Article
Chemistry, Physical
Eduarda Sangiogo Gil, Maurizio Persico, Giovanni Granucci
Summary: We performed computational simulations on the photodynamics of ABPT SAM on a gold surface. Our results showed that excitation energy transfer between chromophores occurs quickly in the pp* manifold, but not between np* states. As a result, excitation transfer does not play a significant role in the quenching of azobenzene photoisomerization in the SAM, which is instead attributed to steric effects.
JOURNAL OF CHEMICAL PHYSICS
(2022)
Article
Chemistry, Analytical
Olivier Aleveque, Eric Levillain
Summary: This methodology is based on the frequency dependence of the phase angle in Alternative Voltammetry to estimate the standard electrochemical rate constant for heterogeneous electron transfer reactions with strong intermolecular interactions occurring between the redox forms.
JOURNAL OF ELECTROANALYTICAL CHEMISTRY
(2022)
Review
Chemistry, Multidisciplinary
Limin Wang, Ulrich S. Schubert, Stephanie Hoeppener
Summary: Surface modification using self-assembled monolayers has seen significant advancement in the past decade, with the introduction of new chemical reactions such as nucleophilic substitution, click chemistry, supramolecular modification, photochemical reaction, and others, enhancing the properties of solid substrates like silicon and glass.
CHEMICAL SOCIETY REVIEWS
(2021)
Article
Chemistry, Multidisciplinary
Christopher A. Petroff, Giuseppe Cassone, Jiri Sponer, Geoffrey R. Hutchison
Summary: This study presents novel piezoelectric force and touch sensors based on self-assembled monolayers of oligopeptides, which show large piezoelectric voltage response and are easily manufactured. Despite modest piezoelectric charge constants, the devices exhibit immense piezoelectric voltage constants. Additionally, a flexible device prototype with high open-circuit voltages is demonstrated, with potential for further improvements in voltage response through peptide selection and device construction.
ADVANCED MATERIALS
(2021)
Article
Chemistry, Multidisciplinary
Dennis Meier, Abhishek K. Adak, Peter Knecht, Joachim Reichert, Sourav Mondal, Nithin Suryadevara, Senthil Kumar Kuppusamy, Keitaro Eguchi, Matthias K. Muntwiler, Francesco Allegretti, Mario Ruben, Johannes V. Barth, Shobhana Narasimhan, Anthoula C. Papageorgiou
Summary: Tailored nano-spaces can control enantioselective adsorption and molecular motion through the spontaneous assembly of a dynamic system on Ag(111) using 2,6-bis(1H-pyrazol-1-yl)pyridine-4-carboxylic acid. The network cavity snugly hosts the chemically modified guest, bestows enantiomorphic adsorption, and allows selective rotational motions. Hydrogen bonding plays a crucial role in stabilizing the rotating guest and influencing the energy landscape formation.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2021)
Article
Nanoscience & Nanotechnology
Mingliang Li, Yingnan Cao, Kefeng Xie, Jinyao Tang
Summary: Self-assembled monolayers (SAMs) have been extensively applied in various functional devices due to their transparency, diversity, stability, sensitivity, selectivity, and great potential in surface passivation. By investigating the relationship between SAM quality and device performance in detail, efficient feedback for system optimization can be provided.
ADVANCED ELECTRONIC MATERIALS
(2023)
Article
Chemistry, Physical
Jin Yang, Mingyong Zhou, Jiezhen Liu, Hao Wang, Can Weng
Summary: It was found that using alkanethiols SAMs to modify the Ni substrate could significantly reduce the surface adhesion of Ni substrate and lower the friction coefficient. Mixed alkanethiols SAMs exhibited better lubricity and wear resistance compared to SAMs of single component.
