Article
Chemistry, Physical
Rui Yun, Huanxin Yang, Yue Li, Yuling Liu, Yiyue Chu, Xiaodan Zhang, Libing Zhang, Xiyan Li, Suli Wu, Xiaowang Liu
Summary: A transformation strategy mediated by an inorganic ligand (NOBF4) was developed to obtain blue-emitting CsPbBr3 nanoplates (NPLs). The transformation process involved the dissolution and recrystallization of Cs4PbBr6 nanocrystals in a nonpolar environment, resulting in the formation of pure blue-emitting NPLs with a line width of about 12 nm. The reorganization of organic ligands tuned by NO+ played a crucial role in the formation of NPLs. This work provides an effective strategy for obtaining pure blue-emitting NPLs and offers a platform for exploring the mechanism of anisotropic growth in perovskite crystals.
CHEMISTRY OF MATERIALS
(2023)
Article
Chemistry, Inorganic & Nuclear
Zixian Wang, Daofu Wu, Qiang Huang, Linfeng Guo, Yijia Wang, Weiwei Chen, Fei Wang, Juan Du, Zhengzheng Liu, Zhiping Hu, Yuxin Leng, Junan Lai, Peng He, Xiaosheng Tang
Summary: The application of organic-inorganic hybrid lead-free perovskite scintillators in X-ray imaging shows potential as a substitute for traditional lead-containing materials with lower costs and reduced self-absorption.
INORGANIC CHEMISTRY
(2023)
Article
Chemistry, Multidisciplinary
Yan Gao, Xiaohong Li, Weiwei Liu, Xiangyuan Xing, Hua Long, Kai Wang, Bing Wang, Peixiang Lu
Summary: In this study, a highly tunable enhancement and switching of nonlinear emission from metal halide perovskites were demonstrated using an asymmetrically biased metal-insulator-semiconductor structure. The enhancement of two-photon-pumped photoluminescence was achieved by electric-field-induced passivation/activation of Br vacancies, ranging from approximately 61.2-fold to 370.3-fold. Efficient modulation of two-photon-pumped lasing with a high on/off ratio of 67:1 was also demonstrated.
Article
Materials Science, Multidisciplinary
Haiping Xu, Xuehua Dong, Zhizhuan Zhang, Ling Huang, Hongmei Zeng, Zhien Lin, Guohong Zou
Summary: In this study, a novel all-inorganic dual halogen emitter Cs2Cd2BrCl5 with a three-dimensional structure was successfully synthesized. It exhibits broadband white-light emission with high correlated color temperature, color rendering index, and photoluminescence quantum yield. The white-light emission originates from self-trapped excitons, and Cs2Cd2BrCl5 shows excellent structural and optical stability, making it a potential candidate for light-emitting diodes.
JOURNAL OF MATERIALS CHEMISTRY C
(2022)
Article
Materials Science, Multidisciplinary
Han K. D. Le, Chung-Kuan Lin, Jianbo Jin, Ye Zhang, Zhenni Lin, Arturas Vailionis, Nobumichi Tamura, Peidong Yang
Summary: The high-temperature phase stability of CsPbI3 nanoplates is enhanced by a strained interface, and the relationship between strain and phase transition kinetics is critical for the design of stable perovskite-based optoelectronic devices.
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, Physical
Xin Mao, Zhongyi Wang, Fen Zhang, Hong Yin, Xin Xu, Junsheng Chen, Zhen Chen, Junhua Luo, Keli Han, Ruiling Zhang
Summary: In this study, high-quality Sb3+-doped 0D Rb2ScCl5(H2O) perovskite single crystals were synthesized and their photophysical properties were investigated. The introduction of Sb3+ dramatically enhanced the emission quantum yield from less than 1% to about 53%. Spectroscopic characterizations revealed that the enhancement was attributed to efficient energy transfer from Sb3+ to the emissive self-trapped excitons (STE). Moreover, 0.2%Sb3+:Rb2ScCl5(H2O) single crystals showed potential applications in direct X-ray detection with a high sensitivity of 58.5 mu C Gy(-1) cm(-2).
