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Self-energy dynamics and mode-specific phonon threshold effect in a Kekule-ordered graphene

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 Added by Hongyun Zhang
 Publication date 2021
  fields Physics
and research's language is English




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Electron-phonon interaction and related self-energy are fundamental to both the equilibrium properties and non-equilibrium relaxation dynamics of solids. Although electron-phonon interaction has been suggested by various time-resolved measurements to be important for the relaxation dynamics of graphene, the lack of energy- and momentum-resolved self-energy dynamics prohibits direct identification of the role of specific phonon modes in the relaxation dynamics. Here by performing time- and angle-resolved photoemission spectroscopy measurements on a Kekule-ordered graphene with folded Dirac cones at the $Gamma$ point, we have succeeded in resolving the self-energy effect induced by coupling of electrons to two phonons at $Omega_1$ = 177 meV and $Omega_2$ = 54 meV and revealing its dynamical change in the time domain. Moreover, these strongly coupled phonons define energy thresholds, which separate the hierarchical relaxation dynamics from ultrafast, fast to slow, thereby providing direct experimental evidence for the dominant role of mode-specific phonons in the relaxation dynamics

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While graphene shows a characteristic conical dispersion with a vanishing density of states (DOS) near the Fermi energy E$_F$, it has been suggested that under extremely-high doping ($sim$ 1/4), the extended flat band can be shifted to near E$_F$, resulting in a diverging DOS with strong many-body interactions and electronic instabilities. Although such highly-doped graphene has attracted tremendous research interests, so far the experimental demonstration of doping-induced flat band as well as its associated intriguing phenomena remains rather limited. Here, we report the observation of an extended flat band around the M point in a Li-intercalated graphene, in which the Li ions not only dope graphene with a high electron concentration, but also induce a Kekule order which breaks the chiral symmetry. At such high electron doping, pronounced electron-phonon and electron-electron interactions are clearly identified by the notable kinks in the band dispersion and a strong reduction of the band width. Moreover, by following the evolution of the band structure upon Li intercalation, we find that the flat band and the Kekule order, with the characteristic flat band near M and folded Dirac cones near $Gamma$ respectively, emerge simultaneously, which indicates that they are strongly coupled. Our work identifies Li-intercalated graphene as a fertile platform for investigating the unique physics of the extended flat band, strong many-body interactions as well as the Kekule order.
The low-energy excitations of graphene are relativistic massless Dirac fermions with opposite chiralities at valleys K and K. Breaking the chiral symmetry could lead to gap opening in analogy to dynamical mass generation in particle physics. Here we report direct experimental evidences of chiral symmetry breaking (CSB) from both microscopic and spectroscopic measurements in a Li-intercalated graphene. The CSB is evidenced by gap opening at the Dirac point, Kekule-O type modulation, and chirality mixing near the gap edge. Our work opens up opportunities for investigating CSB related physics in a Kekule-ordered graphene.
Phonon self-energy corrections have mostly been studied theoretically and experimentally for phonon modes with zone-center (q = 0) wave-vectors. Here, gate-modulated Raman scattering is used to study phonons of a single layer of graphene (1LG) in the frequency range from 2350 to 2750 cm-1, which shows the G* and the G-band features originating from a double-resonant Raman process with q ot= 0. The observed phonon renormalization effects are different from what is observed for the zone-center q = 0 case. To explain our experimental findings, we explored the phonon self-energy for the phonons with non-zero wave-vectors (q ot= 0) in 1LG in which the frequencies and decay widths are expected to behave oppositely to the behavior observed in the corresponding zone-center q = 0 processes. Within this framework, we resolve the identification of the phonon modes contributing to the G* Raman feature at 2450 cm-1 to include the iTO+LA combination modes with q ot= 0 and the 2iTO overtone modes with q = 0, showing both to be associated with wave-vectors near the high symmetry point K in the Brillouin zone.
A Kekule bond texture in graphene modifies the electronic band structure by folding the Brillouin zone and bringing the two inequivalent Dirac points to the center. This can result, in the opening of a gap (Kek-O) or the locking of the valley degree of freedom with the direction of motion (Kek-Y). We analyze the effects of uniaxial strain on the band structure of Kekule-distorted graphene for both textures. Using a tight-binding approach, we introduce strain by considering the hopping renormalization and corresponding geometrical modifications of the Brillouin zone. We numerically evaluate the dispersion relation and present analytical expressions for the low-energy limit. Our results indicate the emergence of a Zeeman-like term due to the coupling of the pseudospin with the pseudomagnetic strain potential which separates the valleys by moving them in opposite directions away from the center of the Brillouin zone. For the Kek-O phase, this results in a competition between the Kekule parameter that opens a gap and the magnitude of strain which closes it. While for the Kek-Y phase, in a superposition of two shifted Dirac cones. As the Dirac cones are much closer in the supperlattice reciprocal space that in pristine graphene, we propose strain as a control parameter for intervalley scattering.
We demonstrate a scanning gate grid measurement technique consisting in measuring the conductance of a quantum point contact (QPC) as a function of gate voltage at each tip position. Unlike conventional scanning gate experiments, it allows investigating QPC conductance plateaus affected by the tip at these positions. We compensate the capacitive coupling of the tip to the QPC and discover that interference fringes coexist with distorted QPC plateaus. We spatially resolve the mode structure for each plateau.
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