Spin-valley dynamics in alloy-based transition metal dichalcogenide heterobilayers

Vasily Kravtsov; Aleksey D. Liubomirov; Roman V. Cherbunin; Alessandro Catanzaro; Armando Genco; Daniel Gillard; Evgeny M. Alexeev; Tatiana Ivanova; Ekaterina Khestanova; Ivan A. Shelykh; Alexander I. Tartakovskii; Maurice S. Skolnick; Dmitry N. Krizhanovskii; Ivan V. Iorsh

doi:10.1088/2053-1583/abcf12

Spin-valley dynamics in alloy-based transition metal dichalcogenide heterobilayers

Vasily Kravtsov, Aleksey D. Liubomirov, Roman V. Cherbunin, Alessandro Catanzaro, Armando Genco, Daniel Gillard, Evgeny M. Alexeev, Tatiana Ivanova, Ekaterina Khestanova, Ivan A. Shelykh, Alexander I. Tartakovskii, Maurice S. Skolnick, Dmitry N. Krizhanovskii, Ivan V. Iorsh

Faculty of Physical Sciences

University of Iceland

Research output: Contribution to journal › Article › peer-review

Abstract

Van der Waals heterobilayers based on 2D transition metal dichalcogenides have been recently shown to support robust and long-lived valley polarization for potential valleytronic applications. However, the roles of the chemical composition and geometric alignment of the constituent layers in the underlying dynamics remain largely unexplored. Here we study spin-valley relaxation dynamics in heterobilayers with different structures and optical properties engineered via the use of alloyed monolayer semiconductors. Through a combination of time-resolved Kerr rotation spectroscopic measurements and theoretical modeling for Mo_{1 − x}W_xSe₂/WSe₂ samples with different chemical compositions and stacking angles, we uncover the contributions of the interlayer exciton recombination and charge carrier spin depolarization to the overall valley dynamics. We show that the corresponding decay rates can be tuned in a wide range in transitions from a misaligned to an aligned structure, and from a hetero- to a homo-bilayer. Our results provide insights into the microscopic spin-valley polarization mechanisms in van der Waals heterostructures for the development of future 2D valleytronic devices.

Original language	English
Article number	025011
Journal	2D Materials
Volume	8
Issue number	2
DOIs	https://doi.org/10.1088/2053-1583/abcf12
Publication status	Published - Apr 2021

Bibliographical note

Funding Information: The authors acknowledge funding from the Ministry of Education and Science of the Russian Federation through Megagrant No. 14.Y26.31.0015. Time-resolved experiments were funded by the Russian Science Foundation, Project No. 19-72-00146. Heterobilayer assembly was funded by the Russian Science Foundation, Project No. 20-72-00157. A.D.L. and R.V.C. acknowledge Saint-Petersburg State University for a research Grant No. 51125686. V.K. acknowledges support by the Government of the Russian Federation through the ITMO Fellowship and Professorship Program. A.C. and A.I.T. thank the financial support of the European Union's Horizon 2020 research and innovation programme under ITN Spin-NANO Marie Sklodowska-Curie Grant Agreement No. 676108. A.G., D.G. and A.I.T. acknowledge funding by EPSRC (EP/P026850/1 and EP/S030751/1). E.M.A. and A.I.T. thank the financial support of the Graphene Flagship Project under Grant Agreements 696656 and 785219. We thank Mikhail M. Glazov for helpful discussion. Funding Information: The authors acknowledge funding from the Ministry of Education and Science of the Russian Federation through Megagrant No. 14.Y26.31.0015. Time-resolved experiments were funded by the Russian Science Foundation, Project No. 19-72-00146. Heterobilayer assembly was funded by the Russian Science Foundation, Project No. 20-72-00157. A.D.L. and R.V.C. acknowledge Saint-Petersburg State University for a research Grant No. 51125686. V.K. acknowledges support by the Government of the Russian Federation through the ITMO Fellowship and Professorship Program. A.C. and A.I.T. thank the financial support of the European Union’s Horizon 2020 research and innovation programme under ITN Spin-NANO Marie Sklodowska-Curie Grant Agreement No. 676108. A.G., D.G. and A.I.T. acknowledge funding by EPSRC (EP/P026850/1 and EP/S030751/1). E.M.A. and A.I.T. thank the financial support of the Graphene Flag-ship Project under Grant Agreements 696656 and 785219. We thank Mikhail M. Glazov for helpful discussion. Publisher Copyright: © 2020 IOP Publishing Ltd

Other keywords

2D alloys
Transition metal dichalcogenides
Ultrafast dynamics
Valleytronics

Access to Document

10.1088/2053-1583/abcf12

Cite this

Kravtsov, V., Liubomirov, A. D., Cherbunin, R. V., Catanzaro, A., Genco, A., Gillard, D., Alexeev, E. M., Ivanova, T., Khestanova, E., Shelykh, I. A., Tartakovskii, A. I., Skolnick, M. S., Krizhanovskii, D. N., & Iorsh, I. V. (2021). Spin-valley dynamics in alloy-based transition metal dichalcogenide heterobilayers. 2D Materials, 8(2), Article 025011. https://doi.org/10.1088/2053-1583/abcf12

