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Whereas most of the reports on the nonlinear properties of micro- and nanostructures address the generation of distinct signals, such as second or third harmonic, we recently demonstrated that the novel generation of dual output lasers developed for microscopy can readily increase the accessible parameter space and enable the simultaneous excitation and detection of multiple emission orders such as several harmonics and signals stemming from various sum and difference frequency mixing processes. [1] This rich response, which in our case features 10 distinct emissions and encompasses the whole spectral range from the deep ultraviolet to the short-wave infrared region, is demonstrated using various nonlinear oxide nanomaterials while being characterized and simulated temporally and spectrally.

Vision in living mice is sensitive to femtosecond pulse shaping., Vision is usually assumed to be sensitive to the light intensity and spectrum but not to its spectral phase. However, experiments performed on retinal proteins in solution showed that the first step of vision consists in an ultrafast photoisomerization that can be coherently controlled by shaping the phase of femtosecond laser pulses, especially in the multiphoton interaction regime. The link between these experiments in solution and the biological process allowing vision was not demonstrated. Here, we measure the electric signals fired from the retina of living mice upon femtosecond multipulse and single-pulse light stimulation. Our results show that the electrophysiological signaling is sensitive to the manipulation of the light excitation on a femtosecond time scale. The mechanism relies on multiple interactions with the light pulses close to the conical intersection, like pump-dump (photoisomerization interruption) and pump-repump (reverse isomerization) processes. This interpretation is supported both experimentally and by dynamics simulations.

We demonstrate femtosecond time–resolved soft–X–ray absorption spectroscopy of liquid samples by combining a sub–micrometer–thin flat liquid jet with a high–harmonic table–top source covering the entire water-window range (284 - 538 eV). Our measurements temporally resolve the gradual appearance of absorption features below the carbon K-edge of ethanol and methanol during strong–field ionization, which trace the valence-shell ionization dynamics of the liquid alcohols with a temporal resolution of ~30 fs.

International audience; Whereas most of the reports on the nonlinear properties of micro- and nanostructures address the generation of distinct signals, such as second or third harmonic, here we demonstrate that the novel generation of dual output lasers recently developed for microscopy can readily increase the accessible parameter space and enable the simultaneous excitation and detection of multiple emission orders such as several harmonics and signals stemming from various sum and difference frequency mixing processes. This rich response, which in our case features 10 distinct emissions and encompasses the whole spectral range from the deep ultraviolet to the short-wave infrared region, is demonstrated using various nonlinear oxide nanomaterials while being characterized and simulated temporally and spectrally. Notably, we show that the response is conserved when the particles are embedded in biological media opening the way to novel biolabeling and phototriggering strategies.

High intensity laser filamentation in air has recently demonstrated that, through plasma generation and its associated shockwave, fog can be cleared around the beam, leaving an optically transparent path to transmit light. However, for practical applications like free-space optical communication (FSO), channels of multi-centimeter diameters over kilometer ranges are required, which is extremely challenging for a plasma based method. Here we report a radically different approach, based on quantum control. We demonstrate that fog clearing can also be achieved by producing molecular quantum wakes in air, and that neither plasma generation nor filamentation are required. The effect is clearly associated with the rephasing time of the rotational wave packet in N2.Pump excitation provided in the form of resonant trains of 8 pulses separated by the revival time are able to transmit optical data through fog with initial extinction as much as −6 dB.

Femtosecond X-ray absorption spectroscopy (XAS) is a powerful method to investigate the dynamical behavior of a system after photoabsorption in real time. So far, the application of this technique has remained limited to large-scale facilities, such as femtosliced synchrotrons and free-electron lasers (FEL). In this work, we demonstrate femtosecond time-resolved soft-X-ray absorption spectroscopy of liquid samples by combining a sub-micrometer-thin flat liquid jet with a high-harmonic tabletop source covering the entire water-window range (284–538 eV). Our work represents the first extension of tabletop XAS to the oxygen edge of a chemical sample in the liquid phase. In the time domain, our measurements resolve the gradual appearance of absorption features below the carbon K-edge of ethanol and methanol during strong-field ionization and trace the valence-shell ionization dynamics of the liquid alcohols with a temporal resolution of ∼30 fs. This technique opens unique opportunities to study molecular dynamics of chemical systems in the liquid phase with elemental, orbital, and site sensitivity. ISSN:1948-7185

