Article
Optics
Peter L. Hagelstein
Summary: A moving nucleus undergoes Lorentz contraction and spin rearrangement due to relativity. Vibrations in a molecule or solid cause minor relativistic modifications in a oscillating nucleus, indicating a relativistic phonon-nuclear interaction. The derivation of the lowest-order interaction is reviewed using the many-particle Dirac model. The lowest-order phonon-nuclear interaction obtained from the covariant two-body Bethe-Salpeter model is similar to the interaction obtained from the Dirac model, indicating that it is not an artifact. Matrix elements of the lowest-order interaction are expressed in terms of one-body operators, facilitating evaluation and quantitative estimation of the magnitude.
JOURNAL OF PHYSICS B-ATOMIC MOLECULAR AND OPTICAL PHYSICS
(2023)
Article
Materials Science, Multidisciplinary
David Amblard, Gabriele D'Avino, Ivan Duchemin, Xavier Blase
Summary: Defect energy levels in hexagonal boron nitride with varying number of layers were studied using a fragment many-body GW formalism. It was found that a single layer can be fragmented to faithfully reproduce the effect of the dielectric environment. The evolution of defect energy levels from monolayer to multilayer systems follows a simple pattern, allowing safe extrapolation of results to few layers, surface, or bulk h-BN.
PHYSICAL REVIEW MATERIALS
(2022)
Article
Computer Science, Information Systems
Pengjia Tu, Junhuai Li, Huaijun Wang, Ting Cao, Kan Wang
Summary: This paper proposes a novel method for human activity recognition based on non-linear chaotic features using human motion accelerometer sensor data. Optimal delay time and embedding dimension are calculated using the C-C method and G-P algorithm, and a two-dimensional chaotic feature matrix is constructed for activity classification. Experimental results show that the chaotic feature outperforms traditional time and frequency domain features in accuracy.
Article
Chemistry, Physical
Iryna Knysh, Kelvine Letellier, Ivan Duchemin, Xavier Blase, Denis Jacquemin
Summary: The study investigates the mixing between charge transfer (CT) and local excited (LE) characters upon twisting of N-phenylpyrrole (N-PP) geometry using theoretical calculations of six low-lying singlet excited states (ES). Results show that the Bethe-Salpeter equation (BSE) formalism is more reliable than Time-Dependent Density Functional Theory (TD-DFT) for close-lying ES with mixed CT/LE nature. BSE/GW provides a more accurate evolution of the excited state potential energy surfaces (PES) with negligible exchange-correlation functional starting point dependency.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2023)
Article
Chemistry, Physical
Yi Yao, Dorothea Golze, Patrick Rinke, Volker Blum, Yosuke Kanai
Summary: We present an accurate computational approach to calculate absolute K-edge core electron excitation energies as measured by X-ray absorption spectroscopy. The method is based on the Bethe-Salpeter equation and GW quasiparticle energies, and takes into account various numerical approximations and basis sets. The results show excellent agreement with experimental data, demonstrating the high accuracy of the method.
JOURNAL OF CHEMICAL THEORY AND COMPUTATION
(2022)
Article
Chemistry, Physical
Johannes Toelle, Johannes Neugebauer
Summary: This Perspective article outlines the theoretical foundations and commonly used practical realizations of photoinduced processes in multichromophoric systems using the subsystem time-dependent density functional theory (sTDDFT). The article also discusses the benefits of recent developments, open issues, prospective applications, and possible methodological developments in the field of sTDDFT.
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
(2022)
Article
Chemistry, Physical
Paul N. Day, Ruth Pachter, Kiet A. Nguyen
Summary: In this study, theoretical investigations were carried out on phosphine-ligated gold clusters using mass-selective electronic absorption photofragmentation spectroscopy. The calculated optical absorption spectra showed good agreement with experimental measurements. The study also included a theoretical evaluation of two-photon absorption cross-sections.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2022)
Article
Chemistry, Physical
Yi Yao, Dorothea Golze, Patrick Rinke, Volker Blum, Yosuke Kanai
Summary: This article presents an accurate computational approach to calculate absolute K-edge core electron excitation energies using numeric atom-centered orbitals (NAOs). The method is validated by comparing the results with experimental data and demonstrates excellent agreement.
