Article
Chemistry, Physical
Min Zhang, Lin Lei, Wei Zhao, Dingyu Yang, Xiaojia Zheng, Wen-Hua Zhang
Summary: By incorporating 4-aminobenzonitrile (ABN) molecules into the BA(2)MA(9)Pb(10)I(31) quasi-2D perovskite, the performance of X-ray detectors can be effectively improved, including enhanced charge transport properties, reduced charge recombination rate, and suppressed ion migration in the perovskite. The ABN additive enables the X-ray detector to exhibit higher sensitivity and lower detection limits at low X-ray dose rates.
JOURNAL OF PHYSICAL CHEMISTRY C
(2023)
Article
Chemistry, Multidisciplinary
Junsang Cho, Preethi S. Mathew, Jeffrey T. DuBose, Prashant Kamat
Summary: 2D lead halide perovskites with tunable bandgap and enhanced chemical stability are useful for designing optoelectronic devices. Reducing dimensionality can increase resistance to light-induced ion migration, but also decreases the efficiency of halide ion segregation and segregation rate constant, leading to a decrease in charge-carrier lifetime.
ADVANCED MATERIALS
(2021)
Article
Nanoscience & Nanotechnology
Maria Morrell, Alec Pickett, Payal Bhattacharya, Suchismita Guha, Yangchuan Xing
Summary: In this study, the optoelectronic properties of all-inorganic CsPbBr3 perovskite nanocrystals with and without RP planar faults were compared. It was found that RP-CsPbBr3 PNCs have higher exciton binding energy and longer exciton lifetimes, attributed to quantum confinement effects and spatial electron-hole separation across the RP faults. Additionally, a significant difference was observed in the up-conversion photoluminescence response of the two types of CsPbBr3 PNCs. The all-inorganic RP-CsPbBr3 PNCs were tested in light-emitting devices for the first time and showed superior performance compared to nonRP CsPbBr3 PNCs.
ACS APPLIED MATERIALS & INTERFACES
(2021)
Article
Chemistry, Physical
Ruben Vazquez-Cardenas, Jesus Rodriguez-Romero, Carlos Echeverria-Arrondo, Jesus Sanchez-Diaz, Vladimir S. Chirvony, Juan P. Martinez-Pastor, Pedro Diaz-Leyva, Juan Reyes-Gomez, Isaac Zarazua, Ivan Mora-Sero
Summary: This study reports a method for fabricating quasi-2D PVK thin films, which effectively reduces the formation of undesired higher n-phases and 3D PVKs without the use of additional reagents or fabrication steps.
CHEMISTRY OF MATERIALS
(2022)
Article
Chemistry, Physical
Debarati Ghosh, Kritiman Marjit, Goutam Ghosh, Srijon Ghosh, Amitava Patra
Summary: This study investigates the impact of bifunctional short-chain aromatic ligands on the charge transfer dynamics of 2D Ruddlesden Popper perovskites. The results reveal that the nature of ligands significantly affects the transfer rates of electrons and holes. These findings provide insights for improving the performance of next-generation optoelectronic devices.
JOURNAL OF PHYSICAL CHEMISTRY C
(2022)
Article
Chemistry, Physical
Debarati Ghosh, Kritiman Marjit, Goutam Ghosh, Srijon Ghosh, Amitava Patra
Summary: This study investigates the impact of bifunctional short-chain aromatic ligands on the charge transfer dynamics of 2D Ruddlesden Popper perovskites. Ultrafast transient absorption spectroscopy reveals evident electron transfer and hole transfer with different ligands, occurring in 900 fs and 1.9 ps, respectively. These findings provide insights for understanding the charge transfer dynamics in 2D Ruddlesden Popper perovskites, which will enhance the performance of next-generation optoelectronic devices.