International audience; Lightning is highly destructive due to its high power density and unpredictable character. Directing lightning away would allow to protect sensitive sites from its direct and indirect impacts (electromagnetic perturbations). Up to now, lasers have been unable to guide lightning efficiently since they were not offering simultaneously terawatt peak powers and kHz repetition rates. In the framework of the Laser Lightning Rod project, we develop a laser system for lightning control, with J-range pulses of 1ps duration at 1kHz. The project aims at investigating its propagation in the multiple filamentation regime and its ability to control high-voltage discharges. In particular, a field campaign at the S ̈antis mountain will assess the laser ability to trigger upward lightning.

We demonstrate femtosecond time–resolved soft–X–ray absorption spectroscopy of liquid samples by combining a sub–micrometer–thin flat liquid jet with a high–harmonic table–top source covering the entire water-window range (284 - 538 eV). Our work represents the first extension of table-top XAS to the oxygen edge of a chemical sample in the liquid phase. In the time domain, our measurements resolve the gradual appearance of absorption features below the carbon K-edge of ethanol and methanol during strong–field ionization, which trace the valence-shell ionization dynamics of the liquid alcohols with a temporal resolution of ~30 fs.

While chemotherapy is one of the most used treatments in oncology, the systemic administration of chemotherapeutics generally results in undesired damages to healthy tissues and cells, side effects such as severe nausea and leukopenia, and reduced efficacy due to multidrug resistance and poor target accessibility. The limitations of conventional chemotherapy formulation have prompted the development of alternative nanomaterials‐based strategies to achieve targeted and stimuli sensitive payload delivery to reach optimal local drug concentration at tumor sites. In this study, the anticancer drug chlorambucil (Clb) was conjugated to the surface of silica coated lithium niobate (LNO) harmonic nanoparticles (HNPs) using a photocaging tether based on coumarin‐4‐yl methyl derivative. Upon laser pulsed femtosecond irradiation at 790 nm, the second harmonic emission from the metal oxide core induced the efficient release of Clb, with concomitant contribution from the nonlinear absorption of the coumarin (CM)‐based moiety.

We present space and time resolved measurements of the air hydrodynamics induced by femtosecond laser pulse excitation of the air gap between two electrodes at high potential difference. We explore both plasma-based and plasma-free gap excitation. The former uses the plasma left in the wake of femtosecond filamentation, while the latter exploits air heating by multiple-pulse resonant excitation of quantum molecular wavepackets. We find that the cumulative electrode-driven air density depression channel plays the dominant role in the gap evolution leading to breakdown. Femtosecond laser heating serves mainly to initiate the depression channel; the presence of filament plasma only augments the early heating.

We introduce a nonlinear all-optical theranostics protocol based on the excitation wavelength decoupling between imaging and photoinduced damage of human cancer cells labeled by bismuth ferrite (BFO) harmonic nanoparticles (HNPs). To characterize the damage process, we rely on a scheme for in situ temperature monitoring based on upconversion nanoparticles: by spectrally resolving the emission of silica coated NaGdF4:Yb3+/Er3+ nanoparticles in close vicinity of a BFO HNP, we show that the photointeraction upon NIR-I excitation at high irradiance is associated with a temperature increase >100 °C. The observed laser–cell interaction implies a permanent change of the BFO nonlinear optical properties, which can be used as a proxy to read out the outcome of a theranostics procedure combining imaging at 980 nm and selective cell damage at 830 nm. The approach has potential applications to monitor and treat lesions within NIR light penetration depth in tissues.

