2012 American Institute of Physics).
Fig.8  Quality factors of single-crystal diamond nano-resonators between 3 and 300 K. Two representative diamond devices are compared with reference devices made from polycrystalline diamond and single-crystal silicon of similar thickness. Reproduced with permission from Ref. [139] (Copyright 2014 Springer Nature).
Fig.9  (a) Operating temperature of different industrial sectors and current silicon-based electronic systems can operate at a maximum temperature of ~200 °C. Reproduced with permission from Ref. [141] (Copyright 2018 Wiley-VCH). Infrared-thermography images of a diamond FET with LG of 0.4 μm and WG of 200 μm when (b) DC and RF powers are off and (c) DC and RF are on. Reproduced with permission from Ref. [142] (Copyright 2006 Elsevier).
Materials grade Nitrogen concentration/ppm Dislocation density/cm–2 Grain size/μm C-vacancy concentration/ppm
1800 W·m–1·K–1 (600 μm) 2.0–5.0 108 100–140 20–30
1800 W·m–1·K–1 (250 μm) 2.0–5.0 108 30–70 20–30
1500 W·m–1·K–1 (250 μm) 12–17 108 30–70 20
1000 W·m–1·K–1 (250 μm) 0.1–0.3 1011 20–30 22–24
Optical 0.1–0.4 108 120–160 9–13
Tab.4  Values for some disruptive properties in diamond grains measured for various grades of CVD diamonds [149]
Fig.10  Correlative EBSD-TDTR microscopy of polycrystalline diamond for directly showing the effect of GB areas on κ. Reproduced with permission from Ref. [161] (Copyright 2018 American Chemical Society).
Fig.11  (a) Optical images of fabricated diamond micro-lenses with large radius of curvature and (b) demonstration of the monolithic diamond Raman laser based on the micro-lens resonator. Reproduced with permission from Ref. [169] (Copyright 2016 Elsevier).
Fig.12  (a) Optical microscopy images of transparent, translucent and opaque PCD films and (b) its IR transmission spectra. (c) EELS spectrum of dark inclusions and (d) HRTEM image of micro-deformation as well as (e) TEM bright fields image of dark features of the opaque sample. Reproduced with permission from Ref. [177] (Copyright 2005 Elsevier).
Element Ea/eV a) Conduction type Comment Refs.
B 0.36–0.37 p Insulative to metallic to superconductive [188–190]
H on surface 0.05 Unstable [191–192]
O 0.32 n Need cold-implantation-rapid-annealing [193]
P 0.57–0.6 Deep donor, limited to the (1?1?1)-oriented diamond lattice structure [194–195]
N 1.7 Deep donor [189,196]
S (S-complex) 0.38 (0.1) S++ c) state cannot act as a donor due to no extra level introduced in the band gap; quite low doping efficiency and solubility (activation energy unstable) [197–198]
Deuterated B 0.23 – [199]
Li 0.1 and 0.4 (~0.2) b) Insoluble, unstable, and likely to form complexes with impurities and vacancies [200–201]
Na 0.3 (0.13–0.42) b) [200,202]
Sn, Te, As, Sb ~0.4–0.5 Unstable, and likely to be compensated by other defects or atom size is large [203]
Tab.5  Doping impurities introduced into synthetic diamond for semiconductor use [188–203]
Fig.13  (a) Nitrogen and vacancy induced deformation in diamond crystal. Reproduced with permission from Ref. [209] (Copyright 2018 American Physical Society). (b)(c) Hall mobility of holes as a function of doping level in homoepitaxial diamond at 300 and 500 K. The symbols indicate experimental data, and the theoretical contributions of various scattering modes are illustrated by dashed and dotted lines for the lattice (lat, acoustic, and optical phonons): a dotted line for the ionized impurities (ii) mode, and a dashed line for the neutral impurities (ni) mode. Reproduced with permission from Ref. [210] (Copyright 2010 American Physical Society). (d) The band electron experiences the depicted CB minimum fluctuation caused by strain fields around an edge dislocation. Reproduced with permission from Ref. [212] (Copyright 2002 American Institute of Physics). (e) TEM analysis of dislocations on off-axis grown diamond without N2 in the gas phase. Reproduced with permission from Ref. [213] (Copyright 2016 Elsevier). (f)(g) Plots of Schubweg and lifetime vs. effective dislocation density. Reproduced with permission from Ref. [214] (Copyright 2020 American Institute of Physics).
Fig.14  (a) Typical CCE map for electron and hole signals affected by nitrogen impurity and dislocation. Reproduced with permission from Ref. [219] (Copyright 2007 American Institute of Physics). (b) Fluorescence microscopy image of “electronic-grade” polycrystalline CVD diamond containing multiple NV centers. Bright regions correspond to grain boundaries and the figure on the right is a higher magnification of the black square. The spatial variation within grains illustrates different defect uptake levels in different growth sectors. A clear example of a sector boundary, or the original facet edge before planarisation, runs between Points 1 and 2. Reproduced with permission from Ref. [229] (Copyright 2011 Elsevier).
Fig.15  (a) Large size freestanding unpolished SCD plate. Reproduced with permission from Ref. [231] (Copyright 2017 Springer Nature). (b) Uniformly and repeatably fabricated inch-sized SCD wafers. Reproduced with permission from Ref. [232] (Copyright 2013 Elsevier). (c) State-of-the-art diamond SCD substrates categorized by growth method, size, and quality. Reproduced with permission from Ref. [45] (Copyright 2019 Wiley-VCH).
Fig.16  (a) A confocal microscope image shows PL from implanted NV centers (with the photon count rate in units of kilocounts per second) containing single NV. Reproduced with permission from Ref. [242] (Copyright 2014 American Institute of Physics). (b) Example photon autocorrelation function obtained from a single NV center at room temperature. Reproduced with permission from Ref. [243] (Copyright 2013 Elsevier). (c) Atomic structure of the NV center in diamond, energy-level diagram of the NV center, and the one-dimensional representation of adiabatic potential energy surfaces in the ground and the excited states. Reproduced with permission from Ref. [244] (Copyright 2021 American Physical Society). In which the points A and D represent equilibrium geometry of the ground state, while the points B and C represent equilibrium geometry of the excited state. ΔEg and ΔEe are lattice relaxation energies. E0 is energy difference between the potential energy minima, and EZPL is the energy of the zero-phonon line. (d) Confocal mapping image and (e) electrical mapping image on a negative single NV center in electronic grade diamond. Reproduced with permission from Ref. [245] (Copyright 2019 American Association for the Advancement of Science).
Fig.17  Detail depth (x–z) and in-plane (x–y) distributions of color centers near one implantation spot of nitrogen ions for NV creation, the SiV– can be detected. Reproduced with permission from Ref. [46] (Copyright 2015 Wiley-VCH).
Fig.18  (a) Schematic of the proximal nuclear spins (arrows) to the NV center: the native nitrogen nuclear spin and the randomly distributed 13C nuclear spins that are naturally 1.1% abundant in diamond. Reproduced with permission from Ref. [243] (Copyright 2013 Elsevier). (b) Free induction decay signal measured on a single nitrogen-vacancy electron spin for diamond with a natural abundance of 13C isotope (12C content 0.989) and isotopically engineered crystal (12C concentration 0.997). Reproduced with permission from Ref. [255] (Copyright 2009 Springer Nature). (c) Fourier-transform spectra of free induction decay signals. The satellites indicated by asterisks are related to the hyperfine interaction with the nitrogen and carbon nuclei. Reproduced with permission from Ref. [255] (Copyright 2009 Springer Nature).
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