Aygar Ayse Melis, Durnan Oliver, Molavi Bahar, Bovey Sam N R, Grüneis Alexander, Szkopek Thomas
Department of Electrical and Computer Engineering, McGill University, Québec, Montréal H3A-0E9, Canada.
Department of Electrical Engineering, Columbia University, New York, New York 10027, United States.
ACS Nano. 2024 Mar 26;18(12):9092-9099. doi: 10.1021/acsnano.3c13187. Epub 2024 Mar 13.
Experimental setups for charge transport measurements are typically not compatible with the ultrahigh vacuum conditions for chemical doping, limiting the charge carrier density that can be investigated by transport methods. Field-effect methods, including dielectric gating and ionic liquid gating, achieve too low a carrier density to induce electronic phase transitions. To bridge this gap, we developed an integrated flip-chip method to dope graphene by alkali vapor in the diffusive regime, suitable for charge transport measurements at ultrahigh charge carrier density. We introduce a cesium droplet into a sealed cavity filled with inert gas to dope a monolayer graphene sample by the process of cesium atom diffusion, adsorption, and ionization at the graphene surface, with doping beyond an electron density of 4.7 × 10 cm monitored by operando Hall measurement. The sealed assembly is stable against oxidation, enabling measurement of charge transport versus temperature and magnetic field. Cyclotron mass inversion is observed via the Hall effect, indicative of the change in Fermi surface geometry associated with the Liftshitz transition at the hyperbolic point of monolayer graphene. The transparent quartz substrate also functions as an optical window, enabling nonresonant Raman scattering. Our findings show that chemical doping, hitherto restricted to ultrahigh vacuum, can be applied in a diffusive regime at ambient pressure in an inert gas environment and thus enable charge transport studies in standard cryogenic environments.
用于电荷传输测量的实验装置通常与化学掺杂所需的超高真空条件不兼容,这限制了通过传输方法能够研究的电荷载流子密度。包括介电栅极和离子液体栅极在内的场效应方法所实现的载流子密度过低,无法诱导电子相变。为了弥补这一差距,我们开发了一种集成倒装芯片方法,在扩散 regime 中通过碱金属蒸汽对石墨烯进行掺杂,适用于在超高电荷载流子密度下进行电荷传输测量。我们将铯液滴引入充满惰性气体的密封腔中,通过铯原子在石墨烯表面的扩散、吸附和电离过程对单层石墨烯样品进行掺杂,并通过原位霍尔测量监测掺杂电子密度超过 4.7×10 cm 的情况。密封组件具有抗氧化稳定性,能够测量电荷传输随温度和磁场的变化。通过霍尔效应观察到回旋质量反转,这表明在单层石墨烯的双曲线点处与 Lifshitz 转变相关的费米面几何形状发生了变化。透明石英衬底还用作光学窗口,能够进行非共振拉曼散射。我们的研究结果表明,迄今为止仅限于超高真空的化学掺杂可以在惰性气体环境中的常压扩散 regime 中应用,从而能够在标准低温环境中进行电荷传输研究。