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Title: Distinguishing attosecond electron–electron scattering and screening in transition metals

Electron–electron interactions are the fastest processes in materials, occurring on femtosecond to attosecond timescales, depending on the electronic band structure of the material and the excitation energy. Such interactions can play a dominant role in light-induced processes such as nano-enhanced plasmonics and catalysis, light harvesting, or phase transitions. However, to date it has not been possible to experimentally distinguish fundamental electron interactions such as scattering and screening. Here, we use sequences of attosecond pulses to directly measure electron–electron interactions in different bands of different materials with both simple and complex Fermi surfaces. By extracting the time delays associated with photoemission we show that the lifetime of photoelectrons from the d band of Cu are longer by ~100 as compared with those from the same band of Ni. We attribute this to the enhanced electron–electron scattering in the unfilled d band of Ni. Using theoretical modeling, we can extract the contributions of electron–electron scattering and screening in different bands of different materials with both simple and complex Fermi surfaces. Our results also show that screening influences high-energy photoelectrons (≈20 eV) significantly less than low-energy photoelectrons. As a result, high-energy photoelectrons can serve as a direct probe of spin-dependent electron–electron scattering bymore » neglecting screening. This can then be applied to quantifying the contribution of electron interactions and screening to low-energy excitations near the Fermi level. In conclusion, the information derived here provides valuable and unique information for a host of quantum materials.« less
Authors:
 [1] ; ORCiD logo [1] ;  [1] ;  [2] ;  [3] ;  [4] ;  [4] ;  [5] ;  [1] ;  [4] ;  [4] ;  [1] ;  [6] ;  [7] ;  [3] ;  [4] ;  [8] ;  [1] ;  [1]
  1. Univ. of Colorado and National Institute of Standards and Technology, Boulder, CO (United States)
  2. Univ. of Colorado and National Institute of Standards and Technology, Boulder, CO (United States); Umea Univ., Umea (Sweden)
  3. Univ. of Wisconsin, Madison, WI (United States)
  4. Univ. of Kaiserslautern, Kaiserslautern (Germany)
  5. National Inst. of Standards and Technology (NIST), Boulder, CO (United States)
  6. Univ. of Kaiserslautern, Kaiserslautern (Germany); Georg-August-Univ. Gottingen, Gottingen (Germany)
  7. Kansas State Univ., Manhattan, KS (United States)
  8. Uppsala Univ., Uppsala (Sweden)
Publication Date:
Grant/Contract Number:
SC0002002
Type:
Published Article
Journal Name:
Proceedings of the National Academy of Sciences of the United States of America
Additional Journal Information:
Journal Volume: 114; Journal Issue: 27; Journal ID: ISSN 0027-8424
Publisher:
National Academy of Sciences, Washington, DC (United States)
Research Org:
Univ. of Colorado, Boulder, CO (United States)
Sponsoring Org:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
Country of Publication:
United States
Language:
English
Subject:
74 ATOMIC AND MOLECULAR PHYSICS; attosecond science; high harmonic generation; ARPES; electron-electron interactions
OSTI Identifier:
1367774
Alternate Identifier(s):
OSTI ID: 1465969

Chen, Cong, Tao, Zhensheng, Carr, Adra, Matyba, Piotr, Szilvási, Tibor, Emmerich, Sebastian, Piecuch, Martin, Keller, Mark, Zusin, Dmitriy, Eich, Steffen, Rollinger, Markus, You, Wenjing, Mathias, Stefan, Thumm, Uwe, Mavrikakis, Manos, Aeschlimann, Martin, Oppeneer, Peter M., Kapteyn, Henry, and Murnane, Margaret. Distinguishing attosecond electron–electron scattering and screening in transition metals. United States: N. p., Web. doi:10.1073/pnas.1706466114.
Chen, Cong, Tao, Zhensheng, Carr, Adra, Matyba, Piotr, Szilvási, Tibor, Emmerich, Sebastian, Piecuch, Martin, Keller, Mark, Zusin, Dmitriy, Eich, Steffen, Rollinger, Markus, You, Wenjing, Mathias, Stefan, Thumm, Uwe, Mavrikakis, Manos, Aeschlimann, Martin, Oppeneer, Peter M., Kapteyn, Henry, & Murnane, Margaret. Distinguishing attosecond electron–electron scattering and screening in transition metals. United States. doi:10.1073/pnas.1706466114.
Chen, Cong, Tao, Zhensheng, Carr, Adra, Matyba, Piotr, Szilvási, Tibor, Emmerich, Sebastian, Piecuch, Martin, Keller, Mark, Zusin, Dmitriy, Eich, Steffen, Rollinger, Markus, You, Wenjing, Mathias, Stefan, Thumm, Uwe, Mavrikakis, Manos, Aeschlimann, Martin, Oppeneer, Peter M., Kapteyn, Henry, and Murnane, Margaret. 2017. "Distinguishing attosecond electron–electron scattering and screening in transition metals". United States. doi:10.1073/pnas.1706466114.
@article{osti_1367774,
title = {Distinguishing attosecond electron–electron scattering and screening in transition metals},
author = {Chen, Cong and Tao, Zhensheng and Carr, Adra and Matyba, Piotr and Szilvási, Tibor and Emmerich, Sebastian and Piecuch, Martin and Keller, Mark and Zusin, Dmitriy and Eich, Steffen and Rollinger, Markus and You, Wenjing and Mathias, Stefan and Thumm, Uwe and Mavrikakis, Manos and Aeschlimann, Martin and Oppeneer, Peter M. and Kapteyn, Henry and Murnane, Margaret},
abstractNote = {Electron–electron interactions are the fastest processes in materials, occurring on femtosecond to attosecond timescales, depending on the electronic band structure of the material and the excitation energy. Such interactions can play a dominant role in light-induced processes such as nano-enhanced plasmonics and catalysis, light harvesting, or phase transitions. However, to date it has not been possible to experimentally distinguish fundamental electron interactions such as scattering and screening. Here, we use sequences of attosecond pulses to directly measure electron–electron interactions in different bands of different materials with both simple and complex Fermi surfaces. By extracting the time delays associated with photoemission we show that the lifetime of photoelectrons from the d band of Cu are longer by ~100 as compared with those from the same band of Ni. We attribute this to the enhanced electron–electron scattering in the unfilled d band of Ni. Using theoretical modeling, we can extract the contributions of electron–electron scattering and screening in different bands of different materials with both simple and complex Fermi surfaces. Our results also show that screening influences high-energy photoelectrons (≈20 eV) significantly less than low-energy photoelectrons. As a result, high-energy photoelectrons can serve as a direct probe of spin-dependent electron–electron scattering by neglecting screening. This can then be applied to quantifying the contribution of electron interactions and screening to low-energy excitations near the Fermi level. In conclusion, the information derived here provides valuable and unique information for a host of quantum materials.},
doi = {10.1073/pnas.1706466114},
journal = {Proceedings of the National Academy of Sciences of the United States of America},
number = 27,
volume = 114,
place = {United States},
year = {2017},
month = {6}
}