Article
Chemistry, Multidisciplinary
Philippe B. Green, Ona Segura Lecina, Petru P. Albertini, Anna Loiudice, Raffaella Buonsanti
Summary: This study presents a method to overcome the limitations of ligand exchange by growing an amorphous alumina shell using colloidal atomic layer deposition (c-ALD). The researchers demonstrate that c-ALD can create colloidally stable composite materials by trapping organic chromophores around the nanocrystal core. This approach allows for unique triplet energy transfer and the assembly of a triplet exciton funnel structure, which cannot be achieved through traditional ligand exchange procedures.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Article
Materials Science, Coatings & Films
Solomon T. Oyakhire, Hayrensa Ablat, Nathaniel E. Richey, Stacey F. Bent
Summary: This study develops a three-precursor molecular layer deposition (MLD) process for synthesizing a hybrid film. By incorporating acrylate and aluminum into the film, the process offers high growth rate, stability, and new insights for the design of multi-precursor films.
JOURNAL OF VACUUM SCIENCE & TECHNOLOGY A
(2022)
Article
Chemistry, Multidisciplinary
Fu Li, Changhao Chen, Shaoyong Lu, Xueguang Chen, Wangyu Liu, Kangkang Weng, Zhong Fu, Dan Liu, Lipeng Zhang, Hannikezi Abudukeremu, Linhan Lin, Yuanyuan Wang, Minlin Zhong, Hao Zhang, Jinghong Li
Summary: In this study, a direct patterning method based on a thermal mechanism called thermally activated ligand chemistry (TALC) is introduced. By triggering local thermal stimuli with near-infrared lasers, various nanocrystals can be patterned with high resolution and nondestructive manner. This method overcomes limitations of traditional and emerging patterning techniques and holds promise for the development of advanced optoelectronic functionalities such as transparent electronics.
Article
Chemistry, Physical
Byeongsu Kim, Se-Woong Baek, Changjo Kim, Junho Kim, Jung-Yong Lee
Summary: To achieve high performance CQD/organic hybrid devices, controlling interfacial properties between CQD and organic matter is crucial. By carefully modulating the electronic band between CQD and polymer layers through inserting an interfacial layer treated with various ligands, local charge accumulation and bimolecular recombination can be suppressed, resulting in a high short-circuit current and fill factor of hybrid solar cells. The optimized CQD/polymer hybrid solar cell demonstrates high power conversion efficiency and stability.
ADVANCED ENERGY MATERIALS
(2022)
Article
Materials Science, Coatings & Films
Partha Sarathi Padhi, R. S. Ajimsha, S. K. Rai, Sushmita Bhartiya, Aniruddha Bose, Bidyadhar Das, Manoj Kumar Tiwari, Pankaj Misra
Summary: In this study, device-grade Al2O3/TiO2 nanolaminates (ATA NLs) were fabricated using an ALD system, and the effect of precursor purging time on interfacial and dielectric properties was investigated. It was found that increasing the purging time improved the interface quality and sublayer density by effectively removing reaction by-products and impurities. Additionally, longer purging time resulted in increased dielectric constant, decreased dielectric loss, and improved conductivity contrast across the Al2O3/TiO2 interfaces.
JOURNAL OF VACUUM SCIENCE & TECHNOLOGY A
(2023)
Article
Chemistry, Physical
Huihui Yang, Yanfei Zhang, Leli Zeng, Wen Yin, Yuzhi Xu, Jun Chen, Si-Yang Liu, Xiaoyong Zou, Zhiyu He, Zong Dai
Summary: This study developed a cell encapsulation strategy using nucleolin aptamer and metal-organic frameworks (MOFs) for the preparation of novel whole-cell vaccines. The encapsulated cancer cells underwent immunogenic cell death, leading to enhanced tumor immunoprophylaxis.
Article
Nanoscience & Nanotechnology
Saidjafarzoda Ilhom, Adnan Mohammad, Deepa Shukla, John Grasso, Brian G. Willis, Ali Kemal Okyay, Necmi Biyikli
Summary: This study demonstrates the low-temperature growth of Ga2O3 films using PEALD technology and the transformation of amorphous films into crystalline films with higher refractive index and density through in situ Ar plasma annealing process.
