757 results on '"Decleva, P."'
Search Results
2. Chiral topological light for detecting robust enantio-sensitive observables
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Mayer, Nicola, Ayuso, David, Decleva, Piero, Khokhlova, Margarita, Pisanty, Emilio, Ivanov, Misha, and Smirnova, Olga
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Physics - Optics ,Physics - Atomic Physics ,Physics - Chemical Physics - Abstract
The topological response of matter to electromagnetic fields is a property in high demand in materials design and metrology due to its robustness against noise and decoherence, stimulating recent advances in ultrafast photonics. Embedding topological properties into the enantio-sensitive optical response of chiral molecules could therefore enhance the efficiency and robustness of chiral optical discrimination. Here we achieve such a topological embedding by introducing the concept of chiral topological light~-- a light beam which displays chirality locally, with an azimuthal distribution of its handedness described globally by a topological charge. The topological charge is mapped onto the azimuthal intensity modulation of the non-linear optical response, where enantio-sensitivity is encoded into its spatial rotation. The spatial rotation is robust against intensity fluctuations and imperfect local polarization states of the driving field. Our theoretical results show that chiral topological light enables detection of percentage-level enantiomeric excesses in randomly oriented mixtures of chiral molecules, opening a way to new, extremely sensitive and robust chiro-optical spectroscopies with attosecond time resolution.
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- 2023
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3. Attosecond metrology of 2D charge distribution in molecules
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Loriot, V., Boyer, A., Nandi, S., González-Collado, C. M., Plésiat, E., Marciniak, A., Garcia, C. L., Hu, Y., Lara-Astiaso, M., Palacios, A., Decleva, P., Martín, F., and Lépine, F.
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Physics - Chemical Physics - Abstract
Photoionization as a half-scattering process is not instantaneous. Usually, time delays in photoionization are of the order of few tens of attoseconds (1 as = 10$^{-18}$ s). While going from a single atom to a nano-object, one can expect the delay to increase since the photoelectron scatters over a larger distance. Here, we show that this is no longer valid in the case of planar systems. Using attosecond interferometry, we find that the time delay in a 2D carbon-based molecule, naphthalene, is significantly smaller compared to its 3D diamond-like counterpart, adamantane. The measured time delay carries the signature of the spatial distribution of the hole created in the residual molecular cation, allowing us to obtain its dimensions with angstrom accuracy. Our findings offer novel opportunities for tracking and manipulating ultrafast charge transport in molecular materials.
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- 2022
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4. The photochemical ring-opening reaction of 1,3-cyclohexadiene: complex dynamical evolution of the reactive state
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Travnikova, O., Piteša, T., Ponzi, A., Sapunar, M., Squibb, R. J., Richter, R., Finetti, P., Di Fraia, M., De Fanis, A., Mahne, N., Manfredda, M., Zhaunerchyk, V., Marchenko, T., Guillemin, R., Journel, L., Prince, K. C., Callegari, C., Simon, M., Feifel, R., Decleva, P., Došlić, N., and Piancastelli, M. N.
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Physics - Chemical Physics - Abstract
The photochemically induced ring-opening isomerization reaction of 1,3-cyclohexadiene (CHD) to 1,3,5-hexatriene (HT) is a textbook example of a pericyclic reaction, and has been amply investigated with advanced spectroscopic techniques. The generally accepted description of the isomerization pathway starts with a valence excitation to the lowest-lying bright state, followed by a passage through a conical intersection to a dark doubly excited state, and finally a branching between either the return to the ground state of the cyclic molecule or the actual ring-opening reaction leading to the open-chain isomer. It was traditionally assumed that the dark reactive state corresponds to the second excited state of CHD at the Franck-Condon geometry. Here in a joint experimental and computational effort we demonstrate that the evolution of the excitation-deexcitation process is much more complex than usually described. In particular, we show that an initially high-lying electronic state smoothly decreasing in energy along the reaction path plays a key role in the ring-opening reaction. The conceptual basis of our work is that the dynamics to consider here is determined by diabatic states, whose populations are the ones closely related to the observed photoelectron signal., Comment: Sumbitted to Nature Communications (under review)
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- 2022
5. Valence-shell photoelectron circular dichroism of ruthenium(iii)-tris-(acetylacetonato) gas-phase enantiomers
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Darquie, Benoit, Saleh, Nidal, Tokunaga, Sean K., Srebro-Hooper, Monika, Ponzi, Aurora, Autschbach, Jochen, Decleva, Piero, Garcia, Gustavo A., Crassous, Jeanne, and Nahon, Laurent
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Physics - Chemical Physics ,Physics - Atomic Physics - Abstract
Chiral transition-metal complexes are of interest in many fields ranging from asymmetric catalysis and molecular materials science to optoelectronic applications or fundamental physics including parity violation effects. We present here a combined theoretical and experimental investigation of gas-phase valence-shell photoelectron circular dichroism (PECD) on the challenging open-shell ruthenium(iii)-tris-(acetylacetonato) complex, Ru(acac)$_3$. Enantiomerically pure $\Delta$- or $\Lambda$-Ru(acac)$_3$, characterized by electronic circular dichroism (ECD), were vaporized and adiabatically expanded to produce a supersonic beam and photoionized by circularly-polarized VUV light from the DESIRS beamline at Synchrotron SOLEIL. Photoelectron spectroscopy (PES) and PECD experiments were conducted using a double imaging electron/ion coincidence spectrometer, and compared to density functional theory (DFT) and time-dependent DFT (TDDFT) calculations. The open-shell character of Ru(acac)$_3$, which is not taken into account in our DFT approach, is expected to give rise to a wide multiplet structure, which is not resolved in our PES signals but whose presence might be inferred from the additional striking features observed in the PECD curves. Nevertheless, the DFT-based assignment of the electronic bands leads to the characterisation of the ionized orbitals. In line with other recent works, the results confirm that PECD persists independently on the localization and/or on the achiral or chiral nature of the initial orbital, but is rather a probe of the molecular potential as a whole. Overall, the measured PECD signals on Ru(acac)$_3$, a system exhibiting D$_3$ propeller-type chirality, are of similar magnitude compared to those on asymmetric-carbon-based chiral organic molecules which constitute the vast majority of species investigated so far, thus suggesting that PECD is a universal mechanism, inherent to any type of chirality.
