Article
Chemistry, Physical
Dawid Grabarek, Tadeusz Andruniow
Summary: The spectral properties of fluorescent proteins are influenced by their protein environment. By studying the interactions between the chromophore and the environment, researchers have found that modifying hydrogen bonds and electrostatic interactions can enhance the absorption spectra of fluorescent proteins. Additionally, creating a more hydrophilic environment for the chromophore may lead to improved spectral characteristics.
Article
Multidisciplinary Sciences
Yusuke Nasu, Ciaran Murphy-Royal, Yurong Wen, Jordan N. Haidey, Rosana S. Molina, Abhi Aggarwal, Shuce Zhang, Yuki Kamijo, Marie-Eve Paquet, Kaspar Podgorski, Mikhail Drobizhev, Jaideep S. Bains, M. Joanne Lemieux, Grant R. Gordon, Robert E. Campbell
Summary: L-Lactate, traditionally considered a metabolic waste product, is now recognized as an important intercellular energy currency in mammals. A genetically encoded biosensor called eLACCO1.1 has been developed to enable cellular resolution imaging of extracellular L-lactate in cultured mammalian cells and brain tissue.
NATURE COMMUNICATIONS
(2021)
Article
Chemistry, Physical
Leandro H. Zucolotto Cocca, Andre Pelosi, Lucas F. Sciuti, Luis M. G. Abegao, Kenji Kamada, Sandrine Piguel, Cleber Renato Mendonca, Leonardo De Boni
Summary: Imidazopyridine derivatives, as unnatural purine isosteres, have attracted considerable attention due to their wide applicability in various scientific fields. They can be used as fluorescent bioprobes for DNA or RNA spectroscopic studies, and their optical properties can be enhanced by incorporating different structures in the central imidazopyridine scaffold. The research revealed high fluorescence quantum yields and two-photon absorption effects in certain imidazopyridine derivatives, indicating their potential as fluorescent probes induced by two-photon excitation.
JOURNAL OF MOLECULAR LIQUIDS
(2022)
Article
Chemistry, Multidisciplinary
Yuanning Feng, Partha Jyoti Das, Ryan M. Young, Paige J. Brown, Jessica E. Hornick, Jacob A. Weber, James S. W. Seale, Charlotte L. Stern, Michael R. Wasielewski, J. Fraser Stoddart
Summary: In this study, a series of fluorescent dyes with quadrupolar A-D-A constitutions were synthesized and characterized. The effects of different electron-withdrawing groups at the termini of a para-terphenylene backbone were investigated. The fluorescence emission wavelengths covered a range from 380 to 557 nm, and the photophysical properties were attributed to intramolecular charge transfer.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2022)
Article
Chemistry, Physical
Marc de Wergifosse, Pierre Beaujean, Stefan Grimme
Summary: This work presents the theoretical background and a new method for evaluating two-photon absorption cross-sections, and demonstrates its effectiveness through benchmarking against experimental data for large molecules and fluorescent proteins.
JOURNAL OF PHYSICAL CHEMISTRY A
(2022)
Article
Chemistry, Physical
Karan Ahmadzadeh, Mikael Scott, Manuel Brand, Olav Vahtras, Xin Li, Zilvinas Rinkevicius, Patrick Norman
Summary: In this work, computationally tractable expressions for the isotropic second-order hyperpolarizability were derived within the self-consistent field approximation. A novel tensor average formulation was used to evaluate isotropic damped cubic response functions, demonstrating a relative error of less than about 5% compared to the full form. Numerical examples for two-photon absorption cross sections in different photon resonance regions were provided, showing the effectiveness of the simplified expressions.
JOURNAL OF CHEMICAL PHYSICS
(2021)
Article
Chemistry, Organic
Jela Nociarova, Patrik Osusky, Erik Rakovsky, Dimitris Georgiou, Ioannis Polyzos, Mihalis Fakis, Peter Hrobarik
Summary: Direct iodination of benzothiazoles under strong oxidative/acidic conditions results in a mixture of iodinated heteroarenes with 1-2 major components, including 4,7-diiodobenzothiazoles with a rare substitution pattern as dominant products. These compounds have been utilized in the synthesis of a new class of highly efficient quasi-quadrupolar fluorophores, exhibiting large two-photon absorption cross sections in the near-infrared region.
