Nonequilibrium Lattice Dynamics in Photoexcited 2D Perovskites

Cuthriell, Shelby A.; Panuganti, Shobhana; Laing, Craig C.; Quintero, Michael A.; Güzeltürk, Burak; Yazdani, Nasser; Traoré, Boubacar; Brumberg, Alexandra; Malliakas, Christos D.; Lindenberg, Aaron M.; Wood, Vanessa; Katan, Claudine; Even, Jacky; Zhang, Xiaoyi; Kanatzidis, Mercouri G.; Schaller, Richard D.

doi:10.1002/adma.202202709

Cited by 11 publications

(10 citation statements)

References 50 publications

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“…Syntheses and crystal structures of the six layered perovskites of interest were reported by Billing et al 2,4,19 As reported in this previous work, changing the organic spacer from four to six carbons, as well as from linear to cyclic carbon chains, induces slight shifts in the equatorial lead-iodide bonds that, in turn, causes blue-or red-shifting of the absorption and emission energies (Figures 1 and S1). 6 These equatorial Pb− I−Pb bond angles lead to emission energies of approximately 520, 515, 524, 493, 515, and 516 nm, respectively (Figure 1f).…”

Section: ■ Results and Discussionsupporting

confidence: 60%

Cyclic versus Linear Alkylammonium Cations: Preventing Phase Transitions at Operational Temperatures in 2D Perovskites

et al. 2023

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Two-dimensional lead halide perovskites offer numerous attractive features for optoelectronics owing to their soft, deformable lattices and high degree of chemical tunability. While alteration of the metal and halide ions gives rise to significant modification of the bandgap energy, the organic spacer cations offer in-roads to tuning phase behavior and more subtle functionalities in ways that remain to be understood. Here, we study six variations of 2D perovskites changing only the organic spacer cations and demonstrate that these components intrinsically impact material response in important ways such as altering crystallographic structure, temperature-induced phase transitions, and photoluminescence emission. Two-dimensional perovskites containing commonly utilized aliphatic linear spacers, such as butylammonium, undergo phase transitions near room temperature. These transitions and temperature changes induce spacer-dependent variations in the emission spectra. Conversely, 2D perovskites comprising cyclic aliphatic spacers, such as cyclobutylammonium, are found to lack first-order phase transitions. These cyclic molecules are more sterically hindered within the crystal lattice, leading to temperature-induced contraction or expansion along certain crystallographic planes but no other significant thermal effects; additionally, they undergo changes in their emission spectra that cannot be explained by simple thermal expansion. Given the similarities in the dielectric and chemical makeup of this set of six alkylammonium molecules, these results are unexpected and suggest a large structural and thermal phase space via spacer manipulation that could lead to improved 2D perovskite functionalization.

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Section: ■ Results and Discussionsupporting

confidence: 60%

Cyclic versus Linear Alkylammonium Cations: Preventing Phase Transitions at Operational Temperatures in 2D Perovskites

et al. 2023

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Section: Optoelectronic Properties Of 3d and 2d Halide Perovskitesmentioning

confidence: 99%

“…Cuthriell et al studied the nonequilibrium lattice response of BA and PEA n = 1 halide perovskites and reveal a suppressing line width narrowing in both transient X-rays and photoluminescent spectra at ∼1 ns time scales, suggesting a transient ordering of distorted octahedra (Figure 18 a,b). 369 Interestingly, Zhang et al has reported lattice dynamics beyond the Mott density and revealed an ultrafast relaxation of the lattice distortion at very short time, via reduced in-lane octahedral tilting (relaxation of antiferro-distortions) in DJ-type 2D halide perovskites (Figure 18 c−e). 370 Such strong carrier−lattice interactions are initiated by dense electron−hole plasma beyond the Mott density.…”

Section: Bulk Ferroelectricity In 2d Halide Perovskitesmentioning

confidence: 99%

Synergy of 3D and 2D Perovskites for Durable, Efficient Solar Cells and Beyond

Metcalf,

Sidhik,

Zhang

et al. 2023

Chem. Rev.

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Three-dimensional (3D) organic–inorganic lead halide perovskites have emerged in the past few years as a promising material for low-cost, high-efficiency optoelectronic devices. Spurred by this recent interest, several subclasses of halide perovskites such as two-dimensional (2D) halide perovskites have begun to play a significant role in advancing the fundamental understanding of the structural, chemical, and physical properties of halide perovskites, which are technologically relevant. While the chemistry of these 2D materials is similar to that of the 3D halide perovskites, their layered structure with a hybrid organic–inorganic interface induces new emergent properties that can significantly or sometimes subtly be important. Synergistic properties can be realized in systems that combine different materials exhibiting different dimensionalities by exploiting their intrinsic compatibility. In many cases, the weaknesses of each material can be alleviated in heteroarchitectures. For example, 3D-2D halide perovskites can demonstrate novel behavior that neither material would be capable of separately. This review describes how the structural differences between 3D halide perovskites and 2D halide perovskites give rise to their disparate materials properties, discusses strategies for realizing mixed-dimensional systems of various architectures through solution-processing techniques, and presents a comprehensive outlook for the use of 3D-2D systems in solar cells. Finally, we investigate applications of 3D-2D systems beyond photovoltaics and offer our perspective on mixed-dimensional perovskite systems as semiconductor materials with unrivaled tunability, efficiency, and technologically relevant durability.

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“…Finally, deformation potential coupling to Pb–X–Pb bends should be present for other LHP systems with differing compositions (other A-cations or X-anions) or dimensions (for example, two-dimensional (2D) LHPs), provided the VB, CB or both consist of sp -bonding of the Pb–X sublattice. For example, photoinduced straightening of Pb–I–Pb bends has recently been reported in 2D LHPs 49 , 50 . The strength of the coupling and interactions, and therefore their relevance, depends on the particular LHP system.…”

Section: Mainmentioning

confidence: 99%

Coupling to octahedral tilts in halide perovskite nanocrystals induces phonon-mediated attractive interactions between excitons

Yazdani,

Bodnarchuk,

Bertolotti

et al. 2023

Nat. Phys.

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Understanding the origin of electron–phonon coupling in lead halide perovskites is key to interpreting and leveraging their optical and electronic properties. Here we show that photoexcitation drives a reduction of the lead–halide–lead bond angles, a result of deformation potential coupling to low-energy optical phonons. We accomplish this by performing femtosecond-resolved, optical-pump–electron-diffraction-probe measurements to quantify the lattice reorganization occurring as a result of photoexcitation in nanocrystals of FAPbBr3. Our results indicate a stronger coupling in FAPbBr3 than CsPbBr3. We attribute the enhanced coupling in FAPbBr3 to its disordered crystal structure, which persists down to cryogenic temperatures. We find the reorganizations induced by each exciton in a multi-excitonic state constructively interfere, giving rise to a coupling strength that scales quadratically with the exciton number. This superlinear scaling induces phonon-mediated attractive interactions between excitations in lead halide perovskites.

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Nonequilibrium Lattice Dynamics in Photoexcited 2D Perovskites

Cited by 11 publications

References 50 publications

Cyclic versus Linear Alkylammonium Cations: Preventing Phase Transitions at Operational Temperatures in 2D Perovskites

Cyclic versus Linear Alkylammonium Cations: Preventing Phase Transitions at Operational Temperatures in 2D Perovskites

Synergy of 3D and 2D Perovskites for Durable, Efficient Solar Cells and Beyond

Coupling to octahedral tilts in halide perovskite nanocrystals induces phonon-mediated attractive interactions between excitons

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