APPLIED SURFACE SCIENCE
(2021)
Article
Materials Science, Multidisciplinary
Xinyan Yang, Junqing Leng, Cheng Sun, Sinan Keten
Summary: Magneto-elastic materials with shape programmability, adaptive stiffness, and tunable strength are crucial for advances in structural and robotic materials. We present a novel design for elastic bars with permanent fixed dipole magnets, which can self-assemble into magneto-elastic networks under random vibrations. The orientation of end dipoles determines the self-assembled network topology, which can range from quasi-ordered lattices to stacks or strings of particles. This work establishes design criteria for stable lightweight 2D networks and paves the way for self-assembled and repaired structural materials with random vibrations, expanding the applications of magneto-elastic soft materials.
ADVANCED MATERIALS TECHNOLOGIES
(2023)
Article
Chemistry, Physical
Rui Yan, Andreas Terfort, Michael Zharnikov
Summary: The study investigated the effect of wavelength on the modification of archetypical nonsubstituted alkanethiolate self-assembled monolayers on gold surfaces by ultraviolet light. The results provided insights into the behavior of UV-induced processes under different wavelengths and offered a useful tool for estimating proper dosage ranges in applications involving modification of AT-SAMs and thiolate SAMs.
JOURNAL OF PHYSICAL CHEMISTRY C
(2021)
Article
Chemistry, Multidisciplinary
Shakil N. N. Afraj, Chun-Hsiao Kuan, Jian-Sing Lin, Jen-Shyang Ni, Arulmozhi Velusamy, Ming-Chou Chen, Eric Wei-Guang Diau
Summary: Four X-shaped quinoxaline-based organic dyes, PQx (1), TQx, (2), PQxD (3), and TQxD (4), are developed as p-type self-assemble monolayer (SAM) for tin perovskite solar cells (TPSC). The thermal, optical, and electrochemical properties of these SAMs are thoroughly investigated. Tin perovskite layers are successfully deposited on these SAM surfaces using a two-step approach, and the achieved device performance follows the order of TQxD (8.3%) > TQx (8.0%) > PQxD (7.1%) > PQx (6.1%). Among them, TQxD (4), with a thiophene pi-extended conjugation unit in the SAM structure, exhibits the highest hole extraction rates, greatest hole mobilities, and slowest charge recombination, leading to the best reported efficiency of 8.3% for SAM-based TPSC. Moreover, all devices except PQx show good enduring stability, retaining approximately 90% of their original values after 1600 hours of shelf storage.
ADVANCED FUNCTIONAL MATERIALS
(2023)
Article
Chemistry, Multidisciplinary
Heng Wang, Li-Peng Zhou, Yu Zheng, Kun Wang, Bo Song, Xuzhou Yan, Lukasz Wojtas, Xu-Qing Wang, Xin Jiang, Ming Wang, Qing-Fu Sun, Bingqian Xu, Hai-Bo Yang, Andrew C. -H. Sue, Yi-Tsu Chan, Jonathan L. Sessler, Yang Jiao, Peter J. Stang, Xiaopeng Li
Summary: Supramolecular cages/vesicles in biology demonstrate complex structures and functions by utilizing a few types of protein subunits quasi-equivalently at distinct geometrical locations. Synthetic supramolecular cages lack comparable complexity to natural systems. Self-assembled giant pentagonal supramolecular prisms with tetratopic pyridinyl subunits exhibit unexpected three-fold rotational symmetry in a novel superstructure, providing a new approach to construct highly sophisticated supramolecular architectures.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2021)
Article
Chemistry, Multidisciplinary
Katarina Marusic, Ena Pezic, Nives Matijakovic Mlinaric, Pavo Dubcek, Jordi Sancho-Parramon, Damir Kralj, Branka Mihaljevic
Summary: Self-assembled monolayers (SAMs) are an important element of modern nanotechnology and surface functionalization. However, their application is limited due to their vulnerability in corrosive environments. This study demonstrates for the first time how to strongly crosslink SAMs made of non-toxic and biodegradable fatty acids on metal surfaces using ionizing radiation, resulting in stable crosslinked nanocoatings with significantly improved properties compared to SAMs. Crosslinking opens up the possibility of using SAMs in various systems and on different materials for achieving stable and durable surface properties.
