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

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

doi:10.1016/j.matt.2023.07.004

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

Journal Article · 28 July 2023 · Matter (Online)

DOI: https://doi.org/10.1016/j.matt.2023.07.004 · OSTI ID:2001120

^[1]; Wong, Cindy Y. ^[2]; McClure, C. Emma ^[3]; Romrell, Blake ^[4]; Flannery, Laura ^[2]; Powell, Daniel ^[1]; Garden, Kelsey ^[1]; Berzansky, Alex ^[1]; Eggleston, Michele ^[4]; King, Daniel J. ^[4]; Shirley, Carter M. ^[4];

^[5]; Nie, Wanyi ^[6]; Schleife, André ^[2]; Colton, John S. ^[4]; Whittaker-Brooks, Luisa ^[1]

Univ. of Utah, Salt Lake City, UT (United States)
Univ. of Illinois at Urbana-Champaign, IL (United States)
Brigham Young Univ., Provo, UT (United States); National Renewable Energy Laboratory (NREL), Golden, CO (United States)
Brigham Young Univ., Provo, UT (United States)
National Renewable Energy Laboratory (NREL), Golden, CO (United States)
Los Alamos National Laboratory (LANL), Los Alamos, NM (United States)

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. Here, 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.

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Research Organization:: National Renewable Energy Laboratory (NREL), Golden, CO (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Materials Sciences & Engineering Division (MSE); National Science Foundation (NSF); USDOE National Nuclear Security Administration (NNSA)

Grant/Contract Number:: AC36-08GO28308; SC0019041; 89233218CNA000001

OSTI ID:: 2001120

Report Number(s):: NREL/JA--5900-87580; MainId:88355; UUID:2296defc-bb65-49ad-8e9f-d2739d348844; MainAdminID:70689

Journal Information:: Matter (Online), Journal Name: Matter (Online) Journal Issue: 10 Vol. 6; ISSN 2590-2385

Publisher:: Cell Press/ElsevierCopyright Statement

Country of Publication:: United States

Language:: English

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

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