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- 2021
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6. Giant chiro-optical response in high harmonic generation
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Ayuso, David, Ordonez, Andres F., Decleva, Piero, Ivanov, Misha, and Smirnova, Olga
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Physics - Optics ,Physics - Atomic Physics - Abstract
High harmonic generation (HHG) records the ultrafast electronic response of matter to light, encoding key properties of the interrogated quantum system, such as chirality. The first implementation of chiral HHG [Cireasa et al. Nat. Phys. 11, 654 (2015)] relied on the weak electronic response of a medium of randomly oriented chiral molecules to the magnetic component of an elliptically polarized wave, yielding relatively weak chiro-optical signals. Here we show that elliptically polarized light can drive a strong chiral response in chiral molecules via purely electric-dipole interactions -- the magnetic component of the wave does not participate at all. This giant chiro-optical response, which remains hidden in standard HHG experiments, can be mapped into the macroscopic far-field signal using a non-collinear configuration, creating new opportunities for bringing the electric-dipole "revolution" to HHG., Comment: 12 pages, 5 figures. arXiv admin note: text overlap with arXiv:1809.01632
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- 2021
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7. Geometric magnetism and anomalous enantio-sensitive observables in photoionization of chiral molecules
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Ordonez, Andres F., Ayuso, David, Decleva, Piero, and Smirnova, Olga
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- 2023
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8. Geometric fields and new enantio-sensitive observables in photoionization of chiral molecules
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Ordonez, Andres F., Ayuso, David, Decleva, Piero, and Smirnova, Olga
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Physics - Chemical Physics ,Physics - Optics - Abstract
Chiral molecules are instrumental for molecular recognition in living organisms. Distinguishing between two opposite enantiomers, the mirror twins of the same chiral molecule, is both vital and challenging. Photoelectron circular dichroism (PECD), an extremely sensitive probe of molecular chirality via photoionization, outperforms standard optical methods by many orders of magnitude. Here we show that the physical origin of PECD in chiral molecules is linked to the concept of geometric magnetism, which enables a broad class of phenomena in solids including the anomalous electron velocity, the Hall effect, and related topological phenomena. We uncover the geometric field in molecular photoionization, which leads to a new class of enantio-sensitive observables emerging due to ultrafast excitation of chiral electronic or vibronic currents prior to ionization. Next, we introduce the first member of this new class: enantio-sensitive orientation of chiral molecules via photoionization. This effect opens new routes to both enantio-separation and imaging of chiral dynamics on ultrafast time scales. Our work suggests that geometric fields in photoionization provide the bridge between the two geometrical properties, chirality and topology.
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- 2021
9. Geometric magnetism and anomalous enantio-sensitive observables in photoionization of chiral molecules
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Andres F. Ordonez, David Ayuso, Piero Decleva, and Olga Smirnova
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Astrophysics ,QB460-466 ,Physics ,QC1-999 - Abstract
Abstract Chiral molecules are instrumental for molecular recognition in living organisms. Distinguishing between two opposite enantiomers, the mirror twins of the same chiral molecule, is both vital and challenging. Geometric magnetism enables a broad class of phenomena in solids including the anomalous electron velocity, the Hall effect, and related topological observables. Here we show that ultrafast electron currents excited in chiral molecules can generate geometric fields which enable a class of anomalous enantio-sensitive observables in photoionization. Next, we introduce the first member of this class: enantio-sensitive orientation of chiral molecules via photoionization. This effect opens unexplored routes to both enantio-separation and imaging of chiral dynamics on ultrafast time scales. Our work suggests that geometric magnetism in photoionization provides the bridge between the two geometrical properties, chirality and topology.
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- 2023
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10. Polarization of chirality
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Ayuso, David, Ordonez, Andres, Decleva, Piero, Ivanov, Misha, and Smirnova, Olga
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Physics - Optics - Abstract
It has been long recognized that the spatial polarization of the electronic clouds in molecules, and the spatial arrangements of atoms into chiral molecular structures, play crucial roles in physics, chemistry and biology. However, these two fundamental concepts - chirality and polarization - have remained unrelated so far. This work connects them by introducing and exploring the concept of polarization of chirality. We show that, like charge, chirality, or handedness, can be polarized, and that such polarization leads to fundamental consequences, demonstrated here using light. First, we analyze how chirality dipoles and higher-order chirality multipoles manifest in experimental observables. Next, we show how to create chirality-polarized optical fields of alternating handedness in space. Despite being achiral, these racemic space-time light structures interact differently with chiral matter of opposite handedness, and the chirality dipole of light controls and quantifies the strength of the enantio-sensitive response. Using nonlinear interactions, we can make a medium of randomly oriented chiral molecules emit light to the left, or to the right, depending on the molecular handedness and on the chirality dipole of light. The chiral dichroism in emission direction reaches its highest possible value of 200%. Our work opens the field of chirality polarization shaping of light and new opportunities for efficient chiral discrimination and control of chiral and chirality-polarized light and matter on ultrafast time scales.
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- 2020
11. Attosecond timing of electron emission from a molecular shape resonance
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Nandi, S., Plésiat, E., Zhong, S., Palacios, A., Busto, D., Isinger, M., Neoričić, L., Arnold, C. L., Squibb, R. J., Feifel, R., Decleva, P., L'Huillier, A., Martín, F., and Gisselbrecht, M.
