19 results
Search Results
Now showing 1 - 10 of 19
- ItemSub-laser-cycle control of coupled electron–nuclear dynamics at a conical intersection([London] : IOP, 2015) Richter, Maria; Bouakline, Foudhil; González-Vázquez, Jesús; Martínez-Fernández, Lara; Corral, Inés; Patchkovskii, Serguei; Morales, Felipe; Ivanov, Misha; Martín, Fernando; Smirnova, OlgaNonadiabatic processes play a fundamental role in the understanding of photochemical processes in excited polyatomic molecules. A particularly important example is that of radiationless electronic relaxation at conical intersections (CIs). We discuss new opportunities for controlling coupled electron–nuclear dynamics at CIs, offered by the advent of nearly single-cycle, phase-stable, mid-infrared laser pulses. To illustrate the control mechanism, a two-dimensional model of the NO2 molecule is considered. The key idea of the control scheme is to match the time scale of the laser field oscillations to the characteristic time scale of the wave packet transit through the CI. The instantaneous laser field changes the shape and position of the CI as the wave packet passes through. As the CI moves in the laser field, it 'slices' through the wave packet, sculpting it in the coordinate and momentum space in a way that is sensitive to the carrier-envelope phase of the control pulse. We find that the electronic coherence imparted on the sub-laser-cycle time scale manifests during much longer nuclear dynamics that follow on the many tens of femtosecond time scale. Control efficiency as a function of molecular orientation is analyzed, showing that modest alignment is sufficient for showing the described effects.
- ItemRecent developments in R-matrix applications to molecular processes(Bristol : IOP Publ., 2015) Mašín, Zdeněk; Harvey, Alex; Houfek, Karel; Brambila, Danilo S.; Morales, Felipe; Gorfinkiel, Jimena D.; Tennyson, Jonathan; Smirnova, OlgaWe report on recent developments of the UKRmol suite, an implementation of the molecular R- matrix method and present examples of the calculations (e.g. electron scattering, photoionization, high harmonic generation, etc.) it has enabled.
- ItemNO2molecular frame photoelectron angular distributions for a range of geometries using the R-matrix method(Bristol : IOP Publ., 2015) Brambila, Danilo S.; Harvey, Alex G.; Mašín, Zdeněk; Smirnova, OlgaWe present R-matrix calculations of photoionization from NO2, resolved in energy, angle, and both neutral and ionic state, for a range of molecular geometries, including in the vicinity of the 2A1/2B2 conical intersection.
- ItemRotational quantum beat lasing without inversion(Washington, DC : OSA, 2020) Richter, Maria; Lytova, Marianna; Morales, Felipe; Haessler, Stefan; Smirnova, Olga; Spanner, Michael; Ivanov, MishaIn standard lasers, light amplification requires population inversion between an upper and a lower state to break the reciprocity between absorption and stimulated emission. However, in a medium prepared in a specific superposition state, quantum interference may fully suppress absorption while leaving stimulated emission intact, opening the possibility of lasing without inversion. Here we show that lasing without inversion arises naturally during propagation of intense femtosecond laser pulses in air. It is triggered by the combination of molecular ionization and molecular alignment, both unavoidable in intense light fields. The effect could enable inversionless amplification of broadband radiation in many molecular gases, opening unusual opportunities for remote sensing. © 2020 Optical Society of America
- ItemSignatures of attosecond electronic–nuclear dynamics in the one-photon ionization of molecular hydrogen: analytical model versusab initiocalculations([London] : IOP, 2015) Medišauskas, Lukas; Morales, Felipe; Palacios, Alicia; González-Castrillo, Alberto; Plimak, Lev; Smirnova, Olga; Martín, Fernando; Ivanov, Misha YuWe present an analytical model based on the time-dependent WKB approximation to reproduce the photoionization spectra of an H2 molecule in the autoionization region. We explore the nondissociative channel, which is the major contribution after one-photon absorption, and we focus on the features arising in the energy differential spectra due to the interference between the direct and the autoionization pathways. These features depend on both the timescale of the electronic decay of the autoionizing state and the time evolution of the vibrational wavepacket created in this state. With full ab initio calculations and with a one-dimensional approach that only takes into account the nuclear wavepacket associated to the few relevant electronic states we compare the ground state, the autoionizing state, and the background continuum electronic states. Finally, we illustrate how these features transform from molecular-like to atomic-like by increasing the mass of the system, thus making the electronic decay time shorter than the nuclear wavepacket motion associated with the resonant state. In other words, autoionization then occurs faster than the molecular dissociation into neutrals.
- ItemSub-cycle valleytronics: control of valley polarization using few-cycle linearly polarized pulses(Washington, DC : OSA, 2021) Jiménez-Galán, Álvaro; Silva, Rui E. F.; Smirnova, Olga; Ivanov, MishaSo far, it has been assumed that selective excitation of a desired valley in the Brillouin zone of a hexagonal two-dimensional material has to rely on using circularly polarized fields. We theoretically demonstrate a way to control the valley excitation in hexagonal 2D materials on a few-femtosecond timescale using a few-cycle, linearly polarized pulse with controlled carrier–envelope phase. The valley polarization is mapped onto the strength of the perpendicular harmonic signal of a weak, linearly polarized pulse, which allows to read this information all-optically without destroying the valley state and without relying on the Berry curvature, making our approach potentially applicable to inversion-symmetric materials. We show applicability of this method to hexagonal boron nitride and MoS2.
