Following a chemical reaction using high-harmonic interferometry.

The study of chemical reactions on the molecular (femtosecond) timescale typically uses pump laser pulses to excite molecules and subsequent probe pulses to interrogate them. The ultrashort pump pulse can excite only a small fraction of molecules, and the probe wavelength must be carefully chosen to discriminate between excited and unexcited molecules. The past decade has seen the emergence of new methods that are also aimed at imaging chemical reactions as they occur, based on X-ray diffraction, electron diffraction or laser-induced recollision--with spectral selection not available for any of these new methods. Here we show that in the case of high-harmonic spectroscopy based on recollision, this apparent limitation becomes a major advantage owing to the coherent nature of the attosecond high-harmonic pulse generation. The coherence allows the unexcited molecules to act as local oscillators against which the dynamics are observed, so a transient grating technique can be used to reconstruct the amplitude and phase of emission from the excited molecules. We then extract structural information from the amplitude, which encodes the internuclear separation, by quantum interference at short times and by scattering of the recollision electron at longer times. The phase records the attosecond dynamics of the electrons, giving access to the evolving ionization potentials and the electronic structure of the transient molecule. In our experiment, we are able to document a temporal shift of the high-harmonic field of less than an attosecond (1 as = 10(-18) s) between the stretched and compressed geometry of weakly vibrationally excited Br(2) in the electronic ground state. The ability to probe structural and electronic features, combined with high time resolution, make high-harmonic spectroscopy ideally suited to measuring coupled electronic and nuclear dynamics occurring in photochemical reactions and to characterizing the electronic structure of transition states.

All-optical measurement of high-harmonic amplitudes and phases in aligned molecules.

We report a new all-optical approach to measuring the phase and amplitude of high-harmonic emission from aligned molecules. We combine the transient grating technique with a continuous rotation of the molecular alignment axis and develop an analytical model that enables the simultaneous determination of phases and amplitudes. Measurements in N(2) molecules are shown to be in qualitative agreement with the results of ab initio quantum scattering calculations.

Revealing the Cooper minimum of N2 by molecular frame high-harmonic spectroscopy.

Molecular frame high-harmonic spectra of aligned N2 molecules reveal a Cooper-like minimum. By deconvolving the laboratory frame alignment distribution, what was previously thought to be a maximum of emission along the molecular axis is found to be maxima at 35 degrees off axis, with a spectral minimum on axis. Both of these features are supported by photoionization calculations that underline the relationship between high-harmonic spectroscopy and photoionization measurements. The calculations reveal that the on axis spectral minimum is a Cooper-like minimum that arises from the destructive interference of the p and f partial wave contributions to high-harmonic photorecombination. Features such as Cooper minima and shape resonances are ubiquitous in molecular photoionization or recombination.

Oriented rotational wave-packet dynamics studies via high harmonic generation.

We produce oriented rotational wave packets in CO and measure their characteristics via high harmonic generation. The wave packet is created using an intense, femtosecond laser pulse and its second harmonic. A delayed 800 nm pulse probes the wave packet, generating even-order high harmonics that arise from the broken symmetry induced by the orientation dynamics. The even-order harmonic radiation that we measure appears on a zero background, enabling us to accurately follow the temporal evolution of the wave packet. Our measurements reveal that, for the conditions optimum for harmonic generation, the orientation is produced by preferential ionization which depletes the sample of molecules of one orientation.

Probing polar molecules with high harmonic spectroscopy.

We bring the methodology of orienting polar molecules together with the phase sensitivity of high harmonic spectroscopy to experimentally compare the phase difference of attosecond bursts of radiation emitted upon electron recollision from different ends of a polar molecule. This phase difference has an impact on harmonics from aligned polar molecules, suppressing emission from the molecules parallel to the driving laser field while favoring the perpendicular ones. For oriented molecules, we measure the amplitude ratio of even to odd harmonics produced when intense light irradiates CO molecules and determine the degree of orientation and the phase difference of attosecond bursts using molecular frame ionization and recombination amplitudes. The sensitivity of the high harmonic spectrum to subtle phase differences in the emitted radiation makes it a detailed probe of polar molecules and will drive major advances in the theory of high harmonic generation.

High-harmonic transient grating spectroscopy of NO2 electronic relaxation.

We study theoretically and experimentally the electronic relaxation of NO(2) molecules excited by absorption of one ∼400 nm pump photon. Semiclassical simulations based on trajectory surface hopping calculations are performed. They predict fast oscillations of the electronic character around the intersection of the ground and first excited diabatic states. An experiment based on high-order harmonic transient grating spectroscopy reveals dynamics occurring on the same time scale. A systematic study of the detected transient is conducted to investigate the possible influence of the pump intensity, pump wavelength, and rotational temperature of the molecules. The quantitative agreement between measured and predicted dynamics shows that, in NO(2), high harmonic transient grating spectroscopy encodes vibrational dynamics underlying the electronic relaxation.

Ultrahigh-order wave mixing in noncollinear high harmonic generation.

We show that noncollinear high harmonic generation (HHG) can be fully understood in terms of nonlinear optical wave mixing. We demonstrate this by superposing on the fundamental ω1 field its second harmonic ω2 of variable intensity in a noncollinear geometry. It allows us to identify, by momentum conservation, each field's contribution (n1,n2) to the extreme ultraviolet emission at frequency Ω = n1ω1 + n2ω2. We observe that the photon (Ω) yield follows an n2 power law on the ω2 intensity, before saturation. It demonstrates that, although HHG is a highly nonperturbative process, a perturbation theory can still be developed around it.