JOURNAL OF PHYSICAL CHEMISTRY C
(2022)
Article
Chemistry, Multidisciplinary
Chris R. Roy, Dongxu Pan, Yining Wang, Matthew P. Hautzinger, Yuzhou Zhao, John C. Wright, Zihua Zhu, Song Jin
Summary: The research reveals that halide miscibility in RPPs decreases with perovskite layer thickness, enabling the preparation of stable lateral heterostructures through anion exchange. Different layer thicknesses of RPPs exhibit different ways of forming lateral heterojunctions, which can help optimize the performance of optoelectronic devices.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2021)
Article
Chemistry, Physical
Deyu Xin, Min Zhang, Zhenghui Fan, Ning Yang, Ruihan Yuan, Bing Cai, Ping Yu, Xiaojia Zheng, Jianguo Zhu
Summary: In this study, sensitive, stable, and portable pixel quasi-two-dimensional (2D) Ruddlesden-Popper (RP) perovskite X-ray imagers were obtained by an advanced solvent-free laminated fabrication approach. A-Site cation engineering of RP perovskites provided a solution to the trade-off between stability and detection performance, resulting in high-performance and stable X-ray imagers capable of 2D multipixel X-ray imaging.
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
(2022)
Article
Chemistry, Physical
Pushpender Yadav, Kyeongdeuk Moon, Anupam Biswas, Christopher K. Herrera, Yunlu Zhang, Scott Calabrese Barton, Richard R. Lunt, Gary J. Blanchard, Seokhyoung Kim
Summary: Researchers have successfully synthesized two-dimensional Ruddlesden-Popper halide perovskite BA2PbBr4 nanowires using chemical vapor deposition for the first time. The nanowires exhibit strong absorption and radiative emission characteristics, making them promising candidates for nanophotonic and optical communication applications.
CHEMISTRY OF MATERIALS
(2023)
Article
Chemistry, Multidisciplinary
Zachary T. Armstrong, Kristel M. Forlano, Chris R. Roy, Miriam Bohlmann Kunz, Kieran Farrell, Dongxu Pan, John C. Wright, Song Jin, Martin T. Zanni
Summary: In this study, the spatial variations of excitons and biexcitons in microcrystals of two-dimensional Ruddlesden-Popper perovskites were systematically investigated using one- and two-quantum two-dimensional white-light microscopy. It was found that the average biexciton binding energy is essentially independent of the perovskite layer thickness. Moreover, spatial variations of the exciton and biexciton energies on micron length scales within individual crystals were resolved, indicating that biexcitons are more sensitive to their environments than excitons.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Article
Chemistry, Physical
Kameron R. Hansen, Blake Romrell, C. Emma McClure, Michele Eggleston, Alex Berzansky, Jeffrey Wayjer Lin, Kelsey Garden, Luisa Whittaker-Brooks, John S. Colton
Summary: Alloying mixed ratios of elements into halide perovskite structure can tune their structural and electronic properties for various optoelectronic applications. Electroabsorption spectroscopy is used to characterize disorder and phase segregation in 2D halide perovskite alloys with mixed-metal and mixed-halide compositions. Coexistence of elemental-rich domains is observed in the alloys, while Br-Cl alloys show sharper spectral features and a more ordered structure compared to their pure counterparts. The band gap energies and exciton binding energies can be continuously tuned by adjusting the Br:Cl ratio.
JOURNAL OF PHYSICAL CHEMISTRY C
(2023)
Article
Multidisciplinary Sciences
Mohammad Rahil, Rashid Malik Ansari, Chandra Prakash, S. S. Islam, Ambesh Dixit, Shahab Ahmad
Summary: This study reports a series of new quasi-two-dimensional perovskite materials with a cyclic carbon group as the organic spacer, demonstrating excellent optoelectronic properties and stability. This research provides potential solution-processed semiconducting materials for optoelectronic devices.
SCIENTIFIC REPORTS
(2022)
Article
Chemistry, Multidisciplinary
Carlo Andrea Riccardo Perini, Esteban Rojas-Gatjens, Magdalena Ravello, Andres-Felipe Castro-Mendez, Juanita Hidalgo, Yu An, Sanggyun Kim, Barry Lai, Ruipeng Li, Carlos Silva-Acuna, Juan-Pablo Correa-Baena
Summary: This study explores the impact of bulky-cation-modified interfaces on the stability of halide perovskite solar cells. The results demonstrate the thermal instability of the bulky-cation interface layers used in state-of-the-art solar cells, which significantly affects the performance and operation of the devices. The type of cation used for surface treatment also influences the extent of these changes, with long carbon chains providing more stable interfaces.
