A5018561362- Spectroscopy and Quantum Chemical Studies
- Advanced Chemical Physics Studies
- Spectroscopy and Laser Applications
- Photochemistry and Electron Transfer Studies
- Molecular spectroscopy and chirality
- Photoreceptor and optogenetics research
- X-ray Spectroscopy and Fluorescence Analysis
- Photosynthetic Processes and Mechanisms
- Advanced X-ray Imaging Techniques
- Machine Learning in Materials Science
- Advanced Electron Microscopy Techniques and Applications
- Laser-Matter Interactions and Applications
- Gastrointestinal Bleeding Diagnosis and Treatment
- Photochromic and Fluorescence Chemistry
- Catalysis and Oxidation Reactions
- Mass Spectrometry Techniques and Applications
- Quantum Electrodynamics and Casimir Effect
- Electrochemical Analysis and Applications
- Force Microscopy Techniques and Applications
- AI in cancer detection
- Helicobacter pylori-related gastroenterology studies
- Optical Polarization and Ellipsometry
- Pancreatic and Hepatic Oncology Research
- Conducting polymers and applications
- Advanced NMR Techniques and Applications
Fondazione IRCCS Ca' Granda Ospedale Maggiore Policlinico
2024-2025
Ospedale Valduce
2024-2025
University of Milan
2024-2025
Ospedale Maggiore
2025
University of Bologna
2017-2024
Boston University
2020
Ono Pharmaceutical (Japan)
2019
University of California, Irvine
2019
European Centre for Theoretical Studies in Nuclear Physics and Related Areas
2017-2018
Istituto Nazionale di Fisica Nucleare, Trento Institute for Fundamental Physics And Applications
2017-2018
MOLCAS/OpenMolcas is an ab initio electronic structure program providing a large set of computational methods from Hartree-Fock and density functional theory to various implementations multiconfigurational theory. This article provides comprehensive overview the main features code, specifically reviewing use code in previously reported chemical applications as well more recent including calculation magnetic properties optimized matrix renormalization group wave functions.
The developments of the open-source OpenMolcas chemistry software environment since spring 2020 are described, with a focus on novel functionalities accessible in stable branch package or via interfaces other packages. These span wide range topics computational and presented thematic sections: electronic structure theory, spectroscopy simulations, analytic gradients molecular optimizations, ab initio dynamics, new features. This report offers an overview chemical phenomena processes can...
We combine sub-20 fs transient absorption spectroscopy with state-of-the-art computations to study the ultrafast photoinduced dynamics of trans-azobenzene (AB). are able resolve lifetime ππ* state, whose decay within ca. 50 is correlated buildup nπ* population and emergence coherences in dynamics, date unobserved. Nonlinear simulations call for CNN in-plane bendings as active modes subps coherent out state. Radiative kinetic energy transfer into these drives system a high-energy planar...
Nonlinear electronic spectroscopies represent one of the most powerful techniques to study complex multichromophoric architectures. For these systems, in fact, linear spectra are too congested be used disentangle many coupled vibroelectronic processes that activated. By using a 2D approach, instead, clear picture can achieved, but only when recorded combined with proper interpretative model. So far, this has been almost always achieved through parametrized exciton Hamiltonians necessarily...
X-ray diffraction is routinely used for structure determination of stationary molecular samples. Modern photon sources, e.g., from free-electron lasers, enable us to add temporal resolution these scattering events, thereby providing a movie atomic motions. We simulate and decipher the various contributions pattern femtosecond isomerization azobenzene, textbook photochemical process. A wealth information encoded besides real-time monitoring charge density cis trans isomerization. In...
Multireference methods are known for their ability to accurately treat states of very different nature in many molecular systems, facilitating high-quality simulations a large variety spectroscopic techniques. Here, we couple the multiconfigurational restricted active space self-consistent field RASSCF/RASPT2 method (of CASSCF/CASPT2 family) displaced harmonic oscillator (DHO) model, simulate soft X-ray spectroscopy. We applied such an RASSCF/RASPT2+DHO approach at K-edges various second-row...
Computation of nonlinear optical response functions allows for an in-depth connection between theory and experiment. Experimentally recorded spectra provide a high density information, but to objectively disentangle overlapping signals reach detailed reliable understanding the system dynamics, measurements must be integrated with theoretical approaches. Here, we present new, highly accurate efficient trajectory-based semiclassical path integral method computing higher order non-Markovian...
We present an accurate and efficient approach to computing the linear nonlinear optical spectroscopy of a closed quantum system subject impulsive interactions with incident electromagnetic field. It incorporates effect ultrafast nonadiabatic dynamics by means explicit numerical propagation nuclear wave packet. The fundamental expressions for evaluation first- higher-order response functions are recast in general form that can be used any code capable overlap packets evolving different...
In this discussion we present a methodology to describe spectral lineshape from first principles, providing insight into the solvent-solute molecular interactions in terms of static and dynamic disorder how these shape signals recorded experimentally linear nonlinear optical spectroscopies, including two-dimensional electronic spectroscopy (2DES). Two different strategies for simulating are compared: both rely on same evaluation coupling between states intra-molecular vibrations, while they...
X-ray spectroscopy is gaining a growing interest in the scientific community, as it represents versatile and powerful experimental toolbox for probing dynamics of both core valence electronic excitations, nuclear motions material structure, with element site specificity. Among various based techniques, near-edge absorption fine structure (NEXAFS) spectroscopy, which investigates energy probability resonant core-to-valence transitions, has started to be applied organic molecules: recent...
