Observation of intravalley phonon scattering of 2s excitons in MoSe2 and WSe2 monolayers
Observation of intravalley phonon scattering of 2s excitons in MoSe2 and WSe2 monolayers
 
  We present a high-resolution resonance Raman study of hBN encapsulated MoSe2 and WSe2 monolayers at 4 K using excitation energies from 1.6 eV to 2.25 eV. We report resonances with the WSe2 A2s and MoSe2 A2s and B2s excited Rydberg states despite their low oscillator strength. When resonant with the 2s states we identify new Raman peaks which are associated with intravalley scattering between different Rydberg states via optical phonons. By calibrating the Raman scattering efficiency and separately constraining the electric dipole matrix elements, we reveal that the scattering rates for k=0 optical phonons are comparable for both 1s and 2s states despite differences in the envelope functions. We also observe multiple new dispersive Raman peaks including a peak at the WSe2 A2s resonance that demonstrates non-linear dispersion and peak-splitting behavior that suggests the dispersion relations for dark excitonic states at energies near the 2s state are extremely complex.
  Rydberg states, dark excitons, excited states, exciton phonon scattering, intervalley scattering, resonance raman spectroscopy, transition metal dichalcogenides
  
  
  
    
      Mcdonnell, Liam
      
        f2c05544-d580-4f52-bdec-1d74be0697d7
      
     
  
    
      Viner, Jacob
      
        0fe62a03-a774-43d2-a864-79af91de17eb
      
     
  
    
      Rivera, Pasqual
      
        e36a10b9-6779-4005-a4a8-ab11934145ae
      
     
  
    
      Xu, Xiaodong
      
        4e3760f2-d24d-47df-b827-8217e25e20ea
      
     
  
    
      Smith, David C.
      
        d9b2c02d-b7ea-498b-9ea1-208a1681536f
      
     
  
  
   
  
  
    
    
  
    
      27 July 2020
    
    
  
  
    
      Mcdonnell, Liam
      
        f2c05544-d580-4f52-bdec-1d74be0697d7
      
     
  
    
      Viner, Jacob
      
        0fe62a03-a774-43d2-a864-79af91de17eb
      
     
  
    
      Rivera, Pasqual
      
        e36a10b9-6779-4005-a4a8-ab11934145ae
      
     
  
    
      Xu, Xiaodong
      
        4e3760f2-d24d-47df-b827-8217e25e20ea
      
     
  
    
      Smith, David C.
      
        d9b2c02d-b7ea-498b-9ea1-208a1681536f
      
     
  
       
    
 
  
    
      
  
  
  
  
  
  
    Mcdonnell, Liam, Viner, Jacob, Rivera, Pasqual, Xu, Xiaodong and Smith, David C.
  
  
  
  
   
    (2020)
  
  
    
    Observation of intravalley phonon scattering of 2s excitons in MoSe2 and WSe2 monolayers.
  
  
  
  
    2D Materials, 7 (4), [045008].
  
   (doi:10.1088/2053-1583/ab98f0). 
  
  
   
  
  
  
  
  
   
  
    
    
      
        
          Abstract
          We present a high-resolution resonance Raman study of hBN encapsulated MoSe2 and WSe2 monolayers at 4 K using excitation energies from 1.6 eV to 2.25 eV. We report resonances with the WSe2 A2s and MoSe2 A2s and B2s excited Rydberg states despite their low oscillator strength. When resonant with the 2s states we identify new Raman peaks which are associated with intravalley scattering between different Rydberg states via optical phonons. By calibrating the Raman scattering efficiency and separately constraining the electric dipole matrix elements, we reveal that the scattering rates for k=0 optical phonons are comparable for both 1s and 2s states despite differences in the envelope functions. We also observe multiple new dispersive Raman peaks including a peak at the WSe2 A2s resonance that demonstrates non-linear dispersion and peak-splitting behavior that suggests the dispersion relations for dark excitonic states at energies near the 2s state are extremely complex.
         
      
      
        
          
            
  
    Text
 Accepted Manuscript
     - Accepted Manuscript
   
  
  
    
  
 
          
            
          
            
           
            
           
        
        
       
    
   
  
  
  More information
  
    
      Accepted/In Press date: 2 June 2020
 
    
      Published date: 27 July 2020
 
    
  
  
    
  
    
     
        Additional Information:
        Publisher Copyright:
© 2020 IOP Publishing Ltd.
Copyright:
Copyright 2020 Elsevier B.V., All rights reserved.
      
    
  
    
  
    
  
    
     
    
  
    
     
        Keywords:
        Rydberg states, dark excitons, excited states, exciton phonon scattering, intervalley scattering, resonance raman spectroscopy, transition metal dichalcogenides
      
    
  
    
  
    
  
  
        Identifiers
        Local EPrints ID: 442813
        URI: http://eprints.soton.ac.uk/id/eprint/442813
        
          
        
        
        
          ISSN: 2053-1583
        
        
          PURE UUID: 4c82d6f4-b4b1-43d0-bbd9-d64a02b18323
        
  
    
        
          
            
              
            
          
        
    
        
          
            
          
        
    
        
          
        
    
        
          
        
    
        
          
            
          
        
    
  
  Catalogue record
  Date deposited: 28 Jul 2020 16:30
  Last modified: 05 Jun 2024 19:39
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      Contributors
      
          
          Author:
          
            
              
              
                Liam Mcdonnell
              
              
                 
              
            
            
          
         
      
          
          Author:
          
            
              
              
                Jacob Viner
              
              
            
            
          
        
      
          
          Author:
          
            
            
              Pasqual Rivera
            
          
        
      
          
          Author:
          
            
            
              Xiaodong Xu
            
          
        
      
        
      
      
      
    
  
   
  
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