Biexcitons do not form in MoS2 monolayers from optical pumping at 6 K

Ryan E. Wood; Lawson T. Lloyd; Fauzia Mujid; Lili Wang; Marco A. Allodi; Hui Gao; Richard Mazuski; Po Chieh Ting; Saien Xie; Jiwoong Park; Gregory S. Engel

doi:10.1117/12.2545200

Biexcitons do not form in MoS₂ monolayers from optical pumping at 6 K

Ryan E. Wood, Lawson T. Lloyd, Fauzia Mujid, Lili Wang, Marco A. Allodi, Hui Gao, Richard Mazuski, Po Chieh Ting, Saien Xie, Jiwoong Park, Gregory S. Engel

Research output: Chapter in Book/Report/Conference proceeding › Conference contribution

Abstract

Transition metal dichalcogenides (TMDs) have attracted much interest in recent years due to their emerging material properties. In monolayer TMDs, such as MoS₂, extreme quantum confinement is achieved in the monolayer limit. Although monolayer TMDs represent an ideal platform to explore excitonic physics using ultrafast spectroscopy, this exploration is currently limited by confusion regarding the origin of certain spectral features, including the below-bandgap PIA feature observed in pump-probe experiments. In this work, we document an absence of PIA features immediately after photoexcitation, indicating a lack of strong optically-induced biexciton formation. Below-bandgap PIA features are observed to grow in with a time constant of 110 ± 10 fs, indicative of other factors responsible for their origin. These results indicate that optically-induced biexciton formation is most likely not responsible for the previously observed PIA features in MoS₂ monolayers.

Original language	English (US)
Title of host publication	Ultrafast Phenomena and Nanophotonics XXIV
Editors	Markus Betz, Abdulhakem Y. Elezzabi
Publisher	SPIE
ISBN (Electronic)	9781510633193
DOIs	https://doi.org/10.1117/12.2545200
State	Published - 2020
Externally published	Yes
Event	Ultrafast Phenomena and Nanophotonics XXIV 2020 - San Francisco, United States Duration: Feb 2 2020 → Feb 4 2020

Publication series

Name	Proceedings of SPIE - The International Society for Optical Engineering
Volume	11278
ISSN (Print)	0277-786X
ISSN (Electronic)	1996-756X

Conference

Conference	Ultrafast Phenomena and Nanophotonics XXIV 2020
Country/Territory	United States
City	San Francisco
Period	2/2/20 → 2/4/20

All Science Journal Classification (ASJC) codes

Electronic, Optical and Magnetic Materials
Condensed Matter Physics
Computer Science Applications
Applied Mathematics
Electrical and Electronic Engineering

Access to Document

10.1117/12.2545200

Cite this

Wood, R. E., Lloyd, L. T., Mujid, F., Wang, L., Allodi, M. A., Gao, H., Mazuski, R., Ting, P. C., Xie, S., Park, J., & Engel, G. S. (2020). Biexcitons do not form in MoS₂ monolayers from optical pumping at 6 K. In M. Betz, & A. Y. Elezzabi (Eds.), Ultrafast Phenomena and Nanophotonics XXIV [1127805] (Proceedings of SPIE - The International Society for Optical Engineering; Vol. 11278). SPIE. https://doi.org/10.1117/12.2545200

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title = "Biexcitons do not form in MoS2 monolayers from optical pumping at 6 K",

abstract = "Transition metal dichalcogenides (TMDs) have attracted much interest in recent years due to their emerging material properties. In monolayer TMDs, such as MoS2, extreme quantum confinement is achieved in the monolayer limit. Although monolayer TMDs represent an ideal platform to explore excitonic physics using ultrafast spectroscopy, this exploration is currently limited by confusion regarding the origin of certain spectral features, including the below-bandgap PIA feature observed in pump-probe experiments. In this work, we document an absence of PIA features immediately after photoexcitation, indicating a lack of strong optically-induced biexciton formation. Below-bandgap PIA features are observed to grow in with a time constant of 110 ± 10 fs, indicative of other factors responsible for their origin. These results indicate that optically-induced biexciton formation is most likely not responsible for the previously observed PIA features in MoS2 monolayers.",

author = "Wood, {Ryan E.} and Lloyd, {Lawson T.} and Fauzia Mujid and Lili Wang and Allodi, {Marco A.} and Hui Gao and Richard Mazuski and Ting, {Po Chieh} and Saien Xie and Jiwoong Park and Engel, {Gregory S.}",

note = "Funding Information: This work was financially supported by the Vannevar Bush Faculty Fellowship Program (Grant No. N00014-16-1-2513 and N00014-15-1-0048), the Air Force Office of Scientific Research (AFOSR) (Grant No. FA9550-14-1-0367 and FA9550-18-1-0099), the NSF MRSEC at the Cornell Center for Materials Research (DMR-1719875) and the University of Chicago (DMR-1420709). R.E.W. acknowledges support from the National Defense Science & Engineering Graduate Fellowship (NDSEG) Program, 32 CFR 168a, funded through the AFOSR and the Department of Defense. F.M. and R.J.M. acknowledge support from the NSF-GRFP program under grant No. DGE-1746045. M.A.A. acknowledges support from a Yen Postdoctoral fellowship from the Institute for Biophysical Dynamics at The University of Chicago and from an Arnold O. Beckman Postdoctoral Fellowship from the Arnold and Mabel Beckman Foundation. The authors would like to thank Dr. Karen M. Watters for scientific editing. Publisher Copyright: {\textcopyright} COPYRIGHT SPIE. Downloading of the abstract is permitted for personal use only.; Ultrafast Phenomena and Nanophotonics XXIV 2020 ; Conference date: 02-02-2020 Through 04-02-2020",