JOURNAL OF CHEMICAL THEORY AND COMPUTATION
(2022)
Article
Materials Science, Multidisciplinary
Michael Winter, Manon H. E. Bousquet, Denis Jacquemin, Ivan Duchemin, Xavier Blase
Summary: The study revealed a luminescence zero-phonon energy of 4.36 eV in the carbon-dimer defect in h-BN monolayer, including contributions from zero-point vibrational energy and reorganization energy. Interlayer screening further decreased the emission energy by about 0.3 eV. The comparisons with optical gaps suggested a large excitonic binding energy of 3 eV for the associated localized Frenkel exciton.
PHYSICAL REVIEW MATERIALS
(2021)
Article
Chemistry, Physical
Pierre-Francois Loos, Massimiliano Comin, Xavier Blase, Denis Jacquemin
Summary: This study provides highly accurate vertical transition energies for intramolecular charge-transfer transitions in (pi-conjugated) molecular compounds, and validates these transitions using a variety of wave functions and methods.
JOURNAL OF CHEMICAL THEORY AND COMPUTATION
(2021)
Article
Engineering, Biomedical
Yong Peng, Honggang Liu, Junhua Li, Jun Huang, Bao-Liang Lu, Wanzeng Kong
Summary: This paper proposes a Joint label-Common and label-Specific Features Exploration (JCSFE) model for semi-supervised cross-session EEG emotion recognition. The experimental results demonstrate that JCSFE achieves superior emotion recognition performance and provides a quantitative method to identify the label-common and label-specific EEG features in emotion recognition.
IEEE TRANSACTIONS ON NEURAL SYSTEMS AND REHABILITATION ENGINEERING
(2023)
Article
Engineering, Electrical & Electronic
M. S. Arun Sankar, P. S. Sathidevi
Summary: There is a growing demand for voice-activated applications due to the significant growth of mobile devices and services. It is important to capture individual speaker characteristics in addition to the relevant information in the speech signal. This paper proposes a wideband scalable bit rate speech coder that efficiently represents excitation using glottal instants and linear predictive coding based on the mel scale.
CIRCUITS SYSTEMS AND SIGNAL PROCESSING
(2023)
Article
Biochemistry & Molecular Biology
Rahul D. Jawarkar, Ravindra L. Bakal, Nobendu Mukherjee, Arabinda Ghosh, Magdi E. A. Zaki, Sami A. AL-Hussain, Aamal A. Al-Mutairi, Abdul Samad, Ajaykumar Gandhi, Vijay H. Masand
Summary: This study develops robust quantitative structure-activity relationship (QSAR) models for LSD1/KDM1A inhibitors, identifying critical pharmacophoric features and confirming their binding to the LSD1 receptor through molecular docking experiments. The findings can be used to produce potential anticancer drugs targeting LSD1/KDM1A.
Article
Chemistry, Physical
Elizaveta F. Petrusevich, Manon H. E. Bousquet, Borys Osmialowski, Denis Jacquemin, Josep M. Luis, Robert Zalesn
Summary: This study proposes an efficient first-principles protocol for simulating vibrationally-resolved absorption spectra. It analyzes the selection of density functional approximation (DFA), vibrational structure schemes, and the use of machine learning for estimating broadening. The results show accurate band shapes and reduced CPU time.
