| 1. |
- Aeschlimann, S., et al.
(author)
-
Ultrafast momentum imaging of pseudospin-flip excitations in graphene
- 2017
-
In: Physical Review B. - 2469-9969 .- 2469-9950. ; 96:2
-
Journal article (peer-reviewed)abstract
- The pseudospin of Dirac electrons in graphene manifests itself in a peculiar momentum anisotropy for photoexcited electron-hole pairs. These interband excitations are in fact forbidden along the direction of the light polarization and are maximum perpendicular to it. Here, we use time-and angle-resolved photoemission spectroscopy to investigate the resulting unconventional hot carrier dynamics, sampling carrier distributions as a function of energy, and in-plane momentum. We first show that the rapidly-established quasithermal electron distribution initially exhibits an azimuth-dependent temperature, consistent with relaxation through collinear electron-electron scattering. Azimuthal thermalization is found to occur only at longer time delays, at a rate that depends on the substrate and the static doping level. Further, we observe pronounced differences in the electron and hole dynamics in n-doped samples. By simulating the Coulomb-and phonon-mediated carrier dynamics we are able to disentangle the influence of excitation fluence, screening, and doping, and develop a microscopic picture of the carrier dynamics in photoexcited graphene. Our results clarify new aspects of hot carrier dynamics that are unique to Dirac materials, with relevance for photocontrol experiments and optoelectronic device applications.
|
|
| 2. |
- Hofmann, Niklas, et al.
(author)
-
Link between interlayer hybridization and ultrafast charge transfer in WS 2 -graphene heterostructures
- 2023
-
In: 2D Materials. - 2053-1583. ; 10:3
-
Journal article (peer-reviewed)abstract
- Ultrafast charge separation after photoexcitation is a common phenomenon in various van-der-Waals (vdW) heterostructures with great relevance for future applications in light harvesting and detection. Theoretical understanding of this phenomenon converges towards a coherent mechanism through charge transfer states accompanied by energy dissipation into strongly coupled phonons. The detailed microscopic pathways are material specific as they sensitively depend on the band structures of the individual layers, the relative band alignment in the heterostructure, the twist angle between the layers, and interlayer interactions resulting in hybridization. We used time- and angle-resolved photoemission spectroscopy combined with tight binding and density functional theory electronic structure calculations to investigate ultrafast charge separation and recombination in WS2-graphene vdW heterostructures. We identify several avoided crossings in the band structure and discuss their relevance for ultrafast charge transfer. We relate our own observations to existing theoretical models and propose a unified picture for ultrafast charge transfer in vdW heterostructures where band alignment and twist angle emerge as the most important control parameters.
|
|
| 3. |
- Krause, R., et al.
(author)
-
Microscopic Understanding of Ultrafast Charge Transfer in van der Waals Heterostructures
- 2021
-
In: Physical Review Letters. - 1079-7114 .- 0031-9007. ; 127:27
-
Journal article (peer-reviewed)abstract
- Van der Waals heterostructures show many intriguing phenomena including ultrafast charge separation following strong excitonic absorption in the visible spectral range. However, despite the enormous potential for future applications in the field of optoelectronics, the underlying microscopic mechanism remains controversial. Here we use time- and angle-resolved photoemission spectroscopy combined with microscopic many-particle theory to reveal the relevant microscopic charge transfer channels in epitaxial WS2/graphene heterostructures. We find that the timescale for efficient ultrafast charge separation in the material is determined by direct tunneling at those points in the Brillouin zone where WS2 and graphene bands cross, while the lifetime of the charge separated transient state is set by defect-assisted tunneling through localized sulphur vacancies. The subtle interplay of intrinsic and defect-related charge transfer channels revealed in the present work can be exploited for the design of highly efficient light harvesting and detecting devices.
|
|