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Physics - Chemical Physics - Abstract
Shape resonances in physics and chemistry arise from the spatial confinement of a particle by a potential barrier. In molecular photoionization, these barriers prevent the electron from escaping instantaneously, so that nuclei may move and modify the potential, thereby affecting the ionization process. By using an attosecond two-color interferometric approach in combination with high spectral resolution, we have captured the changes induced by the nuclear motion on the centrifugal barrier that sustains the well-known shape resonance in valence-ionized N$_2$. We show that despite the nuclear motion altering the bond length by only $2\%$, which leads to tiny changes in the potential barrier, the corresponding change in the ionization time can be as large as $200$ attoseconds. This result poses limits to the concept of instantaneous electronic transitions in molecules, which is at the basis of the Franck-Condon principle of molecular spectroscopy., Comment: 24 pages, 5 figures
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- 2019
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12. Locally and globally chiral fields for ultimate control of chiral light matter interaction
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Ayuso, David, Neufeld, Ofer, Ordonez, Andres F., Decleva, Piero, Lerner, Gavriel, Cohen, Oren, Ivanov, Misha, and Smirnova, Olga
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Physics - Optics - Abstract
Light is one of the most powerful and precise tools allowing us to control, shape and create new phases of matter. In this task, the magnetic component of a light wave has so far played a unique role in defining the wave's helicity, but its influence on the optical response of matter is weak. Chiral molecules offer a typical example where the weakness of magnetic interactions hampers our ability to control the strength of their chiral optical response. It is limited several orders of magnitude below the full potential. Here we introduce freely propagating locally and globally chiral electric fields, which interact with chiral quantum systems extremely efficiently. To demonstrate the degree of control enabled by such fields, we focus on the nonlinear optical response of randomly oriented chiral molecules. We show full control over intensity, polarization and propagation direction of the chiral optical response, enabling its background-free detection. This response can be fully suppressed or enhanced at will depending on the molecular handedness, achieving the ultimate limit in chiral discrimination. Our findings open a way to extremely efficient control of chiral matter and to ultrafast imaging of chiral structure and dynamics in gases, liquids and solids., Comment: Major revision of the manuscript that introduces new concepts and considerably extends the scope of the work
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- 2018
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13. Strong-field control and enhancement of chiral response in bi-elliptical high-order harmonic generation: an analytical model
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Ayuso, David, Decleva, Piero, Patchkovskii, Serguei, and Smirnova, Olga
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Physics - Optics - Abstract
The generation of high-order harmonics in a medium of chiral molecules driven by intense bi-elliptical laser fields can lead to strong chiroptical response in a broad range of harmonic numbers and ellipticities [D. Ayuso et al, J. Phys. B 51, 06LT01 (2018)]. Here we present a comprehensive analytical model that can describe the most relevant features arising in the high-order harmonic spectra of chiral molecules driven by strong bi-elliptical fields. Our model recovers the physical picture underlying chiral high-order harmonic generation based on ultrafast chiral hole motion and identifies the rotationally invariant molecular pseudoscalars responsible for chiral dynamics. Using the chiral molecule propylene oxide as an example, we show that one can control and enhance the chiral response in bi-elliptical high-order harmonic generation by tailoring the driving field, in particular by tuning its frequency, intensity and ellipticity, exploiting a suppression mechanism of achiral background based on the linear Stark effect.
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- 2018
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14. Alterations of color vision and pupillary light responses in age-related macular degeneration
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Diego Decleva, Kallene Summer Vidal, Andre Carvalho Kreuz, Paulo Augusto Hidalgo Leite de Menezes, and Dora Fix Ventura
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age-related macular degeneration (AMD) ,pupillary light reflex (PLR) ,intrinsically photosensitive retinal ganglion cells (ipRGC) ,color vision ,rods (retina) ,cones ,Neurosciences. Biological psychiatry. Neuropsychiatry ,RC321-571 - Abstract
IntroductionAge-related macular degeneration (AMD) is the leading cause of irreversible central vision loss in developed countries and one of the leading causes of blindness. In this work, we evaluated color vision and the pupil light reflex (PLR) to assess visual function in patients with early and neovascular AMD (NVAMD) compared with the control group.MethodsWe recruited 34 early patients with dry AMD and classified them into two groups following AREDS: 13 patients with NVAMD and 24 healthy controls. Controls and patients with early dry AMD had visual acuity (VA) best or equal to 20/25 (0.098 logMAR). Color vision was assessed in controls and patients with early dry AMD using the Cambridge Color Test (CCT) 2.0 through the Trivector protocol. The PLR was evaluated using a Ganzfeld, controlled by the RETI–port system. The stimuli consisted of 1s blue (470 nm) and red (631 nm) light flashes presented alternately at 2-min intervals. To assess the cone contribution, we used a red flash at 2.4 log cd.m–2, with a blue background at 0.78 log cd.m–2. For rods, we used 470-nm flashes at –3 log cd.m–2, and for the melanopsin function of ipRGCs, we used 470 nm at 2.4 log cd.m–2.ResultsPatients with early dry AMD had reduced color discrimination in all three axes: protan (p = 0.0087), deutan (p = 0.0180), and tritan (p = 0.0095) when compared with the control group. The PLR has also been affected in patients with early dry AMD and patients with NVAMD. The amplitude for the melanopsin-driven response was smaller in patients with early dry AMD (p = 0.0485) and NVAMD (p = 0.0035) than in the control group. The melanopsin function was lower in patients with NVAMD (p = 0.0290) than the control group. For the rod-driven response, the latency was lower in the NVAMD group (p = 0.0041) than in the control group. No changes were found in cone-driven responses between the control and AMD groups.ConclusionPatients with early dry AMD present diffusely acquired color vision alteration detected by CCT. Rods and melanopsin contributions for PLR are affected in NVAMD. The CCT and the PLR may be considered sensitive tests to evaluate and monitor functional changes in patients with AMD.
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- 2023
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15. Cluster approach to scattering in MoS2 photoemission
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Ambrosio, M.J., Plesiat, E., Decleva, P., Echenique, P.M., Díez Muiño, R., and Martín, F.
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- 2022
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16. Attosecond photoionisation time delays reveal the anisotropy of the molecular potential in the recoil frame
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Ahmadi, H., Plésiat, E., Moioli, M., Frassetto, F., Poletto, L., Decleva, P., Schröter, C. D., Pfeifer, T., Moshammer, R., Palacios, A., Martin, F., and Sansone, G.
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- 2022
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17. Attosecond photoionisation time delays reveal the anisotropy of the molecular potential in the recoil frame
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H. Ahmadi, E. Plésiat, M. Moioli, F. Frassetto, L. Poletto, P. Decleva, C. D. Schröter, T. Pfeifer, R. Moshammer, A. Palacios, F. Martin, and G. Sansone
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Science - Abstract
Photoionization time delays provide insights on the interaction of photon with the electrons. Here the authors explore the role of the molecular potential to the attosecond time delays in the photoionization of CF4 molecule.