JOURNAL OF CHEMICAL THEORY AND COMPUTATION
(2023)
Article
Chemistry, Physical
Isabella C. D. Merritt, Denis Jacquemin, Morgane Vacher
Summary: In this study, the impact of various approximation schemes for the coupling term in the trajectory surface hopping (TSH) method is investigated. It is found that two tested schemes, the local diabatization scheme and the biorthonormal wave function overlap scheme, can reproduce the dynamics obtained using explicitly calculated nonadiabatic coupling vectors at a much lower cost. The other two schemes can give different and even incorrect dynamics.
JOURNAL OF CHEMICAL THEORY AND COMPUTATION
(2023)
Article
Chemistry, Physical
Iryna Knysh, Jose D. J. Villalobos-Castro, Ivan Duchemin, Xavier Blase, Denis Jacquemin
Summary: The change of molecular dipole moment induced by photon absorption is important for interpreting optical spectra. While time-dependent density functional theory (TD-DFT) is commonly used to predict excited-state dipoles (mu(ES)), this study shows that the many-body Green's function Bethe-Salpeter equation (BSE) is a valuable alternative with decreased dependency on exchange-correlation functional. The BSE method is not only suitable for transition energies and oscillator strengths, but also for properties related to the excited-state density.
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
(2023)
Correction
Chemistry, Physical
Iryna Knysh, Jose D. J. Villalobos-Castro, Ivan Duchemin, Xavier Blase, Denis Jacquemin
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
(2023)
Article
Chemistry, Physical
J. Villalobos-Castro, Iryna Knysh, Denis Jacquemin, Ivan Duchemin, Xavier Blase
Summary: We propose a method for calculating excited-state analytic gradients in the Bethe-Salpeter equation formalism. The method uses an adapted Lagrangian Z-vector approach to achieve a cost independent of the number of perturbations. We evaluate the accuracy of common approximations in the Bethe-Salpeter community and compare the results with time-dependent density-functional theory (TD-DFT) data.
JOURNAL OF CHEMICAL PHYSICS
(2023)
Article
Chemistry, Physical
Manon H. E. Bousquet, Thomas V. V. Papineau, Koen Veys, Daniel Escudero, Denis Jacquemin
Summary: Defining a theoretical model for accurately predicting the fluorescence quantum yields of organic dyes is important in designing improved fluorophores systematically. This study analyzed the impact of different computational parameters on the determination of reliable radiative rates (k (r)) using time-dependent density functional theory calculations. The results showed that the chosen vibronic model, especially the potential energy surface model, had a significant impact on the computed k (r) and the difference observed between different exchange-correlation functionals. However, all evaluated functionals yielded reasonable trends for the treated compounds, fitting the experimental values.
JOURNAL OF CHEMICAL THEORY AND COMPUTATION
(2023)
Article
Chemistry, Physical
Xiaorui Zhao, Isabella C. D. Merritt, Ruiqing Lei, Yinan Shu, Denis Jacquemin, Linyao Zhang, Xuefei Xu, Morgane Vacher, Donald G. Truhlar
Summary: This work discusses nonadiabatic TSH dynamics algorithms employing the curvature-driven approximation and overlap-based time derivative couplings, and presents test calculations on six photochemical reactions. The results show good agreement between the curvature-driven algorithms and overlap-based algorithms.
JOURNAL OF CHEMICAL THEORY AND COMPUTATION
(2023)
Article
Chemistry, Organic
Timothee Stoerkler, Gilles Ulrich, Adele D. Laurent, Denis Jacquemin, Julien Massue
Summary: This study presents the synthesis of fluorophores containing triphenylamine derivatives and explores their photophysical, electrochemical, and electronic structure properties. The compounds exhibit excited-state intramolecular proton transfer, with different photophysical processes observed depending on the nature of the conjugated scaffold. The photophysical properties are further explained by ab initio calculations.
