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Song, Tze-Bin

Publications and source records attributed to Song, Tze-Bin.

14 records
All sourcesNASA NTRSDOE OSTI
DOE OSTI2021

Out-of-equilibrium processes in crystallization of organic-inorganic perovskites during spin coating

Complex phenomena are prevalent during the formation of materials, which affect their processing-structure-function relationships. Thin films of methylammonium lead iodide (CH 3 NH 3 PbI 3 , MAPI) are processed by spin coating, antisolvent drop, and annealing of colloidal precursors. The structure and properties of transient and stable phases formed during the process are reported, and the mechanistic insights of the underlying transitions are revealed by combining in situ data from grazing-incidence wide-angle X-ray scattering and photoluminescence spectroscopy. Here, we report the detailed insights on the embryonic stages of organic-inorganic perovskite formation. The physicochemical evolution during the conversion proceeds in four steps: i) An instant nucleation of polydisperse MAPI nanocrystals on antisolvent drop, ii) the instantaneous partial conversion of metastable nanocrystals into orthorhombic solvent-complex by cluster coalescence, iii) the thermal decomposition (dissolution) of the stable solvent-complex into plumboiodide fragments upon evaporation of solvent from the complex and iv) the formation (recrystallization) of cubic MAPI crystals in thin film.

36 MATERIALS SCIENCE↗
DOE OSTI2018

Slow thermal equilibration in methylammonium lead iodide revealed by transient mid-infrared spectroscopy

Hybrid organic–inorganic perovskites are emerging semiconductors for cheap and efficient photovoltaics and light-emitting devices. Different from conventional inorganic semiconductors, hybrid perovskites consist of coexisting organic and inorganic sub-lattices, which present disparate atomic masses and bond strengths. The nanoscopic interpenetration of these disparate components, which lack strong electronic and vibrational coupling, presents fundamental challenges to the understanding of charge and heat dissipation. Here we study phonon population and equilibration processes in methylammonium lead iodide (MAPbI 3 ) by transiently probing the vibrational modes of the organic sub-lattice following above-bandgap optical excitation. We observe inter-sub-lattice thermal equilibration on timescales ranging from hundreds of pico seconds to a couple of nanoseconds. As supported by a two temperature model based on first-principles calculations, the slow thermal equilibration is attributable to the sequential phonon populations of the inorganic and organic sub-lattices, respectively. The observed long-lasting thermal non-equilibrium offers insights into thermal transport and heat management of the emergent hybrid material class.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗
DOE OSTI2018

Piperazine Suppresses Self-Doping in CsSnI 3 Perovskite Solar Cells

Tin-based halide perovskite materials are promising candidates for lead-free halide perovskite solar cells. However, they suffer from poor device reproducibility and limited overall power conversion efficiencies due to their tendency to become semimetallic from p-type defect states. Herein, we demonstrate an effective approach to address this issue via the addition of piperazine to the precursor solution of tin-based halide perovskite films, to suppress the undesirable p-doping of CsSnI 3 films. Piperazine is found to significantly reduce the conductivity of CsSnI 3 films, improve the film coverage, and at the same time suppress the crystallization of excess SnI 2 . Consequently, short-circuit behaviors are eliminated, with significantly improved CsSnI 3 solar-cell performance. Finally, the effects of incorporating SnCl 2 and SnF 2 into the CsSnI 3 devices were investigated in conjunction with addition of piperazine to achieve CsSnI 3 devices with a maximum power conversion efficiency of 3.83%.

14 SOLAR ENERGY↗
DOE OSTI2018

Weak Electron Phonon Coupling and Deep Level Impurity for High Thermoelectric Performance Pb 1–x Ga x Te

High ZT of 1.34 at 766 K and a record high average ZT above 1 in the temperature range of 300-864 K are attained in n-type PbTe by engineering the temperature-dependent carrier concentration and weakening electron–phonon coupling upon Ga doping. The experimental studies and first principles band structure calculations show that doping with Ga introduces a shallow level impurity contributing extrinsic carriers and imparts a deeper impurity level that ionizes at higher temperatures. This adjusts the carrier concentration closer to the temperature-dependent optimum and thus maximizes the power factor in a wide temperature range. The maximum power factor of 35 μW cm -1 K -2 is achieved for the Pb 0.98 Ga 0.02 Te compound, and is maintained over 20 μWcm-1 K-2 from 300 to 767 K. Band structure calculations and X-ray photoelectron spectroscopy corroborate the amphoteric role of Ga in PbTe as the origin of shallow and deep levels. Additionally, Ga doping weakens the electron–phonon coupling, leading to high carrier mobilities in excess of 1200 cm 2 V -1 s -1 . Enhanced point defect phonon scattering yields a reduced lattice thermal conductivity. Here, we provide a new avenue, beyond the conventional shallow level doping, for further improving the average ZT in thermoelectric materials.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2017

