Growth-Controlled Broad Emission in Phase-Pure Two-Dimensional Hybrid Perovskite Films

Kennard, Rhiannon M.; Dahlman, Clayton J.; Chung, Juil; Cotts, Benjamin L.; Mikhailovsky, Alexander A.; Mao, Lingling; DeCrescent, Ryan A.; Stone, Kevin H.; Venkatesan, Naveen R.; Mohtashami, Yahya; Assadi, Sepanta; Salleo, Alberto; Schuller, Jon A.; Seshadri, Ram; Chabinyc, Michael L.

doi:10.1021/acs.chemmater.1c01641

Title: Growth-Controlled Broad Emission in Phase-Pure Two-Dimensional Hybrid Perovskite Films

Journal Article · 16 September 2021 · Chemistry of Materials

DOI: https://doi.org/10.1021/acs.chemmater.1c01641 · OSTI ID:1825667

Kennard, Rhiannon M. ^[1];

^[2]; Chung, Juil ^[2]; Cotts, Benjamin L. ^[3]; Mikhailovsky, Alexander A. ^[2];

^[2];

^[2]; Mohtashami, Yahya ^[2]; Assadi, Sepanta ^[2]; Salleo, Alberto ^[3];

^[2];

^[2]

Univ. of California, Santa Barbara, CA (United States); University of California, Santa Barbara (UCSB)
Univ. of California, Santa Barbara, CA (United States)
Stanford Univ., CA (United States)

Two-dimensional hybrid metal halide perovskites (2D perovskites) are attractive for light-emitting devices and other applications because their emission is tunable across the visible spectrum. The emission profile of 2D perovskites can be broadened via a variety of mechanisms and is further complicated by the presence of impurities. Here, the challenge of making phase-pure films in Ruddlesden–Popper phases [(A')₂(A)_n–1B_nX_3n+1 structure] is overcome by using a single A/A'-site cation, ethylammonium (EA), whose optimal size also prohibits the formation of off-target phases. In the (EA)₂(EA)_n–1Pb_nBr_3n+1 family, the low-energy, broad emission observed in bulk crystals is reduced in spin-cast, polycrystalline films. This decrease in broad emission, attributed to phonon-mediated processes, is correlated with the strain in polycrystalline films that is observed by X-ray scattering. Photothermal deflection spectroscopy shows that strain also increases the electronic disorder near the free exciton absorbance. Broad emission in films can be recovered by slowing growth kinetics, which removes the strain acquired from spin-casting and increases the domain size. Furthermore, these results help extend the utility of 2D perovskites by suggesting design rules for the growth of thin films with the targeted phase and emission.

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Research Organization:: Univ. of California, Santa Barbara, CA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: SC0012541; AC02-76SF00515

OSTI ID:: 1825667

Journal Information:: Chemistry of Materials, Journal Name: Chemistry of Materials Journal Issue: 18 Vol. 33; ISSN 0897-4756

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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