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An Organic–Inorganic Hybrid Electrolyte as a Cathode Interlayer for Efficient Organic Solar Cells

Angewandte Chemie 2021年第15期133卷

作者： Dr. Chaowei Zhao Zhou Zhang Dr. Faming Han Dongdong Xia Dr. Chengyi Xiao Dr. Jie Fang Yuefeng Zhang Prof. Binghui Wu Prof. Shengyong You Prof. Yonggang Wu Prof. Weiwei Li Institute of Applied Chemistry Jiangxi Academy of Sciences Nanchang 330096 P. R. China Beijing Advanced Innovation Center for Soft Matter Science and Engineering & State Key Laboratory of Organic–Inorganic Composites Beijing University of Chemical Technology Beijing 100029 P. R. China College of Chemistry and Environmental Science Hebei University Baoding 071002 P. R. China Pen-Tung Sah Institute of Micro-Nano Science and Technology College of Chemistry and Chemical Engineering Xiamen University Xiamen 361005 P. R. China

An organic–inorganic hybrid electrolyte based on a cyclic Ti-oxo cluster as the inorganic core and naphthalene-based organic ammonium bromide salts as the electrolyte was developed with easy synthesis and low cost. The new hybrid electrolyte exhibits excellent solubility in methanol, aligned work function, good conductivity, and amorphous state in thin film, enabling its successful application as a cathode interlayer in organic solar cells with a high power conversion efficiency of 17.19 %. This work demonstrates that the hybrid electrolytes are a new kind of semiconductor, exhibiting promising applications in organic electronics.

关键词： cathode interlayers organic–inorganic hybrid electrolytes solar cells Ti-oxo clusters

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Electrocatalytically Activating and Reducing N2Molecule by Tuning Activity of Local Hydrogen Radical

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Angewandte Chemie 2023年第20期135卷

作者： Yuanyuan Yang Cejun Hu Dr. Jieqiong Shan Chuanqi Cheng Prof. Lili Han Prof. Xinzhe Li Ruguang Wang Prof. Wei Xie Prof. Yao Zheng Prof. Tao Ling Key Laboratory for Advanced Ceramics and Machining Technology of Ministry of Education Tianjin Key Laboratory of Composite and Functional Materials School of Materials Science and Engineering Tianjin University Tianjin 300072 China Key Laboratory of Advanced Energy Materials Chemistry (Ministry of Education) Tianjin Key Lab of Molecular Recognition & Biosensing Renewable Energy Conversion and Storage Center College of Chemistry Nankai University Tianjin 300071 China School of Chemical Engineering The University of Adelaide Adelaide SA 5005 Australia State Key Laboratory of Structural Chemistry Fujian Institute of Research on the Structure of Matter Chinese Academy of Sciences Fuzhou 350002 China State Key Laboratory of Multiphase Flow in Power Engineering School of Energy and Power Engineering Xi'an Jiaotong University Xi An Shi Xi'an 710049 China

Decarbonizing N 2 conversion is particularly challenging, but essential for sustainable development of industry and agriculture. Herein, we achieve electrocatalytic activation/reduction of N 2 on X/Fe−N−C (X=Pd, Ir and Pt) dual-atom catalysts under ambient condition. We provide solid experimental evidence that local hydrogen radical (H*) generated on the X site of the X/Fe−N−C catalysts can participate in the activation/reduction of N 2 adsorbed on the Fe site. More importantly, we reveal that the reactivity of X/Fe−N−C catalysts for N 2 activation/reduction can be well adjusted by the activity of H* generated on the X site, i.e., the interaction between the X−H bond. Specifically, X/Fe−N−C catalyst with the weakest X−H bonding exhibits the highest H* activity, which is beneficial to the subsequent cleavage of X−H bond for N 2 hydrogenation. With the most active H*, the Pd/Fe dual-atom site promotes the turnover frequency of N 2 reduction by up to 10 times compared with the pristine Fe site.