Article
Chemistry, Physical
Georgios Stratis, Jordan D. Zesch, Henry S. Pan, Lauren J. Webb, Mark G. Raizen
Summary: This study presents a minimally invasive in situ probe for detecting real-time damage in organic materials. Specifically, metastable excited helium atoms in the S-3(1) state are used to characterize the damage induced by a low-energy electron beam on organic materials.
JOURNAL OF CHEMICAL PHYSICS
(2021)
Article
Chemistry, Physical
Badri P. Mainali, Dhruba K. Pattadar, Francis P. Zamborini
Summary: The oxidation resistance of gold nanoparticles has a unique reverse size dependence for thiolate-coated nanoparticles, where the extent of oxidation increases with size, opposite to weakly stabilized or bare gold nanoparticles.
JOURNAL OF PHYSICAL CHEMISTRY C
(2021)
Article
Chemistry, Physical
A. Brady-Boyd, R. O'Connor, S. Armini, V Selvaraju, M. Pasquali, G. Hughes, J. Bogan
Summary: This study investigates the effects of using self-assembled monolayers (SAMs) for area-selective atomic layer deposition (AS-ALD) by examining the etch rates of two different SAMs. The results show that the etch rate is distinct for each SAM, providing insights for selecting the appropriate SAM for AS-ALD applications.
APPLIED SURFACE SCIENCE
(2022)
Article
Chemistry, Physical
Yuxuan Yao, William L. Hase, Giovanni Granucci, Maurizio Persico
Summary: The research compares algorithms for sampling initial positions and momenta in a molecular system for classical trajectory simulations. The goal is to reproduce the phase space quantum distribution for a vibrational eigenstate, as in Wigner theory. Two approaches are introduced to address the issue of controlling total energy and energy partition among vibrational modes.
JOURNAL OF CHEMICAL PHYSICS
(2021)
Article
Chemistry, Physical
Giovanni Granucci, Giancarlo Padula
Summary: In this study, a computational investigation was conducted on the photoisomerization of SP to merocyanine, with optimized parameters of the semiempirical Hamiltonian and consideration of the impact of excited states on dynamics simulations. The results showed that the photoisomerization quantum yield depends on the electronic state initially populated.
JOURNAL OF CHEMICAL PHYSICS
(2021)
Article
Chemistry, Physical
Davide Accomasso, Serra Arslancan, Lorenzo Cupellini, Giovanni Granucci, Benedetta Mennucci
Summary: Carotenoids, as natural pigments, play multiple important roles in photosynthesis, and their structure and photophysical properties play a key role in their functions.
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
(2022)
Article
Chemistry, Physical
Eduarda Sangiogo Gil, Maurizio Persico, Giovanni Granucci
Summary: We performed computational simulations on the photodynamics of ABPT SAM on a gold surface. Our results showed that excitation energy transfer between chromophores occurs quickly in the pp* manifold, but not between np* states. As a result, excitation transfer does not play a significant role in the quenching of azobenzene photoisomerization in the SAM, which is instead attributed to steric effects.
JOURNAL OF CHEMICAL PHYSICS
(2022)
Article
Chemistry, Physical
Mario Barbatti, Mattia Bondanza, Rachel Crespo-Otero, Baptiste Demoulin, Pavlo O. Dral, Giovanni Granucci, Fabris Kossoski, Hans Lischka, Benedetta Mennucci, Saikat Mukherjee, Marek Pederzoli, Maurizio Persico, Max Pinheiro, Jiri Pittner, Felix Plasser, Eduarda Sangiogo Gil, Ljiljana Stojanovic
Summary: Newton-X is an open-source computational platform that implements nonadiabatic molecular dynamics based on surface hopping and spectrum simulations. It describes the main features of these methods and highlights the latest developments. These methods are widely used in computational chemistry for photo-physical and photochemical investigations, making them of great importance for understanding molecular dynamics.
