2019
DOI: 10.1038/s41467-019-12819-w
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Redox-governed charge doping dictated by interfacial diffusion in two-dimensional materials

Abstract: Controlling extra charge carriers is pivotal in manipulating electronic, optical, and magnetic properties of various two-dimensional materials. Nonetheless, the ubiquitous hole doping of two-dimensional materials in the air and acids has been controversial in its mechanistic details. Here we show their common origin is an electrochemical reaction driven by redox couples of oxygen and water molecules. Using real-time photoluminescence imaging of WS2 and Raman spectroscopy of graphene, we capture molecular diffu… Show more

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Cited by 31 publications
(88 citation statements)
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“…We suspect the opposite gate-dependent PL emissions result from p-doping and n-doping of WSe 2 on Au and SiO 2 , which is caused by charge-transfer effect [21][22][23][24] and chemical-doping effect, [25][26][27] respectively. The work function of Au is about −5.4 eV, [28] which is lower than the conduction band (CB) minimum of WSe 2 (about −3.2 eV).…”
Section: Mechanism Of the Opposite Behavior Of Excitonic Emissions Upon Gate Voltagementioning
confidence: 90%
“…We suspect the opposite gate-dependent PL emissions result from p-doping and n-doping of WSe 2 on Au and SiO 2 , which is caused by charge-transfer effect [21][22][23][24] and chemical-doping effect, [25][26][27] respectively. The work function of Au is about −5.4 eV, [28] which is lower than the conduction band (CB) minimum of WSe 2 (about −3.2 eV).…”
Section: Mechanism Of the Opposite Behavior Of Excitonic Emissions Upon Gate Voltagementioning
confidence: 90%
“…In the air, the main ambient components such as H2O and O2 would adsorb on TMDCs and influence their conduction types. In the characterization of doping result, photoluminescence (PL) spectrum is an effective method because PL peak intensities and positions would be regulated by the carrier distribution [42]. With H2O and O2 adsorbates, the PL spectra demonstrated a significant intensity enhancement for MoS2 and an opposite change for WSe2 (Figs.…”
Section: Surface Adsorptionmentioning
confidence: 99%
“…With H2O and O2 adsorbates, the PL spectra demonstrated a significant intensity enhancement for MoS2 and an opposite change for WSe2 (Figs. 5(a) and 5(b)) that could be specifically explained through the carrier recombination theory [41,42]. The carrier recombinations consist of nonradiative recombination and radiative recombination (PL spectrum) which is further divided into exciton recombination (X 0 ) and trion recombination (X +/-).…”
Section: Surface Adsorptionmentioning
confidence: 99%
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“…Electrical hysteresis has been observed in devices based on two-dimensional materials, such as graphene and TMDs based fieldeffect transistors 29,30 . Generally, electrical hysteresis is attributed to the chemical-doping effect by doping species (O2 and H2O) that are bound at the device/substrate interface, and/or on the surface of the device [31][32][33] . In our case, we propose that the excitonic hysteresis mentioned above is originated from the same scenario.…”
mentioning
confidence: 99%