JOURNAL OF ORGANIC CHEMISTRY
(2023)
Article
Chemistry, Physical
Isabella C. D. Merritt, Denis Jacquemin, Morgane Vacher
Summary: This study benchmarks the impact of different approximations to the nonadiabatic coupling term on the trajectory surface hopping (TSH) dynamics of isomerization and ring-opening reactions. It is found that the popular local diabatization scheme and a scheme based on biorthonormal wave function overlap in the OpenMOLCAS code can reproduce the dynamics obtained using explicitly calculated nonadiabatic coupling vectors at a reduced cost. However, the other two schemes tested can give different and even incorrect results.
JOURNAL OF CHEMICAL THEORY AND COMPUTATION
(2023)
Article
Chemistry, Physical
Iryna Knysh, Kelvine Letellier, Ivan Duchemin, Xavier Blase, Denis Jacquemin
Summary: The study investigates the mixing between charge transfer (CT) and local excited (LE) characters upon twisting of N-phenylpyrrole (N-PP) geometry using theoretical calculations of six low-lying singlet excited states (ES). Results show that the Bethe-Salpeter equation (BSE) formalism is more reliable than Time-Dependent Density Functional Theory (TD-DFT) for close-lying ES with mixed CT/LE nature. BSE/GW provides a more accurate evolution of the excited state potential energy surfaces (PES) with negligible exchange-correlation functional starting point dependency.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2023)
Article
Materials Science, Multidisciplinary
Nicolas Ledos, Denis Tondelier, Bernard Geffroy, Denis Jacquemin, Pierre-Antoine Bouit, Muriel Hissler
Summary: We synthesized and characterized benzophosphole oxides with an ethoxy substituent on the P atom and electro-donating amino groups on the lateral phenyl groups. The optical and redox properties of these compounds were studied experimentally and computationally. The nature of the donor was shown to fine-tune the internal charge transfer and optical properties. These compounds were used in multilayered organic light emitting devices due to their intense fluorescence, favorable redox and thermal properties. One compound even achieved an external quantum efficiency of 5%, highlighting the potential of this novel family of fluorophores for next generation optoelectronic/photonic devices.
JOURNAL OF MATERIALS CHEMISTRY C
(2023)
Review
Chemistry, Physical
Mariana T. do Casal, Koen Veys, Manon H. E. Bousquet, Daniel Escudero, Denis Jacquemin
Summary: In this Perspective, recent advances in evaluating excited-state decay rate constants of organic fluorophores from first-principles are discussed, focusing on the static strategy. The static strategy utilizes Fermi's golden rule to evaluate rate constants at key points of the potential energy surfaces, and the radiative rate constant can be obtained by integrating the fluorescence line shape determined from vibronic calculations. The use of Fermi's golden rule also enables the calculation of internal conversion and intersystem crossing rates, providing estimates of emission yields when complex photophysical phenomena are not present.
JOURNAL OF PHYSICAL CHEMISTRY A
(2023)
Article
Chemistry, Multidisciplinary
Thomas Castaing-Cordier, Selina Crasnier, Damien Dubois, Virginie Ladroue, Audrey Bulete, Cedric Prudhomme, Celine Charvoz, Fabrice Besacier, Denis Jacquemin, Patrick Giraudeau, Jonathan Farjon
Summary: This article introduces an efficient analytical method for identifying new psychoactive substances (NPS) using compact nuclear magnetic resonance (NMR) spectrometry in combination with databases. The article presents an improved strategy that utilizes non-uniform sampling (NUS) to enhance spectral resolution, thus improving the accuracy of NPS identification.
MAGNETIC RESONANCE IN CHEMISTRY
(2023)
Article
Chemistry, Multidisciplinary
John A. Clark, Damian Kusy, Olena Vakuliuk, Maciej Krzeszewski, Krzysztof J. Kochanowski, Beata Koszarna, Omar O'Mari, Denis Jacquemin, Daniel T. Gryko, Valentine I. Vullev
Summary: This study investigates the effects of electronic coupling through biaryl linkers on the excited-state symmetry breaking of hybrid dyes. It is found that strengthening the donor-acceptor electronic coupling decreases the charge transfer rates and the propensity for symmetry breaking. In cases of intermediate electronic coupling, the dyes exhibit white fluorescence.