关键词： Carbon Materials Electrocatalysis Metal-Free Catalysts Nitrogen Reduction Reaction

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Chiral Hybrid Germanium(II) Halide with Strong Nonlinear Chiroptical Properties

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Angewandte Chemie 2023年第41期135卷

作者： Hebin Wang Junzi Li Haolin Lu Sehrish Gull Tianyin Shao Yunxin Zhang Tengfei He Prof. Yongsheng Chen Prof. Tingchao He Prof. Guankui Long School of Materials Science and Engineering Smart Sensing Interdisciplinary Science Center Tianjin Key Lab for Rare Earth Materials and Applications Renewable Energy Conversion and Storage Center (RECAST) National Institute for Advanced Materials Nankai University Tianjin 300350 China Key Laboratory of Optoelectronic Devices and Systems of Ministry of Education and Guangdong Province College of Physics and Optoelectronic Engineering Shenzhen University Shenzhen 518060 China The Centre of Nanoscale Science and Technology and Key Laboratory of Functional Polymer Materials Institute of Polymer Chemistry Renewable Energy Conversion and Storage Center (RECAST) College of Chemistry Nankai University Tianjin 300071 China

Due to the pronounced anisotropic response to circularly polarized light, chiral hybrid organic–inorganic metal halides have been regarded as promising candidates for the application in nonlinear chiroptics, especially for the second-harmonic generation circular dichroism (SHG-CD) effect. However, designing novel lead-free chiral hybrid metal halides with large anisotropy factors and high laser-induced damage thresholds (LDT) of SHG-CD remains challenging. Herein, we develop the first chiral hybrid germanium halide, ( R / S -NEA) 3 Ge 2 I 7 ⋅H 2 O ( R / S -NGI), and systematically investigated its linear and nonlinear chiroptical properties. S -NGI and R -NGI exhibit large anisotropy factors ( g SHG-CD ) of 0.45 and 0.48, respectively, along with a high LDT of 38.46 GW/cm 2 ; these anisotropy factors were the highest values among the reported lead-free chiral hybrid metal halides. Moreover, the effective second-order nonlinear optical coefficient of S -NGI could reach up to 0.86 pm/V, which was 2.9 times higher than that of commercial Y-cut quartz. Our findings facilitate a new avenue toward lead-free chiral hybrid metal halides, and their implementation in nonlinear chiroptical applications.

关键词： Chirality Germanium Nonlinear Chiroptics Perovskites Second-Harmonic Generation

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Non-Equal Ratio Cocrystal Engineering to Improve Charge Transport Characteristics of Organic Semiconductors: A Case Study on Indolo[2,3-a]carbazole

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Angewandte Chemie 2022年第28期134卷

作者： Junfeng Guo Yan Zeng Prof. Yonggang Zhen Prof. Hua Geng Dr. Zongrui Wang Prof. Yuanping Yi Prof. Huanli Dong Prof. Wenping Hu National Laboratory for Molecular Sciences Key Laboratory of Organic Solids Institute of Chemistry Chinese Academy of Sciences Beijing 100190 China University of Chinese Academy of Sciences Beijing 100049 China Beijing Advanced Innovation Center for Soft Matter Science and Engineering State Key Laboratory of Organic-Inorganic Composites Beijing University of Chemical Technology Beijing 100029 China State Key Laboratory of Optoelectronic Materials and Technologies Sun Yat-sen University Guangdong 510275 China Beijing Key Laboratory for Optical Materials and Photonic Devices Department of Chemistry Capital Normal University Beijing 100048 China State Key Laboratory of Luminescent Materials and Devices South China University of Technology Guangzhou 510640 China Tianjin Key Laboratory of Molecular Optoelectronic Sciences Department of Chemistry School of Sciences Tianjin University & Collaborative Innovation Center of Chemical Science and Engineering (Tianjin) Tianjin 300072 China

Rare studies of cocrystal engineering have focused on improving carrier mobility of organic semiconductors mainly because of the generation of ambipolarity, the alteration of the charge carrier polarity or the reduction of electronic couplings. Herein, we utilize indolo[2,3-a]carbazole (IC) as the model compound and 2,6-diphenylanthraquinone (DPAO) and 9-fluorenone (FO) as the coformers to construct IC2-DPAO and IC-FO cocrystals with 2 : 1 or 1 : 1 ratios, respectively, through hydrogen bonds and donor–acceptor interactions. Interestingly, the more appropriate packing structure, possessing not only enhanced electronic couplings but also increased intermolecular distances, is achieved in IC2-DPAO, which shows an improved carrier mobility of 0.11 cm 2 V −1 s −1 by four orders of magnitude relative to the IC crystal. These results suggest that non-equal ratio cocrystal engineering opens up the possibility to develop organic semiconductors with enhanced charge transport behaviors.

