Real-time control of AlN incorporation in epitaxial Hf1−Al N using high-flux, low-energy (10–40 eV) ion bombardment during reactive magnetron sputter deposition from a Hf0.7Al0.3 alloy target

Howe, Brandon M.; Sammann, E.; Wen, Jianguo; Spila, T.; Greene, J. E.; Hultman, Lars; Petrov, I.

doi:10.1016/j.actamat.2010.08.023

Cited by 21 publications

(13 citation statements)

References 40 publications

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“…With larger E i , the Si 2p binding energy shifts to higher values and Si bonding is dominated by more ionic Si-N bonds, resulting in a harder layer. With E i ≥ 50 eV, Si and Al concentrations decrease dramatically due to preferential resputtering of lighter elements, similar to that reported by Howe et al 26 for controlling the AlN incorporation probability in Hf 1−x Al x N films.…”

Section: Introductionsupporting

confidence: 70%

“…This is consistent with the observations of Howe et al who demonstrated real-time control of the AlN concentration in epitaxial pseudobinary Hf 1−x Al x N(001) layers grown from a single Hf 0.7 Al 0.3 alloy target. 26 The AlN incorporation probability varied dramatically (> 200×) due to bombardment of the growing films with high-flux, low-energy ions dur- ing deposition in which E i ranged from 10 to 80 eV. The large ion-to-metal flux ratio, J i /J M e = 8, used in both Howe et al's and the present experiments, results in amplification of the Al and Si resputter yields from the growing film due to the high density of short, overlapping, and nearly isotropic collision cascades.…”

Section: A Hfalsin Film Growth and Nanostructurementioning

confidence: 99%

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Novel hard, tough HfAlSiN multilayers, defined by alternating Si bond structure, deposited using modulated high-flux, low-energy ion irradiation of the growing film

Fager

Howe

Greczyński

et al. 2015

Journal of Vacuum Science &Amp; Technology A: Vacuum, Surfaces, and Films

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Hf 1−x−y Al x Si y N (0 ≤ x ≤ 0.14, 0 ≤ y ≤ 0.12) single layer and multilayer films are grown on Si(001) at 250• C using ultra-high vacuum magnetically-unbalanced reactive magnetron sputtering from a single Hf 0.6 Al 0.2 Si 0.2 target in mixed 5%-N 2 /Ar atmospheres at a total pressure of 20 mTorr (2.67 Pa). The composition and nanostructure of Hf 1−x−y Al x Si y N films are controlled by varying the energy E i of the ions incident at the film growth surface while maintaining the ion-to-metal flux ratio constant at eight. Switching E i between 10 and 40 eV allows the growth of Hf 0.78 Al 0.10 Si 0.12 N/Hf 0.78 Al 0.14 Si 0.08 N multilayers with similar layer compositions, but in which the Si bonding state changes from predominantly Si-Si/Si-Hf for films grown with E i = 10 eV, to primarily Si-N with E i = 40 eV. Multilayer hardness values, which vary inversely with bilayer period Λ, range from 20 GPa with Λ = 20 nm to 27 GPa with Λ = 2 nm, while fracture toughness increases directly with Λ. Multilayers with Λ = 10 nm combine relatively high hardness, H ∼ 24 GPa, with good fracture toughness.

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Section: Introductionsupporting

confidence: 70%

Section: A Hfalsin Film Growth and Nanostructurementioning

confidence: 99%

Novel hard, tough HfAlSiN multilayers, defined by alternating Si bond structure, deposited using modulated high-flux, low-energy ion irradiation of the growing film

Fager

Howe

Greczyński

et al. 2015

Journal of Vacuum Science &Amp; Technology A: Vacuum, Surfaces, and Films

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“…The chemical driving force for the isostructural decomposition into binary cubic nitrides is high since the mixing enthalpy is almost twice as big as in Ti 1−x Al x N, see Figure 2.3 [58,59]. The maximum amount of AlN soluble in Hf 1−x Al x N is reported to be x ≈ 0.5 [25,60,61]. From X-ray diffraction patterns, it is found that the cubic phase is maintained up to x = 0.33, then an amorphous or nanocrystalline material is obtained between x = 0.38 and 0.71, while from x = 0.77 wurtzite single phase field is formed [59].…”

Section: Ternary Pseudo-binary Nitride Alloysmentioning

confidence: 99%

Properties of multilayered and multicomponent nitride alloys from first principles