ACS APPLIED MATERIALS & INTERFACES
(2021)
Article
Energy & Fuels
Qi Xiao, Bing Xia, Peilin Liu, Yang Yang, Gaoyuan Yang, Jing Liu, Shuaicheng Lu, Xuezhi Zhao, Ciyu Ge, Duo Chen, Junrui Yang, Guijie Liang, Kanghua Li, Xinzheng Lan, Zewen Xiao, Jianbing Zhang, Liang Gao, Jiang Tang
Summary: The study proposes a facile patch-passivation strategy for developing efficient PbS CQD IR solar cells. By adding TPPO Lewis base to PbS CQDs, uncoordinated Pb2+ can be passivated, suppressing non-radiative recombination. The TPPO-passivated devices achieve high PCE and promising open-circuit voltage in the IR spectrum.
SOLAR ENERGY MATERIALS AND SOLAR CELLS
(2022)
Article
Nanoscience & Nanotechnology
Jihyung Lee, Byeongsu Kim, Changjo Kim, Min-Ho Lee, Irem Kozakci, Sungjun Cho, Beomil Kim, Sang Yeon Lee, Junho Kim, Jihun Oh, Jung-Yong Lee
Summary: To unlock the potential of CQD/organic hybrid devices, we adjusted the interface properties between the ETL and CQD layers by incorporating an EIL. The EIL with a cascading band offset effectively suppressed potential barriers and local charge accumulation at the interfaces, leading to reduced recombination. An optimal EIL expanded the depletion region and facilitated charge extraction, preventing the formation of shallow traps. Devices with an EIL achieved a maximum power conversion efficiency of 14.01% and maintained over 80% of initial performance after 300 hours of continuous operation.
ACS APPLIED MATERIALS & INTERFACES
(2023)
Article
Chemistry, Inorganic & Nuclear
Jin Young Kim, Woongsik Jang, Jihyun Lim, Dong Hwan Wang
Summary: The synthesis of all-inorganic perovskite quantum dots using a one-pot method without a thermal environment is beneficial for enhancing the crystal structure of the materials. This study presents a novel approach to synthesize CsPbClBr2 blue-emitting quantum dots with excellent optical properties and high quantum yield.
INORGANIC CHEMISTRY
(2023)
Article
Chemistry, Multidisciplinary
Tamara Boltersdorf, Felicity N. E. Gavins, Nicholas J. Long
Summary: The study demonstrates a switchable fluorescence effect through LRET technology with lanthanide, enhancing the brightness of lanthanide emission for cellular imaging applications. This strategy can be used to increase lanthanide emission rates for brighter optical probes.
Article
Chemistry, Inorganic & Nuclear
Daniel J. Sattler, Jake B. Bailey, Douglas B. Grotjahn
Summary: In this study, a hybrid ligand with both phosphine and phosphonate ester moieties was synthesized and a Cp*Ir complex of the ligand was synthesized and characterized.
Article
Chemistry, Physical
Sakiru L. Abiodun, Perry J. Pellechia, Andrew B. Greytak
Summary: The purification of CsPbX3 perovskite quantum dots using gel permeation chromatography (GPC) without exposure to polar solvents has been proven effective, resulting in near-unity quantum yield (QY) and improved colloidal stability. Ligand exchange with DDAB further enhances the QY and stability of the CsPbX3 QDs, making the process precise and repeatable for studying ligand populations and photoluminescence lifetimes.
JOURNAL OF PHYSICAL CHEMISTRY C
(2021)
Article
Computer Science, Artificial Intelligence
Qiang Xi, Xinzhi Liu, Xiaodi Li
Summary: This article investigates the issue of finite-time synchronization of complex dynamical networks (CDNs) and proposes a new control strategy that combines weak finite-time control with finite times of impulsive control to achieve finite-time synchronization of CDNs. The proposed strategy synchronizes the impulses within a maximal impulsive interval (MII), which is different from existing results. Global and local criteria for finite-time synchronization are established using the concept of impulsive degree. The optimal values for the times of impulsive control in the controllers and the settling time are derived based on initial values. The article also introduces a technical lemma that reflects the core idea. Finally, a simulation example is provided to demonstrate the main results.