关键词： Charge Transport Cocrystals Organic Field-Effect Transistors Organic Semiconductors Packing Structures

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Honeycomb Carbon Nanofibers: A Superhydrophilic O2-Entrapping Electrocatalyst Enables Ultrahigh Mass Activity for the Two-Electron Oxygen Reduction Reaction

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Angewandte Chemie 2021年第19期133卷

作者： Kai Dong Jie Liang Yuanyuan Wang Zhaoquan Xu Dr. Qian Liu Yonglan Luo Dr. Tingshuai Li Lei Li Dr. Xifeng Shi Prof. Abdullah M. Asiri Prof. Quan Li Prof. Dongwei Ma Prof. Xuping Sun Institute of Fundamental and Frontier Sciences University of Electronic Science and Technology of China Chengdu 610054 Sichuan China College of Chemistry and Materials Science Sichuan Normal University Chengdu 610068 Sichuan China Key Laboratory for Special Functional Materials of Ministry of Education School of Materials Science and Engineering Henan University Kaifeng 475004 Henan China College of Chemistry Chemical Engineering and Materials Science Shandong Normal University Jinan 250014 Shandong China Chemistry Department Faculty of Science & Center of Excellence for Advanced Materials Research King Abdulaziz University P.O. Box 80203 Jeddah 21589 Saudi Arabia

Electrocatalytic two-electron oxygen reduction has emerged as a promising alternative to the energy- and waste-intensive anthraquinone process for distributed H 2 O 2 production. This process, however, suffers from strong competition from the four-electron pathway leading to low H 2 O 2 selectivity. Herein, we report using a superhydrophilic O 2 -entrapping electrocatalyst to enable superb two-electron oxygen reduction electrocatalysis. The honeycomb carbon nanofibers (HCNFs) are robust and capable of achieving a high H 2 O 2 selectivity of 97.3 %, much higher than that of its solid carbon nanofiber counterpart. Impressively, this catalyst achieves an ultrahigh mass activity of up to 220 A g −1 , surpassing all other catalysts for two-electron oxygen reduction reaction. The superhydrophilic porous carbon skeleton with rich oxygenated functional groups facilitates efficient electron transfer and better wetting of the catalyst by the electrolyte, and the interconnected cavities allow for more effective entrapping of the gas bubbles. The catalytic mechanism is further revealed by in situ Raman analysis and density functional theory calculations.

关键词： density functional theory honeycomb carbon nanofibers hydrogen peroxide electrosynthesis O2 entrapment superhydrophilicity

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Nano-enabled Quenching of Bacterial Communications for the Prevention of Biofilm Formation

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Angewandte Chemie 2023年第27期135卷

作者： Dr. Meng Gao Dr. Bolong Xu Dr. Yang Huang Jiayu Cao Lili Yang Dr. Xi Liu Alisher Djumaev Di Wu Moxichexra Shoxiddinova Xiaoming Cai Behruz Tojiyev Dr. Huizhen Zheng Prof. Xuehua Li Prof. Kunduz Normurodova Prof. Huiyu Liu Prof. Ruibin Li State Key Laboratory of Radiation Medicine and Protection School for Radiological and Interdisciplinary Sciences (RAD-X) Collaborative Innovation Center of Radiological Medicine of Jiangsu Higher Education Institutions Suzhou Medical College Soochow University 215123 Suzhou Jiangsu China Beijing Advanced Innovation Center for Soft Matter Science and Engineering State Key Laboratory of Organic–Inorganic Composites Bionanomaterials & Translational Engineering Laboratory Beijing Key Laboratory of Bioprocess Beijing Laboratory of Biomedical Materials Beijing University of Chemical Technology 100029 Beijing China Key Laboratory of Industrial Ecology and Environmental Engineering School of Environmental Science and Technology Dalian University of Technology 116024 Dalian Liaoning China School of Public Health Jiangsu Key Laboratory of Preventive and Translational Medicine for Geriatric Diseases Soochow University 215123 Suzhou Jiangsu China Department of Microbiology and Biotechnology Faculty of Biology National University of Uzbekistan named after Mirzo Ulugbek 100174 Tashkent Uzbekistan