ADVANCED MATERIALS
(2022)
Article
Energy & Fuels
Hao-Yeu Tsai, Yung-Fang Yang, Hong-Sheng Jiang, Fang-Chung Chen
Summary: 2D perovskites with nearly vertically oriented Ruddlesden-Popper (RP) phases are grown using a vapor venting space-limited crystallization method, minimizing the impact of bulky side chains of the ammonium cations. Surface passivation is used to lower surface defects and improve power conversion efficiency (PCE), resulting in a PCE higher than 16%.
Article
Chemistry, Multidisciplinary
Gill M. Biesold, Shuang Liang, Brent K. Wagner, Zhitao Kang, Zhiqun Lin
Summary: The study successfully designed a flow reactor to continuously produce high-quality two-dimensional RP perovskite nanoplatelets. The synthesis rate of the flow reactor was found to be over 8 times higher than batch synthesis, offering the potential for large-scale production.
Article
Chemistry, Physical
Shaked Dror, Sasha Khalfin, Noam Veber, Arad Lang, Yaron Kauffmann, Maria Koifman Khristosov, Reut Shechter, Boaz Pokroy, Ivano E. Castelli, Yehonadav Bekenstein
Summary: Double-perovskite structures with the composition of Cs2AgBiBr6 are suggested as emerging inorganic semiconductors for solar energy conversion. Colloidal synthesis provides a methodological basis for investigating single monolayer two-dimensional materials and using them as building blocks for a more stable bilayer structure and thicker nanoplates. The colloidal approach enables the use of high-resolution transmission electron microscopy to detect structural defects, which is essential for improving the properties of bismuth-based lead-free double perovskites and bringing them closer to real-life photovoltaic implementation.
CHEMISTRY OF MATERIALS
(2023)
Article
Chemistry, Physical
Supriya Ghosh, Bapi Pradhan, Weihua Lin, Yiyue Zhang, Luca Leoncino, Pavel Chabera, Kaibo Zheng, Eduardo Solano, Johan Hofkens, Tonu Pullerits
Summary: In the past two decades, research has focused on suppressing Auger recombination in metal-chalcogenide and perovskite nanocrystals (PNCs) for photovoltaic and light emitting device (LED) applications. A study examined dodecahedron cesium lead bromide perovskite nanocrystals (DNCs) and found that they exhibit slower Auger recombination compared to hexahedron nanocrystals (HNCs). The research demonstrates that multiexciton recombinations result in lower Auger recombination rates in DNCs than in HNCs.
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
(2023)
Article
Materials Science, Multidisciplinary
Huifang Geng, Zhuanzhuan Huang, Huaxiu Geng, Siyu Liu, Maria A. Naumova, Raffaele Salvia, Siqi Chen, Junli Wei, Lifu Zhang, Xianshao Zou, Weihua Lin, Xinyi Cai, Mingjian Yuan, Zhenpeng Hu, Xi Shen, Richeng Yu, Kaibo Zheng, Sophie E. Canton, Xuewen Fu
Summary: Recently, cesium bismuth halide perovskites have been considered as potential substitutes for cesium lead halide perovskites due to their low toxicity. However, the photophysics of cesium-bismuth halides nanocrystals (NCs) has not been fully understood due to the debated structures. This study successfully synthesized pure Cs3BiBr6 and Cs3Bi2Br9 NCs with controlled structures. The photophysical properties of the Cs3Bi2Br9 NCs were investigated, and their potential for optoelectronic applications was demonstrated.
SCIENCE CHINA-MATERIALS
(2023)
Article
Energy & Fuels
Mingli Liang, Weihua Lin, Qian Zhao, Jun Li, Lin Zhu, Brice Sarpi, Alexei Zakharov, Ivan G. Scheblykin, Tonu Pullerits, Yuran Niu, Sophie E. Canton, Kaibo Zheng
Summary: This study presents the first investigation of spatially resolved electronic structures in 2D LHP single-crystal flakes, with a focus on the contribution from the edge area. The results show a blueshift in the Pb 5d core-level peaks at the edge area compared to the interior area, which is attributed to surface restructuring induced by the release of mechanical strain.