Conical intersections (CoIns) play an important role in ultrafast relaxation channels. Their monitoring remains a formidable experimental challenge. We theoretically compare the probing of S2 → S1 CoIn passage 4-thiouracil by its vibronic coherences, using off-resonant X-ray-stimulated Raman spectroscopy (TRUECARS) and time-resolved X-ray diffraction (TRXD). The quantum nuclear wavepacket (WP) dynamics provides accurate picture photoinduced dynamics. Upon photoexcitation, WP oscillates among...
In this article the recent developments of open-source OpenMolcas chemistry software environment, since spring 2020, are described, with main focus on novel functionalities that accessible in stable branch package and/or via interfaces other packages. These community span a wide range topics computational chemistry, and presented thematic sections associated electronic structure theory, spectroscopy simulations, analytic gradients molecular optimizations, ab initio dynamics, new features....
Abstract We introduce iSPECTRON, a program that parses data from common quantum chemistry software (NWChem, OpenMolcas, Gaussian, Cobramm, etc.), produces the input files for simulation of linear and nonlinear spectroscopy molecules with Spectron code, analyzes spectra broad range tools. Vibronic are expressed in term electronic eigenstates, obtained computations, vibrational/bath effects incorporated framework displaced harmonic oscillator model, where all required quantities computed at...
Linear and nonlinear X-ray spectroscopy hold the promise to provide a complementary tool available ample body of terahertz UV spectroscopic techniques, disclosing information about electronic structure dynamics large variety systems, spanning from transition metals organic molecules. While experimental free electron laser facilities continue develop, theory may take lead in modeling inspiring new cutting edge experiments, paving way their future use. As an example, not-yet-available...
Significance Monitoring the real-space motion of electrons directly involved in ultrafast molecular dynamics is a challenging goal, hindered by strong contributions remaining inactive electrons. Molecular quantum coherences can provide direct window into elementary electronic dynamics, but they could not be separately imaged so far. Here, we demonstrate time- and frequency-resolved X-ray diffraction technique, which employ existing stochastic pulses to image coherence contributions. The...
Core excitations on different atoms are highly localized and therefore decoupled. By placing molecules in an x-ray cavity the core transitions become coupled via exchange of photons form delocalized hybrid light-matter known as polaritons. We demonstrate these effects for two inequivalent carbon 1,1-difluoroethylene. Polariton signatures absorption, two-photon multidimensional four-wave mixing signals predicted.
We study the ultrafast time evolution of cyclobutanone excited to singlet n → Rydberg state through non-adiabatic surface-hopping simulationsperformed at extended multi-state complete active space second-order perturbation (XMS-CASPT2) level theory. These dynamics predict relaxation ground-state with a timescale 822 ± 45 fs minimal involvement triplets. The major path involves three-state degeneracy region and leads variety fragmented photoproducts. simulate resulting time-resolved...
We report the development of a novel diagnostic tool, named wave function overlap tool (WFOT), designed to evaluate between functions computed at single-reference [i.e., time-dependent density functional theory or configuration interaction singles (CIS)] and multireference (i.e., CASSCF/CASPT2) electronic structure levels theory. It relies on truncating single- WFs CIS-like expansions spanning same configurational space maximizing molecular orbital by means unitary transformation. To...
The partially linearized density matrix formalism for nonadiabatic dynamics is adapted to incorporate a classical external electromagentic field into the system Hamiltonian. This advancement encompasses possibility of describing field-driven and computing variety linear nonlinear spectroscopic signals beyond perturbative limit. capabilities developed approach are demonstrated on simple two-state vibronic model coupled bath, which we (a) perform an exhaustive search in parameter space optimal...
We introduce a mesoscopic model to predict the charge mobility of organic semiconductors characterized by coexistence crystalline and amorphous phases. First, we validate our scheme reproducing trends in observed thin films poly(3-hexylthiophene) (P3HT) polymers. Next, address problem predicting morphologies that lead highest mobility. Our main finding is identification region model's multidimensional parameter space, which effectively depends on single morphological feature: average...
The fate of virtually all photochemical reactions is determined by conical intersections. These are energetically degenerate regions molecular potential energy surfaces that strongly couple electronic states, thereby enabling fast relaxation channels. Their direct spectroscopic detection relies on weak features often buried beneath stronger, less interesting contributions. For azobenzene photoisomerization, a textbook reaction, we demonstrate how resonant infrared field can be employed...
Spectroscopy simulations are of paramount importance for the interpretation experimental electronic spectra, disentangling overlapping spectral features, and tracing microscopic origin observed signals. Linear nonlinear based on results drawn from structure calculations that provide necessary parameterization molecular systems probed by light. Here, we investigate applicability excited-state properties obtained linear-response time-dependent density functional theory (TDDFT) in description...
Abstract Quantum dynamics is the natural framework in which accurate simulation of spectroscopy nonadiabatically coupled molecular systems can be obtained. Even if efficient quantum approaches have been developed, number degrees freedom that need to considered realistic typically too high explicitly account for all them. Moreover, open-quantum systems, a quasi-continuum low-frequency environment modes included get proper description spectral bands. Here, we describe an approach large modes,...