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The light-induced ultrafast switching between molecular isomers norbornadiene and quadricyclane can reversibly store and release a substantial amount of chemical energy. Prior work observed signatures of ultrafast molecular dynamics in both isomers upon ultraviolet excitation but could not follow the electronic relaxation all the way back to the ground state experimentally. Here we study the electronic relaxation of quadricyclane after exciting in the ultraviolet (201 nanometres) using time-resolved gas-phase extreme ultraviolet photoelectron spectroscopy combined with non-adiabatic molecular dynamics simulations. We identify two competing pathways by which electronically excited quadricyclane molecules relax to the electronic ground state. The fast pathway (<100 femtoseconds) is distinguished by effective coupling to valence electronic states, while the slow pathway involves initial motions across Rydberg states and takes several hundred femtoseconds. Both pathways facilitate interconversion between the two isomers, albeit on different timescales, and we predict that the branching ratio of norbornadiene/quadricyclane products immediately after returning to the electronic ground state is approximately 3:2.

In this study, we present a complete set of electron scattering cross-sections from 1-Methyl-5-Nitroimidazole (1M5NI) molecules for impact energies ranging from 0.1 to 1000 eV. This information is relevant to evaluate the potential role of 1M5NI as a molecular radiosensitizers. The total electron scattering cross-sections (TCS) that we previously measured with a magnetically confined electron transmission apparatus were considered as the reference values for the present analysis. Elastic scattering cross-sections were calculated by means of two different schemes: The Schwinger multichannel (SMC) method for the lower energies (below 15 eV) and the independent atom model-based screening-corrected additivity rule with interferences (IAM-SCARI) for higher energies (above 15 eV). The latter was also applied to calculate the total ionization cross-sections, which were complemented with experimental values of the induced cationic fragmentation by electron impact. Double differential ionization cross-sections were measured with a reaction microscope multi-particle coincidence spectrometer. Using a momentum imaging spectrometer, direct measurements of the anion fragment yields and kinetic energies by the dissociative electron attachment are also presented. Cross-sections for the other inelastic channels were derived with a self-consistent procedure by sampling their values at a given energy to ensure that the sum of the cross-sections of all the scattering processes available at that energy coincides with the corresponding TCS. This cross-section data set is ready to be used for modelling electron-induced radiation damage at the molecular level to biologically relevant media containing 1M5NI as a potential radiosensitizer. Nonetheless, a proper evaluation of its radiosensitizing effects would require further radiobiological experiments.

We describe an apparatus for investigating the excited-state dissociation dynamics of mass-selected ion-molecule clusters by mass-resolving and detecting photofragment-ions and neutrals, in coincidence, using an ultrafast laser operating at high repetition rates. The apparatus comprises a source that generates ion-molecule clusters, a time-of-flight spectrometer, and a mass filter that selects the desired anions, and a linear-plus-quadratic reflectron mass spectrometer that discriminates the fragment anions after the femtosecond laser excites the clusters. The fragment neutrals and anions are then captured by two channeltron detectors. The apparatus performance is tested by measuring the photofragments: I-, CF3I-, and neutrals from photoexcitation of the ion-molecule cluster CF3I·I- using femtosecond UV laser pulses with a wavelength of 266 nm. The experimental results are compared with our ground state and excited state electronic structure calculations as well as the existing results and calculations, with particular attention to the generation mechanism of the anion fragments and dissociation channels of the ion-molecule cluster CF3I·I- in the charge-transfer excited state.

In this study, we present a complete set of electron scattering cross-sections from 1-Methyl-5- Nitroimidazole (1M5NI) molecules for impact energies ranging from 0.1 to 1000 eV. This information is relevant to evaluate the potential role of 1M5NI as a molecular radiosensitizers. The total electron scattering cross-sections (TCS) that we previously measured with a magnetically confined electron transmission apparatus were considered as the reference values for the present analysis. Elastic scattering cross-sections were calculated by means of two different schemes: The Schwinger multichannel (SMC) method for the lower energies (below 15 eV) and the independent atom model-based screening-corrected additivity rule with interferences (IAM-SCARI) for higher energies (above 15 eV). The latter was also applied to calculate the total ionization cross-sections, which were complemented with experimental values of the induced cationic fragmentation by electron impact. Double differential ionization cross-sections were measured with a reaction microscope multi-particle coincidence spectrometer. Using a momentum imaging spectrometer, direct measurements of the anion fragment yields and kinetic energies by the dissociative electron attachment are also presented. Cross-sections for the other inelastic channels were derived with a self-consistent procedure by sampling their values at a given energy to ensure that the sum of the cross-sections of all the scattering processes available at that energy coincides with the corresponding TCS. This cross-section data set is ready to be used for modelling electron-induced radiation damage at the molecular level to biologically relevant media containing 1M5NI as a potential radiosensitizer. Nonetheless, a proper evaluation of its radiosensitizing effects would require further radiobiological experiments.

