Anisotropic strain relaxation-induced directional ultrafast carrier dynamics in RuO2 films

Seung Gyo Jeong; In Hyeok Choi; Seungjun Lee; Jin Young Oh; Sreejith Nair; Jae Hyuck Lee; Changyoung Kim; Ambrose Seo; Woo Seok Choi; Tony Low; Jong Seok Lee; Bharat Jalan

doi:10.1126/sciadv.adw7125

Anisotropic strain relaxation-induced directional ultrafast carrier dynamics in RuO₂ films

Seung Gyo Jeong
, In Hyeok Choi
, Seungjun Lee
, Jin Young Oh
, Sreejith Nair
, Jae Hyuck Lee
, Changyoung Kim
, Ambrose Seo
, Woo Seok Choi
, Tony Low
, Jong Seok Lee
, Bharat Jalan

Producción científica: Article › revisión exhaustiva

10 Citas (Scopus)

Resumen

Ultrafast light-matter interactions inspire potential functionalities in picosecond optoelectronic applications. However, achieving directional carrier dynamics in metals remains challenging due to strong carrier scattering within a multiband environment, typically expected for isotropic carrier relaxation. In this study, we demonstrate epitaxial RuO₂/TiO₂ (110) heterostructures grown by hybrid molecular beam epitaxy to engineer polarization selectivity of ultrafast light-matter interactions via anisotropic strain engineering. Combining spectroscopic ellipsometry, x-ray absorption spectroscopy, and optical pump-probe spectroscopy, we revealed the strong anisotropic transient optoelectronic response at an excitation energy of 1.58 eV in strain-engineered RuO₂/TiO₂ (110) heterostructures along both in-plane [001] and [110] crystallographic directions. Theoretical analysis identifies strain-induced modifications in band nesting as the underlying mechanism for enhanced anisotropic carrier relaxation observed at this excitation energy. These findings establish epitaxial strain engineering as a powerful tool for tuning anisotropic optoelectronic responses with near-infrared excitations in metallic systems, paving the way for next-generation polarization-sensitive ultrafast optoelectronic devices.

Idioma original	English
Número de artículo	eadw7125
Publicación	Science advances
Volumen	11
N.º	26
DOI	https://doi.org/10.1126/sciadv.adw7125
Estado	Published - jun 27 2025

Nota bibliográfica

Publisher Copyright:
Copyright © 2025 The Authors, some rights reserved.

Financiación

Acknowledgments Funding: Film synthesis (S.G.J and B.J.) was supported by the US department of energy through grant nos. de-Sc0020211 and (partly) de-Sc0024710. Structural characterization, transport, and ellipsometry (at UMn) were supported by the Air Force Office of Scientific Research (AFOSR) through grant nos. FA9550-21-1-0025 and FA9550-24-1-0169. S.n. was supported partially by the UMn MRSec program under award no. dMR-2011401. Parts of this work were carried out at the characterization Facility, University of Minnesota, which receives partial support from the nSF through the MRSec program under award no. dMR-2011401. the work by J.h.l. and c.K. was supported by the Global Research development center (GRdc) cooperative hub Program through the national Research Foundation of Korea (nRF) funded by the Ministry of Science and ict (MSit) (grant no. RS-2023-00258359) and the nRF grant funded by MSit (grant no. nRF-2022R1A3B1077234). this work was supported by the national Research Foundation of Korea (nRF) grant funded by the Korean government (MSit) [nos. RS-2022-nR070254, RS-2024-00486846 (i.h.c. and J.S.l.), 2021R1A2c2011340 (J.Y.O and W.S.c.), RS-2023-00220471 (J.Y.O. and W.S.c.), and RS-2023-00281671 (J.Y.O. and W.S.c.)]. A.S. acknowledges the support of the national Science Foundation grant no. dMR-2104296. Author contributions: conceptualization: S.G.J., i.h.c., S.l., J.S.l., t.l., and B.J. Methodology: S.G.J., i.h.c., S.l., J.Y.O., S.n., J.h.l., c.K., A.S., W.S.c., t.l., J.S.l., and B.J. visualization: S.G.J. and i.h.c. Supervision: J.S.l. and B.J. Writing—original draft: S.G.J., i.h.c., S.l., J.S.l., t.l., and B.J. Writing—review and editing: S.G.J., i.h.c., S.l., J.Y.O., S.n., J.h.l., c.K., A.S., W.S.c., t.l., J.S.l., and B.J. Competing interests: the authors declare that they have no competing interests. Data and materials availability: All data needed to evaluate the conclusions in the paper are present in the paper and/or the Supplementary Materials. Film synthesis (S.G.J and B.J.) was supported by the US Department of Energy through grant nos. DE-SC0020211 and (partly) DE-SC0024710. Structural characterization, transport, and ellipsometry (at UMN) were supported by the Air Force Office of Scientific Research (AFOSR) through grant nos. FA9550-21-1-0025 and FA9550-24-1-0169. S.N. was supported partially by the UMN MRSEC program under award no. DMR-2011401. Parts of this work were carried out at the Characterization Facility, University of Minnesota, which receives partial support from the NSF through the MRSEC program under award no. DMR-2011401. The work by J.H.L. and C.K. was supported by the Global Research Development Center (GRDC) Cooperative Hub Program through the National Research Foundation of Korea (NRF) funded by the Ministry of Science and ICT (MSIT) (grant no. RS-2023-00258359) and the NRF grant funded by MSIT (grant no. NRF-2022R1A3B1077234). This work was supported by the National Research Foundation of Korea (NRF) grant funded by the Korean government (MSIT) [nos. RS-2022-NR070254, RS-2024-00486846 (I.H.C. and J.S.L.), 2021R1A2C2011340 (J.Y.O and W.S.C.), RS-2023-00220471 (J.Y.O. and W.S.C.), and RS-2023-00281671 (J.Y.O. and W.S.C.)]. A.S. acknowledges the support of the National Science Foundation grant no. DMR-2104296.

