2022
DOI: 10.1038/s41467-021-27747-x
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Unlocking surface octahedral tilt in two-dimensional Ruddlesden-Popper perovskites

Abstract: Molecularly soft organic-inorganic hybrid perovskites are susceptible to dynamic instabilities of the lattice called octahedral tilt, which directly impacts their carrier transport and exciton-phonon coupling. Although the structural phase transitions associated with octahedral tilt has been extensively studied in 3D hybrid halide perovskites, its impact in hybrid 2D perovskites is not well understood. Here, we used scanning tunneling microscopy (STM) to directly visualize surface octahedral tilt in freshly ex… Show more

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Cited by 64 publications
(67 citation statements)
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“…Before compression, the sample displays a clear intrinsic excitonic emission at ~ 2.14 eV arising from the bulk-like state (BS), this corresponds to the state where the majority of its BA molecules adopt the trans configuration typical of ground state alkane molecules. A low-energy PL emission centered at ~ 2.06 eV is related to surface state (SS) emission introduced by a small population of relaxed tt-conformer BA molecules 33 . Upon compression to 2.5 GPa, the BS and SS emissions red shift continuously, then they merge into a single peak at 3.9 GPa, which blue shifts with further increase in pressures until a drastic drop in PL intensity occurs due to amorphization (> 5.8 GPa), as shown in Fig.…”
Section: Broadband Photoluminescence Spectra In the Exfoliated Rpp Cr...mentioning
confidence: 99%
“…Before compression, the sample displays a clear intrinsic excitonic emission at ~ 2.14 eV arising from the bulk-like state (BS), this corresponds to the state where the majority of its BA molecules adopt the trans configuration typical of ground state alkane molecules. A low-energy PL emission centered at ~ 2.06 eV is related to surface state (SS) emission introduced by a small population of relaxed tt-conformer BA molecules 33 . Upon compression to 2.5 GPa, the BS and SS emissions red shift continuously, then they merge into a single peak at 3.9 GPa, which blue shifts with further increase in pressures until a drastic drop in PL intensity occurs due to amorphization (> 5.8 GPa), as shown in Fig.…”
Section: Broadband Photoluminescence Spectra In the Exfoliated Rpp Cr...mentioning
confidence: 99%
“…Lowdimensional materials demonstrate the merits of the spatialconfinement effect, versatile interfacial properties, and the unique aspect ratio (thicknesstolateral scale) in contrast to the bulk counterparts. [26,27] Especially, the TMDs nanosheets enrich the 2D materials family with the faradic redox activi ties, facile charge transfer as well as the anisotropic cation diffusion kinetics. [28,29] So far, the compositional ratio and thick ness tailoring of 1T TMDs nanosheets involve two types of approaches.…”
Section: Introductionmentioning
confidence: 99%
“…The obtained STM image of (BA) 2 MA 3 Pb 4 I 13 (Fig. 2i) demonstrated a clear dimer structure corresponding to the iodine atom at the top, which is further veried by the simulated charge density image 53 (Fig. 2j).…”
Section: Surface Statementioning
confidence: 64%
“…Apart from high-resolution AFM, scanning tunnelling microscopy (STM) is another tool to directly visualize the surface states. Shao et al 53 proposed a model based on monolayer (BA) 2 MA 3 Pb 4 I 13 perovskites, suggesting that the stronger out-of-plane tilt of adjacent Pb–I octahedra toward each other will naturally push their apical I atoms closer, forming a “dimer-like” structure eventually (Fig. 2h).…”
Section: Propertiesmentioning
confidence: 99%