DOE PAGES title logo U.S. Department of Energy
Office of Scientific and Technical Information

Title: Microsecond charge separation at heterojunctions between transition metal dichalcogenide monolayers and single-walled carbon nanotubes

Abstract

The use of monolayer transition metal dichalcogenides (TMDCs) for optical-to-electrical or optical-to-chemical energy conversion can be limited by the ultrafast excited state relaxation inherent to neat monolayers. Photoinduced charge separation at nanoscale heterojunctions is an important strategy to extend carrier lifetimes, enabling photodetectors, solar cells, and solar fuel production with these ultrathin materials. We demonstrate TMDC/single-walled carbon nanotube (SWCNT) heterojunctions with exceptionally long, microsecond timescale, charge separation following sub-picosecond interfacial charge transfer. These carrier lifetimes are orders of magnitude longer-lived than in other monolayer TMDC heterojunctions. We further present two unique methodologies for estimating charge-transfer quantum yields in MoS2 that can be broadly applied and refined for other TMDC systems. Our results highlight the promise of TMDC/SWCNT heterojunctions for advanced (photo)catalytic and optoelectronic systems and devices.

Authors:
ORCiD logo [1]; ORCiD logo [1];  [1]; ORCiD logo [1]
  1. National Renewable Energy Lab. (NREL), Golden, CO (United States)
Publication Date:
Research Org.:
National Renewable Energy Laboratory (NREL), Golden, CO (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1543254
Alternate Identifier(s):
OSTI ID: 1543166
Report Number(s):
NREL/JA-5K00-74336
Journal ID: ISSN 2051-6347; MHAOAL
Grant/Contract Number:  
AC36-08GO28308
Resource Type:
Accepted Manuscript
Journal Name:
Materials Horizons
Additional Journal Information:
Journal Volume: none; Journal Issue: none; Journal ID: ISSN 2051-6347
Publisher:
Royal Society of Chemistry
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; 71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSICS; energy conversion; monolayers; charge separation; transition metal dichalcogenides

Citation Formats

Sulas-Kern, Dana B., Zhang, Hanyu, Li, Zhaodong, and Blackburn, Jeffrey L. Microsecond charge separation at heterojunctions between transition metal dichalcogenide monolayers and single-walled carbon nanotubes. United States: N. p., 2019. Web. doi:10.1039/C9MH00954J.
Sulas-Kern, Dana B., Zhang, Hanyu, Li, Zhaodong, & Blackburn, Jeffrey L. Microsecond charge separation at heterojunctions between transition metal dichalcogenide monolayers and single-walled carbon nanotubes. United States. https://doi.org/10.1039/C9MH00954J
Sulas-Kern, Dana B., Zhang, Hanyu, Li, Zhaodong, and Blackburn, Jeffrey L. Tue . "Microsecond charge separation at heterojunctions between transition metal dichalcogenide monolayers and single-walled carbon nanotubes". United States. https://doi.org/10.1039/C9MH00954J. https://www.osti.gov/servlets/purl/1543254.
@article{osti_1543254,
title = {Microsecond charge separation at heterojunctions between transition metal dichalcogenide monolayers and single-walled carbon nanotubes},
author = {Sulas-Kern, Dana B. and Zhang, Hanyu and Li, Zhaodong and Blackburn, Jeffrey L.},
abstractNote = {The use of monolayer transition metal dichalcogenides (TMDCs) for optical-to-electrical or optical-to-chemical energy conversion can be limited by the ultrafast excited state relaxation inherent to neat monolayers. Photoinduced charge separation at nanoscale heterojunctions is an important strategy to extend carrier lifetimes, enabling photodetectors, solar cells, and solar fuel production with these ultrathin materials. We demonstrate TMDC/single-walled carbon nanotube (SWCNT) heterojunctions with exceptionally long, microsecond timescale, charge separation following sub-picosecond interfacial charge transfer. These carrier lifetimes are orders of magnitude longer-lived than in other monolayer TMDC heterojunctions. We further present two unique methodologies for estimating charge-transfer quantum yields in MoS2 that can be broadly applied and refined for other TMDC systems. Our results highlight the promise of TMDC/SWCNT heterojunctions for advanced (photo)catalytic and optoelectronic systems and devices.},
doi = {10.1039/C9MH00954J},
journal = {Materials Horizons},
number = none,
volume = none,
place = {United States},
year = {Tue Jan 01 00:00:00 EST 2019},
month = {Tue Jan 01 00:00:00 EST 2019}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record

