Condensed Matter Systems Exposed to Radiation: Multiscale Theory, Simulations, and Experiment.

This roadmap reviews the new, highly interdisciplinary research field studying the behavior of condensed matter systems exposed to radiation. The Review highlights several recent advances in the field and provides a roadmap for the development of the field over the next decade. Condensed matter systems exposed to radiation can be inorganic, organic, or biological, finite or infinite, composed of different molecular species or materials, exist in different phases, and operate under different thermodynamic conditions.

THz to far-infrared spectra of the known crystal polymorphs of phenylalanine.

There is renewed interest in the structure of the essential amino acid phenylalanine in the solid state. Three new polymorphs were found in the years 2012 to 2014. Here, we investigate the structure, stability, and energetical ordering of these phases using first-principles simulations at the level of density functional theory incorporating van der Waals interactions.

Probing Photoionization Dynamics in Acetylene with Angle-Resolved Attosecond Interferometry.

Photoionization of acetylene by extreme ultraviolet light results in a stand-alone contribution from the outermost valence orbital, followed by well-separated photoelectron bands from deeper molecular orbitals. This makes acetylene an ideal candidate for probing the photoionization dynamics in polyatomic molecules free from the spectral congestion often arising after interaction with an attosecond pulse train. Here, using an angle-resolved attosecond interferometric technique, we extract the photoionization time delays for the outermost valence orbital in acetylene relative to an atomic target, namely argon.

GlAIcomics: a deep neural network classifier for spectroscopy-augmented mass spectrometric glycans data.

Carbohydrate sequencing is a formidable task identified as a strategic goal in modern biochemistry. It relies on identifying a large number of isomers and their connectivity with high accuracy. Recently, gas phase vibrational laser spectroscopy combined with mass spectrometry tools have been proposed as a very promising sequencing approach.

Tackling recalcitrant Pseudomonas aeruginosa infections in critical illness via anti-virulence monotherapy.

Intestinal barrier derangement allows intestinal bacteria and their products to translocate to the systemic circulation. Pseudomonas aeruginosa (PA) superimposed infection in critically ill patients increases gut permeability and leads to gut-driven sepsis. PA infections are challenging due to multi-drug resistance (MDR), biofilms, and/or antibiotic tolerance.

Few-Femtosecond Isotope Effect in Polyatomic Molecules Ionized by Extreme Ultraviolet Attosecond Pulse Trains.

Following ionization by an extreme ultraviolet (XUV) attosecond pulse train, a polyatomic molecule can be promoted to more-than-one excited states of the residual ion. The ensuing relaxation dynamics is often facilitated by several reaction coordinates, making them difficult to disentangle by the usual spectroscopic means. Here, we show that in atto-chemistry isotope labeling can be an efficient tool for unraveling the relaxation pathways in highly excited photoionized molecules.

On-the-fly investigation of XUV excited large molecular ions using a high harmonic generation light source.

We present experiments where extreme ultraviolet femtosecond light pulses are used to photoexcite large molecular ions at high internal energy. This is done by combining an electrospray ionization source and a mass spectrometer with a pulsed light source based on high harmonic generation. This allows one to study the interaction between high energy photons and mass selected ions in conditions that are accessible on large-scale facilities.

Air-photonics terahertz platform with versatile micro-controller based interface and data acquisition.

We present a terahertz (THz) platform employing air plasma produced by an ultrashort two-color laser pulse as a broadband THz source and air biased coherent detection (ABCD) of the THz field. In contrast to previous studies, a simple peak detector connected to a micro-controller board acquires the ABCD-signal coming from the avalanche photodiode. Numerical simulations of the whole setup yield temporal and spectral profiles of the terahertz electric field in both source and detection area.

Anisotropic dynamics of two-photon ionization: An attosecond movie of photoemission.

Imaging in real time the complete dynamics of a process as fundamental as photoemission has long been out of reach because of the difficulty of combining attosecond temporal resolution with fine spectral and angular resolutions. Here, we achieve full decoding of the intricate angle-dependent dynamics of a photoemission process in helium, spectrally and anisotropically structured by two-photon transitions through intermediate bound states. Using spectrally and angularly resolved attosecond electron interferometry, we characterize the complex-valued transition probability amplitude toward the photoelectron quantum state.