Article
Chemistry, Physical
Albin Hedse, Alex Arash Sand Kalaee, Andreas Wacker, Tonu Pullerits
Summary: The double quantum coherence (DQC) signal in nonlinear spectroscopy provides information about many-body correlation effects that are difficult to obtain through other methods. Contrary to intuition, pulse overlap-related artifacts are not filtered out by the Fourier transform. Careful analysis of experiments is necessary to account for the pulse-overlap artifact.
JOURNAL OF CHEMICAL PHYSICS
(2023)
Article
Chemistry, Physical
Daniel Finkelstein-Shapiro, Pierre-Adrien Mante, Sinan Balci, Donatas Zigmantas, Tonu Pullerits
Summary: In polaritons, the properties of matter are modified by mixing molecular transitions with light modes, leading to hybrid light-matter states and modified exciton dynamics. This article rigorously derives non-Hermitian Hamiltonians in the response function formalism of nonlinear spectroscopy and explores spectroscopic signatures of plexcitons. The study reveals interference and Rabi splitting in linear spectroscopy and a qualitative change in the symmetry of the line shape of the nonlinear signal when crossing the exceptional point.
JOURNAL OF CHEMICAL PHYSICS
(2023)
Article
Chemistry, Physical
Xinyue Wang, Hongxiang Wang, Meixia Zhang, Tonu Pullerits, Peng Song
Summary: By studying the photoinduced electron transfer properties of the D-D-A molecule ((TPA-TT)-BODIPY-C60) in an external electric field (Fext), the excited-state properties of the molecule and the charge-transfer processes were investigated. The electronic coupling (VDA), reorganization energy (lambda), and free energy (Delta G) were calculated and simulated. It was found that exciton dissociation occurs in the Marcus inverted region and the charge-transfer rate is influenced by the changes in VDA and Delta G. The results provide a method for the design of a new type of electron transfer process with high efficiency in the D-D-A system.
JOURNAL OF PHYSICAL CHEMISTRY C
(2023)
Article
Chemistry, Physical
Maurizia Palummo, Michele Re Fiorentin, Koichi Yamashita, Ivano E. Castelli, Giacomo Giorgi
Summary: In this paper, we discuss the optoelectronic features and potential applicability of the tin-based oxynitride material InSnO2N for photo-conversion processes. Through the use of Density Functional and Many-Body Perturbation Theory, we calculate the electronic and optical properties and analyze their variations between the nonpolar and polar phases. Additionally, we determine the Spectroscopic Limited Maximum Efficiency of InSnO2N, further highlighting its relevance for solar energy conversion processes.
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
(2023)
Article
Materials Science, Multidisciplinary
Hongyu Zhang, Jijiang He, Weike Zhang, Ivano E. Castelli, Martin Saunders, Jeffrey M. Gordon, Hui Tong Chua
Summary: The generation of boron nitride nano-onions (BNNOs) from hexagonal-BN crystallite powder via a one-pot, non-toxic, catalyst-free, rapid hightemperature lamp ablation procedure is reported. Characterization procedures revealed the shapes, sizes, and composition of the nanoparticles, and a formation mechanism for BNNOs is proposed. Temperature measurements also showed the viable temperature range for BNNO generation.
Article
Chemistry, Multidisciplinary
Sophie E. E. Canton, Mykola Biednov, Matyas Papai, Frederico A. A. Lima, Tae-Kyu Choi, Florian Otte, Yifeng Jiang, Paul Frankenberger, Martin Knoll, Peter Zalden, Wojciech Gawelda, Ahibur Rahaman, Klaus B. B. Moller, Christopher Milne, David J. J. Gosztola, Kaibo Zheng, Marius Retegan, Dmitry Khakhulin
Summary: Ultrafast optical absorption spectroscopy and X-ray emission spectroscopy were used to track the photoinduced spin-state switching of the prototypical complex [Co(terpy)(2)](2+) in solution phase. The study reveals that the complex undergoes ultrafast Jahn-Teller photoswitching between two different spin multiplicities on the femtosecond timescale.