Citation Metrics:
Cited by: 13 works
Citation information provided by
Web of Science

Save / Share:

Works referenced in this record:

Coupled Spin and Valley Physics in Monolayers of MoS 2 and Other Group-VI Dichalcogenides
journal, May 2012


Glotaran : A Java -Based Graphical User Interface for the R Package TIMP
journal, January 2012

  • Snellenburg, Joris J.; Laptenok, Sergey P.; Seger, Ralf
  • Journal of Statistical Software, Vol. 49, Issue 3
  • DOI: 10.18637/jss.v049.i03

Strong Photoluminescence Enhancement of MoS 2 through Defect Engineering and Oxygen Bonding
journal, May 2014

  • Nan, Haiyan; Wang, Zilu; Wang, Wenhui
  • ACS Nano, Vol. 8, Issue 6
  • DOI: 10.1021/nn500532f

Controlled Scalable Synthesis of Uniform, High-Quality Monolayer and Few-layer MoS2 Films
journal, May 2013

  • Yu, Yifei; Li, Chun; Liu, Yi
  • Scientific Reports, Vol. 3, Issue 1
  • DOI: 10.1038/srep01866

Activating and optimizing MoS2 basal planes for hydrogen evolution through the formation of strained sulphur vacancies
journal, November 2015

  • Li, Hong; Tsai, Charlie; Koh, Ai Leen
  • Nature Materials, Vol. 15, Issue 1
  • DOI: 10.1038/nmat4465

Carrier effects on the excitonic absorption in GaAs quantum-well structures: Phase-space filling
journal, September 1990


Investigation of Band-Offsets at Monolayer–Multilayer MoS 2 Junctions by Scanning Photocurrent Microscopy
journal, March 2015

  • Howell, Sarah L.; Jariwala, Deep; Wu, Chung-Chiang
  • Nano Letters, Vol. 15, Issue 4
  • DOI: 10.1021/nl504311p

Noncovalent Functionalization of Monolayer MoS 2 with Carbon Nanotubes: Tuning Electronic Structure and Photocatalytic Activity
journal, September 2017

  • Zhang, Zhaogang; Huang, Wei-Qing; Xie, Zhong
  • The Journal of Physical Chemistry C, Vol. 121, Issue 40
  • DOI: 10.1021/acs.jpcc.7b06793

Large, non-saturating magnetoresistance in WTe2
journal, September 2014

  • Ali, Mazhar N.; Xiong, Jun; Flynn, Steven
  • Nature, Vol. 514, Issue 7521
  • DOI: 10.1038/nature13763

Gate tunable photovoltaic effect in a MoSe 2 homojunction enabled with different thicknesses
journal, January 2017

  • Yang, Yujue; Huo, Nengjie; Li, Jingbo
  • Journal of Materials Chemistry C, Vol. 5, Issue 28
  • DOI: 10.1039/C7TC01806A

Charge Transfer Exciton and Spin Flipping at Organic–Transition-Metal Dichalcogenide Interfaces
journal, October 2017


High Photovoltaic Quantum Efficiency in Ultrathin van der Waals Heterostructures
journal, June 2017


Emerging Photoluminescence in Monolayer MoS2
journal, April 2010

  • Splendiani, Andrea; Sun, Liang; Zhang, Yuanbo
  • Nano Letters, Vol. 10, Issue 4, p. 1271-1275
  • DOI: 10.1021/nl903868w

Spin and pseudospins in layered transition metal dichalcogenides
journal, April 2014

  • Xu, Xiaodong; Yao, Wang; Xiao, Di
  • Nature Physics, Vol. 10, Issue 5
  • DOI: 10.1038/nphys2942

Electrically Driven Tuning of the Dielectric Constant in MoS 2 Layers
journal, November 2013

  • Santos, Elton J. G.; Kaxiras, Efthimios
  • ACS Nano, Vol. 7, Issue 12
  • DOI: 10.1021/nn403738b

The Crystal Structure of Molybdenite
journal, June 1923

  • Dickinson, Roscoe G.; Pauling, Linus
  • Journal of the American Chemical Society, Vol. 45, Issue 6
  • DOI: 10.1021/ja01659a020

