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DOE OSTI · 2531000

Spatially Enhanced Electrostatic Doping in Graphene Realized via Heterointerfacial Precipitated Metals

Liang, Jiayun [University of California, Berkeley, CA (United States)] (ORCID:0000000245701017)·Ma, Ke [University of California, Berkeley, CA (United States)] (ORCID:0009000121632686)·Walker, Edward [Purdue Univ., West Lafayette, IN (United States)] (ORCID:0000000230153329)·Johnson, Cameron [Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). Molecular Foundry]·Zhao, Xiao [University of California, Berkeley, CA (United States); Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)] (ORCID:000000031079664X)·Terlier, Tanguy [Rice Univ., Houston, TX (United States)] (ORCID:0000000240920771)·Thomas, John C. [Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). Molecular Foundry] (ORCID:0000000221517725)·Wan, Jiawei [University of California, Berkeley, CA (United States); Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)] (ORCID:0000000238055133)·Dale, Nicholas [Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). Molecular Foundry] (ORCID:0000000184322135)·Rotenberg, Eli [Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). Advanced Light Source (ALS)] (ORCID:0000000239798844)·Bostwick, Aaron [Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). Advanced Light Source (ALS)] (ORCID:0000000290082980)·Jozwiak, Chris [Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). Advanced Light Source (ALS)] (ORCID:0000000209803753)·Jang, Ji‐Woong [Korea Institute of Materials Science (KIMS) (Korea, Republic of); Pusan National Univ., Busan (Korea, Republic of)]·Salmeron, Miquel [University of California, Berkeley, CA (United States); Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)] (ORCID:0000000228878128)·Ashby, Paul D. [Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). Molecular Foundry] (ORCID:000000034195310X)·Kim, Jongkuk [Korea Institute of Materials Science (KIMS) (Korea, Republic of)] (ORCID:0000000173893207)·Zheng, Haimei [University of California, Berkeley, CA (United States); Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)] (ORCID:0000000338134170)·Weber‐Bargioni, Alexander [Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). Molecular Foundry] (ORCID:0000000329861819)·Beechem, Thomas [Purdue Univ., West Lafayette, IN (United States)] (ORCID:0000000275360719)·Sherburne, Matthew P. [University of California, Berkeley, CA (United States)] (ORCID:0000000239921822)·Al Balushi, Zakaria Y. [University of California, Berkeley, CA (United States); Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)] (ORCID:0000000305891618)
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Abstract

Forming heavily-doped regions in 2D materials, like graphene, is a steppingstone to the design of emergent devices and heterostructures. Here, a selective-area approach is presented to tune the work-function and carrier density in monolayer graphene by spatially synthesizing sub-monolayer gallium beneath the 2D-solid. The localized metallic gallium is formed via precipitation from an underlying diamond-like carbon (DLC) film that is spatially implanted with gallium-ions. By controlling the interfacial precipitation process with annealing temperature, spatially precise ambipolar tuning of the graphene work-function is achieved, and the tunning effect preserved upon cooling to ambient conditions. Consequently, charge carrier densities from ≈1.8 × 10 10 cm -2 (hole-doped) to ≈7 × 10 13 cm -2 (electron-doped) are realized, confirmed by in situ and ex situ measurements. The theoretical studies corroborated the role of gallium at the heterointerface on charge transfer and electrostatic doping of the graphene overlayer. Specifically, sub-monolayer gallium facilitates heavy n-doping in graphene. Extending this doping strategy to other implantable elements in DLC provides a new means of exploring the physics and chemistry of highly-doped 2D materials.

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36 MATERIALS SCIENCEdopinggrapheneimplantationinterfacelow energy electron microscopyselective-area

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Liang, Jiayun [University of California, Berkeley, CA (United States)] (ORCID:0000000245701017), Ma, Ke [University of California, Berkeley, CA (United States)] (ORCID:0009000121632686), Walker, Edward [Purdue Univ., West Lafayette, IN (United States)] (ORCID:0000000230153329), Johnson, Cameron [Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). Molecular Foundry], Zhao, Xiao [University of California, Berkeley, CA (United States); Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)] (ORCID:000000031079664X), Terlier, Tanguy [Rice Univ., Houston, TX (United States)] (ORCID:0000000240920771), Thomas, John C. [Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). Molecular Foundry] (ORCID:0000000221517725), Wan, Jiawei [University of California, Berkeley, CA (United States); Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)] (ORCID:0000000238055133), Dale, Nicholas [Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). Molecular Foundry] (ORCID:0000000184322135), Rotenberg, Eli [Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). Advanced Light Source (ALS)] (ORCID:0000000239798844), Bostwick, Aaron [Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). Advanced Light Source (ALS)] (ORCID:0000000290082980), Jozwiak, Chris [Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). Advanced Light Source (ALS)] (ORCID:0000000209803753), Jang, Ji‐Woong [Korea Institute of Materials Science (KIMS) (Korea, Republic of); Pusan National Univ., Busan (Korea, Republic of)], Salmeron, Miquel [University of California, Berkeley, CA (United States); Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)] (ORCID:0000000228878128), Ashby, Paul D. [Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). Molecular Foundry] (ORCID:000000034195310X), Kim, Jongkuk [Korea Institute of Materials Science (KIMS) (Korea, Republic of)] (ORCID:0000000173893207), Zheng, Haimei [University of California, Berkeley, CA (United States); Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)] (ORCID:0000000338134170), Weber‐Bargioni, Alexander [Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). Molecular Foundry] (ORCID:0000000329861819), Beechem, Thomas [Purdue Univ., West Lafayette, IN (United States)] (ORCID:0000000275360719), Sherburne, Matthew P. [University of California, Berkeley, CA (United States)] (ORCID:0000000239921822), Al Balushi, Zakaria Y. [University of California, Berkeley, CA (United States); Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)] (ORCID:0000000305891618). 2025-03-14. Spatially Enhanced Electrostatic Doping in Graphene Realized via Heterointerfacial Precipitated Metals. https://doi.org/10.1002/smll.202412750

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36 MATERIALS SCIENCE↗