We describe an apparatus for investigating the excited-state dissociation dynamics of mass-selected ion–molecule clusters by mass-resolving and detecting photofragment-ions and neutrals, in coincidence, using an ultrafast laser operating at high repetition rates. The apparatus comprises a source that generates ion–molecule clusters, a time-of-flight spectrometer, and a mass filter that selects the desired anions, and a linear-plus-quadratic reflectron mass spectrometer that discriminates the fragment anions after the femtosecond laser excites the clusters. The fragment neutrals and anions are then captured by two channeltron detectors. The apparatus performance is tested by measuring the photofragments: I−, CF3I−, and neutrals from photoexcitation of the ion–molecule cluster CF3I⋅I− using femtosecond UV laser pulses with a wavelength of 266 nm. The experimental results are compared with our ground state and excited state electronic structure calculations as well as the existing results and calculations, with particular attention to the generation mechanism of the anion fragments and dissociation channels of the ion–molecule cluster CF3I⋅I− in the charge-transfer excited state.

We report the modification of a gas phase ultrafast electron diffraction (UED) instrument that enables experiments with both gas and condensed matter targets, where a time-resolved experiment with sub-picosecond resolution is demonstrated with solid state samples. The instrument relies on a hybrid DC-RF acceleration structure to deliver femtosecond electron pulses on the target, which is synchronized with femtosecond laser pulses. The laser pulses and electron pulses are used to excite the sample and to probe the structural dynamics, respectively. The new system is added with capabilities to perform transmission UED on thin solid samples. It allows for cooling samples to cryogenic temperatures and to carry out time-resolved measurements. We tested the cooling capability by recording diffraction patterns of temperature dependent charge density waves in 1T-TaS2. The time-resolved capability is experimentally verified by capturing the dynamics in photoexcited single-crystal gold.

In this study, we present a complete set of electron scattering cross-sections from 1-Methyl-5-Nitroimidazole (1M5NI) molecules for impact energies ranging from 0.1 to 1000 eV. This information is relevant to evaluate the potential role of 1M5NI as a molecular radiosensitizers. The total electron scattering cross-sections (TCS) that we previously measured with a magnetically confined electron transmission apparatus were considered as the reference values for the present analysis. Elastic scattering cross-sections were calculated by means of two different schemes: The Schwinger multichannel (SMC) method for the lower energies (below 15 eV) and the independent atom model-based screening-corrected additivity rule with interferences (IAM-SCARI) for higher energies (above 15 eV). The latter was also applied to calculate the total ionization cross-sections, which were complemented with experimental values of the induced cationic fragmentation by electron impact. Double differential ionization cross-sections were measured with a reaction microscope multi-particle coincidence spectrometer. Using a momentum imaging spectrometer, direct measurements of the anion fragment yields and kinetic energies by the dissociative electron attachment are also presented. Cross-sections for the other inelastic channels were derived with a self-consistent procedure by sampling their values at a given energy to ensure that the sum of the cross-sections of all the scattering processes available at that energy coincides with the corresponding TCS. This cross-section data set is ready to be used for modelling electron-induced radiation damage at the molecular level to biologically relevant media containing 1M5NI as a potential radiosensitizer. Nonetheless, a proper evaluation of its radiosensitizing effects would require further radiobiological experiments.

The ability to resolve the dynamics of matter on its native temporal and spatial scales constitutes a key challenge and convergent theme across chemistry, biology, and materials science. The last couple of decades have witnessed ultrafast electron diffraction (UED) emerge as one of the forefront techniques with the sensitivity to resolve atomic motions. Increasingly sophisticated UED instruments are being developed that are aimed at increasing the beam brightness in order to observe structural signatures, but so far they have been limited to low average current beams. Here, we present the technical design and capabilities of the HiRES (High Repetition-rate Electron Scattering) instrument, which blends relativistic electrons and high repetition rates to achieve orders of magnitude improvement in average beam current compared to the existing state-of-the-art instruments. The setup utilizes a novel electron source to deliver femtosecond duration electron pulses at up to MHz repetition rates for UED experiments. Instrument response function of sub-500 fs is demonstrated with < 100 fs time resolution targeted in future. We provide example cases of diffraction measurements on solid-state and gas-phase samples, including both micro- and nanodiffraction (featuring 100 nm beam size) modes, which showcase the potential of the instrument for novel UED experiments.