Time-resolved relaxation and cage opening in diamondoids following XUV ultrafast ionization.

Unraveling ultrafast processes induced by energetic radiation is compulsory to understand the evolution of molecules under extreme excitation conditions. To describe these photo-induced processes, one needs to perform time-resolved experiments to follow in real time the dynamics induced by the absorption of light. Recent experiments have demonstrated that ultrafast dynamics on few tens of femtoseconds are expected in such situations and a very challenging task is to identify the role played by electronic and nuclear degrees of freedom, charge, energy flows and structural rearrangements.

Controlled ultrafast ππ*-πσ* dynamics in tryptophan-based peptides with tailored micro-environment.

Ultrafast charge, energy and structural dynamics in molecules are driven by the topology of the multidimensional potential energy surfaces that determines the coordinated electronic and nuclear motion. These processes are also strongly influenced by the interaction with the molecular environment, making very challenging a general understanding of these dynamics on a microscopic level. Here we use electrospray and mass spectrometry technologies to produce isolated molecular ions with a controlled micro-environment.

Experimental Evidence of Sensitivity of the High Harmonic Generation to Hydrogen Bonding.

The influence of hydrogen bonding and the associated attosecond hole delocalization on the high-order harmonic generation (HHG) process is investigated with the help of hydrogen-bonded binary mixture of acetonitrile and chloroform solvent vapors. We observe a strong enhancement of the HH yield compared to the results obtained with pure samples. We propose that the observed increase of HHG efficiency is due to the presence of hydrogen-bonded binary mixture.

On-the-Fly Femtosecond Action Spectroscopy of Charged Cyanine Dyes: Electronic Structure versus Geometry.

Understanding optical properties of molecular dyes is required to drive progress in molecular photonics. This requires a fundamental comprehension of the role of electronic structure, geometry, and interactions with the environment in order to guide molecular engineering strategies. In this context, we studied charged cyanine dye molecules in the gas phase with a controlled microenvironment to unravel the origin of the spectral tuning of this class of molecules.

Delayed Relaxation of Highly Excited Cationic States in Naphthalene.

Rapid energy transfer from electronic to nuclear degrees of freedom underlies many biological processes and astrophysical observations. The efficiency of this energy transfer depends strongly on the complex interplay between electronic and nuclear motions. In this study, we report two-color pump-probe experiments that probe the relaxation dynamics of highly excited cationic states of naphthalene, a prototypical polycyclic aromatic hydrocarbon molecule, which are produced using wavelength-selected, ultrashort extreme ultraviolet pulses.

Electron correlation driven non-adiabatic relaxation in molecules excited by an ultrashort extreme ultraviolet pulse.

The many-body quantum nature of molecules determines their static and dynamic properties, but remains the main obstacle in their accurate description. Ultrashort extreme ultraviolet pulses offer a means to reveal molecular dynamics at ultrashort timescales. Here, we report the use of time-resolved electron-momentum imaging combined with extreme ultraviolet attosecond pulses to study highly excited organic molecules.

Ultrafast Nonadiabatic Cascade and Subsequent Photofragmentation of Extreme Ultraviolet Excited Caffeine Molecule.

Ultrafast XUV chemistry is offering new opportunities to decipher the complex dynamics taking place in highly excited molecular states and thus better understand fundamental natural phenomena as molecule formation in interstellar media. We used ultrashort XUV light pulses to perform XUV pump-IR probe experiments in caffeine as a model of prebiotic molecule. We observed a 40 fs decay of excited cationic states.

Molecular Insights into Function and Competitive Inhibition of Multiple Virulence Factor Regulator.

New approaches to antimicrobial drug discovery are urgently needed to combat intractable infections caused by multidrug-resistant (MDR) bacteria. ultiple irulence actor egulator (MvfR or PqsR), a quorum sensing transcription factor, regulates functions important in both acute and persistent infections. Recently identified non-ligand-based benzamine-benzimidazole (BB) inhibitors of MvfR suppress both acute and persistent infections in mice without perturbing bacterial growth.