year = "2020",

doi = "10.1117/12.2545200",

language = "English (US)",

series = "Proceedings of SPIE - The International Society for Optical Engineering",

publisher = "SPIE",

editor = "Markus Betz and Elezzabi, {Abdulhakem Y.}",

booktitle = "Ultrafast Phenomena and Nanophotonics XXIV",

address = "United States",

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Wood, RE, Lloyd, LT, Mujid, F, Wang, L, Allodi, MA, Gao, H, Mazuski, R, Ting, PC, Xie, S, Park, J & Engel, GS 2020, Biexcitons do not form in MoS₂ monolayers from optical pumping at 6 K. in M Betz & AY Elezzabi (eds), Ultrafast Phenomena and Nanophotonics XXIV., 1127805, Proceedings of SPIE - The International Society for Optical Engineering, vol. 11278, SPIE, Ultrafast Phenomena and Nanophotonics XXIV 2020, San Francisco, United States, 2/2/20. https://doi.org/10.1117/12.2545200

Biexcitons do not form in MoS₂ monolayers from optical pumping at 6 K. / Wood, Ryan E.; Lloyd, Lawson T.; Mujid, Fauzia et al.
Ultrafast Phenomena and Nanophotonics XXIV. ed. / Markus Betz; Abdulhakem Y. Elezzabi. SPIE, 2020. 1127805 (Proceedings of SPIE - The International Society for Optical Engineering; Vol. 11278).

Research output: Chapter in Book/Report/Conference proceeding › Conference contribution

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T1 - Biexcitons do not form in MoS2 monolayers from optical pumping at 6 K

AU - Wood, Ryan E.

AU - Lloyd, Lawson T.

AU - Mujid, Fauzia

AU - Wang, Lili

AU - Allodi, Marco A.

AU - Gao, Hui

AU - Mazuski, Richard

AU - Ting, Po Chieh

AU - Xie, Saien

AU - Park, Jiwoong

AU - Engel, Gregory S.

N1 - Funding Information: This work was financially supported by the Vannevar Bush Faculty Fellowship Program (Grant No. N00014-16-1-2513 and N00014-15-1-0048), the Air Force Office of Scientific Research (AFOSR) (Grant No. FA9550-14-1-0367 and FA9550-18-1-0099), the NSF MRSEC at the Cornell Center for Materials Research (DMR-1719875) and the University of Chicago (DMR-1420709). R.E.W. acknowledges support from the National Defense Science & Engineering Graduate Fellowship (NDSEG) Program, 32 CFR 168a, funded through the AFOSR and the Department of Defense. F.M. and R.J.M. acknowledge support from the NSF-GRFP program under grant No. DGE-1746045. M.A.A. acknowledges support from a Yen Postdoctoral fellowship from the Institute for Biophysical Dynamics at The University of Chicago and from an Arnold O. Beckman Postdoctoral Fellowship from the Arnold and Mabel Beckman Foundation. The authors would like to thank Dr. Karen M. Watters for scientific editing. Publisher Copyright: © COPYRIGHT SPIE. Downloading of the abstract is permitted for personal use only.

PY - 2020

Y1 - 2020

N2 - Transition metal dichalcogenides (TMDs) have attracted much interest in recent years due to their emerging material properties. In monolayer TMDs, such as MoS2, extreme quantum confinement is achieved in the monolayer limit. Although monolayer TMDs represent an ideal platform to explore excitonic physics using ultrafast spectroscopy, this exploration is currently limited by confusion regarding the origin of certain spectral features, including the below-bandgap PIA feature observed in pump-probe experiments. In this work, we document an absence of PIA features immediately after photoexcitation, indicating a lack of strong optically-induced biexciton formation. Below-bandgap PIA features are observed to grow in with a time constant of 110 ± 10 fs, indicative of other factors responsible for their origin. These results indicate that optically-induced biexciton formation is most likely not responsible for the previously observed PIA features in MoS2 monolayers.

AB - Transition metal dichalcogenides (TMDs) have attracted much interest in recent years due to their emerging material properties. In monolayer TMDs, such as MoS2, extreme quantum confinement is achieved in the monolayer limit. Although monolayer TMDs represent an ideal platform to explore excitonic physics using ultrafast spectroscopy, this exploration is currently limited by confusion regarding the origin of certain spectral features, including the below-bandgap PIA feature observed in pump-probe experiments. In this work, we document an absence of PIA features immediately after photoexcitation, indicating a lack of strong optically-induced biexciton formation. Below-bandgap PIA features are observed to grow in with a time constant of 110 ± 10 fs, indicative of other factors responsible for their origin. These results indicate that optically-induced biexciton formation is most likely not responsible for the previously observed PIA features in MoS2 monolayers.

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A2 - Betz, Markus

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Y2 - 2 February 2020 through 4 February 2020

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