Article
Chemistry, Multidisciplinary
Shunhong Dong, Zhi-Yi Hu, Ping Wei, Jingru Han, Zhao Wang, Jing Liu, Bao-Lian Su, Dongyuan Zhao, Yong Liu
Summary: This study reports the engineering of surface structure to tune the optoelectronic properties of halide perovskites. Uniform all-inorganic CsPbBr3 cubic/tetrahedral single-crystals with precise control of (100) and (111) surface anisotropy were designed and fabricated. The (100) surface engineering enables a lowest surface bandgap energy and high-rate carrier mobility, while the (111) surface enhances surface-defects-catalyzed reactions.
ADVANCED MATERIALS
(2022)
Article
Chemistry, Multidisciplinary
Dong Zhang, Takuya Okamoto, Vasudevanpillai Biju
Summary: This study demonstrates the controlled growth of high-quality FA/MAPbBr(3) single microcrystals with desired properties through thermodynamic and kinetic methods using N-cyclohexyl-2-pyrrolidone (CHP) concentration. The size, density, and photoluminescence (PL) properties of the crystals were controlled by varying the CHP concentration and temperature. The single crystals obtained at 190℃ and 20% CHP concentration exhibited the highest PL intensity and the longest PL lifetimes.
Article
Chemistry, Physical
Sarvani Jowhar Khanam, Nishi Parikh, Soumitra Satapathi, Abul Kalam, Murali Banavoth, Pankaj Yadav
Summary: This study improves the optoelectronic properties of methylammonium lead tribromide single crystals by modifying their growth conditions. The electrical response of the modified crystals is systematically investigated, and it is found that the (R)-3-aminopiperidine dihydrochloride (API) additive improves the charge collection efficiency and reduces recombination.
ACS APPLIED ENERGY MATERIALS
(2022)
Article
Chemistry, Physical
Artem Musiienko, Jakub Cizek, Hassan Elhadidy, Petr Praus, Kate Higgins, Bogdan Dryzhakov, Andrii Kanak, Franck Sureau, Jindrich Pipek, Eduard Belas, Marian Betusiak, Mykola Brynza, Eric Lukosi, Bin Hu, Mahshid Ahmadi
Summary: The study found that both hybrid and all-inorganic MHPs exhibit low concentrations of vacancies regardless of their synthesis method, with crystals grown from solution prone to solvent inclusion during synthesis.
CHEMISTRY OF MATERIALS
(2022)
Article
Chemistry, Physical
Yanyan Li, Zhicong Zhou, Fu Kit Sheong, Zengshan Xing, Kam Sing Wong, Herman H. Y. Sung, Ian D. Williams, Jonathan E. Halpert
Summary: In this study, a series of alkali copper(I) iodide (ACuI)-based organic-inorganic hybrid materials with different structures and emission peaks were synthesized by adjusting the alkali atoms and organic molecules. These compounds showed strong photoluminescence (PL) with emission peaks ranging from 530-660 nm, and the highest PL quantum yield (PLQY) of 91% was achieved for KCuI2(C4H8OS)2. The materials were used to fabricate green, yellow, and red light-emitting diodes (LEDs), and a white LED with a high color rendering index of 93 was demonstrated using a mixture of Cs3Cu2I5 and Rb2Cu2I4(C4H8OS)3 powders. This work provides a new strategy for developing hybrid copper halides with tunable structures and high performance, and suggests that these compounds could be promising candidates for emission applications.
CHEMISTRY OF MATERIALS
(2023)
Article
Chemistry, Multidisciplinary
Zexu Xue, Yingrui Wei, Hao Li, Jiali Peng, Fang Yao, Yong Liu, Sheng Wang, Qianghui Zhou, Qianqian Lin, Zhiping Wang
Summary: An additive-enhanced crystallization method is proposed to increase the solubility of cesium bromide in dimethyl sulfoxide (DMSO) and prevent the formation of impurity phases. The additives react with DMSO to generate glyoxylic acid (GLA), which forms stable PbBr2-DMSO-GLA complexes and improves the crystallinity, uniformity, and carrier lifetimes of the single crystals. X-ray detectors using the additive-enhanced crystals exhibit an ultra-high sensitivity.