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
(2023)
Article
Chemistry, Physical
Xin Mao, Zhongyi Wang, Fen Zhang, Hong Yin, Xin Xu, Junsheng Chen, Zhen Chen, Junhua Luo, Keli Han, Ruiling Zhang
Summary: In this paper, the synthesis and photophysical properties of high-quality Sb3+-doped 0D Rb2ScCl5(H2O) perovskite single crystals are reported. It is found that the emission quantum yield can be dramatically enhanced from less than 1% to about 53% via Sb3+ doping. Spectroscopic characterizations indicate that the photoluminescence enhancement is a result of the efficient energy transfer from Sb3+ to the emissive self-trapped excitons. Additionally, 0.2%Sb3+:Rb2ScCl5(H2O) single crystals exhibit potential application in direct X-ray detection with a high sensitivity of 58.5 mu C Gy-1 cm-2.
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
(2023)
Article
Materials Science, Multidisciplinary
Paris Papagiorgis, Marios Sergides, Andreas Manoli, Modestos Athanasiou, Caterina Bernasconi, Fedros Galatopoulos, Apostolos Ioakeimidis, Constantinos Nicolaides, Epameinondas Leontidis, Theodossis Trypiniotis, Stelios Choulis, Maryna I. Bodnarchuk, Maksym V. Kovalenko, Andreas Othonos, Grigorios Itskos
Summary: Ligand exchange during or after the colloidal synthesis of nanocrystals enables the production of conductive nanocrystal solids for optoelectronics. A post-synthetic ligand washing process was developed, leading to increased photoconductance and improved optoelectronic properties for both FAPbI3 and CsPbBr3 nanocrystals.
ADVANCED OPTICAL MATERIALS
(2023)
Article
Thermodynamics
Bin Wang, Alexandra Navrotsky
Summary: Inorganic cesium lead halide perovskites, particularly CsPbX3, have attracted significant interest for photovoltaic applications, despite facing potential issues with chemical and thermodynamic instabilities. Calorimetric studies revealed decreasing thermodynamic stability in the order CsPbCl3, CsPbBr3, and CsPbI3, with CsPbI3 being only marginally stable from a thermodynamic perspective. The variation in stability follows the Goldschmidt tolerance factor, and perovskites are shown to be entropy-stabilized high temperature phases relative to low temperature polymorphs, with phase transitions reflecting the thermodynamic trends.
THERMOCHIMICA ACTA
(2021)
Article
Chemistry, Multidisciplinary
Marina R. Filip, Diana Y. Qiu, Mauro Del Ben, Jeffrey B. Neaton
Summary: Interlayer organic cations play a crucial role in tuning the optoelectronic properties of quasi-two-dimensional halide perovskites, and their effects can be controlled by adjusting the dielectric properties.
Review
Chemistry, Multidisciplinary
Zhixing Gan, Yingchun Cheng, Weijian Chen, Kian Ping Loh, Baohua Jia, Xiaoming Wen
Summary: 2D organic-inorganic hybrid Ruddlesden-Popper perovskites have garnered attention for their unique photophysics, with room for improvement in performance of photoelectronic devices.
Article
Physics, Applied
Ruiqin Huang, Enze Kang, Han Gao, Renbo Guo, Qingsong Hu, Yibo Han
Summary: CsPbBr3 nanoplatelets exhibit large optical nonlinearity, including third-order nonlinear absorption, refraction, and two-photon absorption excited luminescence. The nonlinear absorption cross section is two orders of magnitude larger than that of CsPbBr3 nanocrystals, making them suitable for optical limiting. Furthermore, they show large self-phase modulation-induced nonlinear refraction, allowing for optical switching.
APPLIED PHYSICS LETTERS
(2022)
Article
Chemistry, Multidisciplinary
Xia Cai, Yan Li, Jianfei Liu, Hao Zhang, Jianguo Pan, Yiqiang Zhan
Summary: This study utilizes ensemble machine learning to search for non-toxic and high-performance all-inorganic lead-free perovskites for use in solving the challenges of efficiency, stability, and toxicity in perovskite solar cells. Through the establishment of structure identification and band gap classification models, as well as the proposal of a physics-inspired multi-component neural network, suitable candidates are screened. Based on first principles calculations, 17 candidates with theoretical power conversion efficiencies over 20% are identified.
MATERIALS HORIZONS
(2023)
Article
Chemistry, Physical
Wenlong Yao, Qin Ling, Qing Dai, Shuyan Fang, Cheng Yang, Like Huang, Xiaohui Liu, Houcheng Zhang, Jing Zhang, Yuejin Zhu, Ziyang Hu
Summary: This paper systematically examines the degradation mechanisms of all-inorganic perovskite CsPbI2Br under a humid environment. It is found that the level of relative humidity (RH) is important for the degradation process and it initiates at the grain boundaries and extends toward the grain interiors.