We couple the full 3D ab initio quantum evolution of the light pulse polarization in interaction with an atom with a propagation model to simulate the propagation of ultrashort laser pulses over macroscopic dimensions, in the presence of self-generated harmonics up to order 11. We evidence a clear feedback of the generated harmonics on propagation, with an influence on the ionization probability as well as the yield of the harmonic generation itself., Comment: 9 pages, 4 figures

Science, 355 (6322), ISSN:0036-8075, ISSN:1095-9203

International audience; We study the use of frequency upconversion schemes of near-IR picosecond laser pulses and compare their ability to guide and trigger electric discharges through filamentation in air. Upconversion, such as Second Harmonic Generation, is favorable for triggering electric discharges for given amount of available laser energy, even taking into account the losses inherent to frequency conversion. We focus on the practical question of optimizing the use of energy from a given available laser system and the potential advantage to use frequency conversion schemes.

In this paper we examine the spectral changes in a white light laser filament due to different pulse shapes generated by a pulse shaping setup. We particularly explore how the properties of the filament spectra can be controlled by parametrically tailored white light pulses. The experiments are carried out in a gas cell with up to 9 bar of argon. Plasma generation and self-phase modulation strongly affect the pulse in the spectral and temporal domain. By exploiting these effects we show that the pulse spectrum can be modified in a desired way by either using second order parametric chirp functions to shift the filament spectrum to higher or lower wavelengths, or by optimizing pulse shapes with a genetic algorithm to generate more complex filament spectra. This paper is one of the first examples of the application of complex, parametrically shaped white light pulses., 14 pages, 7 figures

We propose the impingement of non-uniform wavefront curvature as a simple way to improve the longitudinal homogeneity of the plasma density along filaments generated by ultrashort laser pulses. We characterize multiple filamentation of a multiterawatt beam with different wavefront curvatures applied to specific regions in the transverse beam profile. In adequate conditions, the filamenting region is more homogeneously ionized, in the longitudinal direction, than in the case of uniform focusing. Moreover, the ionization maximum is located between the middle and the two thirds of the filaments in all investigated chirps and focus configurations.

We experimentally and numerically characterize multiple filamentation of laser pulses with incident intensities of a few TW/cm2. Propagating 100 TW laser pulses over 42 m in air, we observe a new propagation regime where the filament density saturates. As also evidenced by numerical simulations in the same intensity range, the total number of filaments is governed by geometric constraints and mutual interactions among filaments rather than by the available power in the beam.

We demonstrate the simultaneous generation of second, third, and fourth harmonic from a single dielectric Bismuth Ferrite nanoparticle excited by a telecom fiber laser at 1560 nm. We first characterize the signals associated with different nonlinear orders in terms of spectrum, excitation intensity dependence, and relative signal strengths. Successively, on the basis of the polarization-resolved emission curves of the three harmonics, we discuss the interplay of susceptibility tensor components at the different orders and we show how polarization can be used as an optical handle to control the relative frequency conversion properties., Comment: include S.I. section at the end of the main pdf file

Optics Express, 26 (9), ISSN:1094-4087

Interestingly, while adopted for a long time in the particle physics community as a usual gauge boson, the photon, i.e. the quantum particle associated with light, is still sometimes debated in the photonics community. Some weird questions are associated, like “is this photonic process quantum?”, “is it purely quantum?” or “is it non-trivially quantum?”. In the present chapter, we will not enter these discussions, but rather consider processes in which the state of a system is in a quantum superposition of different states (e.g. a Schroedinger cat) or in which distinct sub-systems are entangled (via non-locality).

We present high flux table-top 220eV HHG source (>109 photons/s/1% bandwidth) driven directly by a

Frequency-dependence and magnitude of second harmonic generation (SHG) from ~4 × 105 nm2 molybdenum disulfide (MoS2) monolayers was examined in presence of single 150 nm plasmonic gold@silica shell@core nanoantenna monomer and dimers. Quantitative agreement between discrete dipole approximation-calculated fields and measured SHG enhancements was found. SHG from MoS2 was enhanced up to 1.88 × upon deposition of a plasmonic nanoantenna-dimer with 170 nm gap, reaching maximal normalized SHG conversion efficiency of 0.0250%/W. Pump losses attributable to plasmonic damping, e.g., scattering and/or hot-electron injection into MoS2, were apparent. Linear and nonlinear optical activity of MoS2 and nanoantenna controls were compared with literature values.

