Browse
Submit Data
Databases
API
Help

Dataset Information

26 Views

0 Connections

0 Citations

0 Reanalyses

0 Downloads

Omics score: 0

Accelerated Hot-Carrier Cooling in MAPbI₃ Perovskite by Pressure-Induced Lattice Compression.

ABSTRACT: Hot-carrier cooling (HCC) in metal halide perovskites above the Mott transition is significantly slower than in conventional semiconductors. This effect is commonly attributed to a hot-phonon bottleneck, but the influence of the lattice properties on the HCC behavior is poorly understood. Using pressure-dependent transient absorption spectroscopy, we find that at an excitation density below the Mott transition, pressure does not affect the HCC. On the contrary, above the Mott transition, HCC in methylammonium lead iodide is around 2-3 times faster at 0.3 GPa than at ambient pressure. Our electron-phonon coupling calculations reveal ∼2-fold stronger electron-phonon coupling for the inorganic cage mode at 0.3 GPa. However, our experiments reveal that pressure promotes faster HCC only above the Mott transition. Altogether, these findings suggest a change in the nature of excited carriers above the Mott transition threshold, providing insights into the electronic behavior of devices operating at such high charge-carrier densities.

SUBMITTER: Muscarella LA

PROVIDER: S-EPMC8154846 | biostudies-literature |

REPOSITORIES: biostudies-literature

ACCESS DATA

Json Xml

Similar Datasets

Confinement and Exciton Binding Energy Effects on Hot Carrier Cooling in Lead Halide Perovskite Nanomaterials.

Project description:The relaxation of the above-gap ("hot") carriers in lead halide perovskites (LHPs) is important for applications in photovoltaics and offers insights into carrier-carrier and carrier-phonon interactions. However, the role of quantum confinement in the hot carrier dynamics of nanosystems is still disputed. Here, we devise a single approach, ultrafast pump-push-probe spectroscopy, to study carrier cooling in six different size-controlled LHP nanomaterials. In cuboidal nanocrystals, we observe only a weak size effect on the cooling dynamics. In contrast, two-dimensional systems show suppression of the hot phonon bottleneck effect common in bulk perovskites. The proposed kinetic model describes the intrinsic and density-dependent cooling times accurately in all studied perovskite systems using only carrier-carrier, carrier-phonon, and excitonic coupling constants. This highlights the impact of exciton formation on carrier cooling and promotes dimensional confinement as a tool for engineering carrier-phonon and carrier-carrier interactions in LHP optoelectronic materials.

| S-EPMC10100565 | biostudies-literature

Hot carrier cooling mechanisms in halide perovskites.

Project description:Halide perovskites exhibit unique slow hot-carrier cooling properties capable of unlocking disruptive perovskite photon-electron conversion technologies (e.g., high-efficiency hot-carrier photovoltaics, photo-catalysis, and photodetectors). Presently, the origins and mechanisms of this retardation remain highly contentious (e.g., large polarons, hot-phonon bottleneck, acoustical-optical phonon upconversion etc.). Here, we investigate the fluence-dependent hot-carrier dynamics in methylammonium lead triiodide using transient absorption spectroscopy, and correlate with theoretical modeling and first-principles calculations. At moderate carrier concentrations (around 1018 cm-3), carrier cooling is mediated by polar Fröhlich electron-phonon interactions through zone-center delayed longitudinal optical phonon emissions (i.e., with phonon lifetime τ LO around 0.6 ± 0.1 ps) induced by the hot-phonon bottleneck. The hot-phonon effect arises from the suppression of the Klemens relaxation pathway essential for longitudinal optical phonon decay. At high carrier concentrations (around 1019 cm-3), Auger heating further reduces the cooling rates. Our study unravels the intricate interplay between the hot-phonon bottleneck and Auger heating effects on carrier cooling, which will resolve the existing controversy.

| S-EPMC5670184 | biostudies-literature

MAPbI3 microneedle-arrays for perovskite photovoltaic application.

Project description:Methyl-ammonium lead iodide perovskite (MAPbI3) was synthesized in the form of micro-needles via a hydrothermal route at a low temperature of 100 °C in a two-step procedure for the first time. The results exhibit that the amount of the surfactant is crucial for the synthesis of the MAPbI3 nanostructures with well-controlled morphologies. In contrast to bulk MAPbI3, the one-dimensional (1-D) micro-needle perovskite with a diameter of 200 nm showed an improved hole injection from the perovskite to the hole transporting layer (HTL), providing a unique platform at the perovskite/HTL interface. The best performing device employing MAPbI3 perovskite micro-needles yielded stable and hysteresis-free devices with a best power conversion efficiency of (PCEbest) of 17.98%. The current findings highlight the potential of perovskite micro-needles as novel absorber systems and lay the basis for future commercialization.

| S-EPMC9473284 | biostudies-literature

Phase transformations and vibrational properties of hybrid organic-inorganic perovskite MAPbI3 bulk at high pressure.

