Direct Observation of Symmetry-Dependent Electron–Phonon Coupling in Black Phosphorus

Mao, Nannan; Wang, Xingzhi; Lin, Yuxuan; Sumpter, Bobby G.; Ji, Qingqing; Palacios, Tomás; Huang, Shengxi; Meunier, Vincent; Dresselhaus, Mildred S.; Tisdale, William A.; Liang, Liangbo; Ling, Xi; Kong, Jing

doi:10.1021/jacs.9b07974

Title: Direct Observation of Symmetry-Dependent Electron–Phonon Coupling in Black Phosphorus

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Abstract

Electron–phonon coupling in two-dimensional nanomaterials plays a fundamental role in determining their physical properties. Such interplay is particularly intriguing in semiconducting black phosphorus (BP) due to the highly anisotropic nature of its electronic structure and phonon dispersions. Here we report the direct observation of symmetry-dependent electron–phonon coupling in BP by performing the polarization-selective resonance Raman measurement in the visible and ultraviolet regimes, focusing on the out-of-plane A_g¹ and in-plane A_g² phonon modes. Their intrinsic resonance Raman excitation profiles (REPs) were extracted and quantitatively compared. The in-plane A_g² mode exhibits remarkably strong resonance enhancement across the excitation wavelengths when the excitation polarization is parallel to the armchair (A_g²//AC) direction. In contrast, a dramatically weak resonance effect was observed for the same mode with the polarization parallel to zigzag (A_g²//ZZ) direction and for the out-of-plane A_g¹ mode (A_g¹//AC and A_g¹//ZZ). Analysis on quantum perturbation theory and first-principles calculations on the anisotropic electron distributions in BP demonstrated that electron–phonon coupling considering the symmetry of the involved excited states and phonon vibration patterns is responsible for this phenomenon. Further analysis of the polarization-dependent REPs for A_g phonons allows us to resolve the existing controversies on the physical origin of Raman anomaly in BP andmore »« less

Authors:

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^[2];

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^[3];

^[5];

^[6]; Dresselhaus, Mildred S. ^[3];

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Massachusetts Inst. of Technology (MIT), Cambridge, MA (United State); Boston Univ., MA (United States)
Boston Univ., MA (United States)
Massachusetts Inst. of Technology (MIT), Cambridge, MA (United State)
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Pennsylvania State Univ., University Park, PA (United States)
Department of Physics, Applied Physics, and Astronomy, Rensselaer Polytechnic Institute, Troy, New York 12180, United States

Publication Date:: Tue Nov 05 00:00:00 EST 2019

Research Org.:: Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)

Sponsoring Org.:: USDOE

OSTI Identifier:: 1607235

Grant/Contract Number:: AC05-00OR22725

Resource Type:: Accepted Manuscript

Journal Name:: Journal of the American Chemical Society

Additional Journal Information:: Journal Volume: 141; Journal Issue: 48; Journal ID: ISSN 0002-7863

Publisher:: American Chemical Society (ACS)

Country of Publication:: United States

Language:: English

Subject:: 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; phonons; electrical energy; energy; resonance structures; polarization; black phosphorus; electron-phonon coupling; electron-photon coupling; resonance Raman scattering; symmetry; crystalline orientation

Citation Formats


                    Mao, Nannan, Wang, Xingzhi, Lin, Yuxuan, Sumpter, Bobby G., Ji, Qingqing, Palacios, Tomás, Huang, Shengxi, Meunier, Vincent, Dresselhaus, Mildred S., Tisdale, William A., Liang, Liangbo, Ling, Xi, and Kong, Jing. Direct Observation of Symmetry-Dependent Electron–Phonon Coupling in Black Phosphorus.  United States: N. p., 2019. 
Web.  doi:10.1021/jacs.9b07974.

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                    Mao, Nannan, Wang, Xingzhi, Lin, Yuxuan, Sumpter, Bobby G., Ji, Qingqing, Palacios, Tomás, Huang, Shengxi, Meunier, Vincent, Dresselhaus, Mildred S., Tisdale, William A., Liang, Liangbo, Ling, Xi, & Kong, Jing. Direct Observation of Symmetry-Dependent Electron–Phonon Coupling in Black Phosphorus.  United States.  https://doi.org/10.1021/jacs.9b07974

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                    Mao, Nannan, Wang, Xingzhi, Lin, Yuxuan, Sumpter, Bobby G., Ji, Qingqing, Palacios, Tomás, Huang, Shengxi, Meunier, Vincent, Dresselhaus, Mildred S., Tisdale, William A., Liang, Liangbo, Ling, Xi, and Kong, Jing. Tue .  
"Direct Observation of Symmetry-Dependent Electron–Phonon Coupling in Black Phosphorus".  United States.  https://doi.org/10.1021/jacs.9b07974.  https://www.osti.gov/servlets/purl/1607235.

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@article{osti_1607235,

  title        = {Direct Observation of Symmetry-Dependent Electron–Phonon Coupling in Black Phosphorus},

  author       = {Mao, Nannan and Wang, Xingzhi and Lin, Yuxuan and Sumpter, Bobby G. and Ji, Qingqing and Palacios, Tomás and Huang, Shengxi and Meunier, Vincent and Dresselhaus, Mildred S. and Tisdale, William A. and Liang, Liangbo and Ling, Xi and Kong, Jing},

  abstractNote = {Electron–phonon coupling in two-dimensional nanomaterials plays a fundamental role in determining their physical properties. Such interplay is particularly intriguing in semiconducting black phosphorus (BP) due to the highly anisotropic nature of its electronic structure and phonon dispersions. Here we report the direct observation of symmetry-dependent electron–phonon coupling in BP by performing the polarization-selective resonance Raman measurement in the visible and ultraviolet regimes, focusing on the out-of-plane Ag1 and in-plane Ag2 phonon modes. Their intrinsic resonance Raman excitation profiles (REPs) were extracted and quantitatively compared. The in-plane Ag2 mode exhibits remarkably strong resonance enhancement across the excitation wavelengths when the excitation polarization is parallel to the armchair (Ag2//AC) direction. In contrast, a dramatically weak resonance effect was observed for the same mode with the polarization parallel to zigzag (Ag2//ZZ) direction and for the out-of-plane Ag1 mode (Ag1//AC and Ag1//ZZ). Analysis on quantum perturbation theory and first-principles calculations on the anisotropic electron distributions in BP demonstrated that electron–phonon coupling considering the symmetry of the involved excited states and phonon vibration patterns is responsible for this phenomenon. Further analysis of the polarization-dependent REPs for Ag phonons allows us to resolve the existing controversies on the physical origin of Raman anomaly in BP and its dependence on excitation energy, sample thickness, phonon modes, and crystalline orientation. Finally, our study gives deep insights into the underlying interplay between electrons and phonons in BP and paves the way for manipulating the electron–phonon coupling in anisotropic nanomaterials for future device applications.},

  doi          = {10.1021/jacs.9b07974},

  journal      = {Journal of the American Chemical Society},

  number       = 48,

  volume       = 141,

  place        = {United States},

  year         = {Tue Nov 05 00:00:00 EST 2019},

  month        = {Tue Nov 05 00:00:00 EST 2019}

}

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