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Title: Direct observation of picosecond melting and disintegration of metallic nanoparticles

Abstract

Despite more than a century of study, the fundamental mechanisms behind solid melting remain elusive at the nanoscale. Ultrafast phenomena in materials irradiated by intense femtosecond laser pulses have revived the interest in unveiling the puzzling processes of melting transitions. However, direct experimental validation of various microscopic models is limited due to the difficulty of imaging the internal structures of materials undergoing ultrafast and irreversible transitions. Here we overcome this challenge through time-resolved single-shot diffractive imaging using X-ray free electron laser pulses. Images of single Au nanoparticles show heterogeneous melting at the surface followed by density fluctuation deep inside the particle, which is directionally correlated to the polarization of the pumping laser. Observation of this directionality links the non-thermal electronic excitation to the thermal lattice melting, which is further verified by molecular dynamics simulations. Lastly, this work provides direct evidence to the understanding of irreversible melting with an unprecedented spatiotemporal resolution.

Authors:
ORCiD logo [1];  [1];  [1]; ORCiD logo [1];  [1];  [2];  [3];  [3];  [3]; ORCiD logo [4];  [5];  [4];  [6];  [1];  [7]; ORCiD logo [6];  [6];  [4];  [8];  [1]
  1. Pohang Univ. of Science and Technology, Pohang (Korea)
  2. Inst. of Physical and Chemical Research (RIKEN), Sayo (Japan). SPring-8 Center; SLAC National Accelerator Lab., Menlo Park, CA (United States). Linac Coherent Light Source (LCLS)
  3. Pohang Accelerator Lab., Pohang (Korea)
  4. Univ. of California, Los Angeles, CA (United States)
  5. Gwangju Inst. of Science and Technology, Gwangju (Korea); European X-ray Free-Electron Laser (XFEL), Hamburg (Germany)
  6. Inst. of Physical and Chemical Research (RIKEN), Sayo (Japan). SPring-8 Center
  7. Japan Synchrotron Radiation Research Inst., Sayo (Japan)
  8. Gwangju Inst. of Science and Technology, Gwangju (Korea)
Publication Date:
Research Org.:
SLAC National Accelerator Lab., Menlo Park, CA (United States)
Sponsoring Org.:
USDOE
OSTI Identifier:
1532469
Grant/Contract Number:  
AC02-76SF00515
Resource Type:
Accepted Manuscript
Journal Name:
Nature Communications
Additional Journal Information:
Journal Volume: 10; Journal Issue: 1; Journal ID: ISSN 2041-1723
Publisher:
Nature Publishing Group
Country of Publication:
United States
Language:
English

Citation Formats

Ihm, Yungok, Cho, Do Hyung, Sung, Daeho, Nam, Daewoong, Jung, Chulho, Sato, Takahiro, Kim, Sangsoo, Park, Jaehyun, Kim, Sunam, Gallagher-Jones, Marcus, Kim, Yoonhee, Xu, Rui, Owada, Shigeki, Shim, Ji Hoon, Tono, Kensuke, Yabashi, Makina, Ishikawa, Tetsuya, Miao, Jianwei, Noh, Do Young, and Song, Changyong. Direct observation of picosecond melting and disintegration of metallic nanoparticles. United States: N. p., 2019. Web. doi:10.1038/s41467-019-10328-4.
Ihm, Yungok, Cho, Do Hyung, Sung, Daeho, Nam, Daewoong, Jung, Chulho, Sato, Takahiro, Kim, Sangsoo, Park, Jaehyun, Kim, Sunam, Gallagher-Jones, Marcus, Kim, Yoonhee, Xu, Rui, Owada, Shigeki, Shim, Ji Hoon, Tono, Kensuke, Yabashi, Makina, Ishikawa, Tetsuya, Miao, Jianwei, Noh, Do Young, & Song, Changyong. Direct observation of picosecond melting and disintegration of metallic nanoparticles. United States. doi:10.1038/s41467-019-10328-4.
Ihm, Yungok, Cho, Do Hyung, Sung, Daeho, Nam, Daewoong, Jung, Chulho, Sato, Takahiro, Kim, Sangsoo, Park, Jaehyun, Kim, Sunam, Gallagher-Jones, Marcus, Kim, Yoonhee, Xu, Rui, Owada, Shigeki, Shim, Ji Hoon, Tono, Kensuke, Yabashi, Makina, Ishikawa, Tetsuya, Miao, Jianwei, Noh, Do Young, and Song, Changyong. Mon . "Direct observation of picosecond melting and disintegration of metallic nanoparticles". United States. doi:10.1038/s41467-019-10328-4. https://www.osti.gov/servlets/purl/1532469.
@article{osti_1532469,
title = {Direct observation of picosecond melting and disintegration of metallic nanoparticles},
author = {Ihm, Yungok and Cho, Do Hyung and Sung, Daeho and Nam, Daewoong and Jung, Chulho and Sato, Takahiro and Kim, Sangsoo and Park, Jaehyun and Kim, Sunam and Gallagher-Jones, Marcus and Kim, Yoonhee and Xu, Rui and Owada, Shigeki and Shim, Ji Hoon and Tono, Kensuke and Yabashi, Makina and Ishikawa, Tetsuya and Miao, Jianwei and Noh, Do Young and Song, Changyong},
abstractNote = {Despite more than a century of study, the fundamental mechanisms behind solid melting remain elusive at the nanoscale. Ultrafast phenomena in materials irradiated by intense femtosecond laser pulses have revived the interest in unveiling the puzzling processes of melting transitions. However, direct experimental validation of various microscopic models is limited due to the difficulty of imaging the internal structures of materials undergoing ultrafast and irreversible transitions. Here we overcome this challenge through time-resolved single-shot diffractive imaging using X-ray free electron laser pulses. Images of single Au nanoparticles show heterogeneous melting at the surface followed by density fluctuation deep inside the particle, which is directionally correlated to the polarization of the pumping laser. Observation of this directionality links the non-thermal electronic excitation to the thermal lattice melting, which is further verified by molecular dynamics simulations. Lastly, this work provides direct evidence to the understanding of irreversible melting with an unprecedented spatiotemporal resolution.},
doi = {10.1038/s41467-019-10328-4},
journal = {Nature Communications},
number = 1,
volume = 10,
place = {United States},
year = {2019},
month = {6}
}

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Works referenced in this record:

Reconstruction of an object from the modulus of its Fourier transform
journal, January 1978