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- 2022
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18. Photoelectron Circular Dichroism as a Probe of Chiral Hydrocarbons
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Piero Decleva
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chirality ,photoemission ,PECD ,absolute configuration ,hydrocarbons ,Chemistry ,QD1-999 - Abstract
The sensitivity of Photoelectron Circular Dichroism (PECD) in the angular distribution of photoelectrons, a recent chiral technique, to detect chirality in pure hydrocarbons is investigated in a number of benchmark molecules. It is found that a very large chiral signal is expected, surpassing most current examples, giving a sure fingerprint of absolute configuration. On the other hand, the sensitivity to specific isomers or closely related molecules is relatively modest.
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- 2022
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19. Ionisation of H$_2$O by a strong ultrashort XUV pulse: a model within the single active electron approximation
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Galstyan, A., Popov, Yu. V., Janssens, N., Mota-Furtado, F., O'Mahony, P. F., Decleva, P., Quadri, N., and Piraux, B.
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Physics - Atomic Physics - Abstract
We present and discuss a new computationally inexpensive method to study, within the single active electron approximation, the interaction of a complex system with an intense ultrashort laser pulse. As a first application, we consider the one photon single ionisation of the highest occupied molecular orbital of the water molecule by a laser pulse. The ionisation yield is calculated for different orientations of the molecule with respect to the field polarization axis and for different carrier envelope phases of the pulse, and compared against predictions of another single active electron approach., Comment: 24 pages, 13 figures
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- 2017
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20. Attosecond electronic and nuclear quantum photodynamics of ozone monitored with time and angle resolved photoelectron spectra
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Decleva, P., Quadri, N., Perveaux, A., Lauvergnat, D., Gatti, F., Lasorne, B., Halász, G. J., and Vibók, Á.
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Physics - Atomic and Molecular Clusters - Abstract
Recently we reported a series of numerical simulations proving that it is possible in principle to create an electronic wave packet and subsequent electronic motion in a neutral molecule photoexcited by a UV pump pulse within a few femtoseconds. We considered the ozone molecule: for this system the electronic wave packet leads to a dissociation process. In the present work, we investigate more specifically the time-resolved photoelectron angular distribution of the ozone molecule that provides a much more detailed description of the evolution of the electronic wave packet. We thus show that this experimental technique should be able to give access to observing in real time the creation of an electronic wave packet in a neutral molecule and its impact on a chemical process., Comment: Accepted in Scientific Report
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- 2016
21. A randomized clinical trial on the effects of exercise on muscle remodelling following bariatric surgery
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Saulo Gil, John P. Kirwan, Igor H. Murai, Wagner S. Dantas, Carlos Alberto Abujabra Merege‐Filho, Sujoy Ghosh, Samuel K. Shinjo, Rosa M.R. Pereira, Walcy R. Teodoro, Sheylla M. Felau, Fabiana B. Benatti, Ana L. deSá‐Pinto, Fernanda Lima, Roberto deCleva, Marco Aurélio Santo, Bruno Gualano, and Hamilton Roschel
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Muscle atrophy ,Obesity ,Bariatric surgery ,Muscle function ,Diseases of the musculoskeletal system ,RC925-935 ,Human anatomy ,QM1-695 - Abstract
Abstract Background Muscle atrophy and strength loss are common adverse outcomes following bariatric surgery. This randomized, controlled trial investigated the effects of exercise training on bariatric surgery‐induced loss of muscle mass and function. Additionally, we investigated the effects of the intervention on molecular and histological mediators of muscle remodelling. Methods Eighty women with obesity were randomly assigned to a Roux‐en‐Y gastric bypass (RYGB: n = 40, age = 42 ± 8 years) or RYGB plus exercise training group (RYGB + ET: n = 40, age = 38 ± 7 years). Clinical and laboratory parameters were assessed at baseline, and 3 (POST3) and 9 months (POST9) after surgery. The 6 month, three‐times‐a‐week, exercise intervention (resistance plus aerobic exercise) was initiated 3 months post‐surgery (for RYGB + ET). A healthy, lean, age‐matched control group was recruited to provide reference values for selected variables. Results Surgery resulted in a similar (P = 0.66) reduction in lower‐limb muscle strength in RYGB and RYGB+ET (−26% vs. −31%), which was rescued to baseline values in RYGB + ET (P = 0.21 vs. baseline) but not in RYGB (P 0.05 vs. baseline) but not RYGB (P > 0.01 vs. baseline). RYGB + ET showed greater Type I (5187 vs. 3898 μm2, P
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- 2021
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22. Effect of the shot-to-shot variation on charge migration induced by sub-fs x-ray free-electron laser pulses
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Gilbert Grell, Zhaoheng Guo, Taran Driver, Piero Decleva, Etienne Plésiat, Antonio Picón, Jesús González-Vázquez, Peter Walter, Jonathan P. Marangos, James P. Cryan, Agostino Marinelli, Alicia Palacios, and Fernando Martín
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Physics ,QC1-999 - Abstract
X-ray free-electron lasers (XFELs) are now able to provide tunable pairs of intense sub-fs pulses in the soft x-ray regime, paving the way for time-resolved investigations of attosecond charge migration in molecules. However, the stochastic shot-to-shot variation of the XFEL pulses may degrade and eventually hide the observable features. We show by means of state-of-the-art calculations that the damping of the charge migration induced by 260 eV pulses in p-aminophenol due to the shot-to-shot variation of pulses generated at the Linac Coherent Light Source is negligible in comparison to the natural damping due to the intrinsic fluctuation of the initial molecular geometry. This result gives us confidence in the utility of XFEL sub-fs pulses for the measurement of charge migration and other ultrafast charge dynamics.
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- 2023
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23. Enantio-sensitive unidirectional light bending
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David Ayuso, Andres F. Ordonez, Piero Decleva, Misha Ivanov, and Olga Smirnova
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Science - Abstract
Developing new methods for structuring light’s chirality in space would be advantageous for various next-generation applications. Here, the authors report enantio-sensitive unidirectional light bending by interacting light with isotropic chiral media.
