We demonstrate that ultrashort and ultraintense light filaments survive their interaction with water droplets as large as 95 μm and that they are transmitted through water clouds having an optical thickness as high as 3.2 (transmission 5%). In contrast with linear optics, this remarkable transmission through optically dense media results from a dynamic energy balance between the quasisolitonic structure and the surrounding laser photon bath, which acts as an energy reservoir. Implications for free-space laser communications, remote sensing, and telemetry are discussed.

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.

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.

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.

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.

We demonstrate theoretically and experimentally that one-, two-, and three-photon excited fluorescence from dye molecules in spherical microcavities has an asymmetrical angular distribution and is enhanced in the backward direction. The enhancement ratios (of intensities at 180 degrees and 90 degrees ) are 9, 5, and 1.8 for three-, two-, and one-photon excitation, respectively. Even larger ratios are expected for microspheres with an index of refraction larger than that used in the experiments. Because of the reciprocity principle and concentration of the incident wave inside particles, the backward enhancement is expected to occur even with nonspherical particles.

We have applied a multiobjective genetic algorithm to the optimization of multiphoton-excited fluorescence. Our study shows the advantages that this approach can offer to experiments based on adaptive shaping of femtosecond pulses. The algorithm outperforms single-objective optimizations, being totally independent from the bias of user defined parameters and giving simultaneous access to a large set of feasible solutions. The global inspection of their ensemble represents a powerful support to unravel the connections between pulse spectral field features and excitation dynamics of the sample.

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.