Article
Multidisciplinary Sciences
Cheng Liu, Xiuhong Sun, Yi Yang, Olga A. Syzgantseva, Maria A. Syzgantseva, Bin Ding, Naoyuki Shibayama, Hiroyuki Kanda, Farzaneh Fadaei Tirani, Rosario Scopelliti, Shunlin Zhang, Keith G. Brooks, Songyuan Dai, Guanglei Cui, Michael D. Irwin, Zhipeng Shao, Yong Ding, Zhaofu Fei, Paul J. Dyson, Mohammad Khaja Nazeeruddin
Summary: Using a thermally stable ionic liquid [PPN][TFSI], the high-temperature solid-state reaction between Cs4PbI6 and DMAPbI3 can be retarded, enabling the preparation of high-quality and large-area CsPbI3 films. [PPN][TFSI] increases the formation energy of superficial vacancies and prevents phase degradation of CsPbI3. The resulting PSCs achieved a power conversion efficiency of 20.64% (certified 19.69%) with long-term operational stability over 1000 hours. A record efficiency of 16.89% for an all-inorganic perovskite solar module was achieved, with an active area of 28.17 cm2.
Article
Chemistry, Multidisciplinary
Chao Ge, Xiaoxin Zheng, Qing Guo, Yang Liu, Xutang Tao
Summary: Single crystals are the most perfect and stable form of material, representing the upper limit of performance when used in various applications. However, producing crystals with desired shape is still challenging for many emerging low-dimensional and molecular materials. This study presents a universal and high-yield method to grow single crystals with controlled dimensions, which can be directly integrated into devices. By using a polymeric flux and compressed growth space, size-controllable single crystalline flakes can be produced in large quantities. This scalable growth method shows promise for the large-scale integration of micro-single-crystals, as demonstrated by the construction of a 5 in. field-effect transistor array.
ADVANCED MATERIALS
(2023)
Article
Optics
Jinghui Li, Peipei Du, Qingxun Guo, Liang Sun, Zixi Shen, Jiaxing Zhu, Chong Dong, Liang Wang, Xin Zhang, Luying Li, Chaoqun Yang, Jie Pan, Zhengzheng Liu, Bing Xia, Zewen Xiao, Juan Du, Boxiang Song, Jiajun Luo, Jiang Tang
Summary: All-thermal evaporation enables the fabrication of perovskite LEDs and active-matrix displays with high efficiency and resolution. A tri-source co-evaporation strategy with a multifunctional Lewis-base additive is developed to improve the quality of perovskite films. Green PeLEDs with a peak external quantum efficiency of 16.4% and active-matrix PeLED displays with high-definition images and videos are achieved.
Article
Chemistry, Multidisciplinary
Marieh B. Al-Handawi, Ghada Dushaq, Patrick Commins, Durga Prasad Karothu, Mahmoud Rasras, Luca Catalano, Pance Naumov
Summary: This study reports the autonomous self-healing capability of centimeter-size single crystals of methylammonium lead(II) iodide (MAPbI(3)) at ambient temperature, with remarkable recovery of their optoelectronic properties. This discovery overcomes the challenges of chemical stability and mechanical robustness, providing a new strategy for the development of durable and stable optoelectronic devices based on single crystals of hybrid perovskites.
ADVANCED MATERIALS
(2022)
Article
Materials Science, Ceramics
J. Bartak, D. Valdes, S. Martinkova, J. Shanelova, P. Kostal
Summary: The study investigates crystal growth in undercooled melts in the GeSe2-rich region of the (GeSe2)x(Sb2Se3)1-x system. Two crystalline phases (Sb2Se3 and GeSe2) were directly observed using infrared microscopy. The growth rates of GeSe2 crystals depend only on temperature and are independent of the system's composition. The competitive growth of Sb2Se3 and GeSe2 is explained using existing crystal growth theories. New viscosity data for the (GeSe2)0.9(Sb2Se3)0.1 composition were obtained to complement the viscosity behavior in the (GeSe2)x(Sb2Se3)1-x system. The combination of growth and viscosity data provides valuable insights into crystal growth and allows for the prediction of crystal growth rates over a wide temperature range in the (GeSe2)x(Sb2Se3)1-x system.