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- 2021
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24. Separable Potentials Model for Atoms and Molecules in Strong Ultrashort Laser Pulses
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Popov, Yu. V., Galstyan, A., Piraux, B., O’Mahony, P. F., Mota-Furtado, F., Decleva, P., Chuluunbaatar, O., Castleman, Albert W, Series Editor, Toennies, Jan Peter, Series Editor, Yamanouchi, Kaoru, Series Editor, Zinth, Wolfgang, Series Editor, Tunik, Sergey, editor, and Makarov, Vladimir, editor
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- 2019
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25. Basic studies toward ultrafast soft x-ray photoelectron diffraction; its application to probing local structure in iodobenzene molecules
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T. Teramoto, S. Minemoto, T. Majima, T. Mizuno, J. H. Mun, A. Yagishita, P. Decleva, and S. Tsuru
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Crystallography ,QD901-999 - Abstract
Ultrafast x-ray photoelectron diffraction (UXPD) for free molecules has a promising potential to probe the local structures of the molecules in an element-specific fashion. Our UXPD scheme consists of three steps: (1) near-infrared laser (NIR) with ns pulse duration aligns sample molecules, (2) ultra-violet laser with fs pulse duration pumps the aligned molecules, and (3) soft x-ray free-electron laser (SXFEL) with fs pulse duration probes the molecules by measuring x-ray photoelectron diffraction (XPD) profiles. Employing steps of (1) and (3), we have measured I 3d XPD profiles from ground state iodobenzene aligned by the NIR laser with the SXFEL. Then, we have intensively calculated I 3d XPD profiles with density functional theory, taking degrees of alignments of the molecules into account, to extract a distance between C and I atoms in iodobenzene from the experimental I 3d XPD profiles. Although we have failed to determine the distance from the comparison between the experimental and theoretical results, we have succeeded in concluding that the degeneracies of the initial state eliminate the sensitivity on molecular structure in the I 3d XPD profiles. Thus, the observation of fine structures in the XPD profiles could be expected, if a nondegenerate molecular orbital is selected for a probe of UXPD. Finally, we have summarized our criteria to perform UXPD successfully: (1) to use SXFEL, (2) to prepare sample molecules with the degree of alignment higher than 0.8, and (3) to select a photoemission process from a nondegenerate inner-shell orbital of sample molecules.
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- 2022
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26. Imaging Molecular Structure through Femtosecond Photoelectron Diffraction on Aligned and Oriented Gas-Phase Molecules
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Boll, R., Rouzee, A., Adolph, M., Anielski, D., Aquila, A., Bari, S., Bomme, C., Bostedt, C., Bozek, J. D., Chapman, H. N., Christensen, L., Coffee, R., Coppola, N., De, S., Decleva, P., Epp, S. W., Erk, B., Filsinger, F., Foucar, L., Gorkhover, T., Gumprecht, L., Hoemke, A., Holmegaard, L., Johnsson, P., Kienitz, J. S., Kierspel, T., Krasniqi, F., Kuehnel, K. -U., Maurer, J., Messerschmidt, M., Moshammer, R., Mueller, Nele L. M., Rudek, B., Savelyev, E., Schlichting, I., Schmidt, C., Scholz, F., Schorb, S., Schulz, J., Seltmann, J., Stener, M., Stern, S., Techert, S., Thogersen, J, Trippel, S., Viefhaus, J., Vrakking, M, Stapelfeldt, H., Kuepper, J., Ullrich, J., Rudenko, A., and Rolles, D.
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Physics - Atomic Physics - Abstract
This paper gives an account of our progress towards performing femtosecond time-resolved photoelectron diffraction on gas-phase molecules in a pump-probe setup combining optical lasers and an X-ray Free-Electron Laser. We present results of two experiments aimed at measuring photoelectron angular distributions of laser-aligned 1-ethynyl-4-fluorobenzene (C8H5F) and dissociating, laseraligned 1,4-dibromobenzene (C6H4Br2) molecules and discuss them in the larger context of photoelectron diffraction on gas-phase molecules. We also show how the strong nanosecond laser pulse used for adiabatically laser-aligning the molecules influences the measured electron and ion spectra and angular distributions, and discuss how this may affect the outcome of future time-resolved photoelectron diffraction experiments., Comment: 24 pages, 10 figures, Faraday Discussions 171
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- 2014
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27. Charge migration in photo-ionized aromatic amino acids
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Trabattoni, A., Galli, M., Lara-Astiaso, M., Palacios, A., Greenwood, J., Tavernelli, I., Decleva, P., Nisoli, M., Martín, F., and Calegari, F.
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- 2019
28. Enantio-sensitive unidirectional light bending
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Ayuso, David, Ordonez, Andres F., Decleva, Piero, Ivanov, Misha, and Smirnova, Olga
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- 2021
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29. Multiple orbital contributions to molecular high-harmonic generation in an asymmetric top
- Author
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Spector, Limor S., Miyabe, Shungo, Magana, Alvaro, Petretti, Simon, Decleva, Piero, Martinez, Todd, Saenz, Alejandro, Guehr, Markus, and Bucksbaum, Philip H.
- Subjects
Physics - Atomic Physics ,Physics - Chemical Physics - Abstract
High-order harmonic generation (HHG) in aligned linear molecules can offer valuable information about strong-field interactions in lower-lying molecular orbitals, but extracting this information is difficult for three-dimensional molecular geometries. Our measurements of the asymmetric top SO2 show large axis dependencies, which change with harmonic order. The analysis shows that these spectral features must be due to field ionization and recombination from multiple orbitals during HHG. We expect that HHG can probe orbital dependencies using this approach for a broad class of asymmetric-top molecules., Comment: Main text and supplemental material
- Published
- 2013
30. Water Molecules in Ultrashort Intense Laser Fields
- Author
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Petretti, Simon, Saenz, Alejandro, Castro, Alberto, and Decleva, Piero
- Subjects
Physics - Atomic Physics - Abstract
Ionization and excitation of water molecules in intense laser pulses is studied theoretically by solving the three-dimensional time-dependent electronic Schr\"odinger equation within the single-active-electron approximation. The possibility to image orbital densities by measurement of the orientation-dependent ionization of H2O in few-cycle, 800nm linear-polarized laser pulses is investigated. While the highest-occupied molecular orbital 1b1 is found to dominate the overall ionization behavior, contributions from the energetically lower lying 3a1 orbital dominate the ionization yield in the nodal plane of the 1b1 orbital. The ratio of the ionization yields of the two orbitals depends on the intensity. Furthermore, even for laser pulses as long as 8 cycles the orientation-dependent ion yield depends on the carrier-envelope phase. In the interpretation of the orientation-dependent ionization as an imaging tool these effects have to be considered.