@article{d729a80de1da4d459ebd24ba3dea70aa,

title = "Spin-valley dynamics in alloy-based transition metal dichalcogenide heterobilayers",

abstract = "Van der Waals heterobilayers based on 2D transition metal dichalcogenides have been recently shown to support robust and long-lived valley polarization for potential valleytronic applications. However, the roles of the chemical composition and geometric alignment of the constituent layers in the underlying dynamics remain largely unexplored. Here we study spin-valley relaxation dynamics in heterobilayers with different structures and optical properties engineered via the use of alloyed monolayer semiconductors. Through a combination of time-resolved Kerr rotation spectroscopic measurements and theoretical modeling for Mo1 − xWxSe2/WSe2 samples with different chemical compositions and stacking angles, we uncover the contributions of the interlayer exciton recombination and charge carrier spin depolarization to the overall valley dynamics. We show that the corresponding decay rates can be tuned in a wide range in transitions from a misaligned to an aligned structure, and from a hetero- to a homo-bilayer. Our results provide insights into the microscopic spin-valley polarization mechanisms in van der Waals heterostructures for the development of future 2D valleytronic devices.",

keywords = "2D alloys, Transition metal dichalcogenides, Ultrafast dynamics, Valleytronics",

author = "Vasily Kravtsov and Liubomirov, \{Aleksey D.\} and Cherbunin, \{Roman V.\} and Alessandro Catanzaro and Armando Genco and Daniel Gillard and Alexeev, \{Evgeny M.\} and Tatiana Ivanova and Ekaterina Khestanova and Shelykh, \{Ivan A.\} and Tartakovskii, \{Alexander I.\} and Skolnick, \{Maurice S.\} and Krizhanovskii, \{Dmitry N.\} and Iorsh, \{Ivan V.\}",

note = "Funding Information: The authors acknowledge funding from the Ministry of Education and Science of the Russian Federation through Megagrant No. 14.Y26.31.0015. Time-resolved experiments were funded by the Russian Science Foundation, Project No. 19-72-00146. Heterobilayer assembly was funded by the Russian Science Foundation, Project No. 20-72-00157. A.D.L. and R.V.C. acknowledge Saint-Petersburg State University for a research Grant No. 51125686. V.K. acknowledges support by the Government of the Russian Federation through the ITMO Fellowship and Professorship Program. A.C. and A.I.T. thank the financial support of the European Union's Horizon 2020 research and innovation programme under ITN Spin-NANO Marie Sklodowska-Curie Grant Agreement No. 676108. A.G., D.G. and A.I.T. acknowledge funding by EPSRC (EP/P026850/1 and EP/S030751/1). E.M.A. and A.I.T. thank the financial support of the Graphene Flagship Project under Grant Agreements 696656 and 785219. We thank Mikhail M. Glazov for helpful discussion. Funding Information: The authors acknowledge funding from the Ministry of Education and Science of the Russian Federation through Megagrant No. 14.Y26.31.0015. Time-resolved experiments were funded by the Russian Science Foundation, Project No. 19-72-00146. Heterobilayer assembly was funded by the Russian Science Foundation, Project No. 20-72-00157. A.D.L. and R.V.C. acknowledge Saint-Petersburg State University for a research Grant No. 51125686. V.K. acknowledges support by the Government of the Russian Federation through the ITMO Fellowship and Professorship Program. A.C. and A.I.T. thank the financial support of the European Union{\textquoteright}s Horizon 2020 research and innovation programme under ITN Spin-NANO Marie Sklodowska-Curie Grant Agreement No. 676108. A.G., D.G. and A.I.T. acknowledge funding by EPSRC (EP/P026850/1 and EP/S030751/1). E.M.A. and A.I.T. thank the financial support of the Graphene Flag-ship Project under Grant Agreements 696656 and 785219. We thank Mikhail M. Glazov for helpful discussion. Publisher Copyright: {\textcopyright} 2020 IOP Publishing Ltd",

year = "2021",

month = apr,

doi = "10.1088/2053-1583/abcf12",

language = "English",

volume = "8",

journal = "2D Materials",

issn = "2053-1583",

publisher = "IOP Publishing Ltd.",

number = "2",

}

TY - JOUR

T1 - Spin-valley dynamics in alloy-based transition metal dichalcogenide heterobilayers

AU - Kravtsov, Vasily

AU - Liubomirov, Aleksey D.

AU - Cherbunin, Roman V.

AU - Catanzaro, Alessandro

AU - Genco, Armando

AU - Gillard, Daniel

AU - Alexeev, Evgeny M.

AU - Ivanova, Tatiana

AU - Khestanova, Ekaterina

AU - Shelykh, Ivan A.