JOURNAL OF NON-CRYSTALLINE SOLIDS
(2023)
Article
Chemistry, Inorganic & Nuclear
Adrian T. Hines, Gregory Morrison, Brandon J. Yarbrough, Natalia B. Shustova, Luiz G. Jacobsohn, Hans-Conrad zur Loye
Summary: Single crystals of rare earth borates, Na3Ln(BO3)2 and K3Ln(BO3)2, were synthesized using a boric acid/hydroxide melt. Na3Ln(BO3)2 crystallized in the monoclinic system with space group P21/n, while K3Ln(BO3)2 crystallized in the orthorhombic system with space group Pnma. The luminescence of these borates under ultraviolet and X-ray excitations was investigated for the first time, and K3Tb(BO3)2 showed the highest radioluminescence intensity.
SOLID STATE SCIENCES
(2023)
Article
Chemistry, Multidisciplinary
Yuan Chen, Haibo Zeng, Peipei Ma, Gaoyuan Chen, Jie Jian, Xing Sun, Xiaoming Li, Haiyan Wang, Wanjian Yin, Quanxi Jia, Guifu Zou
Summary: The study successfully grew freestanding single crystal CsPbBr3 SCHPFs with thickness less than 100 nm and lateral size close to centimeter for the first time. A new growth kinetics model was proposed to address the surface energy and temperature effect on the growth rate, with experimental results and DFT calculations demonstrating the critical role of surfactants in achieving anisotropic growth.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2021)
Article
Chemistry, Multidisciplinary
Nikita I. Selivanov, Anna Yu. Samsonova, Ruslan Kevorkyants, Irina V. Krauklis, Yuri V. Chizhov, Boris V. Stroganov, Marios E. Triantafyllou-Rundell, Detlef W. Bahnemann, Constantinos C. Stoumpos, Alexei V. Emeline, Yury V. Kapitonov
Summary: The study introduces a new family of hybrid organic-inorganic 2D lead halides, reporting the first example of the hybrid organic-inorganic post-perovskite 3-cyanopyridinium lead tribromide (3cp)PbBr3. The new material exhibits unique structural connectivity and optical properties that show significant anisotropy within the inorganic layer plane.
ADVANCED FUNCTIONAL MATERIALS
(2021)
Article
Chemistry, Inorganic & Nuclear
Xing Liu, Hui Li, Ting Zhang, Lei Zhang, Ming Li, Rongxing He
Summary: A zero-dimensional (0D) (H5O2)(C4H14N2S2)(2)BiCl8: Sb3+ single crystal is obtained by the cooling crystallization method, which shows reversible photoluminescence (PL) upon H5O2+Cl- removal and insertion. The significant distortion of [SbCl6](3-) octahedron induced by guest (H5O2+Cl-) removal at the ground state, especially at the excited state, is responsible for the disparate PL performance. Moreover, (C4H14N2S2)(2)BiCl7: Sb3+ exhibits a fast response (<3 s) to dilute hydrochloric acid with naked-eye perceivable PL color changes, making it a potential sensing material for hydrochloric acid.
INORGANIC CHEMISTRY
(2023)
Article
Chemistry, Multidisciplinary
Yihui He, Ido Hadar, Michael C. De Siena, Vladislav V. Klepov, Lei Pan, Duck Young Chung, Mercouri G. Kanatzidis
Summary: This work reports the use of spectroscopic-grade CsPbBr3 detectors for hard X-ray detection, which can register the energies of individual X-ray interactions with superior resolution. The sensitivity of the detectors can be enhanced by controlling the X-ray energies, flux, and voltage, and they have great potential for X-ray photon-counting systems.
ADVANCED FUNCTIONAL MATERIALS
(2022)
Article
Chemistry, Multidisciplinary
Anna A. Berseneva, Vladislav V. Klepov, Koushik Pal, Kelly Seeley, Daniel Koury, Joseph Schaeperkoetter, Joshua T. Wright, Scott T. Misture, Mercouri G. Kanatzidis, Chris Wolverton, Artem Gelis, Hans-Conrad zur Loye
Summary: The behavior of 5f electrons in soft ligand environments makes actinides, and especially transuranium chalcogenides, interesting materials for fundamental studies. However, synthesizing actinide chalcogenides using non-metallic reagents is challenging due to the affinity of actinides for oxygen. This study successfully synthesized transuranium sulfides NaCuNpS3 and NaCuUS3 using the boron chalcogen mixture method, and investigated their structures, hydration processes, and electronic properties.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2022)
Article
Chemistry, Inorganic & Nuclear
Ceren Kutahyali Aslani, Vladislav V. Klepov, Hans-Conrad zur Loye
Summary: Chemical systems with non-centrosymmetric anions containing electron lone pairs promote the formation of non-centrosymmetric phases. By investigating crystallization in iodate-sulfate systems, it was found that the reaction is highly sensitive to the sulfate concentration.