Wang¹

2018

Linköping Studies in Science and Technology. Dissertations

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This thesis is a theoretical exploration of properties of multilayered and multicomponent nitride alloys, in particular their mixing thermodynamics and elastic behaviors. Systematic investigation of properties of a large class of materials, such as the multicomponent nitride solid solutions, is in line with the modern approach of high-throughput search of novel materials. In this thesis we benchmark and utilize simple but efficient methodological frameworks in predicting mixing thermodynamics, Young's moduli distribution of multilayer alloys and the linear thermal expansion of quaternary nitride solid solutions.We demonstrate by accurate ab-initio calculations that Ti 1−x Al x N solid solution is stabilized by interfacial effects if it is coherently sandwiched between TiN layers along (001). For TiN/AlN and ZrN/AlN multilayers we show higher thermodynamic stability with semicoherent interfaces than with isostructural coherent ones.Accurate 0 Kelvin elastic constants of cubic Ti x X y Al 1−x−y N (X=Zr, Hf, Nb, V, Ta) solid solutions and their multilayers are derived and an analytic comparison of strengths and ductility are presented to reveal the potential of these materials in hard coating applications. The Young's moduli variation of the bulk materials has provided a reliable descriptor to screen the Young's moduli of coherent multilayers.The Debye model is used to reveal the high-temperature thermodynamics and spinodal decomposition of Ti x Nb y Al 1−x−y N. We show that though the effect of vibration is large on the mixing Gibbs free energy the local spinoal decomposition tendencies are not altered. A quasi-harmonic Debye model is benchmarked against results of molecular dynamics simulations in predicting the thermal expansion coefficients of Ti x X y Al 1−x−y N (X=Zr, Hf, Nb, V, Ta).v Sammanfattning Denna avhandling är en teoretisk undersökning av egenskaperna hos multilager och multikomponentlegeringar av nitrider, särskilt deras blandningstermodynamik och elastiska egenskaper. Systematiska undersökningar av egenskaperna hos en stor materialfamilj, såsom fasta lösningar av multikomponentnitrider, ligger i linje med den moderna angreppsvinkeln av massundersökningar i sökandet efter nya material. I denna avhandling utvärderar och använder vi enkla men effektiva metodologiska ramverk för att förutsäga blandningstermodynamik, fördelning av Young's moduli multilager och den linjära termiska expansionen i kvaternära fasta lösningar av nitrider.Vi visar med precisa ab-initio-beräkningar att en fast lösning av Ti 1−x Al x N stabiliseras av gränssnittseffekter om den placeras koherent mellan TiN-skikt längs med (001). För multilager av TiN/AlN och ZrN/AlN påvisar vi högre termodynamisk stabilitet med semikoherenta gränsskikt än med isostrukturella koherenta. Precisa elastiska konstanter vid 0 K för kubiska fasta lösningar av Ti x X y Al 1−x−y N (X=Zr, Hf, Nb, V, Ta) och deras multilager beräknas och en analytisk jämförelse av deras hållfasthet och duktilitet presenteras för att visa dessa materials potential ...

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“…The preferential removal of lighter Al atoms is explained by forward sputtering by recoiled Ar + ions that are neutralized and backscattered from heavy Hf atoms. 44,196 In our study, we wanted to extend this technique to vary both the AlN and SiN concentrations in Hf1−x−yAlxSiyN, and grow amorphous films. Then, I would grow alternating amorphous Hf-Al-Si-N and nanocrystalline HfN layers using a single Hf0.6-Al0.2Si0.2 alloy target, by just varying the ion energy.…”

Section: Paper Vmentioning

confidence: 99%

Growth and Characterization of Amorphous Multicomponent Nitride Thin Films

Fager¹

2014

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This thesis explores deposition of amorphous thin films based on the two transition metal nitride systems, TiN and HfN. Additions of Si, Al and B have been investigated using three different deposition techniques: dc magnetron sputtering, cathodic arc evaporation, and high power impulse magnetron sputtering (HIPIMS). The effect of elemental composition, bonding structure, growth temperature, and low-energy ion bombardment during growth has been investigated and correlated to the resulting microstructure and mechanical properties of the films. The thermal stability has been investigated by annealing experiments. Deposition by cathodic arc evaporation yields dense and homogeneous coatings with essentially fully electron-diffraction amorphous structures with additions of either Al+Si, B+Si or B+Al+Si to TiN. The B-containing coatings have unusually few macroparticles. Annealing experiments show that Ti-Al-Si-N coatings have an age hardening behavior, which is not as clear for B-containing coatings. Compositional layering, due to rotation of the sample fixture during deposition, is present but not always visible in the as-deposited state. The layering acts as a template for renucleation during annealing. The coatings recrystallize by growth of TiN-rich domains. Amorphous growth by conventional dc magnetron sputtering is possible over a wide range of compositions for Ti-B-Si-N thin films. The Ti content in the films is reduced compared to the content in the sputtering target. Without Si, the films consist of a BN onion-like structure surrounding TiN nanograins. With additions of Si the films eventually grows fully amorphous. The growth temperature has only minor effect on the microstructure, due to the limited surface diffusion at the investigated temperature range (100-600 °C). Ion assisted growth leads to nanoscale densification of the films and improved mechanical properties. Ti-B-Si-N thin films are also deposited by a hybrid technique where dc magnetron sputtering is combined with HIPIMS. Here, the Ti:B ratio remains equal to the target composition. Films with low Si content are porous with TiN nanograins separated by BN-rich amorphous channels and have low hardness. Increasing Si contents yield fully electron-amorphous films with higher hardness. Finally, Hf-Al-Si-N single-layer and multilayer films are grown by dc magnetron sputtering from a single Hf-Al-Si target. Amorphous growth is achieved when the growth temperature was kept at its minimum. Low-energy substrate bias modulation is used to grow nanocomposite/nanocolumnar multilayers from the single Hf-Al-Si target, where the layers has essentially the same composition but different Si bonding structure, and different degree of crystallinity

show abstract

Real-time control of AlN incorporation in epitaxial Hf1−Al N using high-flux, low-energy (10–40 eV) ion bombardment during reactive magnetron sputter deposition from a Hf0.7Al0.3 alloy target

Cited by 21 publications

References 40 publications

Novel hard, tough HfAlSiN multilayers, defined by alternating Si bond structure, deposited using modulated high-flux, low-energy ion irradiation of the growing film

Novel hard, tough HfAlSiN multilayers, defined by alternating Si bond structure, deposited using modulated high-flux, low-energy ion irradiation of the growing film

Properties of multilayered and multicomponent nitride alloys from first principles

Growth and Characterization of Amorphous Multicomponent Nitride Thin Films

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