ACS APPLIED ENERGY MATERIALS
(2022)
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
Fridtjof Betz, Felix Binkowski, Martin Hammerschmidt, Lin Zschiedrich, Sven Burger
Summary: This study presents a quasinormal mode expansion approach for quadratic observables, utilizing the rigorous Riesz projection method. The applicability of the method is demonstrated through numerical implementation of a state-of-the-art quantum light source, with emphasis on modal expansions outside the underlying nanophotonic resonator.
PHYSICA STATUS SOLIDI A-APPLICATIONS AND MATERIALS SCIENCE
(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, Multidisciplinary
Vanessa Ruck, Mikkel B. Liisberg, Christian Brinch Mollerup, Yanmei He, Junsheng Chen, Cecilia Cerretani, Tom Vosch
Summary: This article presents a DNA-stabilized silver nanocluster (DNA-AgNC) with dual emission in the red and near-infrared regions. Mass spectrometry data shows that two DNA strands stabilize 18 silver atoms with a nanocluster charge of 12+. Steady-state and time-resolved methods were used to characterize the red fluorescence and NIR luminescence, and the luminescence-to-fluorescence ratio was found to be excitation-intensity-dependent, making it a nanoscale excitation intensity probe.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Engineering, Environmental
Hong Yin, Wenzhi Li, Zhongyi Wang, Pengyuan Wang, Xin Xu, Peigeng Han, Xin Mao, Feng Liu, Keli Han, Junsheng Chen, Ruiling Zhang
Summary: In this study, luminescent low-dimensional organic copper halides were developed by introducing three different cations with increasing steric hindrance: 1D ETMACu2I3, 1D TEACu2I3, and 0D TBMACuI2. The dimensionality of the prepared copper halides decreased with the increase of the steric hindrance of the organic cations, while the photoluminescence spectra became broader. Of note, 0D TBMACuI2 emitted bright warm white light with dual emission bands. The mechanism of the unique dual emission was unveiled through systematic spectroscopic study.
CHEMICAL ENGINEERING JOURNAL
(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
Optics
Elena Mikheeva, Remi Colom, Karim Achouri, Adam Overvig, Felix Binkowski, Jean-yves Duboz, Sgbastien Cueff, Shanhui Fan, Sven Burger, Andrea Alu, Patrice Genevet
Summary: In this paper, we use temporal coupled mode theory to predict the location of phase singularities and control the induced phase modulation of light in wavefront-shaping devices. The study shows that breaking spatial inversion symmetry lifts the degeneracy of reflection zeros and introduces a complex singularity with a positive imaginary part. Our work establishes a general framework for predicting and studying the response of resonant systems in photonics and metaoptics.
Article
Chemistry, Physical
Linnea Lindh, Torbjorn Pascher, Samuel Persson, Yogesh Goriya, Kenneth Warnmark, Jens Uhlig, Pavel Chabera, Petter Persson, Arkady Yartsev
Summary: The excited state dynamics of three iron(II) carbene complexes were investigated, revealing differences in dynamics between the complexes and the metal-centered triplet states. The study provides insights into the deactivation processes of the complexes and improves understanding of the photophysical limitations and opportunities for the use of iron(II) based photosensitizers in photochemical applications.
JOURNAL OF PHYSICAL CHEMISTRY A
(2023)
Article
Chemistry, Physical
Li Zhao, Xuehui Geng, Guoxia Han, Yahui Guo, Runze Liu, Junsheng Chen
Summary: This study investigates the excited state decay mechanism of cytidine in both gas phase and aqueous solution using high-level electronic structure calculations and non-adiabatic dynamic simulations. It is found that cytidine undergoes barrierless decay driven by ring-puckering motion and relaxation channel with a small energy barrier driven by elongation motion of C=O bond. The presence of water molecules significantly reduces the energy barrier, suggesting that the long-lived decay channel in aqueous solution is likely attributed to the cytidine-water intermolecular hydrogen/proton transfer process. These findings contribute to a better understanding of the photostability of DNAs and RNAs and resolve the debate on the cytidine excited-state decay mechanism.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2023)