- Published
- 2011
31. Strong field ionization to multiple electronic states in water
- Author
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Farrell, Joe P., Petretti, Simon, Förster, Johann, McFarland, Brian K., Spector, Limor S., Vanne, Yulian V., Decleva, Piero, Bucksbaum, Philip H., Saenz, Alejandro, and Gühr, Markus
- Subjects
Physics - Atomic Physics - Abstract
High harmonic spectra show that laser-induced strong field ionization of water has a significant contribution from an inner-valence orbital. Our experiment uses the ratio of H2O and D2O high harmonic yields to isolate the characteristic nuclear motion of the molecular ionic states. The nuclear motion initiated via ionization of the highest occupied molecular orbital (HOMO) is small and is expected to lead to similar harmonic yields for the two isotopes. In contrast, ionization of the second least bound orbital (HOMO-1) exhibits itself via a strong bending motion which creates a significant isotope effect. We elaborate on this interpretation by simulating strong field ionization and high harmonic generation from the water isotopes using the time-dependent Schr\"odinger equation. We expect that this isotope marking scheme for probing excited ionic states in strong field processes can be generalized to other molecules.
- Published
- 2011
- Full Text
- View/download PDF
32. Alignment-Dependent Ionization of N$_2$, O$_2$, and CO$_2$ in Intense Laser Fields
- Author
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Petretti, Simon, Vanne, Yulian V., Saenz, Alejandro, Castro, Alberto, and Decleva, Piero
- Subjects
Physics - Atomic Physics - Abstract
The ionization probability of N$_2$, O$_2$, and CO$_2$ in intense laser fields is studied theoretically as a function of the alignment angle by solving the time-dependent Schr\"odinger equation numerically assuming only the single-active-electron approximation. The results are compared to recent experimental data [D.~Pavi{\v{c}}i{\'c} et al., Phys.\,Rev.\,Lett.\ {\bf 98}, 243001 (2007)] and good agreement is found for N$_2$ and O$_2$. For CO$_2$ a possible explanation is provided for the failure of simplified single-active-electron models to reproduce the experimentally observed narrow ionization distribution. It is based on a field-induced coherent core-trapping effect., Comment: 5 pages, 2 figures
- Published
- 2010
- Full Text
- View/download PDF
33. Auger–Meitner and X‑ray Absorption Spectra of Ethylene Cation: Insight into Conical Intersection Dynamics.
- Author
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Cabral Tenorio, Bruno Nunes, Pedersen, Jacob, Barbatti, Mario, Decleva, Piero, and Coriani, Sonia
- Published
- 2024
- Full Text
- View/download PDF
34. Density Functional Theory for the Photoionization Dynamics of Uracil
- Author
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Toffoli, D., Decleva, P., Gianturco, F. A., and Lucchese, R. R.
- Subjects
Physics - Chemical Physics - Abstract
Photoionization dynamics of the RNA base Uracil is studied in the framework of Density Functional Theory (DFT). The photoionization calculations take advantage of a newly developed parallel version of a multicentric approach to the calculation of the electronic continuum spectrum which uses a set of B-spline radial basis functions and a Kohn-Sham density functional hamiltonian. Both valence and core ionizations are considered. Scattering resonances in selected single-particle ionization channels are classified by the symmetry of the resonant state and the peak energy position in the photoelectron kinetic energy scale; the present results highlight once more the site specificity of core ionization processes. We further suggest that the resonant structures previously characterized in low-energy electron collision experiments are partly shifted below threshold by the photoionization processes. A critical evaluation of the theoretical results providing a guide for future experimental work on similar biosystems.
- Published
- 2007
- Full Text
- View/download PDF
35. Discrimination of Excited States of Acetylacetone through Theoretical Molecular-Frame Photoelectron Angular Distributions
- Author
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Aurora Ponzi, Marin Sapunar, Nadja Došlić, and Piero Decleva
- Subjects
photoelectron angular distribution ,MFPADs ,photoionization ,photodynamics ,excited states ,acetylacetone ,Organic chemistry ,QD241-441 - Abstract
Photoelectron angular distribution (PAD) in the laboratory frame for randomly oriented molecules is typically described by a single anisotropy parameter, the so-called asymmetry parameter. However, especially from a theoretical perspective, it is more natural to consider molecular photoionization by using a molecular frame. The molecular frame PADs (MFPADs) may be used to extract information about the electronic structure of the system studied. In the last decade, significant experimental efforts have been directed to MFPAD measurements. MFPADs are highly characterizing signatures of the final ionic states. In particular, they are very sensitive to the nature of the final state, which is embodied in the corresponding Dyson orbital. In our previous work on acetylacetone, a prototype system for studying intra-molecular hydrogen bond interactions, we followed the dynamics of the excited states involved in the photoexcitation–deexcitation process of this molecule. It remains to be explored the possibility of discriminating between different excited states through the MFPAD profiles. The calculation of MFPADs to differentiate excited states can pave the way to the possibility of a clear discrimination for all the cases where the recognition of excited states is otherwise intricate.
- Published
- 2022
- Full Text
- View/download PDF
36. Continuum Electronic States: The Tiresia Code
- Author
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Piero Decleva, Mauro Stener, and Daniele Toffoli
- Subjects
molecular photoionization ,electronic continuum states ,theoretical chemistry ,Organic chemistry ,QD241-441 - Abstract
A multicenter (LCAO) B-spline basis is described in detail, and its capabilities concerning affording convergent solutions for electronic continuum states and wavepacket propagation are presented. It forms the core of the Tiresia code, which implements static-DFT and TDDFT hamiltonians, as well as single channel Dyson-DFT and Dyson-TDDFT descriptions to include correlation in the bound states. Together they afford accurate and computationally efficient descriptions of photoionization properties of complex systems, both in the single photon and strong field environments. A number of examples are provided.