SOLID STATE SCIENCES
(2022)
Article
Chemistry, Physical
Ping Fu, Michael A. Quintero, Claire Welton, Xiaotong Li, Bruno Cucco, Michael C. De Siena, Jacky Even, George Volonakis, Mikael Kepenekian, Runze Liu, Craig C. Laing, Vladislav Klepov, Yukun Liu, Vinayak P. Dravid, G. N. Manjunatha Reddy, Can Li, Mercouri G. Kanatzidis
Summary: In this paper, two-dimensional lead bromide perovskites and one-dimensional compounds based on short aromatic diammonium cations are reported, and their white-light emission is studied. The results indicate that the distortion of the Pb octahedra is influenced by the stereochemistry of the cations and their interactions with the perovskite layers.
CHEMISTRY OF MATERIALS
(2022)
Article
Computer Science, Interdisciplinary Applications
Lei Pan, Yihui He, Vladislav V. Klepov, Michael C. De Siena, Mercouri G. Kanatzidis
Summary: This study reports the performance of CsPbBr3 single-crystal semiconductor detectors capable of resolving the energies of single X-ray photons. By fine-tuning the working conditions, the detector demonstrates a high count rate for X-ray photon counting and exhibits low polarization over a typical timescale of multiple clinical X-ray scans. This demonstrates the potential of CsPbBr3 detectors for X-ray photon-counting applications in medical and industrial diagnostics, with lower cost compared to current state-of-the-art detectors.
IEEE TRANSACTIONS ON MEDICAL IMAGING
(2022)
Article
Materials Science, Multidisciplinary
Lei Pan, Indra Raj Pandey, Antonino Miceli, Vladislav V. Klepov, Duck Young Chung, Mercouri G. Kanatzidis
Summary: A perovskite CsPbBr3 single-crystal detector capable of operating at high X-ray fluxes is reported. The detector shows good performance in terms of gamma-ray energy resolution, dark current, photocurrent linearity, and reproducibility at different X-ray energy levels. It is anticipated that CsPbBr3 detectors will have wide application in high-flux X-ray detection.
ADVANCED OPTICAL MATERIALS
(2023)
Article
Nanoscience & Nanotechnology
Vladislav V. Klepov, Michael C. De Siena, Indra R. Pandey, Lei Pan, Khasim Saheb Bayikadi, Serkan Butun, Duck Young Chung, Mercouri G. Kanatzidis
Summary: The practical application of laser scribing in electrode patterning on perovskite CsPbBr3 detectors is explored. The experimental results show that laser scribing can achieve high-quality patterns with minimal damage to the crystal and low interpixel cross-talk. The energy resolution in gamma-ray spectra is up to 6.1% at 122 keV.
ACS APPLIED MATERIALS & INTERFACES
(2023)
Article
Chemistry, Multidisciplinary
Lei Pan, Zhifu Liu, Claire Welton, Vladislav V. Klepov, John A. Peters, Michael C. De Siena, Alessandro Benadia, Indra Pandey, Antonino Miceli, Duck Young Chung, G. N. Manjunatha Reddy, Bruce W. Wessels, Mercouri G. Kanatzidis
Summary: A solution-grown all-inorganic perovskite CsPbBr3 single-crystal semiconductor detector capable of operating under extremely intense X-rays is reported. The detector exhibits high sensitivity, low detection limit, excellent photocurrent linearity, and reproducibility.
ADVANCED MATERIALS
(2023)
Article
Physics, Applied
Zhifu Liu, John A. Peters, Lei Pan, Vladislav Klepov, Michael De Siena, Alessandro Benadia, Duck Young Chung, Mercouri G. Kanatzidis, Bruce W. Wessels
Summary: Recently, the focus has been on developing x-ray and gamma ray detectors with large volume and high energy resolution that can operate at room temperature. To achieve this, it is necessary to increase the carrier mobility-lifetime product and minimize the concentration of electronic trap states. Thorough measurements and comparisons were conducted on CsPbBr3 halide perovskite single crystals to understand their origins and trap parameters. The results showed that crystals with trap concentrations below 1 x 10(14) cm(-3) exhibited appreciable detector performance.