Controlling the interference of multiple molecular orbitals in high-harmonic generation.

We demonstrate a new method to investigate the origin of spectral structures in high-harmonic generation. We report detailed measurements of high-harmonic spectra in aligned nitrogen and carbon dioxide molecules. Varying the wavelength and intensity of the generating laser field, we show that the minimum in aligned N2 molecules is nearly unaffected, whereas the minimum in aligned CO2 molecules shifts over more than 15 eV. Our quantitative analysis shows that both the interference of multiple orbitals and their structural characteristics affect the position of the minimum. Our method provides a simple approach to the investigation of the high-harmonic generation process in more complex molecules.

High-harmonic homodyne detection of the ultrafast dissociation of Br2 molecules.

We report the time-resolved observation of the photodissociation of Br2 using high-harmonic generation (HHG) as a probe. The simultaneous measurement of the high-harmonic and ion yields shows that high harmonics generated by the electronically excited state interfere with harmonics generated by the ground state. The resulting homodyne effect provides a high sensitivity to the excited state dynamics. We present a simple theoretical model that accounts for the main observations. Our experiment paves the way towards the dynamic imaging of molecules using HHG.

The stop null mice model for schizophrenia displays [corrected] cognitive and social deficits partly alleviated by neuroleptics.

Recently evidence has accumulated that schizophrenia can arise from primary synaptic defects involving structural proteins particularly, microtubule associated proteins. Previous experiments have demonstrated that a STOP (stable tubule only peptide) gene deletion in mice leads to a phenotype mimicking some aspects of positive symptoms classically observed in schizophrenic patients. In the current study, we determined if STOP null mice demonstrate behavioral abnormalities related to the social and cognitive impairments of schizophrenia. Compared with wild-type mice, STOP null mice exhibited deficits in the non-aggressive component of social recognition, short term working memory and social and spatial learning. As described in humans, learning deficits in STOP null mice were poorly sensitive to long term treatment with typical neuroleptics. Since social and cognitive dysfunction have consistently been considered as central features of schizophrenia, we propose that STOP null mice may provide a useful model to understand the neurobiological correlates of social and cognitive defects in schizophrenia and to develop treatments that better target these symptoms.

Soft x-ray excitonics.

The dynamic response of excitons in solids is central to modern condensed-phase physics, material sciences, and photonic technologies. However, study and control have hitherto been limited to photon energies lower than the fundamental band gap. Here we report application of attosecond soft x-ray and attosecond optical pulses to study the dynamics of core-excitons at the L2,3 edge of Si in silicon dioxide (SiO2). This attosecond x-ray absorption near-edge spectroscopy (AXANES) technique enables direct probing of the excitons' quasiparticle character, tracking of their subfemtosecond relaxation, the measurement of excitonic polarizability, and observation of dark core-excitonic states. Direct measurement and control of core-excitons in solids lay the foundation of x-ray excitonics.

[Nonalcoholic fatty liver disease in a severely obese adolescent. An arguable liver biopsy]. / Stéatohépatite non alcoolique chez une adolescente obèse: une biopsie hépatique discutable.

The growing epidemic of juvenile obesity has prompted pediatricians to investigate obesity-related conditions in obese teenagers. We report a clinical case of severe hepatic fibrosis in an adolescent with severe and recent obesity. Because of elevated serum aminotransferase levels, abnormal hepatic ultrasonography and insulin resistance (impaired glucose tolerance), we suspected nonalcoholic steatohepatitis (NASH). Disease activity and fibrosis were confirmed on liver biopsy. Considering the risk of progression toward cirrhosis and its complications, and the pathological liver lesions, we started long-term medical monitoring and drug therapy to control weight loss. At present, although biopsy is the only validated way to establish the diagnosis of NASH, there is no consensus on its indication when NASH is suspected. Noninvasive strategies are attractive but require validation in children.

[Initial descriptive analysis of 200 obese adolescents in an adolescent care unit]. / Qui sont les adolescents consultant pour demande de prise en charge d'une obésité dans une Maison des adolescents ? Phénotypes d'une cohorte de 200 patients.

Common obesity is a frequent reason for outpatient visits to adolescent clinics. Its high risk of persistence or progression into adulthood is well known. This article is a study of 200 clinical charts of obese adolescents that visited our clinic. The physical, metabolic, psychological, and social characteristics of these patients when they first started their follow-up are described. Body image disturbance and the everyday psychosocial impact of obesity were the most frequent reasons for the first visit. Two-thirds of the adolescent girls had already had unsuccessful follow-ups by other teams or doctors. The average age was 14.5 years and the average body mass index z-score was above 7.4. They suffered from musculoskeletal or respiratory disorders but had few metabolic complications at that stage. Various personal or family psychological and social characteristics were frequently observed as well as certain types of eating disorders. This data may be useful in establishing different profiles that could be used to adapt obese patient care for adolescents.

Conical intersection dynamics in NO2 probed by homodyne high-harmonic spectroscopy.

Conical intersections play a crucial role in the chemistry of most polyatomic molecules, ranging from the simplest bimolecular reactions to the photostability of DNA. The real-time study of the associated electronic dynamics poses a major challenge to the latest techniques of ultrafast measurement. We show that high-harmonic spectroscopy reveals oscillations in the electronic character that occur in nitrogen dioxide when a photoexcited wave packet crosses a conical intersection. At longer delays, we observe the onset of statistical dissociation dynamics. The present results demonstrate that high-harmonic spectroscopy could become a powerful tool to highlight electronic dynamics occurring along nonadiabatic chemical reaction pathways.