Improved Hydrogen Evolution Reaction Performance using MoS 2 –WS 2 Heterostructures by Physicochemical Process
journal, May 2018

  • Vikraman, Dhanasekaran; Hussain, Sajjad; Akbar, Kamran
  • ACS Sustainable Chemistry & Engineering, Vol. 6, Issue 7
  • DOI: 10.1021/acssuschemeng.8b00524

Single-layer MoS2
journal, April 1986


Nonlinear manipulation of surface plasmons on graphene-TMDC Bragg reflectors
journal, December 2018


Mutual Photoluminescence Quenching and Photovoltaic Effect in Large-Area Single-Layer MoS 2 –Polymer Heterojunctions
journal, October 2016


Gate-tunable carbon nanotube-MoS2 heterojunction p-n diode
journal, October 2013

  • Jariwala, D.; Sangwan, V. K.; Wu, C. -C.
  • Proceedings of the National Academy of Sciences, Vol. 110, Issue 45
  • DOI: 10.1073/pnas.1317226110

Defect passivation of transition metal dichalcogenides via a charge transfer van der Waals interface
journal, October 2017


Long-Lived Charge Separation at Heterojunctions between Semiconducting Single-Walled Carbon Nanotubes and Perylene Diimide Electron Acceptors
journal, December 2017

  • Kang, Hyun Suk; Sisto, Thomas J.; Peurifoy, Samuel
  • The Journal of Physical Chemistry C, Vol. 122, Issue 25
  • DOI: 10.1021/acs.jpcc.8b01400

Tunable Photoluminescence of Monolayer MoS 2 via Chemical Doping
journal, November 2013

  • Mouri, Shinichiro; Miyauchi, Yuhei; Matsuda, Kazunari
  • Nano Letters, Vol. 13, Issue 12
  • DOI: 10.1021/nl403036h

Quantum-Confined Stark Effect in a MoS 2 Monolayer van der Waals Heterostructure
journal, January 2018


Recent development of two-dimensional transition metal dichalcogenides and their applications
journal, April 2017


Atomically Thin MoS2 A New Direct-Gap Semiconductor
journal, September 2010


MoS2 Heterojunctions by Thickness Modulation
journal, June 2015

  • Tosun, Mahmut; Fu, Deyi; Desai, Sujay B.
  • Scientific Reports, Vol. 5, Issue 1
  • DOI: 10.1038/srep10990

Ultrafast Spectroscopic Signature of Charge Transfer between Single-Walled Carbon Nanotubes and C 60
journal, July 2014

  • Dowgiallo, Anne-Marie; Mistry, Kevin S.; Johnson, Justin C.
  • ACS Nano, Vol. 8, Issue 8
  • DOI: 10.1021/nn503271k

Honeycomb Carbon: A Review of Graphene
journal, January 2010

  • Allen, Matthew J.; Tung, Vincent C.; Kaner, Richard B.
  • Chemical Reviews, Vol. 110, Issue 1, p. 132-145
  • DOI: 10.1021/cr900070d

Charging and discharging processes of carbon nanotubes probed by electrostatic force microscopy
journal, January 2006

  • Zdrojek, M.; Mélin, T.; Diesinger, H.
  • Journal of Applied Physics, Vol. 100, Issue 11
  • DOI: 10.1063/1.2392674

An Optimal Driving Force for Converting Excitons into Free Carriers in Excitonic Solar Cells
journal, April 2012

  • Coffey, David C.; Larson, Bryon W.; Hains, Alexander W.
  • The Journal of Physical Chemistry C, Vol. 116, Issue 16
  • DOI: 10.1021/jp302275z

Hydrogen Evolution Reaction on Hybrid Catalysts of Vertical MoS 2 Nanosheets and Hydrogenated Graphene
journal, January 2018


Transport properties of spin-triplet superconducting monolayer MoS 2
journal, March 2016


Tuning the driving force for exciton dissociation in single-walled carbon nanotube heterojunctions
journal, April 2016

  • Ihly, Rachelle; Mistry, Kevin S.; Ferguson, Andrew J.
  • Nature Chemistry, Vol. 8, Issue 6
  • DOI: 10.1038/nchem.2496

Broadband atomic-layer MoS_2 optical modulators for ultrafast pulse generations in the visible range
journal, January 2017


