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

Abstract

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. The information derived here provides valuable and unique information for a host of quantum materials.« less

Authors:
; ORCiD logo; ; ; ; ; ; ; ; ; ; ; ; ; ; ; ; ;
Publication Date:
Research Org.:
Univ. of Colorado, Boulder, CO (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES); USDOE Office of Science (SC), Basic Energy Sciences (BES). Materials Sciences & Engineering Division
OSTI Identifier:
1367774
Alternate Identifier(s):
OSTI ID: 1465969; OSTI ID: 1680043
Grant/Contract Number:  
SC0002002
Resource Type:
Published Article
Journal Name:
Proceedings of the National Academy of Sciences of the United States of America
Additional Journal Information:
Journal Name: Proceedings of the National Academy of Sciences of the United States of America Journal Volume: 114 Journal Issue: 27; Journal ID: ISSN 0027-8424
Publisher:
National Academy of Sciences
Country of Publication:
United States
Language:
English
Subject:
74 ATOMIC AND MOLECULAR PHYSICS; 75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND SUPERFLUIDITY; Attosecond science; high harmonic generation; ARPES; electron-electron interactions

Citation Formats

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., 2017. Web. doi:10.1073/pnas.1706466114.
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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. https://doi.org/10.1073/pnas.1706466114
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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. Mon . "Distinguishing attosecond electron–electron scattering and screening in transition metals". United States. https://doi.org/10.1073/pnas.1706466114.
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@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. 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 = {Mon Jun 19 00:00:00 EDT 2017},
month = {Mon Jun 19 00:00:00 EDT 2017}
}
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Journal Article:
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https://doi.org/10.1073/pnas.1706466114
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Figures / Tables:

Fig. 1 Fig. 1: Influence of the material band structure on attosecond electron dynamics. (A) Illustration of the photoemission process from Cu(111) and Ni(111) surfaces. Using HHG pulse trains, photoelectrons are excited either from a Cu(111) or Ni(111) surface. Due to the different band structure in these two materials, photoelectrons from Ni(111)more » experience more electron–electron scattering, which reduces the lifetime of photoelectrons by 100 as compared with Cu(111) as they escape from the material surface. The enhanced scattering also reduces the inelastic mean free path. (B) Band structure of Cu(111) along the Г–L direction from DFT calculation (dashed lines), compared with experimental results of band mapping [open symbols; see S3. Static HHG Photoelectron Spectra Analysis of Cu(111)]. The interband transition $Λ^{β}_{3}$ →$Λ^{B}_{1}$ is highlighted by the blue arrow, which corresponds to the spectral enhancement of the photoelectron spectrum at harmonic orders $ω$15 and $ω$17 as shown in D. (C) Band structure of Cu along the Г–L direction for Cu(111), and Г–X for Cu(100), showing the evolution of the $Λ$ bands to $Δ$ bands across the Г point. Due to the photoemission selection rules, transitions from $Δ$2 bands are forbidden in the normal emission geometry from Cu(100). The colored areas indicate the perpendicular momentum regions measured in our experiments. Blue arrows indicate the direction in which the HHG photon energy ($\hbarω_X$) increases. (D) Static ARPES spectra excited by an s-polarized HHG field, generated using different noble gases (Xe, Kr, and Ar). Photoemission from two initial bands ($Λ^{α}_{3}$ and $Λ^{β}_{3}$) can be clearly distinguished.« less
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