Non-metallic dopant modulation of conductivity in substoichiometric tantalum pentoxide: A first-principles study

Bondi, Robert J.; Fox, Brian P.; Marinella, Matthew J.

doi:10.1063/1.4983850

Non-metallic dopant modulation of conductivity in substoichiometric tantalum pentoxide: A first-principles study

Journal Article · Thu Jun 01 00:00:00 EDT 2017 · Journal of Applied Physics

DOI:https://doi.org/10.1063/1.4983850· OSTI ID:1361046

Bondi, Robert J. ^[1]; Fox, Brian P. ^[1]; Marinella, Matthew J. ^[1]

Sandia National Lab. (SNL-NM), Albuquerque, NM (United States)

Here, we apply density-functional theory calculations to predict dopant modulation of electrical conductivity (σ_o) for seven dopants (C, Si, Ge, H, F, N, and B) sampled at 18 quantum molecular dynamics configurations of five independent insertion sites into two (high/low) baseline references of σo in amorphous Ta₂O₅, where each reference contains a single, neutral O vacancy center (V_O⁰). From this statistical population (n = 1260), we analyze defect levels, physical structure, and valence charge distributions to characterize nanoscale modification of the atomistic structure in local dopant neighborhoods. C is the most effective dopant at lowering Ta₂O_x σ_o, while also exhibiting an amphoteric doping behavior by either donating or accepting charge depending on the host oxide matrix. Both B and F robustly increase Ta₂O_x σ_o, although F does so through elimination of Ta high charge outliers, while B insertion conversely creates high charge O outliers through favorable BO₃ group formation, especially in the low σ_o reference. While N applications to dope and passivate oxides are prevalent, we also found that N exacerbates the stochasticity of σ_o we sought to mitigate; sensitivity to the N insertion site and some propensity to form N-O bond chemistries appear responsible. Finally, we use direct first-principles predictions of σ_o to explore feasible Ta₂O₅ dopants to engineer improved oxides with lower variance and greater repeatability to advance the manufacturability of resistive memory technologies.

View Accepted Manuscript (DOE)

Research Organization:: Sandia National Laboratories (SNL-NM), Albuquerque, NM (United States)

Sponsoring Organization:: USDOE; USDOE National Nuclear Security Administration (NNSA)

Grant/Contract Number:: AC04-94AL85000

OSTI ID:: 1361046

Alternate ID(s):: OSTI ID: 1366554

Report Number(s):: SAND2017--3842J; 652423

Journal Information:: Journal of Applied Physics, Journal Name: Journal of Applied Physics Journal Issue: 21 Vol. 121; ISSN 0021-8979

Publisher:: American Institute of Physics (AIP)Copyright Statement

Country of Publication:: United States

Language:: English

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