Dielectric properties of hexagonal boron nitride and transition metal dichalcogenides: from monolayer to bulk
journal, March 2018

  • Laturia, Akash; Van de Put, Maarten L.; Vandenberghe, William G.
  • npj 2D Materials and Applications, Vol. 2, Issue 1
  • DOI: 10.1038/s41699-018-0050-x

Exciton complexes in low dimensional transition metal dichalcogenides
journal, August 2014


Electrotunable artificial molecules based on van der Waals heterostructures
journal, October 2017

  • Zhang, Zhuo-Zhi; Song, Xiang-Xiang; Luo, Gang
  • Science Advances, Vol. 3, Issue 10
  • DOI: 10.1126/sciadv.1701699

Integrated Circuits Based on Bilayer MoS2 Transistors
journal, January 2012

  • Wang, Han; Yu, Lili; Lee, Yi-Hsien
  • Nano Letters, Vol. 12, Issue 9, p. 4674-4680
  • DOI: 10.1021/nl302015v

Ultrafast Exciton Dissociation and Long-Lived Charge Separation in a Photovoltaic Pentacene–MoS 2 van der Waals Heterojunction
journal, December 2016


Extraordinary Sunlight Absorption and One Nanometer Thick Photovoltaics Using Two-Dimensional Monolayer Materials
journal, July 2013

  • Bernardi, Marco; Palummo, Maurizia; Grossman, Jeffrey C.
  • Nano Letters, Vol. 13, Issue 8, p. 3664-3670
  • DOI: 10.1021/nl401544y

2D transition metal dichalcogenides
journal, June 2017

  • Manzeli, Sajedeh; Ovchinnikov, Dmitry; Pasquier, Diego
  • Nature Reviews Materials, Vol. 2, Issue 8
  • DOI: 10.1038/natrevmats.2017.33

The organic–2D transition metal dichalcogenide heterointerface
journal, January 2018

  • Huang, Yu Li; Zheng, Yu Jie; Song, Zhibo
  • Chemical Society Reviews, Vol. 47, Issue 9
  • DOI: 10.1039/C8CS00159F

Probing photoresponse of aligned single-walled carbon nanotube doped ultrathin MoS 2
journal, June 2018


Strain engineering in functional 2-dimensional materials
journal, February 2019

  • Sun, Yufei; Liu, Kai
  • Journal of Applied Physics, Vol. 125, Issue 8
  • DOI: 10.1063/1.5053795

Strongly coupled MoS 2 nanoflake–carbon nanotube nanocomposite as an excellent electrocatalyst for hydrogen evolution reaction
journal, January 2017

  • Huang, Haoliang; Huang, Weihao; Yang, Zhuohong
  • Journal of Materials Chemistry A, Vol. 5, Issue 4
  • DOI: 10.1039/C6TA09612C

Interlayer Excitons and Band Alignment in MoS 2 /hBN/WSe 2 van der Waals Heterostructures
journal, January 2017


Direct determination of monolayer MoS 2 and WSe 2 exciton binding energies on insulating and metallic substrates
journal, January 2018


Ultrafast charge transfer in atomically thin MoS2/WS2 heterostructures
journal, August 2014

  • Hong, Xiaoping; Kim, Jonghwan; Shi, Su-Fei
  • Nature Nanotechnology, Vol. 9, Issue 9
  • DOI: 10.1038/nnano.2014.167

Mechanisms of Ultrafast Charge Separation in a PTB7/Monolayer MoS 2 van der Waals Heterojunction
journal, April 2018

  • Zhong, Chengmei; Sangwan, Vinod K.; Wang, Chen
  • The Journal of Physical Chemistry Letters, Vol. 9, Issue 10
  • DOI: 10.1021/acs.jpclett.8b00628

Exciton-hole interactions in hole-doped single-walled carbon nanotubes evaluated by absorption spectral changes
journal, May 2012

  • Mouri, Shinichiro; Matsuda, Kazunari
  • Journal of Applied Physics, Vol. 111, Issue 9
  • DOI: 10.1063/1.4710532

Exciton-dominated Dielectric Function of Atomically Thin MoS2 Films
journal, November 2015

  • Yu, Yiling; Yu, Yifei; Cai, Yongqing
  • Scientific Reports, Vol. 5, Issue 1
  • DOI: 10.1038/srep16996