Article
Chemistry, Analytical
Yong-Peng Yang, Fu-Jian Qi, Yi-Ping Qian, Xia-Zhen Bao, Han-Chen Zhang, Bin Ma, Fang Dai, Sheng-Xiang Zhang, Bo Zhou
Summary: The newly developed two-photon probe QBMP showed good binding with NQO1 and exhibited superior properties such as rapid response, large Stokes shift, ultra-low detection limit, favorable two-photon cross section, and deep tissue penetration.
ANALYTICAL CHEMISTRY
(2021)
Article
Chemistry, Physical
Banana Tejendra, Swati Singh Rajput, M. Mehboob Alam
Summary: n-Helicenes and n-Phenylenes are twisted molecules with hindered pi-conjugation. We studied the two-photon absorption in these molecules and found a unique feature in n=7 systems. Our computation reveals a different mechanism of two-photon absorption in twisted n-helicenes and n-phenylenes.
Review
Chemistry, Inorganic & Nuclear
Vinayak Juvekar, Sang Jun Park, Juyoung Yoon, Hwan Myung Kim
Summary: Two-photon microscopy combined with two-photon fluorescent probes enables visualization of metal ion distribution in live tissues, facilitating the development of probes for metal ion detection. Recent progress between 2014 and 2020, including design strategies, history, and specific applications, was summarized in this review.
COORDINATION CHEMISTRY REVIEWS
(2021)
Article
Polymer Science
Martyna Durko-Maciag, Gilles Ulrich, Julien Massue, Jaroslaw Mysliwiec, Konrad Cyprych
Summary: This work demonstrates the successful application of Excited-State Intramolecular Proton Transfer (ESIPT) fluorophores as photoinitiators for microfabrication. The influence of chemical structure on this application was investigated, followed by analysis of two-photon polymerization. The study determined the quality of fabricated structures and polymerization thresholds, with one of the chromophores having an impressively low value of 11 nJ.
EUROPEAN POLYMER JOURNAL
(2023)
Article
Multidisciplinary Sciences
Amr A. A. Attia, Peter Reinholdt, Jacob Kongsted
Summary: The study investigates the application of the polarizable embedding method in DNA complexes and aqueous solutions, finding that the ESO issue affects result accuracy and can be addressed by using ECPs.
ADVANCED THEORY AND SIMULATIONS
(2021)
Article
Chemistry, Physical
Shaoting Guo, Wen Liu, Yuling Wu, Jing Sun, Jie Li, Hongyu Jiang, Mengfan Zhang, Senhao Wang, Zuyuan Liu, Long Wang, Hua Wang, Hongbing Fu, Jiannian Yao
Summary: Understanding the structure-property relationships in organic semiconductors is crucial for controlling their photophysical properties and developing new optoelectronic materials. Quadrupolar molecules, donor-acceptor-donor (DAD), have attracted extensive attention in various optoelectronic applications. The comparative study on the excited state dynamics of DA and DAD fluorescence systems reveals that they exhibit similar excited state dynamics, which are attributed to the distinctive excited-state symmetry breaking (ESSB) phenomenon observed in a DAD system.
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
(2022)
Article
Optics
Xu Zhi, Wenhui Xiang, Ying Qian
Summary: The photosensitizer Lys-PtzFP was designed and synthesized with a unique phenothiazine-anchored strategy, showing high specificity for lysosomes, good photostability, and low cytotoxicity. Under irradiation, Lys-PtzFP can produce singlet oxygen in lysosomes and induce apoptosis.
JOURNAL OF LUMINESCENCE
(2021)
Article
Chemistry, Multidisciplinary
Yanqi Ban, Linhong Hao, Zhenbo Peng, Lishui Sun, Lihua Teng, Yingjie Zhao
Summary: Two star-type push-pull chromophores (T1, T2) based on triphenylamine were designed and synthesized. The structures and molecular arrangement of the chromophores were confirmed by single-crystal X-ray diffraction. The photophysical research of T1 and T2 absorption characteristics and density functional theory (DFT) calculations verified their excellent two-photon absorption (TPA) properties. By adjusting the electronic structures of the chromophores, the TPA performance of the small organic molecule could be greatly enhanced, making them promising candidates for various two-photon applications.
