Birefringence phase-matched direct third-harmonic generation in a ridge optical waveguide based on a KTiOPO4 single crystal.

Birefringence phase-matched third-harmonic generation at 1594 nm is performed for the first time in a KTiOPO4 single crystal micrometric ridge waveguide. The energy conversion efficiency reaches 3.4% for a pump energy as low as 2 µJ over a pulse duration of 15 ps at a repetition rate of 10 Hz. Strong agreements between theory and experiments for both phase-matching and conversion efficiency is obtained, which let us envision future triple photon generation quantum experiments.

Phase-matched second-harmonic generation in a flux grown KTP crystal ridge optical waveguide.

Type II second-harmonic generation was performed in a 15.8-mm-long KTiOPO4 (KTP) micrometric ridge waveguide with an average transversal section of 38 µm2. Theoretical predictions are compared with experiments. Strong agreements are obtained for both phase-matching wavelengths and second-harmonic intensity. This work opens wide perspectives for integrated parametric optics.

Profiling an electrospray plume by laser-induced fluorescence and Fraunhofer diffraction combined to mass spectrometry: influence of size and composition of droplets on charge-state distributions of electrosprayed proteins.

We investigated how physico-chemical properties of charged droplets are affected by the electrospray process, using simultaneous in situ measurements by laser-induced fluorescence (LIF), Fraunhofer diffraction and mass spectrometry. For this purpose, we implemented a laser-induced-fluorescence profiling setup in conjunction with a fast, high-resolution particle sizing scheme on a modified Agilent Jet Stream electrospray source coupled to a single quadrupole mass analyser. The optical setup permits us to profile the solvent fractionation and the size of the droplets as they evaporate in an electrospray plume by measuring both the angular scattering pattern and emission spectra of a solvatochromic fluorescent dye. Mass spectra are recorded simultaneously. These mass spectrometry and optical spectroscopy investigations allow us to study the relation between the observed charge-state distributions of protein anions and physico-chemical properties of evaporating droplets in the spray plume. By mixing water with methanol, a refolding of cytochrome C is observed as the water percentage increases in the plume due to the preponderant evaporation of volatile methanol.

Resolution of strongly competitive product channels with optimal dynamic discrimination: application to flavins.

Fundamental molecular selectivity limits are probed by exploiting laser-controlled quantum interferences for the creation of distinct spectral signatures in two flavin molecules, erstwhile nearly indistinguishable via steady-state methods. Optimal dynamic discrimination (ODD) uses optimally shaped laser fields to transiently amplify minute molecular variations that would otherwise go unnoticed with linear absorption and fluorescence techniques. ODD is experimentally demonstrated by combining an optimally shaped UV pump pulse with a time-delayed, fluorescence-depleting IR pulse for discrimination amongst riboflavin and flavin mononucleotide in aqueous solution, which are structurally and spectroscopically very similar. Closed-loop, adaptive pulse shaping discovers a set of UV pulses that induce disparate responses from the two flavins and allows for concomitant flavin discrimination of ∼16σ. Additionally, attainment of ODD permits quantitative, analytical detection of the individual constituents in a flavin mixture. The successful implementation of ODD on quantum systems of such high complexity bodes well for the future development of the field and the use of ODD techniques in a variety of demanding practical applications.

Quantum control of tightly competitive product channels.

Fundamental selectivity limits of quantum control are pushed by introducing laser driven optimal dynamic discrimination to create distinguishing excitations on two nearly identical flavin molecules. Even with modest spectral resources, significant specificity is achieved with optimal pulse shapes, which amplify small molecular differences to create distinct, identifying signals. Rather than being a hindrance, system complexity appears to aid the control process and augments control field capability, which bodes well for implementation of quantum control in a variety of demanding applications.

Femtosecond pump-probe experiments on trapped flavin: optical control of dissociation.