Charge transport and mobility engineering in two-dimensional transition metal chalcogenide semiconductors
journal, January 2016

  • Li, Song-Lin; Tsukagoshi, Kazuhito; Orgiu, Emanuele
  • Chemical Society Reviews, Vol. 45, Issue 1
  • DOI: 10.1039/C5CS00517E

Superconductivity emerging from a suppressed large magnetoresistant state in tungsten ditelluride
journal, July 2015

  • Kang, Defen; Zhou, Yazhou; Yi, Wei
  • Nature Communications, Vol. 6, Issue 1
  • DOI: 10.1038/ncomms8804

Field-induced charge separation dynamics in monolayer MoS 2
journal, July 2017


Monolayer MoS2 Heterojunction Solar Cells
journal, July 2014

  • Tsai, Meng-Lin; Su, Sheng-Han; Chang, Jan-Kai
  • ACS Nano, Vol. 8, Issue 8, p. 8317-8322
  • DOI: 10.1021/nn502776h

Extraordinary Mobility in Semiconducting Carbon Nanotubes
journal, January 2004

  • Dürkop, T.; Getty, S. A.; Cobas, Enrique
  • Nano Letters, Vol. 4, Issue 1, p. 35-39
  • DOI: 10.1021/nl034841q

Computational 2D Materials Database: Electronic Structure of Transition-Metal Dichalcogenides and Oxides
journal, June 2015

  • Rasmussen, Filip A.; Thygesen, Kristian S.
  • The Journal of Physical Chemistry C, Vol. 119, Issue 23
  • DOI: 10.1021/acs.jpcc.5b02950

Approaching the Schottky–Mott limit in van der Waals metal–semiconductor junctions
journal, May 2018


Order of magnitude enhancement of monolayer MoS2 photoluminescence due to near-field energy influx from nanocrystal films
journal, February 2017

  • Guo, Tianle; Sampat, Siddharth; Zhang, Kehao
  • Scientific Reports, Vol. 7, Issue 1
  • DOI: 10.1038/srep41967

Subnanometer Molybdenum Sulfide on Carbon Nanotubes as a Highly Active and Stable Electrocatalyst for Hydrogen Evolution Reaction
journal, January 2016

  • Li, Ping; Yang, Zhi; Shen, Juanxia
  • ACS Applied Materials & Interfaces, Vol. 8, Issue 5
  • DOI: 10.1021/acsami.5b08816

Single-layer MoS2 transistors
journal, January 2011

  • Radisavljevic, B.; Radenovic, A.; Brivio, J.
  • Nature Nanotechnology, Vol. 6, Issue 3, p. 147-150
  • DOI: 10.1038/nnano.2010.279

Ultrathin molybdenum disulfide/carbon nitride nanosheets with abundant active sites for enhanced hydrogen evolution
journal, January 2018

  • Qian, Xingyue; Ding, Junfei; Zhang, Jianli
  • Nanoscale, Vol. 10, Issue 4
  • DOI: 10.1039/C7NR07213A

Quantized electronic transitions in electrodeposited copper indium selenide nanocrystalline homojunctions
journal, February 2021


Defect passivation of transition metal dichalcogenides via a charge transfer van der Waals interface.
text, January 2017

  • Park, Jun Hong; Sanne, Atresh; Guo, Yuzheng
  • Apollo - University of Cambridge Repository
  • DOI: 10.17863/cam.21977

Quantum-Confined Stark Effect in a MoS2 Monolayer van der Waals Heterostructure
text, January 2018

  • G., Roch, Jonas; Nadine, Leisgang,; Guillaume, Froehlicher,
  • American Chemical Society
  • DOI: 10.5451/unibas-ep68124

Theory of Neutral and Charged Excitons in Monolayer Transition Metal Dichalcogenides
text, January 2013


Interlayer excitons and Band Alignment in MoS$_2$/hBN/WSe$_2$ van der Waals Heterostructures
text, January 2016


High Photovoltaic Quantum Efficiency in Ultrathin van der Waals Heterostructures
text, January 2017


Quantum confined Stark effect in a MoS$_2$ monolayer van der Waals heterostructure
text, January 2017


Mechanisms of Ultrafast Charge Separation in a PTB7/Monolayer MoS2 van der Waals Heterojunction
text, January 2018