AU - Tartakovskii, Alexander I.

AU - Skolnick, Maurice S.

AU - Krizhanovskii, Dmitry N.

AU - Iorsh, Ivan V.

N1 - Funding Information: The authors acknowledge funding from the Ministry of Education and Science of the Russian Federation through Megagrant No. 14.Y26.31.0015. Time-resolved experiments were funded by the Russian Science Foundation, Project No. 19-72-00146. Heterobilayer assembly was funded by the Russian Science Foundation, Project No. 20-72-00157. A.D.L. and R.V.C. acknowledge Saint-Petersburg State University for a research Grant No. 51125686. V.K. acknowledges support by the Government of the Russian Federation through the ITMO Fellowship and Professorship Program. A.C. and A.I.T. thank the financial support of the European Union's Horizon 2020 research and innovation programme under ITN Spin-NANO Marie Sklodowska-Curie Grant Agreement No. 676108. A.G., D.G. and A.I.T. acknowledge funding by EPSRC (EP/P026850/1 and EP/S030751/1). E.M.A. and A.I.T. thank the financial support of the Graphene Flagship Project under Grant Agreements 696656 and 785219. We thank Mikhail M. Glazov for helpful discussion. Funding Information: The authors acknowledge funding from the Ministry of Education and Science of the Russian Federation through Megagrant No. 14.Y26.31.0015. Time-resolved experiments were funded by the Russian Science Foundation, Project No. 19-72-00146. Heterobilayer assembly was funded by the Russian Science Foundation, Project No. 20-72-00157. A.D.L. and R.V.C. acknowledge Saint-Petersburg State University for a research Grant No. 51125686. V.K. acknowledges support by the Government of the Russian Federation through the ITMO Fellowship and Professorship Program. A.C. and A.I.T. thank the financial support of the European Union’s Horizon 2020 research and innovation programme under ITN Spin-NANO Marie Sklodowska-Curie Grant Agreement No. 676108. A.G., D.G. and A.I.T. acknowledge funding by EPSRC (EP/P026850/1 and EP/S030751/1). E.M.A. and A.I.T. thank the financial support of the Graphene Flag-ship Project under Grant Agreements 696656 and 785219. We thank Mikhail M. Glazov for helpful discussion. Publisher Copyright: © 2020 IOP Publishing Ltd

PY - 2021/4

Y1 - 2021/4

N2 - Van der Waals heterobilayers based on 2D transition metal dichalcogenides have been recently shown to support robust and long-lived valley polarization for potential valleytronic applications. However, the roles of the chemical composition and geometric alignment of the constituent layers in the underlying dynamics remain largely unexplored. Here we study spin-valley relaxation dynamics in heterobilayers with different structures and optical properties engineered via the use of alloyed monolayer semiconductors. Through a combination of time-resolved Kerr rotation spectroscopic measurements and theoretical modeling for Mo1 − xWxSe2/WSe2 samples with different chemical compositions and stacking angles, we uncover the contributions of the interlayer exciton recombination and charge carrier spin depolarization to the overall valley dynamics. We show that the corresponding decay rates can be tuned in a wide range in transitions from a misaligned to an aligned structure, and from a hetero- to a homo-bilayer. Our results provide insights into the microscopic spin-valley polarization mechanisms in van der Waals heterostructures for the development of future 2D valleytronic devices.

AB - Van der Waals heterobilayers based on 2D transition metal dichalcogenides have been recently shown to support robust and long-lived valley polarization for potential valleytronic applications. However, the roles of the chemical composition and geometric alignment of the constituent layers in the underlying dynamics remain largely unexplored. Here we study spin-valley relaxation dynamics in heterobilayers with different structures and optical properties engineered via the use of alloyed monolayer semiconductors. Through a combination of time-resolved Kerr rotation spectroscopic measurements and theoretical modeling for Mo1 − xWxSe2/WSe2 samples with different chemical compositions and stacking angles, we uncover the contributions of the interlayer exciton recombination and charge carrier spin depolarization to the overall valley dynamics. We show that the corresponding decay rates can be tuned in a wide range in transitions from a misaligned to an aligned structure, and from a hetero- to a homo-bilayer. Our results provide insights into the microscopic spin-valley polarization mechanisms in van der Waals heterostructures for the development of future 2D valleytronic devices.

KW - 2D alloys

KW - Transition metal dichalcogenides

KW - Ultrafast dynamics

KW - Valleytronics

UR - https://www.scopus.com/pages/publications/85099199629

U2 - 10.1088/2053-1583/abcf12

DO - 10.1088/2053-1583/abcf12

M3 - Article

SN - 2053-1583

VL - 8

JO - 2D Materials

JF - 2D Materials

IS - 2

M1 - 025011

ER -

Spin-valley dynamics in alloy-based transition metal dichalcogenide heterobilayers

Abstract

Bibliographical note

Other keywords

Access to Document

Fingerprint

Cite this