Biofilm formation is a major threat to industry, the environment and human health. While killing of embedded microbes in biofilms may inevitably lead to the evolution of antimicrobial resistance (AMR), catalytic quenching of bacterial communications by lactonase is a promising antifouling approach. Given the shortcomings of protein enzymes, it is attractive to engineer synthetic materials to mimic the activity of lactonase. Herein, an efficient lactonase-like Zn−N x −C nanomaterial was synthesized by tuning the coordination environment around zinc atoms to mimic the active domain of lactonase for catalytical interception of bacterial communications in biofilm formation. The Zn−N x −C material could selectively catalyze 77.5 % hydrolysis of N-acylated-L-homoserine lactone (AHL), a critical bacterial quorum sensing (QS) signal in biofilm construction. Consequently, AHL degradation downregulated the expression of QS-related genes in antibiotic resistant bacteria and significantly prevented biofilm formation. As a proof of concept, Zn−N x −C-coated iron plates prevented 80.3 % biofouling after a month exposure in river. Overall, our study provides a nano-enabled contactless antifouling insight to avoid AMR evolution by engineering nanomaterials for mimicking the key bacterial enzymes (e.g., lactonase) functioning in biofilm construction.

关键词： Antibacterial Antimicrobial Resistance Biocatalysis Biofilm Nanozyme

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A Dual‐Surface Amidoximated Halloysite Nanotube for High‐Efficiency Economical Uranium Extraction from Seawater

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Angewandte Chemie 2019年第42期131卷

作者： Shilei Zhao Yihui Yuan Qiuhan Yu Biye Niu Jianhe Liao Zhanhu Guo Ning Wang State Key Laboratory of Marine Resource Utilization in South China Sea Hainan University Haikou 570228 P. R. China College of Materials Science and Engineering Hainan University Haikou 570228 P. R. China Integrated Composites Laboratory (ICL) Department of Chemical & Biomolecular Engineering University of Tennessee Knoxville TN 37996 USA National Engineering Research Center for Advanced Polymer Processing Technology Zhengzhou University Zhengzhou 450001 P. R. China

By chemical cross‐linking the amidoxime group onto dual‐surfaces of natural ore materials, namely halloysite nanotubes (HNTs), an efficient adsorbent, AO‐HNTs, is developed. AO‐HNTs show high uranium adsorption capacity of 456.24 mg g −1 in 32 ppm uranium‐spiked simulated seawater. In natural seawater, AO‐HNTs reach the high uranium extraction capacity of 9.01 mg g −1 after 30 days’ field test. The dual‐surface amidoximated hollow nanotubular AO‐HNTs exhibit more coordination active sites for uranium adsorption, which is attributed to the high and fast uranium adsorption capacity. Because of the stable natural ore structure, AO‐HNTs also show long service life. Benefiting from the low cost of HNTs, the cost for uranium extraction from seawater is close to the uranium price in the spot uranium market, suggesting that AO‐HNTs could be used for economical extraction of uranium from the oceans.

关键词： Amidoxim Halloysit Meerwasser Nanoröhren Uran

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Volatile Perovskite Precursor Ink Enables Window Printing of Phase-Pure FAPbI3Perovskite Solar Cells and Modules in Ambient Atmosphere

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Angewandte Chemie 2023年第7期136卷