Financiadores	Número del financiador
National Research Foundation of Korea
Global Center for Research and Development
Ministry of Science and Technology
NSF
UMN MRSEC	DMR-2011401
National Science Foundation Arctic Social Science Program	DMR-2104296
U.S. Department of Energy	DE-SC0024710, DE-SC0020211
Ministry of Science and ICT, South Korea	RS-2023-00220471, RS-2023-00281671, RS-2024-00486846, 2021R1A2C2011340, RS-2022-NR070254, NRF-2022R1A3B1077234, RS-2023-00258359
Air Force Office of Scientific Research, United States Air Force	FA9550-21-1-0025, FA9550-24-1-0169

ASJC Scopus subject areas

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Near-IR Module for Ellipsometry
Seo, A. (Manager)
Energy Research Priority Area
Equipo / instalación: Equipment

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title = "Anisotropic strain relaxation-induced directional ultrafast carrier dynamics in RuO2 films",

abstract = "Ultrafast light-matter interactions inspire potential functionalities in picosecond optoelectronic applications. However, achieving directional carrier dynamics in metals remains challenging due to strong carrier scattering within a multiband environment, typically expected for isotropic carrier relaxation. In this study, we demonstrate epitaxial RuO2/TiO2 (110) heterostructures grown by hybrid molecular beam epitaxy to engineer polarization selectivity of ultrafast light-matter interactions via anisotropic strain engineering. Combining spectroscopic ellipsometry, x-ray absorption spectroscopy, and optical pump-probe spectroscopy, we revealed the strong anisotropic transient optoelectronic response at an excitation energy of 1.58 eV in strain-engineered RuO2/TiO2 (110) heterostructures along both in-plane [001] and [110] crystallographic directions. Theoretical analysis identifies strain-induced modifications in band nesting as the underlying mechanism for enhanced anisotropic carrier relaxation observed at this excitation energy. These findings establish epitaxial strain engineering as a powerful tool for tuning anisotropic optoelectronic responses with near-infrared excitations in metallic systems, paving the way for next-generation polarization-sensitive ultrafast optoelectronic devices.",

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AU - Nair, Sreejith

AU - Lee, Jae Hyuck

AU - Kim, Changyoung

AU - Seo, Ambrose

AU - Choi, Woo Seok

AU - Low, Tony

AU - Lee, Jong Seok

AU - Jalan, Bharat

PY - 2025/6/27

Y1 - 2025/6/27

N2 - Ultrafast light-matter interactions inspire potential functionalities in picosecond optoelectronic applications. However, achieving directional carrier dynamics in metals remains challenging due to strong carrier scattering within a multiband environment, typically expected for isotropic carrier relaxation. In this study, we demonstrate epitaxial RuO2/TiO2 (110) heterostructures grown by hybrid molecular beam epitaxy to engineer polarization selectivity of ultrafast light-matter interactions via anisotropic strain engineering. Combining spectroscopic ellipsometry, x-ray absorption spectroscopy, and optical pump-probe spectroscopy, we revealed the strong anisotropic transient optoelectronic response at an excitation energy of 1.58 eV in strain-engineered RuO2/TiO2 (110) heterostructures along both in-plane [001] and [110] crystallographic directions. Theoretical analysis identifies strain-induced modifications in band nesting as the underlying mechanism for enhanced anisotropic carrier relaxation observed at this excitation energy. These findings establish epitaxial strain engineering as a powerful tool for tuning anisotropic optoelectronic responses with near-infrared excitations in metallic systems, paving the way for next-generation polarization-sensitive ultrafast optoelectronic devices.

AB - Ultrafast light-matter interactions inspire potential functionalities in picosecond optoelectronic applications. However, achieving directional carrier dynamics in metals remains challenging due to strong carrier scattering within a multiband environment, typically expected for isotropic carrier relaxation. In this study, we demonstrate epitaxial RuO2/TiO2 (110) heterostructures grown by hybrid molecular beam epitaxy to engineer polarization selectivity of ultrafast light-matter interactions via anisotropic strain engineering. Combining spectroscopic ellipsometry, x-ray absorption spectroscopy, and optical pump-probe spectroscopy, we revealed the strong anisotropic transient optoelectronic response at an excitation energy of 1.58 eV in strain-engineered RuO2/TiO2 (110) heterostructures along both in-plane [001] and [110] crystallographic directions. Theoretical analysis identifies strain-induced modifications in band nesting as the underlying mechanism for enhanced anisotropic carrier relaxation observed at this excitation energy. These findings establish epitaxial strain engineering as a powerful tool for tuning anisotropic optoelectronic responses with near-infrared excitations in metallic systems, paving the way for next-generation polarization-sensitive ultrafast optoelectronic devices.

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