Multichannel Interdiffusion Driven FASnI 3 Film Formation Using Aqueous Hybrid Salt/Polymer Solutions toward Flexible Lead-Free Perovskite Solar Cells

Tin (Sn)-based perovskites are increasingly attractive because they offer lead-free alternatives in perovskite solar cells. Yet, depositing high-quality Sn-based perovskite films is still a challenge, particularly for low-temperature planar heterojunction (PHJ) devices. In this work, a “multichannel interdiffusion” protocol is demonstrated by annealing stacked layers of aqueous solution deposited formamidinium iodide (FAI)/polymer layer followed with an evaporated SnI 2 layer to create uniform FASnI 3 films. In this protocol, tiny FAI crystals, significantly inhibited by the introduced polymer, can offer multiple interdiffusion pathways for complete reaction with SnI 2 . What is more, water, rather than traditional aprotic organic solvents, is used to dissolve the precursors. The best-performing FASnI 3 PHJ solar cell assembled by this protocol exhibits a power conversion efficiency (PCE) of 3.98%. In addition, a flexible FASnI 3 -based flexible solar cell assembled on a polyethylene naphthalate–indium tin oxide flexible substrate with a PCE of 3.12% is demonstrated. This novel interdiffusion process can aid to further boost the performance of lead-free Sn-based perovskites.

14 SOLAR ENERGY↗
DOE OSTI2017

Performance Enhancement of Lead-Free Tin-Based Perovskite Solar Cells with Reducing Atmosphere-Assisted Dispersible Additive

Sn-based halide perovskite materials have attracted tremendous attention and have been employed successfully in solar cells. However, their high conductivities resulting from the unstable divalent Sn state in the structure cause poor device performance and poor reproducibility. Herein, we used excess tin iodide (SnI 2 ) in Sn-based halide perovskite solar cells (ASnI 3 , A = Cs, methylammonium and formamidinium tin iodide as the representative light absorbers), combined with a reducing atmosphere to stabilize the Sn 2+ state. Excess SnI 2 can disperse uniformly into the perovskite films and functions as a compensator as well as a suppressor of Sn 2+ vacancies thereby effectively reducing the p-type conductivity. This process significantly improved the solar-cell performances of all the ASnI3 materials on mesoporous TiO 2 . Optimized CsSnI3 devices achieved a maximum power conversion efficiency of 4.81%, which is the highest among all inorganic Pb-free perovskite solar cells to date.

14 SOLAR ENERGY↗
DOE OSTI2017

In Situ Synthesis of Highly Dispersed and Ultrafine Metal Nanoparticles from Chalcogels

We report a unique reaction type for facile synthesis of ultrafine and well-dispersed Pt nanoparticles supported on chalcogel surfaces. The nanoparticles are obtained by in-situ Pt 2+ reduction of a chalcogel network formed by the metathesis reaction between K 2 PtCl 4 and Na 4 SnS 4 . The rapid catalytic ability of the chalcogelsupported Pt nanoparticles is demonstrated in a recyclable manner by using 4-nitrophenol reduction as a probe reaction.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2016

Importance of Reducing Vapor Atmosphere in the Fabrication of Tin-Based Perovskite Solar Cells

Tin-based halide perovskite materials have been successfully employed in lead-free perovskite solar cells, but the tendency of these materials to form leakage pathways from p-type defect states, mainly Sn 4+ and Sn vacancies, causes poor device reproducibility and limits the overall power conversion efficiencies. Here, we present an effective process that involves a reducing vapor atmosphere during the preparation of tin-based halide perovskite solar cells to solve this problem, using MASnI 3 , CsSnI 3 and CsSnBr 3 as the representative absorbers. This process enables the fabrication of remarkably improved solar cells with power conversion efficiencies of 3.89%, 1.83% and 3.04% for MASnI 3 , CsSnI 3 and CsSnBr 3 respectively. The reducing vapor atmosphere process results in more than 20% reduction of Sn 4+ /Sn 2+ ratios, which leads to greatly suppressed carrier recombination, to a level comparable to their lead-based counterparts. These results mark an important step towards a deeper understanding of the intrinsic tin-based halide perovskite materials, paving the way to the realization of low-cost and lead-free Sn-based halide perovskite solar cells.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