Cortical layer-specific critical dynamics triggering perception.

Perceptual experiences may arise from neuronal activity patterns in mammalian neocortex. We probed mouse neocortex during visual discrimination using a red-shifted channelrhodopsin (ChRmine, discovered through structure-guided genome mining) alongside multiplexed multiphoton-holography (MultiSLM), achieving control of individually specified neurons spanning large cortical volumes with millisecond precision. Stimulating a critical number of stimulus-orientation-selective neurons drove widespread recruitment of functionally related neurons, a process enhanced by (but not requiring) orientation-discrimination task learning. Optogenetic targeting of orientation-selective ensembles elicited correct behavioral discrimination. Cortical layer-specific dynamics were apparent, as emergent neuronal activity asymmetrically propagated from layer 2/3 to layer 5, and smaller layer 5 ensembles were as effective as larger layer 2/3 ensembles in eliciting orientation discrimination behavior. Population dynamics emerging after optogenetic stimulation both correctly predicted behavior and resembled natural internal representations of visual stimuli at cellular resolution over volumes of cortex.

Effect of pulse temporal shape on optical trapping and impulse transfer using ultrashort pulsed lasers.

We investigate the effects of pulse duration on optical trapping with high repetition rate ultrashort pulsed lasers, through Lorentz-Mie theory, numerical simulation, and experiment. Optical trapping experiments use a 12 femtosecond duration infrared pulsed laser, with the trapping microscope's temporal dispersive effects measured and corrected using the Multiphoton Intrapulse Interference Phase Scan method. We apply pulse shaping to reproducibly stretch pulse duration by 1.5 orders of magnitude and find no material-independent effects of pulse temporal profile on optical trapping of 780nm silica particles, in agreement with our theory and simulation. Using pulse shaping, we control two-photon fluorescence in trapped fluorescent particles, opening the door to other coherent control applications with trapped particles.

Control of molecular fragmentation using shaped femtosecond pulses.

The possibility that chemical reactions may be controlled by tailored femtosecond laser pulses has inspired recent studies that take advantage of their short pulse duration, comparable to intramolecular dynamics, and high peak intensity to fragment and ionize molecules. In this article, we present an experimental quest to control the chemical reactions that take place when isolated molecules interact with shaped near-infrared laser pulses with peak intensities ranging from 1013 to 1016 W/cm2. Through the exhaustive evaluation of hundreds of thousands of experiments, we methodically evaluated the molecular response of 16 compounds, including isomers, to the tailored light fields, as monitored by time-of-flight mass spectrometry. Analysis of the experimental data, taking into account its statistical significance, leads us to uncover important trends regarding the interaction of isolated molecules with an intense laser field. Despite the energetics involved in fragmentation and ionization, the integrated second-harmonic generation of a given laser pulse (ISHG), which was recorded as an independent diagnostic parameter, was found to be linearly proportional to the total ion yield (IMS) generated by that pulse in all of our pulse shaping measurements. Order of magnitude laser control over the relative yields of different fragment ions was observed for most of the molecules studied; the fragmentation yields were found to vary monotonically with IMS and/or ISHG. When the extensive changes in fragmentation yields as a function of IMS were compared for different phase functions, we found essentially identical results. This observation implies that fragmentation depends on a parameter that is responsible for IMS and independent from the particular time-frequency structure of the shaped laser pulse. With additional experiments, we found that individual ion yields depend only on the average pulse duration, implying that coherence does not play a role in the observed changes in yield as a function of pulse shaping. These findings were consistently observed for all molecules studied (p-, m-, o-nitrotoluene, 2,4-dinitrotoluene, benzene, toluene, naphthalene, azulene, acetone, acetyl chloride, acetophenone, p-chrolobenzonitrile, N,N-dimethylformamide, dimethyl phosphate, 2-chloroethyl ethyl sulfide, and tricarbonyl-[eta5-1-methyl-2,4-cyclopentadien-1-yl]-manganese). The exception to our conclusion is that the yield of small singly-charged fragments resulting from a multiple ionization process in a subset of molecules, were found to be highly sensitive to the phase structure of the intense pulses. This coherent process plays a minimal role in photofragmentation; therefore, we consider it an exception rather than a rule. Changes in the fragmentation process are dependent on molecular structure, as evidenced in a number of isomers, therefore femtosecond laser fragmentation could provide a practical dimension to analytical chemistry techniques.

Automated phase characterization and adaptive pulse compression using multiphoton intrapulse interference phase scan in air.

We introduce a non-interferometric single beam method for automated spectral phase characterization and adaptive pulse compression of amplified ultrashort femtosecond pulses taking advantage of third order harmonic generation in air. This new method, air-MIIPS, compensates high-order phase distortions based on multiphoton intrapulse interference phase scan (MIIPS).

Search space mapping: getting a picture of coherent laser control.

Search space mapping is a method for quickly visualizing the experimental parameters that can affect the outcome of a coherent control experiment. We demonstrate experimental search space mapping for the selective fragmentation and ionization of para-nitrotoluene and show how this method allows us to gather information about the dominant trends behind our achieved control.

Advantages of ultrashort phase-shaped pulses for selective two-photon activation and biomedical imaging.

Two-photon excitation using ultrashort laser pulses can selectively activate nanoparticles or excite fluorophores within thick biological samples. We show how the use of methods such as multiphoton intrapulse interference phase scan (MIIPS) to compensate phase distortions caused by microscope objectives with a high numerical aperture increases signal intensity and reproducibility in two-photon imaging. Using phase shaping of our compensated pulses, we demonstrate selective excitation of fluorophores within a mouse kidney sample, increasing the contrast between different subcellular structures compared to unshaped pulses.

Spectral phase optimization of femtosecond laser pulses for narrow-band, low-background nonlinear spectroscopy.

We use experimental search space mapping to examine the problem of selective nonlinear excitation with binary phase shaped femtosecond laser pulses. The search space maps represent a graphical view of all the possible solutions to the selective nonlinear excitation problem along with their experimental degrees of success. Using the information learned from these maps, we generate narrow lines with low background in second harmonic generation and stimulated Raman scattering spectra.