作者： Linhao Yuan Xining Chen Xianming Guo Shihao Huang Xiaoxiao Wu Yunxiu Shen Hao Gu Yujin Chen Guixiang Zeng Hans-Joachim Egelhaaf Christoph J. Brabec Fu Yang Yaowen Li Yongfang Li Laboratory of Advanced Optoelectronic Materials Suzhou Key Laboratory of Novel Semiconductor-optoelectronics Materials and Devices College of Chemistry Chemical Engineering and Materials Science Soochow University Suzhou 215123 China School of Chemistry and Chemical Engineering Nanjing University Nanjing 210008 China Suzhou Sunflex New Energy Company Limited Suzhou 215100 China Kuang Yaming Honors School Nanjing University Nanjing 210023 China Institute of Materials for Electronics and Energy Technology (i-MEET) Friedrich-Alexander University Erlangen-Nürnberg Martensstrasse 7 91058 Erlangen Germany Helmholtz Institute Erlangen-Nürnberg for Renewable Energy (HI ERN) Immerwahrstrasse 2 91058 Erlangen Germany Jiangsu Key Laboratory of Advanced Negative Carbon Technologies Soochow University Suzhou 215123 Jiangsu P. R. China State and Local Joint Engineering Laboratory for Novel Functional Polymeric Materials Jiangsu Key Laboratory of Advanced Functional Polymer Design and Application College of Chemistry Chemical Engineering and Materials Science Soochow University Suzhou 215123 China Beijing National Laboratory for Molecular Sciences CAS Key Laboratory of Organic Solids Institute of Chemistry Chinese Academy of Sciences Beijing 100190 China

Despite the great success of perovskite photovoltaics in terms of device efficiency and stability using laboratory-scale spin-coating methods, the demand for high-throughput and cost-effective solutions remains unresolved and rarely reported because of the complicated nature of perovskite crystallization. In this work, we propose a stable precursor ink design strategy to control the solvent volatilization and perovskite crystallization to enable the wide speed window printing (0.3 to 18.0 m/min) of phase-pure FAPbI 3 perovskite solar cells (pero-SCs) in ambient atmosphere. The FAPbI 3 perovskite precursor ink uses volatile acetonitrile (ACN) as the main solvent with DMF and DMSO as coordination additives is beneficial to improve the ink stability, inhibit the coffee rings, and the complicated intermediate FAPbI 3 phases, delivering high-quality pin-hole free and phase-pure FAPbI 3 perovskite films with large-scale uniformity. Ultimately, small-area FAPbI 3 pero-SCs (0.062 cm 2 ) and large-area modules (15.64 cm 2 ) achieved remarkable efficiencies of 24.32 % and 21.90 %, respectively, whereas the PCE of the devices can be maintained at 23.76 % when the printing speed increases to 18.0 m/min. Specifically, the unencapsulated device exhibits superior operational stability with T 90 >1350 h. This work represents a step towards the scalable, cost-effective manufacturing of perovskite photovoltaics with both high performance and high throughput.

关键词： Large-Area Printing Perovskite Solar Cells Solar Module Volatile Solvent Wide Speed Window

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Ultrafast charge transfer processes accompanying KLL Auger decay in aqueous KCl solution

arXiv

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arXiv 2017年

作者： Céolin, D. Kryzhevoi, N.V. Nicolas, Ch Pokapanich, W. Choksakulporn, S. Songsiriritthigul, P. Saisopa, Th Rattanachai, Y. Utsumi, Y. Palaudoux, J. Öhrwall, G. Rueff, J.P. Synchrotron SOLEIL l’Orme des Merisiers Saint-Aubin Gif-sur-Yvette CedexF-91192 France Theoretical Chemistry Institute of Physical Chemistry Heidelberg University Im Neuenheimer Feld 229 Heidelberg69120 Germany Faculty of Science Nakhon Phanom University Nakhon Phanom48000 Thailand Synchrotron Light Research Institute Nakhon Ratchasima30000 Thailand NANOTEC-SUT Center of Excellence on Advanced Functional Nanomaterials School of Physics Suranaree University of Technology Nakhon Ratchasima30000 Thailand Department of Applied Physics Faculty of Sciences and Liberal Arts Rajamangala University of Technology Isan Nakhon Ratchasima30000 Thailand CNRS UMR 7614 Laboratoire de Chimie Physique-Matière et Rayonnement ParisF-75005 France Sorbonne Universités UPMC Université Paris 06 UMR 7614 Laboratoire de Chimie Physique-Matière et Rayonnement ParisF-75005 France MAX IV Laboratory P.O. Box 118 LundSE-22100 Sweden