JOURNAL OF CHEMICAL THEORY AND COMPUTATION
(2022)
Article
Multidisciplinary Sciences
Giacomo Salvadori, Veronica Macaluso, Giulia Pellicci, Lorenzo Cupellini, Giovanni Granucci, Benedetta Mennucci
Summary: The authors use computational simulations to uncover the molecular mechanism of photoactivation in phytochromes, the photoreceptors responsible for sensing light in plants, fungi, and bacteria. They find that chromophore-protein interactions play a crucial role in controlling the mechanism and timescale of the photoisomerization process.
NATURE COMMUNICATIONS
(2022)
Article
Chemistry, Physical
Manuel Perez-Escribano, Joanna Jankowska, Giovanni Granucci, Daniel Escudero
Summary: In this article, the radiative surface hopping algorithm is presented, which allows modeling fluorescence within a semi-classical non-adiabatic molecular dynamics framework. The algorithm has been tested for the photodeactivation dynamics of trans-4-dimethylamino-4'-cyanostilbene (DCS). By treating radiative and non-radiative processes equally, the method provides a complete molecular movie of the excited-state deactivation. The proposed approach successfully captures the first fluorescence processes in DCS and reproduces the experimental fluorescence lifetime and quantum yield.
JOURNAL OF CHEMICAL PHYSICS
(2023)
Article
Chemistry, Physical
Carlotta Pieroni, Filippo Becuzzi, Luigi Creatini, Giovanni Granucci, Maurizio Persico
Summary: We tested different sampling methods of initial conditions in surface hopping simulations, focusing on initial energy distributions and the treatment of zero point energy (ZPE). Using the gas phase photodynamics of azomethane as a test case, we found that most quantum mechanical (QM) and classical Boltzmann (CB) approaches yielded similar results in short time dynamics and decay lifetimes. However, the sampling method significantly affected the rate of ground state dissociation reaction, with QM samplings showing higher rates due to the leaking of ZPE.
JOURNAL OF CHEMICAL THEORY AND COMPUTATION
(2023)
Article
Chemistry, Physical
Davide Accomasso, Nadia Ben Amor, Maurizio Persico, Giovanni Granucci
Summary: We describe two computational approaches for designing covalently bound dimers for singlet fission. The goal is to maximize the coupling between the singlet excited state and the double triplet state by adjusting the interaction between the chromophore units. In Design I, we search for optimal arrangements of chromophores in a stacked pair geometry and then connect them covalently. In Design II, we consider all viable ways to bind the chromophores covalently and identify the most promising dimers for singlet fission from our tested candidates. These approaches have successfully led to the design of promising dimers with large singlet-triplet couplings and favorable energetics.
JOURNAL OF PHOTOCHEMISTRY AND PHOTOBIOLOGY A-CHEMISTRY
(2023)
Article
Materials Science, Biomaterials
Silvio Osella, Giovanni Granucci, Maurizio Persico, Stefan Knippenberg
Summary: This computational study investigates the photoisomerization mechanism of the azobenzene molecule in a DPPC lipid membrane. The trans-to-cis isomerization is shown to be a slow process controlled by a torsional mechanism due to strong environmental interaction, while the cis-to-trans mechanism occurs rapidly in sub-ps time scale and is governed by a pedal-like mechanism involving weaker environmental interactions and a different potential energy surface geometry.
JOURNAL OF MATERIALS CHEMISTRY B
(2023)
Article
Chemistry, Multidisciplinary
Luca D'Amario, Maria Bruna Stella, Tomas Edvinsson, Maurizio Persico, Johannes Messinger, Holger Dau
Summary: This study describes a transient spectro-electrochemical Raman setup that achieves sub-ms time resolution, allowing for the study of electrochemical processes. The technique was validated through experiments and confirmed to be effective in assigning spectral properties to transient species. This research provides a foundational contribution to the development of next generation electrolizers, fuel cells, and batteries.