Article
Chemistry, Physical
Iryna Knysh, Jose D. J. Villalobos-Castro, Ivan Duchemin, Xavier Blase, Denis Jacquemin
Summary: In this study, the accuracy of BSE/evGW method for the calculation of excited state and excess dipole moments in organic dyes is assessed and compared with other methods. The results demonstrate that BSE/evGW method exhibits higher accuracy in calculating excess dipole moments of dyes and outperforms other methods in certain cases.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2023)
Article
Chemistry, Multidisciplinary
Alexander M. Prophet, Kritanjan Polley, Gary J. Van Berkel, David T. Limmer, Kevin R. Wilson
Summary: The oxidation kinetics of iodide by ozone at the air-water interface is studied in single microdroplets. Molecular simulations and kinetic modeling are used to understand the underlying multiphase mechanism.
Article
Chemistry, Multidisciplinary
Rong Zhang, Jiajing Lan, Fei Wang, Shumei Chen, Jian Zhang
Summary: By utilizing 1,1'-ferrocene dicarboxylic acid as a chelating and surface protection ligand, we have synthesized multi-nuclear indium oxide clusters with varying nuclear sizes, including heptanuclear and thirteen-nuclear clusters. These clusters possess labile coordination sites, allowing for structural modification and self-assembly, resulting in the formation of various cluster structures.
Article
Chemistry, Multidisciplinary
Hui Wang, Hui Liu, Mingsen Wang, Jiaheng Hou, Yongjun Li, Yuancheng Wang, Yingjie Zhao
Summary: Two supramolecular complexes were prepared using CBs and M1, and their single-crystal structures were analyzed by SCXRD. The unexpected 1:2 self-assembly structure between M1 and CB[8] was discovered for the first time. These complexes exhibit unique photophysical properties and provide valuable information about the structure and photophysical properties of supramolecular complexes.
Article
Chemistry, Multidisciplinary
Chang-Hee Lee, Sookil Park, Sanggil Kim, Ji Young Hyun, Hyun Soo Lee, Injae Shin
Summary: The epidermal growth factor receptor (EGFR) is a cell-surface glycoprotein involved in cell proliferation and tumor development. This study used a fluorescently labeled EGFR to investigate its time-dependent endocytosis in live cells and found that appended glycans affect EGFR internalization. Additionally, the study detected sialic acid residues attached to EGFR on the live cell surface using FRET-based imaging. This research provides valuable insights into the cellular functions of EGFR.
Article
Chemistry, Multidisciplinary
Subhankar Sahu, Lokesh Kumar, Sumita Das, Dipti Gupta, Ruchi Anand
Summary: This study proposes a strategy that combines organic electronics with biosensor scaffolds to create a compact device for monitoring environmental aromatic pollution. By coupling biosensing protein MopR with an organic electrochemical transistor (OECT), a sensor module capable of efficient detection of phenol was designed. Exclusive phenol detection with minimal loss of sensitivity could be achieved in complex pollutant mixtures and real environmental samples.
Review
Chemistry, Multidisciplinary
Changseok Lee, Hyung-Joon Kang, Sungwoo Hong
Summary: The formation of C-N bonds through hydroamination reactions catalyzed by nickel hydrides has been a topic of recent interest. This approach offers a way to efficiently transform a variety of alkene and alkyne substrates into compounds enriched with C-N bonds. The review provides a concise overview of the underlying reaction mechanisms and aims to stimulate further progress in NiH-catalytic techniques and catalyst design.