CHINESE CHEMICAL LETTERS
(2023)
Article
Chemistry, Physical
Antoine Aerts, Pascal Kockaert, Simon-Pierre Gorza, Alex Brown, Jean Vander Auwera, Nathalie Vaeck
Summary: This study proposes a methodology to control a non-stationary dark ro-vibrational state of acetylene using laser pulse shaping. The quality of the control parameters is assessed, and the effects of experimental limitations on the control performance are investigated. The results provide insights into the control mechanism and lay the foundation for future realistic experiments.
JOURNAL OF CHEMICAL PHYSICS
(2022)
Article
Chemistry, Physical
Antoine Aerts, Moritz R. Schaefer, Alex Brown
Summary: A semi-automatic sampling and fitting procedure is presented for generating sum-of-product potential energy surfaces based on a high-dimensional model representation. The method relies on energies only and can be used for re-fitting existing analytic potential energy surfaces or for direct fits from ab initio computations. The results show that the procedure leads to accurate potential energy surfaces with fewer sampling points and fitting parameters.
JOURNAL OF CHEMICAL PHYSICS
(2022)
Article
Chemistry, Physical
Antoine Aerts, Alex Brown, Fabien Gatti
Summary: The intramolecular vibrational relaxation dynamics of formic acid and its deuterated isotopologues were simulated on a full-dimensional potential energy surface. Couplings between the C-O stretch and torsion vibrational modes were observed, and the possibility of laser-induced trans-to-cis isomerization was discussed. Strong isotopic effects were found, with deuteration of the hydroxyl group destroying the coupling in certain cases.
JOURNAL OF CHEMICAL PHYSICS
(2022)
Article
Chemistry, Physical
Nathanael J. King, Alex Brown
Summary: In this work, the conformer-rotamer ensemble sampling tool (CREST) with the GFN2-xtb method was used to explore the geometry of homodimers and heterodimers of pyrene compounds. The effects of oxidation on the dimerization process and the accuracy of the omega B97X-D4 approach were also investigated.
JOURNAL OF PHYSICAL CHEMISTRY A
(2022)
Article
Nanoscience & Nanotechnology
Geng Xie, Minh Tang, Shihong Xu, Alex Brown, Lingzi Sang
Summary: All-solid-state sodium batteries are sustainable systems for large-scale energy storage and electric transportation, utilizing earth-abundant elements. The use of solid-state electrolytes instead of flammable carbonate-based electrolytes enhances battery safety and does not require packaging for fabricating tandem cells, potentially leading to improved energy density.
ACS APPLIED MATERIALS & INTERFACES
(2022)
Article
Chemistry, Physical
Labanya Bhattacharya, Alex Brown, Sagar Sharma, Sridhar Sahu
Summary: This study designs a series of nonfullerene acceptors for photovoltaic applications. The investigated acceptors show air-stability, sufficient open-circuit voltage, and fill factor. They also exhibit better electron mobility and efficient light-harvesting when blended with PM6.
JOURNAL OF PHYSICAL CHEMISTRY A
(2022)
Article
Chemistry, Physical
Shyam Parshotam, Benjamin Rehl, Franziska Busse, Alex Brown, Julianne M. Gibbs
Summary: Vibrational spectroscopy is a powerful tool for determining local hydrogen-bonding environment, but vibrational coupling in H2O makes it difficult to apply. This study reveals the influence of vibrational coupling on interface spectra and investigates the effect of pH variation on the spectra.
