Theory of Raman enhancement by two-dimensional materials: Applications for graphene-enhanced Raman spectroscopy
We propose a third-order time-dependent perturbation theory approach to describe the chemical surface-enhanced Raman spectroscopy of molecules interacting with two-dimensional (2D) surfaces such as an ideal 2D metal and graphene, which are both 2D metallic monolayers. A detailed analysis is performe...
| Main Authors: | , |
|---|---|
| Other Authors: | |
| Format: | Article |
| Language: | English |
| Published: |
American Physical Society
2014
|
| Online Access: | http://hdl.handle.net/1721.1/88659 https://orcid.org/0000-0001-8492-2261 |
| _version_ | 1826207083477860352 |
|---|---|
| author | Barros, Eduardo B. Dresselhaus, Mildred |
| author2 | Massachusetts Institute of Technology. Department of Physics |
| author_facet | Massachusetts Institute of Technology. Department of Physics Barros, Eduardo B. Dresselhaus, Mildred |
| author_sort | Barros, Eduardo B. |
| collection | MIT |
| description | We propose a third-order time-dependent perturbation theory approach to describe the chemical surface-enhanced Raman spectroscopy of molecules interacting with two-dimensional (2D) surfaces such as an ideal 2D metal and graphene, which are both 2D metallic monolayers. A detailed analysis is performed for all the possible scattering processes involving both electrons and holes and considering the different time orderings for the electron-photon and electron-phonon interactions. We show that for ideal 2D metals a surface enhancement of the Raman scattering is possible if the Fermi energy of the surface is near the energy of either the HOMO or the LUMO states of the molecule and that a maximum enhancement is obtained when the Fermi energy matches the energy of either the HOMO or the LUMO energies plus or minus the phonon energy. The graphene-enhanced Raman spectroscopy effect is then explained as a particular case of a 2D surface, on which the density of electronic states is not constant, but increases linearly with the energy measured from the charge neutrality point. In the case of graphene, the Raman enhancement can occur for any value of the Fermi energy between the HOMO and LUMO states of the molecule. The proposed model allows for a formal approach for calculating the Raman intensity of molecules interacting with different 2D materials. |
| first_indexed | 2024-09-23T13:43:38Z |
| format | Article |
| id | mit-1721.1/88659 |
| institution | Massachusetts Institute of Technology |
| language | English |
| last_indexed | 2024-09-23T13:43:38Z |
| publishDate | 2014 |
| publisher | American Physical Society |
| record_format | dspace |
| spelling | mit-1721.1/886592022-10-01T16:44:56Z Theory of Raman enhancement by two-dimensional materials: Applications for graphene-enhanced Raman spectroscopy Barros, Eduardo B. Dresselhaus, Mildred Massachusetts Institute of Technology. Department of Physics Barros, Eduardo B. Dresselhaus, Mildred We propose a third-order time-dependent perturbation theory approach to describe the chemical surface-enhanced Raman spectroscopy of molecules interacting with two-dimensional (2D) surfaces such as an ideal 2D metal and graphene, which are both 2D metallic monolayers. A detailed analysis is performed for all the possible scattering processes involving both electrons and holes and considering the different time orderings for the electron-photon and electron-phonon interactions. We show that for ideal 2D metals a surface enhancement of the Raman scattering is possible if the Fermi energy of the surface is near the energy of either the HOMO or the LUMO states of the molecule and that a maximum enhancement is obtained when the Fermi energy matches the energy of either the HOMO or the LUMO energies plus or minus the phonon energy. The graphene-enhanced Raman spectroscopy effect is then explained as a particular case of a 2D surface, on which the density of electronic states is not constant, but increases linearly with the energy measured from the charge neutrality point. In the case of graphene, the Raman enhancement can occur for any value of the Fermi energy between the HOMO and LUMO states of the molecule. The proposed model allows for a formal approach for calculating the Raman intensity of molecules interacting with different 2D materials. National Science Foundation (U.S.) (Grant DMR-1004147) MIT-Brazil Collaboration program 2014-08-11T15:43:00Z 2014-08-11T15:43:00Z 2014-07 2014-07 2014-07-25T22:00:03Z Article http://purl.org/eprint/type/JournalArticle 1098-0121 1550-235X http://hdl.handle.net/1721.1/88659 Barros, E. B., and M. S. Dresselhaus. “Theory of Raman Enhancement by Two-Dimensional Materials: Applications for Graphene-Enhanced Raman Spectroscopy.” Phys. Rev. B 90, no. 3 (July 2014). © 2014 American Physical Society https://orcid.org/0000-0001-8492-2261 en http://dx.doi.org/10.1103/PhysRevB.90.035443 Physical Review B Article is made available in accordance with the publisher's policy and may be subject to US copyright law. Please refer to the publisher's site for terms of use. American Physical Society application/pdf American Physical Society American Physical Society |
| spellingShingle | Barros, Eduardo B. Dresselhaus, Mildred Theory of Raman enhancement by two-dimensional materials: Applications for graphene-enhanced Raman spectroscopy |
| title | Theory of Raman enhancement by two-dimensional materials: Applications for graphene-enhanced Raman spectroscopy |
| title_full | Theory of Raman enhancement by two-dimensional materials: Applications for graphene-enhanced Raman spectroscopy |
| title_fullStr | Theory of Raman enhancement by two-dimensional materials: Applications for graphene-enhanced Raman spectroscopy |
| title_full_unstemmed | Theory of Raman enhancement by two-dimensional materials: Applications for graphene-enhanced Raman spectroscopy |
| title_short | Theory of Raman enhancement by two-dimensional materials: Applications for graphene-enhanced Raman spectroscopy |
| title_sort | theory of raman enhancement by two dimensional materials applications for graphene enhanced raman spectroscopy |
| url | http://hdl.handle.net/1721.1/88659 https://orcid.org/0000-0001-8492-2261 |
| work_keys_str_mv | AT barroseduardob theoryoframanenhancementbytwodimensionalmaterialsapplicationsforgrapheneenhancedramanspectroscopy AT dresselhausmildred theoryoframanenhancementbytwodimensionalmaterialsapplicationsforgrapheneenhancedramanspectroscopy |