A detailed-balance model for thermionic emission from polyanions: The case of fullerene dianions.

A detailed-balance model for thermionic emission from polyanions has been developed and applied to fullerene dianions. The specificity of this delayed decay process is electron tunneling through the repulsive Coulomb barrier (RCB). An analytical expression of the RCB is derived from electrostatic modeling of the fullerene cage.

Liquid Chromatography/Mass Spectrometry (LC/MS) for the Detection and Quantification of N-Acyl-L-Homoserine Lactones (AHLs) and 4-Hydroxy-2-Alkylquinolines (HAQs).

High-performance liquid chromatography (HPLC) coupled in-line with mass spectrometry (MS) permits rapid and specific identification and quantification of N-acyl-L-homoserine lactones (AHLs) and 4-hydroxy-2-alkylquinolines (HAQs). We are presenting here methods for the analysis of these molecules directly from biological samples using LC/MS.

Few-femtosecond passage of conical intersections in the benzene cation.

Observing the crucial first few femtoseconds of photochemical reactions requires tools typically not available in the femtochemistry toolkit. Such dynamics are now within reach with the instruments provided by attosecond science. Here, we apply experimental and theoretical methods to assess the ultrafast nonadiabatic vibronic processes in a prototypical complex system-the excited benzene cation.

Influence of long-range Coulomb interaction in velocity map imaging.

The standard velocity-map imaging (VMI) analysis relies on the simple approximation that the residual Coulomb field experienced by the photoelectron ejected from a neutral or ion system may be neglected. Under this almost universal approximation, the photoelectrons follow ballistic (parabolic) trajectories in the externally applied electric field, and the recorded image may be considered as a 2D projection of the initial photoelectron velocity distribution. There are, however, several circumstances where this approximation is not justified and the influence of long-range forces must absolutely be taken into account for the interpretation and analysis of the recorded images.

XUV-induced reactions in benzene on sub-10 fs timescale: nonadiabatic relaxation and proton migration.

Unraveling ultrafast dynamical processes in highly excited molecular species has an impact on our understanding of chemical processes such as combustion or the chemical composition of molecular clouds in the universe. In this article we use short (<7 fs) XUV pulses to produce excited cationic states of benzene molecules and probe their dynamics using few-cycle VIS/NIR laser pulses. The excited states produced by the XUV pulses lie in an especially complex spectral region where multi-electronic effects play a dominant role.

Indoor swimming pool environments and self-reported irritative and respiratory symptoms among lifeguards.

A web survey was conducted among 870 lifeguards (current and former) to assess the relationship between exposure to indoor swimming pool environments and respiratory health. Associations between respiratory symptoms and asthma with varying lengths of occupational exposure were assessed by multiple logistic regression. Lifeguards exposed more than 500 hours in the previous 12 months experienced more cough (adjustedOR = 2.

Polypharmacology Approaches against the Pseudomonas aeruginosa MvfR Regulon and Their Application in Blocking Virulence and Antibiotic Tolerance.

Pseudomonas aeruginosa is an important nosocomial pathogen that is frequently recalcitrant to available antibiotics, underlining the urgent need for alternative therapeutic options against this pathogen. Targeting virulence functions is a promising alternative strategy as it is expected to generate less-selective resistance to treatment compared to antibiotics. Capitalizing on our nonligand-based benzamide-benzimidazole (BB) core structure compounds reported to efficiently block the activity of the P.

An instrument combining an electrospray ionization source and a velocity-map imaging spectrometer for studying delayed electron emission of polyanions.

An instrument combining an electrospray ionization source and a velocity-map imaging (VMI) spectrometer has been developed in order to study the delayed electron emission of molecular anions and especially of polyanions. It operates at a high repetition rate (kHz) in order to increase the acquisition speed. The VMI spectrometer has been upgraded for nanosecond time resolution by gating the voltages applied on the position-sensitive detector.