JOURNAL OF PHYSICAL CHEMISTRY C
(2022)
Article
Chemistry, Physical
Shyam Parshotam, Wentong Zhang, Benjamin Rehl, Akemi Darlington, Md. Delwar H. Sikder, Alex Brown, Julianne M. Gibbs
Summary: Isolating the contribution of silica in second harmonic generation (SHG) studies at the silica/water interface remains a challenge. Here, we compare SHG intensities with zeta potentials and vibrational sum frequency generation (SFG) intensities to understand the silica contribution in SHG measurements. The results suggest a significant pH-dependent increase in the silica contribution, which can interfere constructively or destructively with water. The study also demonstrates the direct sensitivity of SHG to surface charging, indicating its potential as a powerful tool in studying other mineral oxides.
JOURNAL OF PHYSICAL CHEMISTRY C
(2023)
Editorial Material
Chemistry, Multidisciplinary
Russell J. Boyd, Alex Brown, Gino A. DiLabio, Stacey D. Wetmore
CANADIAN JOURNAL OF CHEMISTRY
(2023)
Article
Energy & Fuels
Nathanael J. J. King, Alex Brown
Summary: This paper investigated the aggregation of asphaltene model compounds using a combination of GFN2-xtb and DFT. The possible stoichiometries and conformations of the complexes were explored and compared to experimental results. The study found that there are four possible complexes with large equilibrium constants of formation, and both hydrogen bonding and π-π stacking play important roles in this aggregation. Water-mediated aggregation and coordination to open porphyrin sites were not significant in this system. The Gibbs free energies of association were determined for various complexes, and factors influencing NMR chemical shift were briefly explored.
Article
Chemistry, Physical
Mahsa Nazemi Ashani, Qinan Huang, A. Mackenzie Flowers, Alex Brown, Antoine Aerts, Alberto Otero-de-la-Roza, Gino A. Dilabio
Summary: The β-density functional theory (β-DFT) approach based on atom-centered potentials (ACPs) is shown to be a computationally inexpensive and accurate method for representing potential energy surfaces (PESs) and calculating vibrational frequencies for HONO and HFCO molecules. The ACP-corrected PESs produce small mean absolute errors and compared favorably to the results obtained with higher level of theory. This approach shows promise for representing accurate molecular PESs and calculating molecular properties.
JOURNAL OF PHYSICAL CHEMISTRY A
(2023)
Article
Chemistry, Physical
Ismael. A. A. Elayan, Alex Brown
Summary: The study investigates the cross-sections (sigma(2PA)) of two-photon absorption (2PA) spectroscopy using TD-DFT and 2-state model (2SM). It reveals that the cross-sections of ND-2PA are enhanced compared to D-2PA. This work is important for future research on the photophysical properties of different fluorophores and the application of ND-2PA.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2023)
Article
Chemistry, Physical
Shyam Parshotam, Benjamin Rehl, Alex Brown, Julianne M. Gibbs
Summary: Nonlinear optical methods are powerful techniques for studying structures at charged buried interfaces. This study provides a physically motivated understanding of the error phase and shows its correlation with the response of the interface. The results highlight the sensitivity of the error phase to interface variations and the possibility of using the error phase model to predict complex spectra.
JOURNAL OF CHEMICAL PHYSICS
(2023)
Article
Chemistry, Physical
Labanya Bhattacharya, Alex Brown, Sagar Sharma, Sridhar Sahu
Summary: This study aims to design and evaluate a series of nonfullerene acceptors for photovoltaic applications. The results show that these acceptors exhibit air stability, sufficient open-circuit voltage and fill factor, and have the potential to be promising electron transporting acceptor materials in organic photovoltaic cells.
JOURNAL OF PHYSICAL CHEMISTRY A
(2022)
Article
Biochemistry & Molecular Biology
Landon Zarowny, Damien Clavel, Ryan Johannson, Kevin Duarte, Hadrien Depernet, Jerome Dupuy, Heather Baker, Alex Brown, Antoine Royant, Robert E. Campbell
Summary: In this study, we successfully created a new fluorescent protein, NeonCyan1, and two additional mutants with distinct spectral hues through modification of mNeonGreen. Structural, computational, and photophysical characterization of these proteins provided insight into the factors that control the fluorescence emission color. Although not recommended as replacements for contemporary fluorescent proteins, these new variants demonstrate potential suitability for live cell imaging applications.
PROTEIN ENGINEERING DESIGN & SELECTION
(2022)