Femtosecond pump-probe experiments are performed on flavin biomolecules isolated in an ion trap. Mass spectra of the photoinduced fragments show that the fragmentation pathways can be modified using two-color two-photon excitation. In particular, when an infrared probe pulse (810 nm) is added subsequent to the first excitation step (excitation of the S(1) state of flavin mononucleotide at 405 nm), branching ratios between lumichrome and lumiflavin production are inverted relative to the single excitation case.

Identification of biological microparticles using ultrafast depletion spectroscopy.

We show how an ultrafast pump-pump excitation induces strong fluorescence depletion in biological samples, such as bacteria-containing droplets, in contrast with fluorescent interferents, such as polycyclic aromatic compounds, despite similar spectroscopic properties. Application to the optical remote discrimination of biotic versus non-biotic particles is proposed. Further improvement is required to allow the discrimination of one pathogenic among other non-pathogenic micro-organisms. This improved selectivity may be reached with optimal coherent control experiments, as discussed in the paper.

Laser noise compression by filamentation at 400 nm in argon.

Filamentation is an efficient way to produce an intense and spectrally broad, but poorly stable, source for coherent control spectroscopy. We first described both theoretically and experimentally the filamentation and broadening of a 410 nm ultrashort laser pulse in Argon. By observing the theoretical and experimental spectral cross-correlation in the filament, we then show that the stability of the source can be improved. The Signal-to-Noise Ratio of the intensity inside the filament is increased up to 7 dB by its spectral filtering which provide a low noise broad spectrum source.

Measuring the electric charge in cloud droplets by use of second-harmonic generation.

We report on the observation of second-harmonic generation (SHG) from electrically charged microdroplets while they are excited with femtosecond laser pulses. The intense SHG emission results from chi(3) coupling between two photons of the incident laser pulse and the electrostatic field induced by the surface charges. For Iinc= 2 x 10(12) W/cm2, we estimate the second-harmonic emission to be ISHG= 2.5 x 10(3) photons per droplet and per pulse. The possibility of using SHG to measure remotely the electric charge of water droplets in thunderclouds is discussed.

Application of light-emitting diodes for aerosol fluorescence detection.

We demonstrate a proof-of-concept optical spectroscopic system for bioaerosol-particle fluorescence detection, in which a pulsed high-power laser is replaced by a highly compact linear array of sequentially fired light from blue light-emitting diodes. The results suggest that low-cost, compact optical aerosol detection may be feasible with the contemporary emergence of efficient UV light-emitting diodes.

Plasma formation dynamics within a water microdroplet on femtosecond time scales.

We demonstrate that a highly confined plasma inclusion is formed inside a micrometric water droplet that is excited by a femtosecond laser. An 800-nm laser pulse generates a plasma inclusion by laser-induced breakdown that is subsequently probed by the elastic scattering of a second (400-nm) time-delayed ultrashort pulse. For a 25-microm-radius droplet and an incident intensity of 7 x 10(12) W/cm2 the radius of the highly localized plasma is 1.9 +/- 0.4 microm. We probed the plasma formation dynamics on femtosecond time scales by varying the delay between the pump and the probe pulses. Good agreement with numerical simulations of the process was found.

Sonographic probing of laser filaments in air.

The acoustic wave emitted from the plasma channel associated with a filament induced by a femtosecond laser pulse in air was detected with a microphone. This sonographic detection provides a new method to determine the length and the spatial profile of the free-electron density of a filament. The acoustic wave is emitted owing to the expansion of the gas in the filament, which is heated through collisions with high-energy photoelectrons generated by multiphoton ionization. Compared with other methods, the acoustic detection is simpler, more sensitive, and with higher spatial resolution, making it suitable for field measurements over kilometer-range distances or laboratory-scale studies on the fine structure of a filament.

White-light nanosource with directional emission.

We report the first observation of white-light emission from femtosecond laser-induced plasma in a water droplet. Such emission is not observed with water in a cell. The microdroplet acts as a lens, focusing the incident light to nanosized regions within itself and directing the emission from these regions primarily back toward the laser source. This focusing increases the intensity so that multiphoton ionization generates plasma and causes it to reach the critical density during the initial part of the pulse, enabling the rest of the pulse to heat the plasma enough to emit in the visible.