Article
Chemistry, Multidisciplinary
Yueci Wu, Lu-Lu Sun, Hai-Hao Han, Xiao-Peng He, Weiguo Cao, Tony D. James
Summary: Drug-induced liver injury (DILI) is a common cause of acute liver failure in the USA and Europe, but most cases can be recovered or prevented by discontinuing the offending drug. Recent research has found that peroxynitrite (ONOO-) can be used as a potential indicator for early diagnosis of DILI, and there is an urgent need to establish a method to detect and track peroxynitrite in DILI cases. In this study, a FRET-based nano fluorescent probe CD-N-I was developed, which showed high selectivity and sensitivity in detecting peroxynitrite. The probe successfully detected exogenous peroxynitrite in live cells and endogenous peroxynitrite in APAP-induced liver injury of HepG2 cells.
Article
Chemistry, Multidisciplinary
Dmitry L. Lipilin, Mikhail O. Zubkov, Mikhail D. Kosobokov, Alexander D. Dilman
Summary: This article describes a direct photocatalytic method for the thiolation of unprotected acids, which was previously challenging. By using a thionocarbonate reagent with an N-O bond, the efficient conversion of carboxylic acids to thiols is achieved.
Article
Chemistry, Multidisciplinary
Jason Malenfant, Lucille Kuster, Yohann Gagne, Kouassi Signo, Maxime Denis, Sylvain Canesi, Mathieu Frenette
Summary: Raman microscopy can reveal compound-specific vibrational fingerprints without sample preparation. The combination of efficient theoretical calculations and a user-friendly software can accurately predict peak positions and provide match scores to assist with structure determination.
Article
Chemistry, Multidisciplinary
Jayoh A. Hernandez, Paul S. Micus, Sean Alec Lois Sunga, Luca Mazzei, Stefano Ciurli, Gabriele Meloni
Summary: Essential trace metals play crucial roles in the survival and virulence of bacterial pathogens. Helicobacter pylori requires nickel for colonization and persistence in the stomach, and NixA is an essential nickel transporter in this process. This study characterizes the selectivity and electrogenic nature of NixA-mediated nickel transport.
Article
Chemistry, Multidisciplinary
Tarali Devi, Kuheli Dutta, Jennifer Deutscher, Stefan Mebs, Uwe Kuhlmann, Michael Haumann, Beatrice Cula, Holger Dau, Peter Hildebrandt, Kallol Ray
Summary: This study emphasizes the importance of subtle electronic changes and secondary interactions in the stability of biologically relevant metal-dioxygen intermediates. It also shows that the role of the chloride ligand in stabilizing the Fe-III-(OOBu)-Bu-t moiety can extend to other anions, including the thiolate ligand.
Article
Chemistry, Multidisciplinary
Jacqueline R. Santhouse, Jeremy M. G. Leung, Lillian T. Chong, W. Seth Horne
Summary: By studying the folding kinetics and mechanism of the BdpA sequence, researchers found that altering the backbone connectivity can affect protein folding. This suggests that protein mimetic chains have a significant degree of plasticity in transitioning between unfolded and folded states.
Article
Chemistry, Multidisciplinary
Divanshu Gupta, Ralf Einholz, Holger F. Bettinger
Summary: This study presents the first direct spectroscopic evidence of a cyclic seven-membered iminoborane. Compared to linear amino-iminoboranes, this cyclic iminoborane exhibits weakened bond strength and lower Lewis acidity value. The study suggests that the reduced ring strain of cyclic iminoborane prevents nitrogen fixation but allows facile (2 + 2) cycloaddition reaction with C2H4.
Article
Chemistry, Multidisciplinary
Renny Mathew, Aniruddha Mazumder, Praveen Kumar, Julie Matula, Sharmarke Mohamed, Petr Brazda, Mahesh Hariharan, Brijith Thomas
Summary: This study reveals the packing arrangement of partially disordered nitro-perylenediimide (NO2-PDI) using a synergistic approach that combines 3D ED, ssNMR, and DFT techniques. By overcoming these challenges, this methodology opens up new avenues for material characterization, driving exciting advancements in the field.