Project description:The structural stability and internal properties of hybrid organic-inorganic perovskites (HOIPs) have been widely investigated over the past few years. The interplay between organic cations and inorganic framework is one of the prominent features. Herein we report the evolution of Raman modes under pressure in the hybrid organic-inorganic perovskite MAPbI[Formula: see text] by combining the experimental approach with the first-principles calculations. A bulk MAPbI[Formula: see text] single crystal was synthesized via inverse temperature crystallization (ITC) technique and characterized by Raman spectroscopy, while the diamond anvil cells (DACs) was employed to compress the sample. The classification and behaviours of their Raman modes are presented. At ambient pressure, the vibrations of inorganic PbI[Formula: see text] octahedra and organic MA dominate at a low-frequency range (60-760 cm[Formula: see text]) and a fingerprint range (900-1500 cm[Formula: see text]), respectively. The applied pressure exhibits two significant changes in the Raman spectrum and indicates of phase transition. The results obtained from both experiment and calculations of the second phase at 3.26 GPa reveal that the internal vibration intensity of the PbI[Formula: see text] octahedra (< 110 cm[Formula: see text]) reduces as absences of MA libration (150-270 cm[Formula: see text]) and internal vibration of MA (450-750 cm[Formula: see text]). Furthermore, the hydrogen interactions around 1300 cm[Formula: see text] remain strong high pressure up to 5.34 GPa.

| S-EPMC10558557 | biostudies-literature

Hot Carrier Cooling and Trapping in Atomically Thin WS2 Probed by Three-Pulse Femtosecond Spectroscopy.

Project description:Transition metal dichalcogenides (TMDs) have shown outstanding semiconducting properties which make them promising materials for next-generation optoelectronic and electronic devices. These properties are imparted by fundamental carrier-carrier and carrier-phonon interactions that are foundational to hot carrier cooling. Recent transient absorption studies have reported ultrafast time scales for carrier cooling in TMDs that can be slowed at high excitation densities via a hot-phonon bottleneck (HPB) and discussed these findings in the light of optoelectronic applications. However, quantitative descriptions of the HPB in TMDs, including details of the electron-lattice coupling and how cooling is affected by the redistribution of energy between carriers, are still lacking. Here, we use femtosecond pump-push-probe spectroscopy as a single approach to systematically characterize the scattering of hot carriers with optical phonons, cold carriers, and defects in a benchmark TMD monolayer of polycrystalline WS2. By controlling the interband pump and intraband push excitations, we observe, in real-time (i) an extremely rapid "intrinsic" cooling rate of ∼18 ± 2.7 eV/ps, which can be slowed with increasing hot carrier density, (ii) the deprecation of this HPB at elevated cold carrier densities, exposing a previously undisclosed role of the carrier-carrier interactions in mediating cooling, and (iii) the interception of high energy hot carriers on the subpicosecond time scale by lattice defects, which may account for the lower photoluminescence yield of TMDs when excited above band gap.

| S-EPMC10100566 | biostudies-literature

Dual Passivation of Perovskite and SnO2 for High-Efficiency MAPbI3 Perovskite Solar Cells.

Project description:So far, most techniques for modifying perovskite solar cells (PSCs) focus on either the perovskite or electron transport layer (ETL). For the sake of comprehensively improving device performance, a dual-functional method of simultaneously passivating trap defects in both the perovskite and ETL films is proposed that utilizes guidable transfer of Eu3+ in SnO2 to perovskite. Europium ions are distributed throughout the SnO2 film during the formation process of SnO2, and they can diffuse directionally through the SnO2/perovskite interface into the perovskite, while most of the europium ions remain at the interface. Under the synergistic effect of distributed Eu3+ in the SnO2 and aggregated Eu3+ at the interface, the electron mobilities of ETLs are evidently improved. Meanwhile, diffused Eu3+ ions passivate the perovskite to reduce trap densities at the grain boundaries, which can dramatically elevate the open-circuit voltage (V oc) of PSCs. Finally, the mainly PSCs coated on SnO2:Eu3+ ETL achieve a power conversion efficiency of 20.14%. Moreover, an unsealed device degrades by only 13% after exposure to ambient atmosphere for 84 days.

| S-EPMC7927604 | biostudies-literature

Slow Cooling of Hot Polarons in Halide Perovskite Solar Cells.

