In Situ TEM Study of the Amorphous-to-Crystalline Transition during Dielectric Breakdown in TiO2 Film

Tian，Xinchun1; Cook，Chloe2; Hong，Wei3; Ma，Tao4; Brennecka，Geoff L.2; Tan，Xiaoli1

2019

10.1021/acsami.9b08146

ACS Applied Materials & Interfaces   影响因子和分区

1944-8244

1944-8252

Dielectric breakdown of oxides is a main limiting factor for improvement of the performance of electronic devices. Present understanding suggests that defects produced by intense voltage accumulate in the oxide to form a percolation path connecting the two electrodes and trigger the dielectric breakdown. However, reports on directly visualizing the process at nanoscale are very limited. Here, we apply in situ transmission electron microscopy to characterize the structural and compositional changes of amorphous TiO under extreme electric field (∼100 kV/mm) in a Si/TiO/W system. Upon applying voltage pulses, the amorphous TiO gradually transformed into crystalline substoichiometric rutile TiO and the Magnéli phase TiO. The transitions started from the anode/oxide interface under both field polarities. Preferred growth orientation of rutile TiO with respect to the Si substrate was observed when Si was the anode, while oxidation and melting of the W probe occurred when W was the anode. We associate the TiO crystallization process with the electrochemical reduction of TiO, polarity-dependent oxygen migration, and Joule heating. The experimental results are supported by our phase-field modeling. These findings provide direct details of the defect formation process during dielectric breakdown in amorphous oxides and will help the design of electronic devices with higher efficiency and reliability.

amorphous-to-crystallization transformation dielectric breakdown in situ TEM oxygen migration TiO2

SCI ; EI

英语

其他

U.S. Department of Energy, Office of Science, Basic Energy Sciences[DE-SC0017839]

Science & Technology - Other Topics ; Materials Science

Nanoscience & Nanotechnology ; Materials Science, Multidisciplinary

WOS:000493869700135

AMER CHEMICAL SOC

20194307589361

Amorphous silicon ; Anodes ; Chromium compounds ; Crystalline materials ; Defects ; Electric breakdown ; Electrolytic reduction ; High resolution transmission electron microscopy ; In situ processing ; Oxide minerals ; Silicon ; Solvents ; Thermoelectric equipment ; Titanium dioxide

Minerals:482.2 ; Ore Treatment:533.1 ; Nonferrous Metals and Alloys excluding Alkali and Alkaline Earth Metals:549.3 ; Thermoelectric Energy:615.4 ; Electricity: Basic Concepts and Phenomena:701.1 ; Electron Tubes:714.1 ; Optical Devices and Systems:741.3 ; Chemical Agents and Basic Industrial Chemicals:803 ; Inorganic Compounds:804.2 ; Crystalline Solids:933.1 ; Materials Science:951

2-s2.0-85073880863

Scopus

1.Department of Materials Science and EngineeringIowa State University,Ames,50011,United States
2.Department of Metallurgical and Materials EngineeringColorado School of Mines,Golden,80401,United States
3.Department of Mechanics and Aerospace EngineeringSouthern University of Science and Technology,Shenzhen, Guangdong,518055,China
4.US Department of EnergyAmes Laboratory,Ames,50011,United States

Tian，Xinchun,Cook，Chloe,Hong，Wei,et al. In Situ TEM Study of the Amorphous-to-Crystalline Transition during Dielectric Breakdown in TiO2 Film[J]. ACS Applied Materials & Interfaces,2019,11(43):40726-40733.

Tian，Xinchun,Cook，Chloe,Hong，Wei,Ma，Tao,Brennecka，Geoff L.,&Tan，Xiaoli.(2019).In Situ TEM Study of the Amorphous-to-Crystalline Transition during Dielectric Breakdown in TiO2 Film.ACS Applied Materials & Interfaces,11(43),40726-40733.

Tian，Xinchun,et al."In Situ TEM Study of the Amorphous-to-Crystalline Transition during Dielectric Breakdown in TiO2 Film".ACS Applied Materials & Interfaces 11.43(2019):40726-40733.