APPLIED PHYSICS LETTERS
(2023)
Article
Chemistry, Physical
Eugenia S. Vasileiadou, Imra S. Tajuddin, Michael C. De Siena, Vladislav V. Klepov, Mikael Kepenekian, George Volonakis, Jacky Even, Lukasz Wojtas, Ioannis Spanopoulos, Xiuquan Zhou, Abishek K. Iyer, Julie L. Fenton, William R. Dichtel, Mercouri G. Kanatzidis
Summary: A new family of 3D cubic hybrid metal halides has been reported, which exhibits luminescent properties. The materials are synthesized through a one-step solvothermal reaction and an in situ N-alkylation process. The structure of the materials consists of unprecedented [Pb11X31]^9- one-dimensional chains embedded with [T-Et-6]^3+ cations, resulting in weak broad emission centered at 660nm observed at 78K.
CHEMISTRY OF MATERIALS
(2023)
Article
Chemistry, Multidisciplinary
Sergei A. Novikov, James Casey, Hope A. Long, Joshua C. Bledsoe, Jason J. Locklin, Vladislav V. Klepov
Summary: The physical properties of copper chalcogenides are influenced by the covalent nature of Cu-S bonds. The oxidation states of Cu and S/Se in these compounds are still debated. Recent studies on covellite CuS showed strong hybridization and almost equal distribution of electron deficiency on Cu1+ and S2- ions. This article reports the synthesis of a new compound NaCu4S3 and its metallic properties and magnetic behavior.
CRYSTAL GROWTH & DESIGN
(2023)
Article
Materials Science, Multidisciplinary
Joshua Bledsoe, Grant Crane, Jessica Drewke, James Casey, Vladislav Klepov, Jason Locklin
Summary: A nicotinic acid concentration of 2 w/w% was found to be the optimal concentration for achieving the best nucleation performance in a poly(hydroxy-butyrate-co-hydroxy-hexanoate) copolymer, resulting in rapid recrystallization and the formation of highly active crystals.
ACS APPLIED POLYMER MATERIALS
(2023)
Article
Chemistry, Multidisciplinary
Anna A. Berseneva, Vladislav V. Klepov, Hunter B. Tisdale, Hans-Conrad zur Loye
Summary: Two polytypic heterolayered salt-inclusion chalcogenides, o-[Na2Cl]GaQ(2) and t-[Na2Cl]GaQ(2), were synthesized via a NaCl/NaI flux-assisted method in the Na-Ga-Q (Q = S and Se) system. In the Na-Ga-Se system, the use of NaBr/NaI flux did not produce salt-inclusion phases, but resulted in the formation of Na2GaSe3 and Na4Ga2Se5 phases instead. The thermal and electronic properties of [Na2Cl]GaS2 materials were investigated, and the heterolayered [Na2Cl]GaS2 single crystals were tested as a sorbent for UO22+ uptake.
Article
Chemistry, Inorganic & Nuclear
Darren Carone, Vladislav V. Klepov, Scott T. Misture, Joseph C. Schaeperkoetter, Luiz G. Jacobsohn, Mina Aziziha, Juliano Schorne-Pinto, Stuart A. J. Thomson, Adrian T. Hines, Theodore M. Besmann, Hans-Conrad Zur Loye
Summary: A new niobium-doped inorganic scintillating oxyfluoride has been synthesized by high-temperature flux growth. The doped material exhibits bright blue luminescence and scintillation, with the niobium located in an octahedral coordination environment.
Article
Biochemistry & Molecular Biology
Navindra Keerthisinghe, Matthew S. Christian, Anna A. Berseneva, Gregory Morrison, Vladislav V. Klepov, Mark D. Smith, Hans-Conrad zur Loye
Summary: The solvothermal synthesis, structure determination and optical characterization of five new metastable halometallate compounds with rich structural diversity have been reported. The optical behavior of these materials depends on their structural dimensionalities, making them potential candidates for semiconductor applications.
