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Title: Non-thermal fluence threshold for femtosecond pulsed x-ray radiation damage in perovskite complex oxide epitaxial heterostructures

Abstract

Intense hard x-ray pulses from a free-electron laser induce irreversible structural damage in a perovskite oxide epitaxial heterostructure when pulse fluences exceed a threshold value. The intensity of x-ray diffraction from a 25-nm thick epitaxial BiFeO3 layer on a SrTiO3 (STO) substrate measured using a series of pulses decreases abruptly with a per-pulse fluence of 2.7 x 10(6) photons mu m-2 at a photon energy of 9.7 keV but remains constant for 1.3 x 106 photons mu m-2 or less. The damage resulted in the destruction of the BiFeO3 thin film within the focal spot area and the formation of a deep cavity penetrating into the STO substrate via the removal of tens of nanometers of material per pulse. The damage threshold occurs at a fluence that is insufficient to heat the absorption volume to the melting point. The morphology of the ablated sample is consistent with fracture rather than melting. Together, these results indicate that the damage occurs via a nonthermal process consistent with ultrafast ionization of the absorption volume.

Authors:
ORCiD logo [1];  [1];  [1];  [2];  [3];  [3]; ORCiD logo [3];  [3];  [4];  [4];  [4]; ORCiD logo [4];  [5]; ORCiD logo [6];  [7]; ORCiD logo [1]
  1. Univ. of Wisconsin, Madison, WI (United States)
  2. DePaul Univ., Chicago, IL (United States)
  3. Gwangju Inst. of Science and Technology (Korea, Republic of)
  4. Pohang Accelerator Lab. (PAL) (Korea, Republic of)
  5. Stanford Univ., CA (United States). Dept. of Applied Physics
  6. Cornell Univ., Ithaca, NY (United States). Dept. of Materials Science and Engineering
  7. Argonne National Lab. (ANL), Argonne, IL (United States)
Publication Date:
Research Org.:
Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Materials Sciences & Engineering Division
OSTI Identifier:
1630101
Alternate Identifier(s):
OSTI ID: 1579771
Grant/Contract Number:  
AC02-06CH11357
Resource Type:
Accepted Manuscript
Journal Name:
Applied Physics Letters
Additional Journal Information:
Journal Volume: 115; Journal Issue: 25; Journal ID: ISSN 0003-6951
Publisher:
American Institute of Physics (AIP)
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; Radiation damage; X-ray diffraction; Perovskites; Epitaxy; Laser theory; Scanning electron; microscopy; Heterostructures; Thin films; Hard X-rays; Free electron lasers

Citation Formats

Lee, Hyeon Jun, Ahn, Youngjun, Marks, Samuel D., Landahl, Eric C., Lee, Jun Young, Kim, Tae Yeon, Unithrattil, Sanjith, Jo, Ji Young, Chun, Sae Hwan, Kim, Sunam, Park, Sang-Yeon, Eom, Intae, Adamo, Carolina, Schlom, Darrell G., Wen, Haidan, and Evans, Paul G. Non-thermal fluence threshold for femtosecond pulsed x-ray radiation damage in perovskite complex oxide epitaxial heterostructures. United States: N. p., 2019. Web. https://doi.org/10.1063/1.5128509.
Lee, Hyeon Jun, Ahn, Youngjun, Marks, Samuel D., Landahl, Eric C., Lee, Jun Young, Kim, Tae Yeon, Unithrattil, Sanjith, Jo, Ji Young, Chun, Sae Hwan, Kim, Sunam, Park, Sang-Yeon, Eom, Intae, Adamo, Carolina, Schlom, Darrell G., Wen, Haidan, & Evans, Paul G. Non-thermal fluence threshold for femtosecond pulsed x-ray radiation damage in perovskite complex oxide epitaxial heterostructures. United States. https://doi.org/10.1063/1.5128509
Lee, Hyeon Jun, Ahn, Youngjun, Marks, Samuel D., Landahl, Eric C., Lee, Jun Young, Kim, Tae Yeon, Unithrattil, Sanjith, Jo, Ji Young, Chun, Sae Hwan, Kim, Sunam, Park, Sang-Yeon, Eom, Intae, Adamo, Carolina, Schlom, Darrell G., Wen, Haidan, and Evans, Paul G. Mon . "Non-thermal fluence threshold for femtosecond pulsed x-ray radiation damage in perovskite complex oxide epitaxial heterostructures". United States. https://doi.org/10.1063/1.5128509. https://www.osti.gov/servlets/purl/1630101.
@article{osti_1630101,
title = {Non-thermal fluence threshold for femtosecond pulsed x-ray radiation damage in perovskite complex oxide epitaxial heterostructures},
author = {Lee, Hyeon Jun and Ahn, Youngjun and Marks, Samuel D. and Landahl, Eric C. and Lee, Jun Young and Kim, Tae Yeon and Unithrattil, Sanjith and Jo, Ji Young and Chun, Sae Hwan and Kim, Sunam and Park, Sang-Yeon and Eom, Intae and Adamo, Carolina and Schlom, Darrell G. and Wen, Haidan and Evans, Paul G.},
abstractNote = {Intense hard x-ray pulses from a free-electron laser induce irreversible structural damage in a perovskite oxide epitaxial heterostructure when pulse fluences exceed a threshold value. The intensity of x-ray diffraction from a 25-nm thick epitaxial BiFeO3 layer on a SrTiO3 (STO) substrate measured using a series of pulses decreases abruptly with a per-pulse fluence of 2.7 x 10(6) photons mu m-2 at a photon energy of 9.7 keV but remains constant for 1.3 x 106 photons mu m-2 or less. The damage resulted in the destruction of the BiFeO3 thin film within the focal spot area and the formation of a deep cavity penetrating into the STO substrate via the removal of tens of nanometers of material per pulse. The damage threshold occurs at a fluence that is insufficient to heat the absorption volume to the melting point. The morphology of the ablated sample is consistent with fracture rather than melting. Together, these results indicate that the damage occurs via a nonthermal process consistent with ultrafast ionization of the absorption volume.},
doi = {10.1063/1.5128509},
journal = {Applied Physics Letters},
number = 25,
volume = 115,
place = {United States},
year = {2019},
month = {12}
}

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