Superposition of intra- and inter-layer excitons in twistronic MoSe2/WSe2 bilayers probed by resonant Raman scattering
Superposition of intra- and inter-layer excitons in twistronic MoSe2/WSe2 bilayers probed by resonant Raman scattering
 
  Hybridisation of electronic bands of two-dimensional materials, assembled into twistronic heterostructures, enables one to tune their optoelectronic properties by selecting conditions for resonant interlayer hybridisation. Resonant interlayer hybridisation qualitatively modifies the excitons in such heterostructures, transforming these optically active modes into superposition states of interlayer and intralayer excitons. For MoSe2/WSe2 heterostructures, strong hybridization of both single particle and excitonic states can occur via single particle tunneling. Here we use resonance Raman scattering to provide direct evidence for the hybridisation of excitons in twistronic MoSe2/WSe2 structures, by observing scattering of specific excitons by phonons in both WSe2 and MoSe2. We also demonstrate that resonance Raman scattering spectroscopy opens up a wide range of possibilities for quantifying the layer composition of the superposition states of the exciton and the interlayer hybridisation parameters in heterostructures of two-dimensional materials.
  Heterobilayers, Hybridised excitons, Resonance Raman spectroscopy, Transition metal dichalcogenides
  
  
  
    
      Mcdonnell, Liam
      
        f2c05544-d580-4f52-bdec-1d74be0697d7
      
     
  
    
      Viner, Jacob
      
        0fe62a03-a774-43d2-a864-79af91de17eb
      
     
  
    
      Ruiz-Tijerina, David
      
        bd7e7b38-4dcd-4191-98f1-fca5173ef7e5
      
     
  
    
      Rivera, Pasqual
      
        8363e6c4-4d7d-4c9e-bf5d-7d08249edf85
      
     
  
    
      Xu, Xiaodong
      
        870f9465-8fb6-42c0-857e-0f834f9a7c96
      
     
  
    
      Fal'ko, Vladimir
      
        2bcc7a4b-d57c-4bd4-8516-15f82727f5e4
      
     
  
    
      Smith, David C.
      
        d9b2c02d-b7ea-498b-9ea1-208a1681536f
      
     
  
  
   
  
  
    
    
  
    
      July 2021
    
    
  
  
    
      Mcdonnell, Liam
      
        f2c05544-d580-4f52-bdec-1d74be0697d7
      
     
  
    
      Viner, Jacob
      
        0fe62a03-a774-43d2-a864-79af91de17eb
      
     
  
    
      Ruiz-Tijerina, David
      
        bd7e7b38-4dcd-4191-98f1-fca5173ef7e5
      
     
  
    
      Rivera, Pasqual
      
        8363e6c4-4d7d-4c9e-bf5d-7d08249edf85
      
     
  
    
      Xu, Xiaodong
      
        870f9465-8fb6-42c0-857e-0f834f9a7c96
      
     
  
    
      Fal'ko, Vladimir
      
        2bcc7a4b-d57c-4bd4-8516-15f82727f5e4
      
     
  
    
      Smith, David C.
      
        d9b2c02d-b7ea-498b-9ea1-208a1681536f
      
     
  
       
    
 
  
    
      
  
  
  
  
  
  
    Mcdonnell, Liam, Viner, Jacob, Ruiz-Tijerina, David, Rivera, Pasqual, Xu, Xiaodong, Fal'ko, Vladimir and Smith, David C.
  
  
  
  
   
    (2021)
  
  
    
    Superposition of intra- and inter-layer excitons in twistronic MoSe2/WSe2 bilayers probed by resonant Raman scattering.
  
  
  
  
    2D Materials, 8 (3), [035009].
  
   (doi:10.1088/2053-1583/abe778). 
  
  
   
  
  
  
  
  
   
  
    
    
      
        
          Abstract
          Hybridisation of electronic bands of two-dimensional materials, assembled into twistronic heterostructures, enables one to tune their optoelectronic properties by selecting conditions for resonant interlayer hybridisation. Resonant interlayer hybridisation qualitatively modifies the excitons in such heterostructures, transforming these optically active modes into superposition states of interlayer and intralayer excitons. For MoSe2/WSe2 heterostructures, strong hybridization of both single particle and excitonic states can occur via single particle tunneling. Here we use resonance Raman scattering to provide direct evidence for the hybridisation of excitons in twistronic MoSe2/WSe2 structures, by observing scattering of specific excitons by phonons in both WSe2 and MoSe2. We also demonstrate that resonance Raman scattering spectroscopy opens up a wide range of possibilities for quantifying the layer composition of the superposition states of the exciton and the interlayer hybridisation parameters in heterostructures of two-dimensional materials.
         
      
      
        
          
            
  
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     - Accepted Manuscript
   
  
  
    
  
 
          
            
          
            
           
            
           
        
        
       
    
   
  
  
  More information
  
    
      Accepted/In Press date: 18 February 2021
 
    
      Published date: July 2021
 
    
  
  
    
  
    
     
        Additional Information:
        Funding Information:
This research was supported by UK Engineering and Physical Sciences Research Council via program grant EP/N035437/1 and grants EP/S019367/1, EP/S030719/1, EP/N010345/1, EP/V007033/1. VF acknowledges ERC Synergy Grant Hetero2D and EU Quantum Technology Flagship project 2D-SIPC. Both L P M and J V were supported by EPSRC DTP funding. The work at U Washington was funded by the Department of Energy, Basic Energy Sciences, Materials Sciences and Engineering Division (DESC0018171). D R-T was funded by UNAM-DGAPA.
Publisher Copyright:
© 2021 The Author(s). Published by IOP Publishing Ltd
Copyright:
Copyright 2021 Elsevier B.V., All rights reserved.
      
    
  
    
  
    
  
    
     
    
  
    
     
        Keywords:
        Heterobilayers, Hybridised excitons, Resonance Raman spectroscopy, Transition metal dichalcogenides
      
    
  
    
  
    
  
  
        Identifiers
        Local EPrints ID: 448342
        URI: http://eprints.soton.ac.uk/id/eprint/448342
        
          
        
        
        
          ISSN: 2053-1583
        
        
          PURE UUID: c5b7c887-1a4b-4237-b2ea-248d6a4b6919
        
  
    
        
          
            
              
            
          
        
    
        
          
            
          
        
    
        
          
        
    
        
          
        
    
        
          
        
    
        
          
        
    
        
          
            
          
        
    
  
  Catalogue record
  Date deposited: 20 Apr 2021 16:34
  Last modified: 06 Jun 2024 04:21
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      Contributors
      
          
          Author:
          
            
              
              
                Liam Mcdonnell
              
              
                 
              
            
            
          
         
      
          
          Author:
          
            
              
              
                Jacob Viner
              
              
            
            
          
        
      
          
          Author:
          
            
            
              David Ruiz-Tijerina
            
          
        
      
          
          Author:
          
            
            
              Pasqual Rivera
            
          
        
      
          
          Author:
          
            
            
              Xiaodong Xu
            
          
        
      
          
          Author:
          
            
            
              Vladimir Fal'ko
            
          
        
      
        
      
      
      
    
  
   
  
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