Article
Electrochemistry
Benjamin H. H. Sjolin, Peter B. B. Jorgensen, Andrea Fedrigucci, Tejs Vegge, Arghya Bhowmik, Ivano E. E. Castelli
Summary: We developed a multi-target multi-fidelity workflow to search for stable high-performance solid state electrolytes for all-solid state batteries. The workflow utilizes thermodynamic and kinetic properties calculations, including phase and electrochemical stability, semiconducting behavior, and ionic diffusivity. By using a surrogate model to predict the transition state structure, the calculation of kinetic properties is greatly accelerated without significant loss of accuracy.
BATTERIES & SUPERCAPS
(2023)
Editorial Material
Electrochemistry
Benjamin H. H. Sjolin, Peter B. B. Jorgensen, Andrea Fedrigucci, Tejs Vegge, Arghya Bhowmik, Ivano E. E. Castelli
Summary: We developed and implemented a multi-target multi-fidelity workflow to explore the chemical space of antiperovskite materials as solid state electrolytes for all-solid state batteries. The workflow includes calculations of thermodynamic and kinetic properties, and uses a surrogate model to predict the transition state structure during ionic diffusion, significantly reducing calculation cost. This approach identified 14 materials that agree with experimental results as promising solid state electrolytes.
BATTERIES & SUPERCAPS
(2023)
Article
Chemistry, Physical
Yanmei He, Siping Liu, Zehan Yao, Qian Zhao, Pavel Chabera, Kaibo Zheng, Bin Yang, Tonu Pullerits, Junsheng Chen
Summary: Low-dimensional perovskite-inspired materials with self-trapped exciton (STE) emission have sparked cutting-edge research in optoelectronics. However, there has been little focus on the intrinsic dynamics of broad emission based on STE in these materials. In this study, through femtosecond transient absorption spectroscopy, we directly observed the ultrafast process of STE formation in Cs2ZrCl6 nanocrystals, and obtained the dynamic rules of ultrafast STE formation. The formed STEs relax to an intermediate STE state with a lifetime of approximately 180 ps before reaching the emissive STE state with a lifetime of about 15 μs. Our work provides a comprehensive and precise dynamic picture of STE emission in low-dimensional metal halides and sheds light on expanding their potential applications.
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
(2023)
Article
Chemistry, Physical
Milena Martins, Dominik Haering, Justin G. Connell, Hao Wan, Katrine L. Svane, Bostjan Genorio, Pedro Farinazzo Bergamo Dias Martins, Pietro P. Lopes, Brian Gould, Filippo Maglia, Roland Jung, Vojislav Stamenkovic, Ivano E. Castelli, Nenad M. Markovic, Jan Rossmeisl, Dusan Strmcnik
Summary: Compared to aqueous electrolytes, the understanding of chemical and electrochemical processes in non-aqueous electrolytes, particularly in Li-ion battery electrolytes, is limited. In this study, a comprehensive investigation of the electrochemistry of ethylene carbonate (EC) and its interaction with trace amounts of water and HF is conducted across various electrode materials. The electrocatalytic nature of EC, HF, and water electroreductions at different interfaces is revealed, and the catalytic role of water in EC electroreduction is also discovered. The composition of the solid-electrolyte interphase (SEI) is found to depend primarily on the balance between the (electro)chemistry of EC, water, and HF.
Article
Nanoscience & Nanotechnology
Jie Meng, Qian Zhao, Weihua Lin, Tonu Pullerits, Kaibo Zheng
Summary: This study demonstrates the biexciton dynamics of core/shell quantum dots with submonolayer shell coverage. The results show that these quantum dots have a prolonged Auger lifetime. However, unlike conventional quantum dots, the dependence of the Auger recombination time on quantum dot size features two constant stages. This study provides a reference for the application of core-shell quantum dots in optoelectronic devices.
ADVANCED ELECTRONIC MATERIALS
(2023)