- Published
- 2022
- Full Text
- View/download PDF
37. Photoionization Observables from Multi-Reference Dyson Orbitals Coupled to B-Spline DFT and TD-DFT Continuum
- Author
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Bruno Nunes Cabral Tenorio, Aurora Ponzi, Sonia Coriani, and Piero Decleva
- Subjects
electron correlation ,photoelectron spectroscopy ,dyson orbitals ,photoionization ,Organic chemistry ,QD241-441 - Abstract
We present a theoretical model to compute the accurate photoionization dynamical parameters (cross-sections, asymmetry parameters and orbital, or cross-section, ratios) from Dyson orbitals obtained with the multi-state complete active space perturbation theory to the second order (MS-CASPT2) method. Our new implementation of Dyson orbitals in OpenMolcas takes advantage of the full Abelian symmetry point group and has the corrected normalization. The Dyson orbitals are coupled to an accurate description of the electronic continuum obtained with a multicentric B-spline basis at the DFT and TD-DFT levels. Two prototype diatomic molecules, i.e., CS and SiS, have been chosen due to their smallness, which hides important correlation effects. These effects manifest themselves in the appearance of well-characterized isolated satellite bands in the middle of the valence region. The rich satellite structures make CS and SiS the perfect candidates for a computational study based on our highly accurate MS-CASPT2/B-spline TD-DFT protocol.
- Published
- 2022
- Full Text
- View/download PDF
38. Acetylacetone photodynamics at a seeded free-electron laser
- Author
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R. J. Squibb, M. Sapunar, A. Ponzi, R. Richter, A. Kivimäki, O. Plekan, P. Finetti, N. Sisourat, V. Zhaunerchyk, T. Marchenko, L. Journel, R. Guillemin, R. Cucini, M. Coreno, C. Grazioli, M. Di Fraia, C. Callegari, K. C. Prince, P. Decleva, M. Simon, J. H. D. Eland, N. Došlić, R. Feifel, and M. N. Piancastelli
- Subjects
Science - Abstract
The first steps in photochemical processes involve changes in electronic and geometric structure on extremely short timescales. Here, the authors report femtosecond dynamics in prototypical acetylacetone, by pump-probe photoexcitation-photoemission experiments and static and dynamics calculations.
- Published
- 2018
- Full Text
- View/download PDF
39. Chiral topological light for detection of robust enantiosensitive observables
- Author
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Mayer, Nicola, Ayuso, David, Decleva, Piero, Khokhlova, Margarita, Pisanty, Emilio, Ivanov, Misha, and Smirnova, Olga
- Abstract
The topological response of matter to electromagnetic fields is a highly demanded property in materials design and metrology due to its robustness against noise and decoherence, stimulating recent advances in ultrafast photonics. Embedding topological properties into the enantiosensitive optical response of chiral molecules could therefore enhance the efficiency and robustness of chiral optical discrimination. Here we achieve such a topological embedding by introducing the concept of chiral topological light—a light beam which displays chirality locally, with an azimuthal distribution of its handedness described globally by a topological charge. The topological charge is mapped onto the azimuthal intensity modulation of the non-linear optical response, where enantiosensitivity is encoded into its spatial rotation. The spatial rotation is robust against intensity fluctuations and imperfect local polarization states of the driving field. Our theoretical results show that chiral topological light enables detection of percentage-level enantiomeric excesses in randomly oriented mixtures of chiral molecules, opening a way to new, extremely sensitive and robust chiro-optical spectroscopies with attosecond time resolution.
- Published
- 2024
- Full Text
- View/download PDF
40. Photoelectron circular dichroism of isopropanolamine
- Author
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Catone, D., Turchini, S., Contini, G., Prosperi, T., Stener, M., Decleva, P., and Zema, N.
- Published
- 2017
- Full Text
- View/download PDF
41. Photoionization of pyrrole from the B2 state: a computational study on the effects of Rydberg–valence mixing
- Author
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Ponzi, Aurora, Sapunar, Marin, Došlić, Nađa, and Decleva, Piero
- Published
- 2020
- Full Text
- View/download PDF
42. Sub-4-fs Charge Migration in Phenylalanine
- Author
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Calegari, F., Ayuso, D., Belshaw, L., Trabattoni, A., Anumula, S., De Camillis, S., Frassetto, F., Poletto, L., Palacios, A., Decleva, P., Greenwood, J., Martín, F., Nisoli, M., Yamanouchi, Kaoru, editor, Cundiff, Steven, editor, de Vivie-Riedle, Regina, editor, Kuwata-Gonokami, Makoto, editor, and DiMauro, Louis, editor
- Published
- 2015
- Full Text
- View/download PDF
43. Attosecond spectroscopy of bio-chemically relevant molecules
- Author
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Calegari, F., Trabattoni, A., Månsson, E., Greenwood, J. B., Decleva, P., Martìn, F., and Nisoli, M.
- Published
- 2018
- Full Text
- View/download PDF
44. Full-dimensional theoretical description of vibrationally resolved valence-shell photoionization of H2O
- Author
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Selma Engin, Jesús González-Vázquez, Gianluigi Grimaldi Maliyar, Aleksandar R. Milosavljević, Taishi Ono, Saikat Nandi, Denys Iablonskyi, Kuno Kooser, John D. Bozek, Piero Decleva, Edwin Kukk, Kiyoshi Ueda, and Fernando Martín
- Subjects
Crystallography ,QD901-999 - Abstract
We have performed a full-dimensional theoretical study of vibrationally resolved photoelectron emission from the valence shell of the water molecule by using an extension of the static-exchange density functional theory that accounts for ionization as well as for vibrational motion in the symmetric stretching, antisymmetric stretching, and bending modes. At variance with previous studies performed in centrosymmetric molecules, where vibrationally resolved spectra are mostly dominated by the symmetric stretching mode, in the present case, all three modes contribute to the calculated spectra, including intermode couplings. We have found that diffraction of the ejected electron by the various atomic centers is barely visible in the ratios between vibrationally resolved photoelectron spectra corresponding to different vibrational states of the remaining H2O+ cation (the so-called v-ratios), in contrast to the prominent oscillations observed in K-shell ionization of centrosymmetric molecules, including those that only contain hydrogen atoms around the central atoms, e.g., CH4. To validate the conclusions of our work, we have carried out synchrotron radiation experiments at the SOLEIL synchrotron and determined photoelectron spectra and v-ratios for H2O in a wide range of photon energies, from threshold up to 150 eV. The agreement with the theoretical predictions is good.
