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. 2023 Mar 28;17(6):5956-5962.
doi: 10.1021/acsnano.3c00180. Epub 2023 Mar 10.

Control of Raman Scattering Quantum Interference Pathways in Graphene

Xue Chen  1   2 , Sven Reichardt  3 , Miao-Ling Lin  1 , Yu-Chen Leng  1 , Yan Lu  1 , Heng Wu  1   2 , Rui Mei  1   2 , Ludger Wirtz  3 , Xin Zhang  1   2 , Andrea C Ferrari  4 , Ping-Heng Tan  1   2
Affiliations

Control of Raman Scattering Quantum Interference Pathways in Graphene

Xue Chen et al. ACS Nano. .

Abstract

Graphene is an ideal platform to study the coherence of quantum interference pathways by tuning doping or laser excitation energy. The latter produces a Raman excitation profile that provides direct insight into the lifetimes of intermediate electronic excitations and, therefore, on quantum interference, which has so far remained elusive. Here, we control the Raman scattering pathways by tuning the laser excitation energy in graphene doped up to 1.05 eV. The Raman excitation profile of the G mode indicates its position and full width at half-maximum are linearly dependent on doping. Doping-enhanced electron-electron interactions dominate the lifetimes of Raman scattering pathways and reduce Raman interference. This will provide guidance for engineering quantum pathways for doped graphene, nanotubes, and topological insulators.

Keywords: electron−electron interaction; electron−phonon coupling; graphite intercalation compounds; quantum interference; resonant Raman scattering.

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Conflict of interest statement

The authors declare no competing financial interest.

Figures

Figure 1
Figure 1
(a) Optical image of sample S4, with the area of interest indicated by the white box. (b) Schematic illustration of intercalation process, where Cl, Fe, and C atoms are color coded in green, purple, and dark-gray, respectively. (c) Raman spectra of samples S1–S4, with different EF, SLG (EF ∼ −0.08 eV) and graphite, for EL = 2.41 eV. (d) FWHM(G) and (e) I(2D)/I(G) as a function of Pos(G) for SLG in samples S1–S4.
Figure 2
Figure 2
(a) Contour plots of I(G) of S4 as a function of Pos(G) and EL. (b) Experimental G REP and fit based on eq 1. Calculated (c) phase of Rk and (d) magnitude |Rk| for each pathway at EL = 2.6 eV and γ = 0.225 eV for SLG with 2|EF|= 2.1 eV. (e) Calculated |Rk| for EL = 1.8 eV. The diagonal and shaded areas indicate the blocking region imposed by the Pauli exclusion principle and the pathways contributing to I(G).
Figure 3
Figure 3
(a) Experimental REPs for S1–S4 along with the fitted curves based on eq 1. (b) Correlation between |EFREP| and |EF|. The solid line corresponds to |EFREP| = |EF|. (c) γ as a function of |EFREP|. The solid line is a linear fit.
Figure 4
Figure 4
Absolute value (logarithmic scale) and phase (color-encoded) of formula image (formula image) in the high-symmetry line Γ – K – M – Γ at EL = 2 eV by including Mk (a) (Full cal.), and setting the dipole and EPMEs to a constant (b) (Constant numerator), both for a constant broadening of γ = 0.225 eV. The shaded area represents the value of the joint density of states at Ek. (c) Experimental REP (open circles) and theoretical REPs calculated by ab initio (Full cal., dashed line) and the SM (solid line). (d) Rescaled experimental REPs for S2–S4 as a function of (EL – EG/2)/2|EFREP|.
Figure 5
Figure 5
Raman spectra of samples S1–S4 and unintentionally doped SLG with no background subtracted, for EL = 2.41 eV. The Raman peaks of graphene are identified as well as those from FeCl3 and Si substrate labeled by gray # and *, respectively. The broadband backgrounds in samples S2–S4 are PL emission near 2|EF| of heavily doped SLG.
See this image and copyright information in PMC

References

    1. Ficek Z.; Swain S.. Quantum Interference and Coherence: Theory and Experiments; Springer: New York, 2005; Chapter 1, pp 1–44.
    1. Liu R. C.; Odom B.; Yamamoto Y.; Tarucha S. Quantum Interference in Electron Collision. Nature 1998, 391, 263–265. 10.1038/34611. - DOI
    1. Zheng H.; Hou S.; Xin C.; Wu Q.; Jiang F.; Tan Z.; Zhou X.; Lin L.; He W.; Li Q.; Zheng J.; Zhang L.; Liu J.; Yang Y.; Shi J.; Zhang X.; Zhao Y.; Li Y.; Lambert C.; Hong W. Room-Temperature Quantum Interference in Single Perovskite Quantum Dot Junctions. Nat. Commun. 2019, 10, 5458.10.1038/s41467-019-13389-7. - DOI - PMC - PubMed
    1. Guédon C. M.; Valkenier H.; Markussen T.; Thygesen K. S.; Hummelen J. C.; van der Molen S. J. Observation of Quantum Interference in Molecular Charge Transport. Nat. Nanotechnol. 2012, 7, 305–309. 10.1038/nnano.2012.37. - DOI - PubMed
    1. Bai J.; Daaoub A.; Sangtarash S.; Li X.; Tang Y.; Zou Q.; Sadeghi H.; Liu S.; Huang X.; Tan Z.; Liu J.; Yang Y.; Shi J.; Meszaros G.; Chen W.; Lambert C.; Hong W. Anti-Resonance Features of Destructive Quantum Interference in Single-Molecule Thiophene Junctions Achieved by Electrochemical Gating. Nat. Mater. 2019, 18, 364–369. 10.1038/s41563-018-0265-4. - DOI - PubMed