IEEE TRANSACTIONS ON NEURAL NETWORKS AND LEARNING SYSTEMS
(2022)
Article
Chemistry, Inorganic & Nuclear
Agnideep Das, Hannah Jobelius, Jules Schleinitz, Stefani Gamboa-Ramirez, Geordie Creste, Gwendal Kervern, Jesus Raya, Nolwenn Le Breton, Aurelie Guenet, Zahia Boubegtiten-Fezoua, Laurence Grimaud, Maylis Orio, Guillaume Rogez, Petra Hellwig, Sylvie Choua, Sylvie Ferlay, Marine Desage-El Murr
Summary: The design of a unique bioinspired ligand was reported, merging redox-active catechol and flavin-related alloxazine substructures to form a trinuclear complex with three Ni-II centers and redox-active ligands. A multidisciplinary approach was used to study this air-stable metallic triangle, supporting the presence of protons located on the organic ligands and an electronic structure involving high spin Ni(ii) ions strongly ferromagnetically coupled with radicals. The ligand and complex provide a new design for molecular bricks and bioinspired energy storage devices.
INORGANIC CHEMISTRY FRONTIERS
(2021)
Article
Chemistry, Multidisciplinary
Min Wang, Anna Loiudice, Valery Okatenko, Ian D. D. Sharp, Raffaella Buonsanti
Summary: The coupling of CO-generating molecular catalysts with copper electrodes in tandem schemes is a promising strategy to boost the formation of multi-carbon products in the electrocatalytic reduction of CO2. The spatial distribution of the two components in molecular-based tandem systems has not been well explored. This study examines the importance of the relative spatial distribution of Co-phthalocyanine (CoPc) and Cu nanocubes (Cu-cub) on the performance of tandem catalysts. It is found that a direct contact between the CO-generating molecular catalyst and the Cu is crucial for promoting C-C coupling, indicating a surface transport mechanism between the two components of the tandem catalyst.
Article
Chemistry, Physical
Essa A. Alharbi, Anurag Krishna, Nikolaos Lempesis, Mathias Dankl, Irea Mosquera-Lois, Michael A. Hope, Thomas P. Baumeler, George Kakavelakis, Aditya Mishra, Felix T. Eickemeyer, Olivier Ouellette, Thanyarat Chawanpunyawat, Anders Hagfeldt, Shaik M. Zakeeruddin, Lyndon Emsley, Lukas Pfeifer, Ursula Roethlisberger, Michael Gratzel
Summary: We present two alkylammonium halide modulators that improve the power conversion efficiency (PCE) and stability of perovskite solar cells (PSCs), while also suppressing light-induced halide phase segregation. The champion PCEs of a-FAPbI3 and FA0.65MA0.35Pb(I0.65Br0.35)3 are reported to be 24.9% and 21.2% respectively, with retained PCEs of -90% and -80% after 1,200 and 250 hours of continuous operation. Our results address the critical issue of stability and pave the way for large-scale practical applications of PSCs.
Article
Chemistry, Multidisciplinary
Pinelopi Moutzouri, Manuel Cordova, Bruno Simoes de Almeida, Daria Torodii, Lyndon Emsley
Summary: One key bottleneck of solid-state NMR spectroscopy is the broadness of H-1 NMR spectra of organic solids due to dipolar couplings. A new approach called PIP was suggested to address this problem by mapping errors leading to dipolar broadening and removing them in a correlation experiment. By extending the PIP approach to a second dimension using deep learning, high resolution H-1-H-1 double-quantum/single-quantum dipolar correlation and spin-diffusion spectra were obtained with significantly higher resolution than the corresponding spectra at 100 kHz MAS, allowing the identification of previously overlapped isotropic correlation peaks.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Editorial Material
Chemistry, Physical
Raffaella Buonsanti
CHEMISTRY OF MATERIALS
(2023)
Article
Chemistry, Physical
Aditya Mishra, Michael A. Hope, Gabriele Stevanato, Dominik J. Kubicki, Lyndon Emsley
Summary: Researchers studied cesium lead chloride and found that metal-ion DNP provides the highest bulk sensitivity in this case, while highly surface-selective NMR spectra can be acquired using impregnation DNP. The performance of both methods is explained in terms of the relaxation times, particle size, dopant concentration, and surface wettability.