X-ray photoelectron spectroscopy (XPS) and KLL Auger spectra of aqueous KCl solution were measured for the K+ and Cledges. While the XPS spectra of potassium and chloride have similar structures, both exhibiting only weak satellite structures near the main line, the Auger spectra of these isoelectronic ions differ dramatically. A very strong satellite peak was found in the K+ KLL Auger spectrum at the low kinetic energy side of the 1D state. Using equivalent core models and ab initio calculations this spectral structure was assigned to electron transfer processes from solvent water molecules to the solvated K+ cation. Contrary to the potassium case, no extra peak was found in the KLL Auger spectrum of solvated Cl- indicating on a strong dependence of the underlying processes on ionic charge. The observed charge transfer processes are suggested to play an important role in charge redistribution following single and multiple core-hole creation in atomic and molecular systems placed into an environment. Copyright © 2017, The Authors. All rights reserved.

关键词： Charge transfer

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Collective nature of orbital excitations in layered cuprates in the absence of apical oxygens

arXiv

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arXiv 2023年

作者： Martinelli, Leonardo Wohlfeld, Krzysztof Pelliciari, Jonathan Arpaia, Riccardo Brookes, Nicholas B. Di Castro, Daniele Fernandez, Mirian G. Kang, Mingu Krockenberger, Yoshiharu Kummer, Kurt McNally, Daniel E. Paris, Eugenio Schmitt, Thorsten Yamamoto, Hideki Walters, Andrew Zhou, Ke-Jin Braicovich, Lucio Comin, Riccardo Sala, Marco Moretti Devereaux, Thomas P. Daghofer, Maria Ghiringhelli, Giacomo Dipartimento di Fisica Politecnico di Milano piazza Leonardo da Vinci 32 MilanoI-20133 Italy Institute of Theoretical Physics Faculty of Physics University of Warsaw Pasteura 5 WarsawPL-02093 Poland National Synchrotron Light Source II Brookhaven National Laboratory UptonNY11973 United States Department of Physics Massachusetts Institute of Technology CambridgeMA United States Quantum Device Physics Laboratory Department of Microtechnology and Nanoscience Chalmers University of Technology GöteborgSE-41296 Sweden ESRF-The European Synchrotron 71 Avenue des Martyrs CS 40220 GrenobleF-38043 France CNR-SPIN Dipartimento di Ingegneria Civile e Ingegneria Informatica Universit`a di Roma Tor Vergata Via del Politecnico 1 RomaI-00133 Italy Diamond Light Source Harwell Campus DidcotOX11 0DE United Kingdom NTT Basic Research Laboratories NTT Corporation Atsugi Kanagawa243-0198 Japan Photon Science Division Paul Scherrer Institut Villigen PSI5232 Switzerland Stanford Institute for Materials and Energy Sciences SLAC Menlo ParkCA94025 United States Department of Materials Science and Engineering Stanford University StanfordCA94305 United States Geballe Laboratory for Advanced Materials Stanford University StanfordCA94305 United States Institute for Functional Matter and Quantum Technologies University of Stuttgart Pfaffenwaldring 57 StuttgartD-70550 Germany Center for Integrated Quantum Science and Technology University of Stuttgart Pfaffenwaldring 57 StuttgartD-70550 Germany CNR-SPIN Dipartimento di Fisica Politecnico di Milano MilanoI-20133 Italy

We have investigated the 3d orbital excitations in CaCuO2 (CCO), Nd2CuO4 (NCO), and La2CuO4 (LCO) using high-resolution resonant inelastic x-ray scattering. In LCO they behave as well-localized excitations, similarly to several other cuprates. On the contrary, in CCO and NCO the dxy orbital clearly disperse, pointing to a collective character of this excitation (orbiton) in compounds without apical oxygen. We ascribe the origin of the dispersion as stemming from a substantial next-nearest-neighbor (NNN) orbital superexchange. Such an exchange leads to the liberation of the orbiton from its coupling to magnons, which is associated with the orbiton hopping between nearest neighbor copper sites. Finally, we show that the exceptionally large NNN orbital superexchange can be traced back to the absence of apical oxygens suppressing the charge transfer energy. Copyright © 2023, The Authors. All rights reserved.

关键词： Copper compounds

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