Theory of Hydrogen-Related Levels in Semiconductors and Oxides
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1 Theory of Hydrogen-Related Levels in Semiconductors and Oxides Chris G. Van de Walle Materials Department University of California, Santa Barbara
2 Acknowledgments Computations J. Neugebauer (Max-Planck-Institut, Düsseldorf) A. Janotti (UCSB) S. Limpijumnong (Suranaree U. Tech., Thailand) B. Tuttle (Penn State University) Support AFOSR; ONR Palo Alto Research Center Alexander von Humboldt Foundation Fritz-Haber-Institut & Paul-Drude-Institut, Berlin
3 Motivation for studying hydrogen Omnipresent impurity Growth vapor-phase transport, hydrothermal growth, MOCVD, MBE, sputtering (H 2 atmosphere), Processing: forming gas anneal, Beneficial effects & applications Passivation of defects Si/ Reliability? (deuterium) High-k dielectrics? C. G. Van de Walle and B. Tuttle, IEEE Trans. Electr. Dev. 47, 1779 (2000). hydrogen source gate silicon drain
4 Motivation for studying hydrogen Unintended / detrimental effects Passivation of dopant impurities DRAM variable retention time Nanoscale MOSFETs Source: Intel
5 Motivation for studying hydrogen Unintended / detrimental effects Passivation of dopant impurities DRAM variable retention time Nanoscale MOSFETs Trapping of hydrogen in oxide Stress-induced leakage currents Blöchl and Stathis, Phys. Rev. Lett. 83, 372 (1999). Charging of interface Afanas ev and Stesmans, Appl. Phys. Lett. 72, 79 (1998).
6 Hydrogen impurities Understanding interstitial hydrogen interactions with defects and impurities Hydrogen is electrically active! H 0 : rarely important H + donor H - acceptor Amphoteric impurity relative stability of H + /H - depends on Fermi level E F ε(+/0) = ε D ε(0/-) = ε A CB VB
7 Example: interstitial H in GaN E F H - H + ε(+/0) = ε D ε(+/-) ε(0/-) = ε A CB Amphoteric impurity: H + in p-type / H - in n-type Always counteracts prevailing conductivity VB First-principles calculations Density-functional theory Pseudopotentials / Atomic relaxations Applies to: Si, ; GaAs, AlAs, GaN, AlN, ; ZnSe, What about?
8 Zinc oxide devices Applications in optoelectronics Zinc oxide: typically n-type Conductivity due to electrons Cause: heavily debated Traditionally attributed to oxygen vacancies First-principles calculations: oxygen vacancies are not shallow donors! So what is the cause?
9 Hydrogen in ε(+/-) E F CB H + VB H + is the only stable charge state Phys. Rev. Lett. 85, 1012 (2000) Confirmed by more than 20 experiments to date
10 Why is different? Position of ε(+/-) in the band gap E F H - H + ε(+/-) CB VB E F H + ε(+/-) CB VB GaN Question: Why is ε(+/-) so much higher in energy in?
11 Why is different? Band lineups! ε(+/-) CB VB GaN
12 Why is different? Band lineups! ε(+/-) CB VB GaN
13 Band lineups 0 E (ev) Si Ge SiC AlN GaN InN GaSb GaAs ZnSe -10 Use natural band lineups to align band structures C. G. Van de Walle, Phys. Rev. B 39, 1871 (1989)
14 Band lineups 0 E (ev) Si Ge SiC AlN GaN InN GaSb GaAs hydrogen ε(+/-) level Nature 423, 626 (2003) ZnSe
15 0-2 Band lineups E (ev) Si Ge SiC AlN GaN InN GaSb GaAs ZnSe hydrogen ε(+/-) level Nature 423, 626 (2003) P. Blöchl, Phys. Rev. B 62, 6158 (2000)
16 0-2 Band lineups E (ev) Si Ge SiC AlN GaN InN GaSb GaAs hydrogen ε(+/-) level Nature 423, 626 (2003) ZnSe C. G. Van de Walle, Phys. Rev. Lett. 85, 1012 (2000)
17 Band lineups 0 E (ev) InN H exclusively a donor Si Ge SiC AlN GaN InN GaSb GaAs hydrogen ε(+/-) level Nature 423, 626 (2003) ZnSe Experiment: Appl. Phys. Lett. 82, 592 (2003).
18 0-2 Band lineups E (ev) GaSb H exclusively an acceptor Si Ge SiC AlN GaN InN GaSb GaAs ZnSe hydrogen ε(+/-) level Nature 423, 626 (2003)
19 Band lineups 0 E (ev) Si Ge SiC AlN GaN InN GaSb GaAs hydrogen ε(+/-) level Nature 423, 626 (2003) ZnSe
20 Band lineups 0 E (ev) Si Ge SiC -8 AlN -10
21 Band lineups 0 E (ev) Si Ge SiC -8 AlN In 2 O 3 TiO 2 HfO 2 ZrO 2-10 SnO 2
22 0-2 Band lineups E (ev) SnO 2 H exclusively a donor -4-6 Si Ge SiC -8 AlN In 2 O 3 SnO 2 TiO 2 HfO 2 ZrO 2-10 Transparent conductors
23 0-2 Band lineups E (ev) ZrO Si Ge SiC AlN In 2 O 3 SnO 2 TiO 2 HfO 2 ZrO 2 High-k dielectrics
24 Conclusions Hydrogen strongly interacts with defects and impurities Understanding this behavior: First-principles calculations Interstitial hydrogen: basis for understanding complex interactions Towards general understanding: Universal alignment Predictive model Connection with band lineups
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