Real-time GW-BSE investigations on spin-valley exciton dynamics in monolayer transition metal dichalcogenide.
TLDR
In this paper, an ab initio nonadiabatic molecular dynamics method based on GW plus real-time Bethe-Salpeter equation (GW + rtBSE-NAMD) was developed for the spin-resolved exciton dynamics where the electron-phonon (eph) scattering, spin-orbit interaction (SOI), and electron-hole (e-h) interactions come into play collectively.Abstract:
We develop an ab initio nonadiabatic molecular dynamics (NAMD) method based on GW plus real-time Bethe-Salpeter equation (GW + rtBSE-NAMD) for the spin-resolved exciton dynamics. From investigations on MoS2, we provide a comprehensive picture of spin-valley exciton dynamics where the electron-phonon (e-ph) scattering, spin-orbit interaction (SOI), and electron-hole (e-h) interactions come into play collectively. In particular, we provide a direct evidence that e-h exchange interaction plays a dominant role in the fast valley depolarization within a few picoseconds, which is in excellent agreement with experiments. Moreover, there are bright-to-dark exciton transitions induced by e-ph scattering and SOI. Our study proves that e-h many-body effects are essential to understand the spin-valley exciton dynamics in transition metal dichalcogenides and the newly developed GW + rtBSE-NAMD method provides a powerful tool for exciton dynamics in extended systems with time, space, momentum, energy, and spin resolution.read more
Citations
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References
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BerkeleyGW: A massively parallel computer package for the calculation of the quasiparticle and optical properties of materials and nanostructures
Jack Deslippe,Jack Deslippe,Georgy Samsonidze,Georgy Samsonidze,David A. Strubbe,David A. Strubbe,Manish Jain,Manish Jain,Marvin L. Cohen,Marvin L. Cohen,Steven G. Louie,Steven G. Louie +11 more
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Pasqual Rivera,Kyle L. Seyler,Hongyi Yu,John Schaibley,Jiaqiang Yan,Jiaqiang Yan,David Mandrus,David Mandrus,Wang Yao,Xiaodong Xu +9 more
TL;DR: This work created interlayer exciton spin-valley polarization by means of circularly polarized optical pumping and determined a valley lifetime of 40 nanoseconds, which enables the visualization of the expansion of a valley-polarized exciton cloud over several micrometers.
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Theoretical studies of photoinduced electron transfer in dye-sensitized TiO2.
Walter R. Duncan,Oleg V. Prezhdo +1 more
TL;DR: This review describes recent research into the properties of the chromophore-TiO2 interface that forms the basis for photoinduced charge separation in dye-sensitized semiconductor solar cells, focusing particularly on an atomistic picture of the electron-injection dynamics.
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Alexey V. Akimov,Oleg V. Prezhdo +1 more
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Many-body effects in valleytronics: direct measurement of valley lifetimes in single-layer MoS2.
TL;DR: Direct measurements of valley relaxation dynamics in single layer MoS2 are reported by using ultrafast transient absorption spectroscopy, showing that strong Coulomb interactions significantly impact valley population dynamics and biexcitons form with more than an order of magnitude larger binding energy compared to conventional semiconductors.