- Published
- 2019
- Full Text
- View/download PDF
45. A study of the valence shell electronic states of s-triazine by photoabsorption spectroscopy and ab initio calculations
- Author
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Holland, D.M.P., Shaw, D.A., Stener, M., Decleva, P., and Coriani, S.
- Published
- 2016
- Full Text
- View/download PDF
46. The OpenMolcas Web: A Community-Driven Approach to Advancing Computational Chemistry
- Author
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Li Manni, Giovanni, Fdez. Galván, Ignacio, Alavi, Ali, Aleotti, Flavia, Aquilante, Francesco, Autschbach, Jochen, Avagliano, Davide, Baiardi, Alberto, Bao, Jie J., Battaglia, Stefano, Birnoschi, Letitia, Blanco-González, Alejandro, Bokarev, Sergey I., Broer, Ria, Cacciari, Roberto, Calio, Paul B., Carlson, Rebecca K., Carvalho Couto, Rafael, Cerdán, Luis, Chibotaru, Liviu F., Chilton, Nicholas F., Church, Jonathan Richard, Conti, Irene, Coriani, Sonia, Cuéllar-Zuquin, Juliana, Daoud, Razan E., Dattani, Nike, Decleva, Piero, de Graaf, Coen, Delcey, Mickaël G., De Vico, Luca, Dobrautz, Werner, Dong, Sijia S., Feng, Rulin, Ferré, Nicolas, Filatov(Gulak), Michael, Gagliardi, Laura, Garavelli, Marco, González, Leticia, Guan, Yafu, Guo, Meiyuan, Hennefarth, Matthew R., Hermes, Matthew R., Hoyer, Chad E., Huix-Rotllant, Miquel, Jaiswal, Vishal Kumar, Kaiser, Andy, Kaliakin, Danil S., Khamesian, Marjan, King, Daniel S., Kochetov, Vladislav, Krośnicki, Marek, Kumaar, Arpit Arun, Larsson, Ernst D., Lehtola, Susi, Lepetit, Marie-Bernadette, Lischka, Hans, López Ríos, Pablo, Lundberg, Marcus, Ma, Dongxia, Mai, Sebastian, Marquetand, Philipp, Merritt, Isabella C. D., Montorsi, Francesco, Mörchen, Maximilian, Nenov, Artur, Nguyen, Vu Ha Anh, Nishimoto, Yoshio, Oakley, Meagan S., Olivucci, Massimo, Oppel, Markus, Padula, Daniele, Pandharkar, Riddhish, Phung, Quan Manh, Plasser, Felix, Raggi, Gerardo, Rebolini, Elisa, Reiher, Markus, Rivalta, Ivan, Roca-Sanjuán, Daniel, Romig, Thies, Safari, Arta Anushirwan, Sánchez-Mansilla, Aitor, Sand, Andrew M., Schapiro, Igor, Scott, Thais R., Segarra-Martí, Javier, Segatta, Francesco, Sergentu, Dumitru-Claudiu, Sharma, Prachi, Shepard, Ron, Shu, Yinan, Staab, Jakob K., Straatsma, Tjerk P., Sørensen, Lasse Kragh, Tenorio, Bruno Nunes Cabral, Truhlar, Donald G., Ungur, Liviu, Vacher, Morgane, Veryazov, Valera, Voß, Torben Arne, Weser, Oskar, Wu, Dihua, Yang, Xuchun, Yarkony, David, Zhou, Chen, Zobel, J. Patrick, and Lindh, Roland
- Abstract
The developments of the open-source OpenMolcaschemistry software environment since spring 2020 are described, with a focus on novel functionalities accessible in the stable branch of the package or via interfaces with other packages. These developments span a wide range of topics in computational chemistry and are presented in thematic sections: electronic structure theory, electronic spectroscopy simulations, analytic gradients and molecular structure optimizations, ab initio molecular dynamics, and other new features. This report offers an overview of the chemical phenomena and processes OpenMolcascan address, while showing that OpenMolcasis an attractive platform for state-of-the-art atomistic computer simulations.
- Published
- 2023
- Full Text
- View/download PDF
47. A study of the valence shell electronic structure and photoionisation dynamics of s-triazine
- Author
-
Coriani, S., Stener, M., Decleva, P., Holland, D.M.P., Potts, A.W., and Karlsson, L.
- Published
- 2015
- Full Text
- View/download PDF
48. Controlling Fragmentation of the Acetylene Cation in the Vacuum Ultraviolet via Transient Molecular Alignment
- Author
-
Varvarezos, L., primary, Delgado-Guerrero, J., additional, Di Fraia, M., additional, Kelly, T. J., additional, Palacios, A., additional, Callegari, C., additional, Cavalieri, A. L., additional, Coffee, R., additional, Danailov, M., additional, Decleva, P., additional, Demidovich, A., additional, DiMauro, L., additional, Düsterer, S., additional, Giannessi, L., additional, Helml, W., additional, Ilchen, M., additional, Kienberger, R., additional, Mazza, T., additional, Meyer, M., additional, Moshammer, R., additional, Pedersini, C., additional, Plekan, O., additional, Prince, K. C., additional, Simoncig, A., additional, Schletter, A., additional, Ueda, K., additional, Wurzer, M., additional, Zangrando, M., additional, Martín, F., additional, and Costello, J. T., additional
- Published
- 2022
- Full Text
- View/download PDF
49. Ultrafast electron dynamics in phenylalanine initiated by attosecond pulses
- Author
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Calegari, F., Ayuso, D., Trabattoni, A., Belshaw, L., De Camillis, S., Anumula, S., Frassetto, F., Poletto, L., Palacios, A., Decleva, P., Greenwood, J. B., Martín, F., and Nisoli, M.
- Published
- 2014
50. Interference and diffraction in photoelectron spectra
- Author
-
Decleva, P., Ponzi, A., and Santizo, I.
- Published
- 2014
- Full Text
- View/download PDF
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