We demonstrate the simultaneous generation of more than four harmonics from individual dielectric nanoparticles excited by a telecom fiber laser at 1560. We discuss the possibility to control their relative intensities by the laser polarization.

In femtosecond optical transfection and nanosurgery, cell survival critically depends on phototoxicity. It is therefore of primary importance to optimize the laser-cell interaction in order to increase the membrane poration efficiency while reducing collateral cell damage. Baumert group studied the impact of spectral phase modulation of femtosecond for machining on glass substrate. They demonstrated that the use of third order phase pulses (Airy pulses) could modulate the photon-interaction leading to holes of higher aspect ratio, compared to those produced by femtosecond bandwidth limited pulses. Following this approach, we showed that optimally shaped temporal Airy pulses display better performances also on fixed biological samples. In fact, Airy pulses can increase the cell membrane poration efficiency for a lower peak intensity and a similar energy per pulse than bandwith limited femtosecond pulses. We also discuss results from a live cell experiment. We set up a protocol where we investigate cells poration efficiency and cell viability as a function of pulse spectral phase. Hence, we present a protocol based on the use of three fluorophores to assess cells viability at different time points after poration.

Light can be used to modify and control properties of media, as in the case of electromagnetically induced transparency or, more recently, for the generation of slow light or bright coherent XUV and X-ray radiation. Particularly unusual states of matter can be created by light fields with strengths comparable to the Coulomb field that binds valence electrons in atoms, leading to nearly-free electrons oscillating in the laser field and yet still loosely bound to the core [1,2]. These are known as Kramers-Henneberger states [3], a specific example of laser-dressed states [2]. Here, we demonstrate that these states arise not only in isolated atoms [4,5], but also in rare gases, at and above atmospheric pressure, where they can act as a gain medium during laser filamentation. Using shaped laser pulses, gain in these states is achieved within just a few cycles of the guided field. The corresponding lasing emission is a signature of population inversion in these states and of their stability against ionization. Our work demonstrates that these unusual states of neutral atoms can be exploited to create a general ultrafast gain mechanism during laser filamentation., Comment: 9 pages, 4 figures, 10 pages supplementary material, 8 supplementary figures

Atmospheric clearness is a key issue for free space optical communications (FSO). We present the first active method to achieve FSO through clouds and fog, using ultrashort high intensity laser filaments. The laser filaments opto-mechanically expel the droplets out of the beam and create a cleared channel for transmitting high bit rate telecom data at 1.55 microns. The low energy required for the process allows considering applications to Earth-satellite FSO and secure ground based optical communication, with classical or quantum protocols., 4 pages + 2 pages supplementary text and movies

We present laser-induced condensation as a method for detecting of ultra-low concentrations of volatile organic compounds featuring a detection threshold well below 1 ppb. The method was tested in lab scale experiments and compared with quantitative photo-ionization detection measurements. The method was shown to be sensitive to the laser excitation wavelength between 1.6’2.0 um range.

Filamentation of ultra-short TW-class lasers recently opened new perspectives in atmospheric research. Laser filaments are self-sustained light structures of 0.1-1 mm in diameter, spanning over hundreds of meters in length, and producing a low density plasma (1015-1017 cm-3) along their path. They stem from the dynamic balance between Kerr self-focusing and defocusing by the self-generated plasma and/or non-linear polarization saturation. While non-linearly propagating in air, these filamentary structures produce a coherent supercontinuum (from 230 nm to 4 µm, for a 800 nm laser wavelength) by self-phase modulation (SPM), which can be used for remote 3D-monitoring of atmospheric components by Lidar (Light Detection and Ranging). However, due to their high intensity (1013-1014 W cm-2), they also modify the chemical composition of the air via photo-ionization and photo-dissociation of the molecules and aerosols present in the laser path. These unique properties were recently exploited for investigating the capability of modulating some key atmospheric processes, like lightning from thunderclouds, water vapor condensation, fog formation and dissipation, and light scattering (albedo) from high altitude clouds for radiative forcing management. Here we review recent spectacular advances in this context, achieved both in the laboratory and in the field, reveal their underlying mechanisms, and discuss the applicability of using these new non-linear photonic catalysts for real scale weather control.

