Chiral topological light for detection of robust enantiosensitive observables.

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.

Attosecond impulsive stimulated X-ray Raman scattering in liquid water.

We report the measurement of impulsive stimulated x-ray Raman scattering in neutral liquid water. An attosecond pulse drives the excitations of an electronic wavepacket in water molecules. The process comprises two steps: a transition to core-excited states near the oxygen atoms accompanied by transition to valence-excited states.

Capturing electron-driven chiral dynamics in UV-excited molecules.

Chiral molecules, used in applications such as enantioselective photocatalysis, circularly polarized light detection and emission and molecular switches, exist in two geometrical configurations that are non-superimposable mirror images of each other. These so-called (R) and (S) enantiomers exhibit different physical and chemical properties when interacting with other chiral entities. Attosecond technology might enable influence over such interactions, given that it can probe and even direct electron motion within molecules on the intrinsic electronic timescale and thereby control reactivity.

Ultrafast control over chiral sum-frequency generation.

We introduce an ultrafast all-optical approach for efficient chiral recognition that relies on the interference between two low-order nonlinear processes that are ubiquitous in nonlinear optics: sum-frequency generation and third-harmonic generation. In contrast to traditional sum-frequency generation, our approach encodes the medium's handedness in the intensity of the emitted harmonic signal, rather than in its phase, and it enables full control over the enantiosensitive response. We show how, by sculpting the sub-optical-cycle oscillations of the driving laser field, we can force one molecular enantiomer to emit bright light while its mirror twin remains dark, thus reaching the ultimate efficiency limit of chiral sensitivity via low-order nonlinear light-matter interactions.

Tilting light's polarization plane to spatially separate the ultrafast nonlinear response of chiral molecules.

Distinguishing between the left- and right-handed versions of a chiral molecule (enantiomers) is vital, but also inherently difficult. Traditional optical methods using elliptically/circularly polarized light rely on linear effects which arise beyond the electric-dipole approximation, posing major limitations for ultrafast spectroscopy. Here we show how to turn an ultrashort elliptical pulse into an efficient chiro-optical tool: by tilting its polarization plane towards its propagation direction.

Ultrafast chirality: the road to efficient chiral measurements.

Today we are witnessing the electric-dipole revolution in chiral measurements. Here we reflect on its lessons and outcomes, such as the perspective on chiral measurements using the complementary principles of "chiral reagent" and "chiral observer", the hierarchy of scalar, vectorial and tensorial enantio-sensitive observables, the new properties of the chiro-optical response in the ultrafast and non-linear domains, and the geometrical magnetism associated with the chiral response in photoionization. The electric-dipole revolution is a landmark event.

New opportunities for ultrafast and highly enantio-sensitive imaging of chiral nuclear dynamics enabled by synthetic chiral light.

Synthetic chiral light [D. Ayuso , , 2019, , 866-871] has opened up new opportunities for ultrafast and highly efficient imaging and control of chiral matter. Here we show that the giant enantio-sensitivity enabled by such light could be exploited to probe chiral nuclear rearrangements during chemical reactions in a highly enantio-sensitive manner.

Strong chiral response in non-collinear high harmonic generation driven by purely electric-dipole interactions.

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.

Enantio-sensitive unidirectional light bending.

Structured light, which exhibits nontrivial intensity, phase, and polarization patterns in space, has key applications ranging from imaging and 3D micromanipulation to classical and quantum communication. However, to date, its application to molecular chirality has been limited by the weakness of magnetic interactions. Here we structure light's local handedness in space to introduce and realize an enantio-sensitive interferometer for efficient chiral recognition without magnetic interactions, which can be seen as an enantio-sensitive version of Young's double slit experiment.

Attosecond Pump-Probe Spectroscopy of Charge Dynamics in Tryptophan.

Attosecond pump-probe experiments performed in small molecules have allowed tracking charge dynamics in the natural time scale of electron motion. That this is also possible in biologically relevant molecules is still a matter of debate, because the large number of available nuclear degrees of freedom might destroy the coherent charge dynamics induced by the attosecond pulse. Here we investigate extreme ultraviolet-induced charge dynamics in the amino acid tryptophan.

Validation to Spanish of the Caring Assessment Tool (CAT-V).

Objective: to translate and validate to Spanish the Caring Assessment Scale tool, CAT-V, by Joanne Duffy, within the framework of Jean Watson; as a secondary objective, it is proposed to evaluate its psychometric properties. There are tools designed to measure the patient's perception of provided cares, including CAT-V, the subject of our interest, in a way that it can be used in Spanish-speaking patients.

Methods: to meet the objectives, it was performed sequential translation and retro-translation of the scale to be validated, through a standardized procedure.

Ultrafast charge dynamics in glycine induced by attosecond pulses.

The combination of attosecond pump-probe techniques with mass spectrometry methods has recently led to the first experimental demonstration of ultrafast charge dynamics in a biomolecule, the amino acid phenylalanine [Calegari et al., Science, 2014, 346, 336]. Using an extension of the static-exchange density functional theory (DFT) method, the observed dynamics was explained as resulting from the coherent superposition of ionic states produced by the broadband attosecond pulse.

Decoherence, control and attosecond probing of XUV-induced charge migration in biomolecules. A theoretical outlook.

The sudden ionization of a molecule by an attosecond pulse is followed by charge redistribution on a time scale from a few femtoseconds down to hundreds of attoseconds. This ultrafast redistribution is the result of the coherent superposition of electronic continua associated with the ionization thresholds that are reached by the broadband attosecond pulse. Thus, a correct theoretical description of the time evolution of the ensuing wave packet requires the knowledge of the actual ionization amplitudes associated with all open ionization channels, a real challenge for large and medium-size molecules.