An official website of the United States government
Chemical doping can be used to control the charge-carrier polarity and concentration in two-dimensional van der Waals materials. However, conventional methods based on substitutional doping or surface functionalization result in the degradation of electrical mobility due to structural disorder, and the maximum doping density is set by the solubility limit of dopants. Here we show that a reversible laser-assisted chlorination process can be used to create high doping concentrations (above 3 × 1013 cm−2) in graphene monolayers with minimal drops in mobility. The approach uses two lasers—with distinct photon energies and geometric configurations—that are designed for chlorination and subsequent chlorine removal, allowing highly doped patterns to be written and erased without damaging the graphene. To illustrate the capabilities of our approach, we use it to create rewritable photoactive junctions for graphene-based photodetectors.
more »
« less
Modulation Doping via a Two-Dimensional Atomic Crystalline Acceptor
Two-dimensional nanoelectronics, plasmonics, and emergent phases require clean and local charge control, calling for layered, crystalline acceptors or donors. Our Raman, photovoltage, and electrical conductance measurements combined with ab initio calculations establish the large work function and narrow bands of α-RuCl3 enable modulation doping of exfoliated single and bilayer graphene, chemical vapor deposition grown graphene and WSe2, and molecular beam epitaxy grown EuS. We further demonstrate proof of principle photovoltage devices, control via twist angle, and charge transfer through hexagonal boron nitride. Short-ranged lateral doping (≤65 nm) and high homogeneity are achieved in proximate materials with a single layer of α-RuCl3. This leads to the best-reported monolayer graphene mobilities (4900 cm2 /(V s)) at these high hole densities (3 × 1013 cm−2 ) and yields larger charge transfer to bilayer graphene (6 × 1013 cm−2).
more »
« less
- Award ID(s):
- 1700137
- PAR ID:
- 10251486
- Date Published:
- Journal Name:
- Nano letters
- Volume:
- 20
- ISSN:
- 1530-6992
- Page Range / eLocation ID:
- 8446-8452
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
More Like this
-
-
Charge transfer is a fundamental interface process that can be harnessed for light detection, photovoltaics, and photosynthesis. Recently, charge transfer was exploited in nanophotonics to alter plasmon polaritons by involving additional non-polaritonic materials to activate the charge transfer. Yet, direct charge transfer between polaritonic materials has not been demonstrated. We report the direct charge transfer in pure polaritonic van der Waals (vdW) heterostructures of α-MoO3/graphene. We extracted the Fermi energy of 0.6 eV for graphene by infrared nano-imaging of charge transfer hyperbolic polaritons in the vdW heterostructure. This unusually high Fermi energy is attributed to the charge transfer between graphene and α-MoO3. Moreover, we have observed charge transfer hyperbolic polaritons in multiple energy–momentum dispersion branches with a wavelength elongation of up to 150%. With the support from the density functional theory calculation, we find that the charge transfer between graphene and α-MoO3, absent in mechanically assembled vdW heterostructures, is attributed to the relatively pristine heterointerface preserved in the epitaxially grown vdW heterostructure. The direct charge transfer and charge transfer hyperbolic polaritons demonstrated in our work hold great promise for developing nano-optical circuits, computational devices, communication systems, and light and energy manipulation devices.more » « less
-
Surface-enhanced Raman spectroscopy (SERS) is an important analytical tool with ultrahigh sensitivity that depends on electromagnetic mechanism (EM) and chemical mechanism (CM). The CM relies on efficient charge transfer between the probe molecules and SERS substrates, which means engineering the molecule attachment and the energy level alignment at the molecule/substrate interface is critical to optimal CM enhancement. Herein, we report enhanced CM of Rhodamine 6G (R6G) on graphene SERS substrates using combined C-band ultraviolet (UVC) irradiation and Pt nanoparticle (Pt-NPs) decoration using atomic layer deposition (ALD). An enhancement of 270% was obtained in the former, which is ascribed to the graphene surface activation and p-doping on graphene for improved R6G molecule attachment and charge transfer by its surface change from hydrophobic to hydrophilic and the down-shift of the Fermi energy (p-doping) after UVC exposure. The Pt-NPs decoration adds an additional enhancement of 250% by further p-doping graphene, which shifts the graphene’s Fermi energy to promote charge (hole) transfer at the R6G/graphene interface. Remarkably, the combination of the UVC irradiation and Pt-NPs decoration has led to enhanced R6G SERS sensitivity of 5 × 10−9 M, which represents a two-orders of magnitude enhancement over that on the pristine graphene and illustrates the importance of graphene engineering for optimal probe molecule attachment and the energy level alignment at the molecule/graphene interface toward achieving high-performance SERS biosensing.more » « less
-
Abstract Colloidal quantum dots (QDs)/graphene nanohybrids provide a unique platform to design photodetectors of high performance. These photodetectors are quantum sensors due to the strong quantum confinement in QDs for spectral tunability, and in graphene for high charge mobility. Quantitatively, the high carrier mobility of graphene plays a critical role to enable high photoconductive gain and understanding its impact on the photodetector performance is imperative. Herein, we report a comparative study of PbS QDs/graphene nanohybrids with monolayer and bilayer graphene for broadband photodetection ranging from ultraviolet, visible, near-infrared to short-wave infrared spectra (wavelength: 400 nm–1750 nm) to determine if a specific advantage exists for one over the other. This study has revealed that both the monolayer and bilayer graphene grown in chemical vapor deposition can provide a highly efficient charge transfer channel for photo-generated carriers for high broadband photoresponse.more » « less
-
Capsaicin is used to modify SnO 2 quantum dots and then used as an electron-transfer material for perovskite solar cells. After capsaicin modification, the power conversion efficiency of the devices increases from 19.90 (± 0.47)% to 21.87 (± 0.28)% with a champion device of 22.24% (AM 1.5G, 100 mW/cm 2 ). Transient photovoltage and photocurrent decay show that, after the capsaicin doping, the lifetime increases from 21.55 (± 1.54) to 27.63 (± 1.45) μs, while the charge extraction time reduces from 1.90 (± 0.09) to 1.67 (± 0.06) μs. Time-resolved photoluminescence and impedance spectrum studies show similar results. The accelerated charge transfer and retarded recombination are due to defect passivation. Space charge limited current study shows that, after modification, the trap density of devices is reduced from 2.24 × 10 15 to 1.28 × 10 15 cm −3 . X-ray photoelectron spectroscopy and theoretical calculation indicate that the reduced trap density is due to the chemical interaction between carbonyl group (from capsaicin) and Sn atom, and that between carbonyl group and Pb atom.more » « less
- Free Publicly Accessible Full Text
-
Accepted Manuscript1.0
- Journal Article:
- The DOI is not currently available.
