摘要
Platinum diselenide(PtSe_(2))is a promising two-dimensional(2D)material for the terahertz(THz)range as,unlike other transition metal dichalcogenides(TMDs),its bandgap can be uniquely tuned from a semiconductor in the nearinfrared to a semimetal with the number of atomic layers.This gives the material unique THz photonic properties that can be layer-engineered.Here,we demonstrate that a controlled THz nonlinearity—tuned from monolayer to bulk PtSe_(2)—can be realized in wafer size polycrystalline PtSe_(2)through the generation of ultrafast photocurrents and the engineering of the bandstructure valleys.This is combined with the PtSe_(2)layer interaction with the substrate for a broken material centrosymmetry,permitting a second order nonlinearity.Further,we show layer dependent circular dichroism,where the sign of the ultrafast currents and hence the phase of the emitted THz pulse can be controlled through the excitation of different bandstructure valleys.In particular,we show that a semimetal has a strong dichroism that is absent in the monolayer and few layer semiconducting limit.The microscopic origins of this TMD bandstructure engineering are highlighted through detailed DFT simulations,and shows the circular dichroism can be controlled when PtSe_(2)becomes a semimetal and when the K-valleys can be excited.As well as showing that PtSe_(2)is a promising material for THz generation through layer controlled optical nonlinearities,this work opens up a new class of circular dichroism materials beyond the monolayer limit that has been the case of traditional TMDs,and impacting a range of domains from THz valleytronics,THz spintronics to harmonic generation.
出处
《InfoMat》
SCIE
CSCD
2023年第11期49-63,共15页
信息材料(英文)
基金
H2020 Future and Emerging Technologies,Grant/Award Number:964735
H2020 Excellent Science,Grant/Award Number:881603
Agence Nationale de la Recherche,Grant/Award Numbers:ANR-16-CE24-0023,ANR-2018-CE08-018-05
National Research Foundation Singapore,Grant/Award Number:NRF-CRP26-2021-0004
Region Ile de France
EquipMeso,Grant/Award Number:ANR-10-EQPX-29-01。