Title: Ultrafast Charge Transfer Cascade in a Mixed-Dimensionality Nanoscale Trilayer

Abstract

Innovation in optoelectronic semiconductor devices is driven by a fundamental understanding of how to move charges and/or excitons (electron–hole pairs) in specified directions for doing useful work, e.g., for making fuels or electricity. The diverse and tunable electronic and optical properties of two-dimensional (2D) transition metal dichalcogenides (TMDCs) and one-dimensional (1D) semiconducting single-walled carbon nanotubes (s-SWCNTs) make them good quantum confined model systems for fundamental studies of charge and exciton transfer across heterointerfaces. Here we demonstrate a mixeddimensionality 2D/1D/2D MoS₂/SWCNT/WSe₂ heterotrilayer that enables ultrafast photoinduced exciton dissociation, followed by charge diffusion and slow recombination. Importantly, the heterotrilayer serves to double charge carrier yield relative to a MoS₂/SWCNT heterobilayer and also demonstrates the ability of the separated charges to overcome interlayer exciton binding energies to diffuse from one TMDC/SWCNT interface to the other 2D/1D interface, resulting in Coulombically unbound charges. Interestingly, the heterotrilayer also appears to enable efficient hole transfer from SWCNTs to WSe₂, which is not observed in the identically prepared WSe₂/SWCNT heterobilayer, suggesting that increasing the complexity of nanoscale trilayers may modify dynamic pathways. Our work suggests ”mixed-dimensionality” TMDC/SWCNT based heterotrilayers as both interesting model systems for mechanistic studies of carrier dynamics at nanoscale heterointerfaces and for potential applicationsmore » in advanced optoelectronic systems.« less

Authors:

Myers, Alexis R. ^[1]; Li, Zhaodong ^[2]; Gish, Melissa K.  ^[3];

• Search DOE PAGES for author "Gish, Melissa K."
• Search DOE PAGES for ORCID "0000-0002-9886-3626"

Earley, Justin D.  ^[1];

• Search DOE PAGES for author "Earley, Justin D."
• Search DOE PAGES for ORCID "0000-0003-0492-4692"

Johnson, Justin C.  ^[3];

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• Search DOE PAGES for ORCID "0000-0002-8874-6637"

Hermosilla-Palacios, M. Alejandra  ^[3];

• Search DOE PAGES for author "Hermosilla-Palacios, M. Alejandra"
• Search DOE PAGES for ORCID "0000-0002-7169-9360"

Blackburn, Jeffrey L.  ^[3]

• Search DOE PAGES for author "Blackburn, Jeffrey L."
• Search DOE PAGES for ORCID "0000-0002-9237-5891"

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+ Show Author Affiliations

1. National Renewable Energy Laboratory, Golden, Colorado 80401, United States, Department of Chemistry, University of Colorado−Boulder, Boulder, Colorado 80309, United States
2. National Renewable Energy Laboratory, Golden, Colorado 80401, United States, The Institute of Technological Sciences, Wuhan University, Wuhan, Hubei 430072, China
3. National Renewable Energy Laboratory, Golden, Colorado 80401, United States

Publication Date:

Mon Mar 11 00:00:00 EDT 2024

Research Org.:

National Renewable Energy Laboratory (NREL), Golden, CO (United States)

Sponsoring Org.:

USDOE; USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division (CSGB)

OSTI Identifier:

2322587

Alternate Identifier(s):

OSTI ID: 2324902; OSTI ID: 2329426

Report Number(s):

NREL/JA-5K00-88449
Journal ID: ISSN 1936-0851

Grant/Contract Number:  

AC36-08GO28308

Resource Type:

Published Article

Journal Name:

ACS Nano

Additional Journal Information:

Journal Name: ACS Nano Journal Volume: 18 Journal Issue: 11; Journal ID: ISSN 1936-0851

Publisher:

American Chemical Society

Country of Publication:

United States

Language:

English

Subject:

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; 14 SOLAR ENERGY; transition metal dichalcogenides; charge transfer; heterojunctions; carbon nanotubes; excitons; interfaces; vesicles