JOURNAL OF PHYSICAL CHEMISTRY C
(2023)
Article
Chemistry, Multidisciplinary
Valery Okatenko, Anna Loiudice, Mark A. Newton, Dragos C. Stoian, Anastasia Blokhina, Alexander N. Chen, Kevin Rossi, Raffaella Buonsanti
Summary: Researchers have successfully synthesized CuGa nanoparticles and demonstrated that alloying Cu with Ga greatly improves the stability of the nanocatalysts. In particular, CuGa nanoparticles containing 17% Ga preserved most of their CO2RR activity for at least 20 hours, while Cu nanoparticles of the same size reconstructed and lost their CO2RR activity within 2 hours.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Article
Chemistry, Multidisciplinary
Philippe B. Green, Ona Segura Lecina, Petru P. Albertini, Anna Loiudice, Raffaella Buonsanti
Summary: This study presents a method to overcome the limitations of ligand exchange by growing an amorphous alumina shell using colloidal atomic layer deposition (c-ALD). The researchers demonstrate that c-ALD can create colloidally stable composite materials by trapping organic chromophores around the nanocrystal core. This approach allows for unique triplet energy transfer and the assembly of a triplet exciton funnel structure, which cannot be achieved through traditional ligand exchange procedures.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Article
Chemistry, Physical
Kunal Datta, Alessandro Caiazzo, Michael A. Hope, Junyu Li, Aditya Mishra, Manuel Cordova, Zehua Chen, Lyndon Emsley, Martijn M. Wienk, Rene A. J. Janssen
Summary: Photoinduced halide segregation limits the widespread application of three-dimensional mixed-halide perovskites. In this study, we investigate the phenomenon of photoinduced halide segregation in lower-dimensional mixed iodide-bromide perovskites. We find that layered two-dimensional structures exhibit additional stability against halide demixing due to reduced halide mobility, which is supported by solid-state NMR analysis.
ACS ENERGY LETTERS
(2023)
Article
Biochemical Research Methods
Bruno Simoes de Almeida, Daria Torodii, Pinelopi Moutzouri, Lyndon Emsley
Summary: The role of 1H solid-state NMR in structure elucidation of solids is becoming more important, especially with the availability of faster magic-angle spinning rates (MAS) which improve 1H detected assignment strategies. However, the current 1H spectral resolution is still relatively low. This study investigates the factors limiting proton linewidths and line shapes in MAS experiments with five different samples and identifies the different contributions through one-and two-dimensional experiments.
JOURNAL OF MAGNETIC RESONANCE
(2023)
Article
Biochemical Research Methods
Michael A. Hope, Yuxuan Zhang, Amrit Venkatesh, Lyndon Emsley
Summary: Dynamic nuclear polarisation (DNP) using high-spin metal ions, such as Gd3+, can enhance nuclear magnetic resonance (NMR) sensitivity. Spin diffusion and metal site symmetry are factors affecting DNP efficiency. In this study, cubic In(OH)3 was investigated as a high-symmetry proton-containing material for DNP using endogenous Gd3+. A 1H enhancement of up to 9 was achieved, and the clustering of Gd3+ dopants and the local reduction in symmetry of the metal site induced by proton disorder were identified as the reasons for the enhancement. This is the first example of 1H DNP using Gd3+ dopants in an inorganic solid.
JOURNAL OF MAGNETIC RESONANCE
(2023)
Article
Chemistry, Multidisciplinary
Valery Okatenko, Anna Loiudice, Mark A. Newton, Dragos C. Stoian, Anastasia Blokhina, Alexander N. Chen, Kevin Rossi, Raffaella Buonsanti
Summary: Researchers synthesized tunable CuGa nanoparticles and found that alloying Cu with Ga greatly improves the stability of the nanocatalysts in the electrochemical CO2 reduction reaction. Various characterization techniques suggest that the addition of Ga can suppress Cu oxidation and enhance electronic interactions, resulting in the stabilized CuGa nanoparticles.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Article
Chemistry, Multidisciplinary
Valery Okatenko, Coline Boulanger, Alexander N. Chen, Krishna Kumar, Pascal Schouwink, Anna Loiudice, Raffaella Buonsanti
Summary: Studied the chemical reactivity of liquid Ga and Cu nanoparticles and found that the applied voltage and spatial proximity of the particle precursors affected the reaction outcome. The use of liquid Ga/Cu nanodimer precursors resulted in more uniform mixing and reaction products. Adjusting the stoichiometry of Ga and Cu in the nanodimer precursors produced CuGa2 alloys or solid@liquid CuGa2@Ga core@shell nanoparticles. The voltage-driven synthesis was extended to the combination of Ga with other elements.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)