Project description:Halide perovskites show unusual thermalization kinetics for above-bandgap photoexcitation. We explain this as a consequence of excess energy being deposited into discrete large polaron states. The crossover between low-fluence and high-fluence "phonon bottleneck" cooling is due to a Mott transition where the polarons overlap (n ≥ 1018 cm-3) and the phonon subpopulations are shared. We calculate the initial rate of cooling (thermalization) from the scattering time in the Fröhlich polaron model to be 78 meV ps-1 for CH3NH3PbI3. This rapid initial thermalization involves heat transfer into optical phonon modes coupled by a polar dielectric interaction. Further cooling to equilibrium over hundreds of picoseconds is limited by the ultralow thermal conductivity of the perovskite lattice.

| S-EPMC5727468 | biostudies-literature

Quantifying Charge Carrier Recombination Losses in MAPbI3/C60 and MAPbI3/Spiro-OMeTAD with and without Bias Illumination.

Project description:To increase the open-circuit voltage in perovskite-based solar cells, recombination processes at the interface with transport layers (TLs) should be identified and reduced. We investigated the charge carrier dynamics in bilayers of methylammonium lead iodide (MAPbI3) with C60 or Spiro-OMeTAD using time-resolved microwave conductance (TRMC) measurements with and without bias illumination (BI). By modeling the results, we quantified recombination losses in bare MAPbI3 and extraction into the TLs. Only under BI did we find that the density of deep traps increases in bare MAPbI3, substantially enhancing trap-mediated losses. This reversible process is prevented in a bilayer with C60 but not with Spiro-OMeTAD. While under BI extraction rates reduce significantly in both bilayers, only in MAPbI3/Spiro-OMeTAD does interfacial recombination also increases, substantially reducing the quasi Fermi level splitting. This work demonstrates the impact of BI on charge dynamics and shows that adjusting the Fermi level of TLs is imperative to reduce interfacial recombination losses.

| S-EPMC9393883 | biostudies-literature

Ultrafast Intraband Spectroscopy of Hot-Carrier Cooling in Lead-Halide Perovskites.

Project description:The rapid relaxation of above-band-gap "hot" carriers (HCs) imposes the key efficiency limit in lead-halide perovskite (LHP) solar cells. Recent studies have indicated that HC cooling in these systems may be sensitive to materials composition, as well as the energy and density of excited states. However, the key parameters underpinning the cooling mechanism are currently under debate. Here we use a sequence of ultrafast optical pulses (visible pump-infrared push-infrared probe) to directly compare the intraband cooling dynamics in five common LHPs: FAPbI3, FAPbBr3, MAPbI3, MAPbBr3, and CsPbBr3. We observe ?100-900 fs cooling times, with slower cooling at higher HC densities. This effect is strongest in the all-inorganic Cs-based system, compared to the hybrid analogues with organic cations. These observations, together with band structure calculations, allow us to quantify the origin of the "hot-phonon bottleneck" in LHPs and assert the thermodynamic contribution of a symmetry-breaking organic cation toward rapid HC cooling.

| S-EPMC6231231 | biostudies-literature

Fast and Accurate Artificial Neural Network Potential Model for MAPbI3 Perovskite Materials.

Project description:Hybrid organic-inorganic perovskite materials are promising materials for photovoltaic and optoelectronic applications. Nevertheless, the construction of a computationally efficient potential model for atomistic simulations of perovskite with high fidelity to ab initio calculations is not a trivial task given the chemically complex nature of perovskite in terms of its chemical components and interatomic interactions. In the present study, we demonstrate that artificial neural network (ANN) models can be employed for efficient and accurate potential energy evaluation of MAPbI3 perovskite materials. The ANN models were trained using training sets composed of thousands of atomic images of tetragonal MAPbI3 crystals, with their respective energies and atomic forces obtained from ab initio calculations. The trained ANN models were validated by predicting the lattice parameters and energies/atomic forces of cubic MAPbI3 perovskite and had excellent agreement with ab initio calculations. The phonon modes could also be extracted using the trained ANN model with good agreement with ab initio calculations, provided that the atomic forces were incorporated into the training processes. Finally, we demonstrate that for a given system size, the trained ANN model offers 104 to 105 faster time consumption per energy evaluation relative to ab initio calculations using Vienna Ab initio Simulation Package, demonstrating the potential of the ANN model for exhaustively sampling the configuration spaces of chemically complex materials for predictions of thermodynamic properties and phase stabilities.

| S-EPMC6648651 | biostudies-literature