Real-time monitoring of individual particles from atmospheric aerosols was performed by means of a specifically developed single-particle fluorescence spectrometer (SPFS). The observed fluorescence was assigned to particles bearing polycyclic aromatic hydrocarbons (PAH). This assignment was supported by an intercomparison with classical speciation on filters followed by gas chromatography-mass spectrometry (GC-MS) analysis. As compared with daily-averaged data, our time resolved approach provided information about the physicochemical dynamics of the particles. In particular, distinctions were made between background emissions related to heating, and traffic peaks during rush hours. Also, the evolution of the peak fluorescence wavelength provided an indication of the aging of the particles during the day., 8 pages, 6 figures

Light is used to modify or control properties in many quantum systems, leading to phenomena such as electromagnetically induced transparency, the generation of slow light or bright coherent XUV radiation. Using light fields, with strengths comparable to the Coulomb field which binds valence electrons in atoms, particularly unusual quantum states can be created which describe a nearly free electron oscillating in the laser field yet still loosely bound to the core1, 2. We demonstrate that such states can arise not only in isolated atoms3, but also in gases at a few atmospheric pressures, guiding intense laser pulses, where they can act as a gain medium. This gain is created within just a few cycles of the guided field. Using shaped pulses4 with 5–10 fs risetimes, we create pulse conditions, within a laser filament, where these states can persist, and we observe in the corresponding emission, the signatures of these states. This work demonstrates a general, new, ultrafast gain mechanism during filamentation, in which any driven atom can achieve inversion intra-pulse, using pulse shaping techniques.

Time-resolved spectroscopy at element-specific absorption edges provides a powerful tool to study ultrafast phenomena of matter on the atomic scale in the gas, solid or liquid phase. Combining element sensitivity of core-to-valence transitions due to the very localized initial core state and femtosecond/attosecond time resolution of new soft X-ray sources based on high-harmonic generation from long-wavelength drivers, accurate electronic and structural information is now accessible.

We demonstrate an approach for a real-time, consumable-free optical system operating on a liquid jet which can be easily derived from the water distribution infrastructure. We apply a pump-probe scheme based on the acquisition and nanosecond manipulation of UV-excited fluorescence to increase the selective identification of bacterial against organic pollutants in water.

Organometal halide perovskite-based solar cells have recently been reported to be highly efficient, giving an overall power conversion efficiency of up to 15%. However, much of the fundamental photophysical properties underlying this performance has remained unknown. Here, we apply photoluminescence, transient absorption, time-resolved terahertz and microwave conductivity measurements to determine the time scales of generation and recombination of charge carriers as well as their transport properties in solution-processed CH3NH3PbI3 perovskite materials. We found that electron-hole pairs are generated almost instantaneously after photoexcitation and dissociate in 2 ps forming highly mobile charges (25 cm(2) V(-1) s(-1)) in the neat perovskite and in perovskite/alumina blends; almost balanced electron and hole mobilities remain very high up to the microsecond time scale. When the perovskite is introduced into a TiO2 mesoporous structure, electron injection from perovskite to the metal oxide is efficient in less than a picosecond, but the lower intrinsic electron mobility of TiO2 leads to unbalanced charge transport. Microwave conductivity measurements showed that the decay of mobile charges is very slow in CH3NH3PbI3, lasting up to tens of microseconds. These results unravel the remarkable intrinsic properties of CH3NH3PbI3 perovskite material if used as light absorber and charge transport layer. Moreover, finding a metal oxide with higher electron mobility may further increase the performance of this class of solar cells.