Mechanistic origins of excitonic properties in 2D perovskites: Implications for exciton engineering

Kameron R. Hansen; Cindy Y. Wong; C. Emma McClure; Blake Romrell; Laura Flannery; Daniel Powell; Kelsey Garden; Alex Berzansky; Michele Eggleston; Daniel J. King; Carter M. Shirley; Matthew C. Beard; Wanyi Nie; André Schleife; John S. Colton; Luisa Whittaker-Brooks

doi:10.1016/j.matt.2023.07.004

Mechanistic origins of excitonic properties in 2D perovskites: Implications for exciton engineering

Kameron R. Hansen, Cindy Y. Wong, C. Emma McClure, Blake Romrell, Laura Flannery, Daniel Powell, Kelsey Garden, Alex Berzansky, Michele Eggleston, Daniel J. King, Carter M. Shirley, Matthew C. Beard, Wanyi Nie, André Schleife, John S. Colton, Luisa Whittaker-Brooks

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

Abstract

As the field of 2D halide perovskites (HPs) matures, state-of-the-art techniques to measure important properties, such as the band gap (E_g) and exciton binding energy (E_b), continue to produce inconsistent values. Here, we tackle this long-standing problem by obtaining direct measurements of E_g and E_b for 31 unique HP structures. The E_b values are lower than in previous literature reports and lower than expected from standard theory that assumes excitons are screened by optical-frequency dielectric constants. These low E_b values are shown to be a consequence of unique screening effects, such as superlattice screening and phonon screening. We find a strikingly strong correlation between E_b and E_g and provide design principles to a priori tune E_g and E_b to their optimal values. As such, this work offers a blueprint for E_g-E_b engineering of low-dimensional semiconductors as an even more useful replacement for simply band-gap engineering.

Original language	English (US)
Pages (from-to)	3463-3482
Number of pages	20
Journal	Matter
Volume	6
Issue number	10
DOIs	https://doi.org/10.1016/j.matt.2023.07.004
State	Published - Oct 4 2023

Keywords

2D semiconductor
MAP3: Understanding
Wannier exciton
band-gap engineering
charge-lattice interactions
dielectric function
electroabsorption
halide perovskite
phonon screening
quantum well
superlattice

ASJC Scopus subject areas

General Materials Science

Online availability

10.1016/j.matt.2023.07.004

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Hansen, K. R., Wong, C. Y., McClure, C. E., Romrell, B., Flannery, L., Powell, D., Garden, K., Berzansky, A., Eggleston, M., King, D. J., Shirley, C. M., Beard, M. C., Nie, W., Schleife, A., Colton, J. S., & Whittaker-Brooks, L. (2023). Mechanistic origins of excitonic properties in 2D perovskites: Implications for exciton engineering. Matter, 6(10), 3463-3482. https://doi.org/10.1016/j.matt.2023.07.004

Hansen, KR, Wong, CY, McClure, CE, Romrell, B, Flannery, L, Powell, D, Garden, K, Berzansky, A, Eggleston, M, King, DJ, Shirley, CM, Beard, MC, Nie, W, Schleife, A, Colton, JS & Whittaker-Brooks, L 2023, 'Mechanistic origins of excitonic properties in 2D perovskites: Implications for exciton engineering', Matter, vol. 6, no. 10, pp. 3463-3482. https://doi.org/10.1016/j.matt.2023.07.004

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abstract = "As the field of 2D halide perovskites (HPs) matures, state-of-the-art techniques to measure important properties, such as the band gap (Eg) and exciton binding energy (Eb), continue to produce inconsistent values. Here, we tackle this long-standing problem by obtaining direct measurements of Eg and Eb for 31 unique HP structures. The Eb values are lower than in previous literature reports and lower than expected from standard theory that assumes excitons are screened by optical-frequency dielectric constants. These low Eb values are shown to be a consequence of unique screening effects, such as superlattice screening and phonon screening. We find a strikingly strong correlation between Eb and Eg and provide design principles to a priori tune Eg and Eb to their optimal values. As such, this work offers a blueprint for Eg-Eb engineering of low-dimensional semiconductors as an even more useful replacement for simply band-gap engineering.",

keywords = "2D semiconductor, MAP3: Understanding, Wannier exciton, band-gap engineering, charge-lattice interactions, dielectric function, electroabsorption, halide perovskite, phonon screening, quantum well, superlattice",

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AU - Hansen, Kameron R.

AU - Wong, Cindy Y.

AU - McClure, C. Emma

AU - Romrell, Blake

AU - Flannery, Laura

AU - Powell, Daniel

AU - Garden, Kelsey

AU - Berzansky, Alex

AU - Eggleston, Michele

AU - King, Daniel J.

AU - Shirley, Carter M.

AU - Beard, Matthew C.

AU - Nie, Wanyi

AU - Schleife, André

AU - Colton, John S.

AU - Whittaker-Brooks, Luisa

PY - 2023/10/4

Y1 - 2023/10/4

N2 - As the field of 2D halide perovskites (HPs) matures, state-of-the-art techniques to measure important properties, such as the band gap (Eg) and exciton binding energy (Eb), continue to produce inconsistent values. Here, we tackle this long-standing problem by obtaining direct measurements of Eg and Eb for 31 unique HP structures. The Eb values are lower than in previous literature reports and lower than expected from standard theory that assumes excitons are screened by optical-frequency dielectric constants. These low Eb values are shown to be a consequence of unique screening effects, such as superlattice screening and phonon screening. We find a strikingly strong correlation between Eb and Eg and provide design principles to a priori tune Eg and Eb to their optimal values. As such, this work offers a blueprint for Eg-Eb engineering of low-dimensional semiconductors as an even more useful replacement for simply band-gap engineering.

AB - As the field of 2D halide perovskites (HPs) matures, state-of-the-art techniques to measure important properties, such as the band gap (Eg) and exciton binding energy (Eb), continue to produce inconsistent values. Here, we tackle this long-standing problem by obtaining direct measurements of Eg and Eb for 31 unique HP structures. The Eb values are lower than in previous literature reports and lower than expected from standard theory that assumes excitons are screened by optical-frequency dielectric constants. These low Eb values are shown to be a consequence of unique screening effects, such as superlattice screening and phonon screening. We find a strikingly strong correlation between Eb and Eg and provide design principles to a priori tune Eg and Eb to their optimal values. As such, this work offers a blueprint for Eg-Eb engineering of low-dimensional semiconductors as an even more useful replacement for simply band-gap engineering.

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KW - MAP3: Understanding

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KW - band-gap engineering

KW - charge-lattice interactions

KW - dielectric function

KW - electroabsorption

KW - halide perovskite

KW - phonon screening

KW - quantum well

KW - superlattice

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Mechanistic origins of excitonic properties in 2D perovskites: Implications for exciton engineering

Abstract

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