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Title: Phase transformation pathways of ultrafast-laser-irradiated Ln 2 O 3 ( Ln = Er Lu )

Ultrafast laser irradiation causes intense electronic excitations in materials, leading to transient high temperatures and pressures. Here, we show that ultrafast laser irradiation drives an irreversible cubic-to-monoclinic phase transformation in Ln 2O 3 ( Ln = Er – Lu ) , and explore the mechanism by which the phase transformation occurs. A combination of grazing incidence x-ray diffraction and transmission electron microscopy are used to determine the magnitude and depth-dependence of the phase transformation, respectively. Although all compositions undergo the same transformation, their transformation mechanisms differ. The transformation is pressure-driven for Ln = Tm – Lu , consistent with the material's phase behavior under equilibrium conditions. However, the transformation is thermally driven for Ln = Er , revealing that the nonequilibrium conditions of ultrafast laser irradiation can lead to novel transformation pathways. Ab initio molecular-dynamics simulations are used to examine the atomic-scale effects of electronic excitation, showing the production of oxygen Frenkel pairs and the migration of interstitial oxygen to tetrahedrally coordinated constitutional vacancy sites, the first step in a defect-driven phase transformation.
Authors:
 [1] ;  [1] ;  [1] ;  [2] ;  [2] ;  [3] ;  [4] ;  [1]
  1. Stanford Univ., CA (United States)
  2. Univ. of California, Berkeley, CA (United States)
  3. Stanford Univ., CA (United States); SLAC National Accelerator Lab., Menlo Park, CA (United States)
  4. Univ. of Michigan, Ann Arbor, MI (United States)
Publication Date:
Grant/Contract Number:
SC0001089; AC02-76SF00515; AC02-05CH11231; FA9550-16-1-0312; ECCS-1542152
Type:
Accepted Manuscript
Journal Name:
Physical Review B
Additional Journal Information:
Journal Volume: 97; Journal Issue: 2; Journal ID: ISSN 2469-9950
Publisher:
American Physical Society (APS)
Research Org:
SLAC National Accelerator Lab., Menlo Park, CA (United States); Energy Frontier Research Centers (EFRC) (United States). Materials Science of Actinides (MSA)
Sponsoring Org:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
Country of Publication:
United States
Language:
English
Subject:
75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND SUPERFLUIDITY
OSTI Identifier:
1424744

Rittman, Dylan R., Tracy, Cameron L., Chen, Chien-Hung, Solomon, Jonathan M., Asta, Mark, Mao, Wendy L., Yalisove, Steven M., and Ewing, Rodney C.. Phase transformation pathways of ultrafast-laser-irradiated Ln2O3(Ln=Er–Lu). United States: N. p., Web. doi:10.1103/physrevb.97.024104.
Rittman, Dylan R., Tracy, Cameron L., Chen, Chien-Hung, Solomon, Jonathan M., Asta, Mark, Mao, Wendy L., Yalisove, Steven M., & Ewing, Rodney C.. Phase transformation pathways of ultrafast-laser-irradiated Ln2O3(Ln=Er–Lu). United States. doi:10.1103/physrevb.97.024104.
Rittman, Dylan R., Tracy, Cameron L., Chen, Chien-Hung, Solomon, Jonathan M., Asta, Mark, Mao, Wendy L., Yalisove, Steven M., and Ewing, Rodney C.. 2018. "Phase transformation pathways of ultrafast-laser-irradiated Ln2O3(Ln=Er–Lu)". United States. doi:10.1103/physrevb.97.024104.
@article{osti_1424744,
title = {Phase transformation pathways of ultrafast-laser-irradiated Ln2O3(Ln=Er–Lu)},
author = {Rittman, Dylan R. and Tracy, Cameron L. and Chen, Chien-Hung and Solomon, Jonathan M. and Asta, Mark and Mao, Wendy L. and Yalisove, Steven M. and Ewing, Rodney C.},
abstractNote = {Ultrafast laser irradiation causes intense electronic excitations in materials, leading to transient high temperatures and pressures. Here, we show that ultrafast laser irradiation drives an irreversible cubic-to-monoclinic phase transformation in Ln2O3 ( Ln = Er – Lu ) , and explore the mechanism by which the phase transformation occurs. A combination of grazing incidence x-ray diffraction and transmission electron microscopy are used to determine the magnitude and depth-dependence of the phase transformation, respectively. Although all compositions undergo the same transformation, their transformation mechanisms differ. The transformation is pressure-driven for Ln = Tm – Lu , consistent with the material's phase behavior under equilibrium conditions. However, the transformation is thermally driven for Ln = Er , revealing that the nonequilibrium conditions of ultrafast laser irradiation can lead to novel transformation pathways. Ab initio molecular-dynamics simulations are used to examine the atomic-scale effects of electronic excitation, showing the production of oxygen Frenkel pairs and the migration of interstitial oxygen to tetrahedrally coordinated constitutional vacancy sites, the first step in a defect-driven phase transformation.},
doi = {10.1103/physrevb.97.024104},
journal = {Physical Review B},
number = 2,
volume = 97,
place = {United States},
year = {2018},
month = {1}
}