- ItemReconstruction of the time-dependent electronic wave packet arising from molecular autoionization(Washington, DC [u.a.] : Assoc., 2018) Bello, Roger Y.; Canton, Sophie E.; Jelovina, Denis; Bozek, John D.; Rude, Bruce; Smirnova, Olga; Ivanov, Mikhail Y.; Palacios, Alicia; Martín, FernandoAutoionizing resonances are paradigmatic examples of two-path wave interferences between direct photoionization, which takes a few attoseconds, and ionization via quasi-bound states, which takes much longer. Time-resolving the evolution of these interferences has been a long-standing goal, achieved recently in the helium atom owing to progress in attosecond technologies. However, already for the hydrogen molecule, similar time imaging has remained beyond reach due to the complex interplay between fast nuclear and electronic motions. We show how vibrationally resolved photoelectron spectra of H2 allow one to reconstruct the associated subfemtosecond autoionization dynamics by using the ultrafast nuclear dynamics as an internal clock, thus forgoing ultrashort pulses. Our procedure should be general for autoionization dynamics in molecules containing light nuclei, which are ubiquitous in chemistry and biology.
- ItemCross-polarized common-path temporal interferometry for high-sensitivity strong-field ionization measurements(Washington, DC : Soc., 2022) Nie, Zan; Nambu, Noa; Marsh, Kenneth A.; Welch, Eric; Matteo, Daniel; Zhang, Chaojie; Wu, Yipeng; Patchkovskii, Serguei; Morales, Felipe; Smirnova, Olga; Joshi, ChanAbsolute density measurements of low-ionization-degree or low-density plasmas ionized by lasers are very important for understanding strong-field physics, atmospheric propagation of intense laser pulses, Lidar etc. A cross-polarized common-path temporal interferometer using balanced detection was developed for measuring plasma density with a sensitivity of ∼0.6 mrad, equivalent to a plasma density-length product of ∼2.6 × 1013 cm-2 if using an 800 nm probe laser. By using this interferometer, we have investigated strong-field ionization yield versus intensity for various noble gases (Ar, Kr, and Xe) using 800 nm, 55 fs laser pulses with both linear (LP) and circular (CP) polarization. The experimental results were compared to the theoretical models of Ammosov-Delone-Krainov (ADK) and Perelomov-Popov-Terent'ev (PPT). We find that the measured phase change induced by plasma formation can be explained by the ADK theory in the adiabatic tunneling ionization regime, while PPT model can be applied to all different regimes. We have also measured the photoionization and fractional photodissociation of molecular (MO) hydrogen. By comparing our experimental results with PPT and MO-PPT models, we have determined the likely ionization pathways when using three different pump laser wavelengths of 800 nm, 400 nm, and 267 nm.
- ItemRole of electronic correlations in photoionization of NO2 in the vicinity of the 2A1/2B2 conical intersection(Cambridge : The Royal Soc. of Chemistry, 2017) Brambila, Danilo S.; Harvey, Alex G.; Houfek, Karel; Mašín, Zdeněk; Smirnova, OlgaWe present the first ab initio multi-channel photoionization calculations for NO2 in the vicinity of the 2A1/2B2 conical intersection, for a range of nuclear geometries, using our newly developed set of tools based on the ab initio multichannel R-matrix method. Electronic correlation is included in both the neutral and the scattering states of the molecule via configuration interaction. Configuration mixing is especially important around conical intersections and avoided crossings, both pertinent for NO2, and manifests itself via significant variations in photoelectron angular distributions. The method allows for a balanced and accurate description of the photoionization/photorecombination for a number of different ionic channels in a wide range of photoelectron energies up to 100 eV. Proper account of electron correlations is crucial for interpreting time-resolved signals in photoelectron spectroscopy and high harmonic generation (HHG) from polyatomic molecules.
- ItemChiral dichroism in bi-elliptical high-order harmonic generation(Bristol : IOP Publ., 2018-02-28) Ayuso, David; Decleva, Piero; Patchkovskii, Serguei; Smirnova, OlgaThe application of strong bi-elliptically polarized laser fields to the generation of high-order harmonics in organic molecules offers exceptional opportunities for chiral recognition and chiral discrimination. These fields are made by combining an elliptically polarized fundamental, typically in the infrared range, with its counter-rotating second harmonic. Here we present a theoretical study of the harmonic emission from the chiral molecule propylene oxide in bi-elliptical fields. Our calculations include, for the first time in such a complex system, accurate photorecomination matrix elements, evaluated using the static-exchange density functional theory method. We show that bi-elliptical light can induce strong chiral dichroism in the harmonic spectra of chiral molecules in a broad range of harmonic numbers and ellipticities.