Directly imaging structural dynamics involving hydrogen atoms by ultrafast diffraction methods is complicated by their low scattering cross sections. Here we demonstrate that megaelectronvolt ultrafast electron diffraction is sufficiently sensitive to follow hydrogen dynamics in isolated molecules. In a study of the photodissociation of gas phase ammonia, we simultaneously observe signatures of the nuclear and corresponding electronic structure changes resulting from the dissociation dynamics in the time-dependent diffraction. Both assignments are confirmed by ab initio simulations of the photochemical dynamics and the resulting diffraction observable. While the temporal resolution of the experiment is insufficient to resolve the dissociation in time, our results represent an important step towards the observation of proton dynamics in real space and time.

Ultrafast electron diffraction (UED) from aligned molecules in the gas phase has successfully retrieved structures of both linear and symmetric top molecules. Alignment of asymmetric tops has been recorded with UED but no structural information was retrieved. We present here the extraction of two-dimensional structural information from simple transformations of experimental diffraction patterns of aligned molecules as a proof-of-principle for the recovery of the full structure. We align 4-fluorobenzotrifluoride with a linearly polarized laser and show that we can distinguish between atomic pairs with equal distances that are parallel and perpendicular to the aligned axis. We additionally show with numerical simulations that by cooling the molecules to a rotational temperature of 1 K, more distances and angles can be resolved through direct transformations.

Since the discovery of electron-wave duality, electron scattering instrumentation has developed into a powerful array of techniques for revealing the atomic structure of matter. Beyond detecting local lattice variations in equilibrium structures with the highest possible spatial resolution, recent research efforts have been directed toward the long-sought-after dream of visualizing the dynamic evolution of matter in real time. The atomic behavior at ultrafast timescales carries critical information on phase transition and chemical reaction dynamics, the coupling of electronic and nuclear degrees of freedom in materials and molecules, and the correlation among structure, function, and previously hidden metastable or nonequilibrium states of matter. Ultrafast electron pulses play an essential role in this scientific endeavor, and their generation has been facilitated by rapid technical advances in both ultrafast laser and particle accelerator technologies. This review presents a summary of the noteworthy developments in this field in the last few decades. The physics and technology of ultrafast electron beams is presented with an emphasis on the figures of merit most relevant for ultrafast electron diffraction experiments. Recent developments in the generation, manipulation, and characterization of ultrashort electron beams aimed at improving the combined spatiotemporal resolution of these measurements are discussed. The fundamentals of electron scattering from atomic matter and the theoretical frameworks for retrieving dynamic structural information from solid-state and gas-phase samples is described. Essential experimental techniques and several landmark works that have applied these approaches are also highlighted to demonstrate the widening applicability of these methods. Ultrafast electron probes with ever-improving capabilities, combined with other complementary photon-based or spectroscopic approaches, hold tremendous potential for revolutionizing our ability t

Imaging laser-induced rotational dynamics is an important and active field due to its applications in capturing reactions in the molecular frame and in molecular imaging. Experimental measurement of the molecular orientation distribution, as a function of the Euler angles, has been demonstrated for special cases when the detectable signal is generated along the molecular symmetry axis. Here we developed the general theory that maps the probability density distribution of the molecular orientation to the atom-pair angular distributions for nonlinear molecules. With the theory, the molecular orientation distribution can be retrieved from the measured atom-pair angular distribution, which we demonstrate experimentally using ultrafast electron diffractive imaging of impulsively aligned trifluoro-iodomethane molecules. The retrieved molecular orientation distribution is in good agreement with direct numerical simulations of the time-dependent Schrödinger equation using the experimental conditions. Unlike the existing retrieval methods, the retrieval method does not require solving the Schrödinger equation, works for any alignment method, and is in principle applicable to asymmetric top molecules.

Water is one of the most important, yet least understood, liquids in nature. Many anomalous properties of liquid water originate from its well-connected hydrogen bond network1, including unusually efficient vibrational energy redistribution and relaxation2. An accurate description of the ultrafast vibrational motion of water molecules is essential for understanding the nature of hydrogen bonds and many solution-phase chemical reactions. Most existing knowledge of vibrational relaxation in water is built upon ultrafast spectroscopy experiments2-7. However, these experiments cannot directly resolve the motion of the atomic positions and require difficult translation of spectral dynamics into hydrogen bond dynamics. Here, we measure the ultrafast structural response to the excitation of the OH stretching vibration in liquid water with femtosecond temporal and atomic spatial resolution using liquid ultrafast electron scattering. We observed a transient hydrogen bond contraction of roughly 0.04 Å on a timescale of 80 femtoseconds, followed by a thermalization on a timescale of approximately 1 picosecond. Molecular dynamics simulations reveal the need to treat the distribution of the shared proton in the hydrogen bond quantum mechanically to capture the structural dynamics on femtosecond timescales. Our experiment and simulations unveil the intermolecular character of the water vibration preceding the relaxation of the OH stretch.

Water is one of the most important, yet least understood, liquids in nature. Many anomalous properties of liquid water originate from its well-connected hydrogen bond network, including unusually efficient vibrational energy redistribution and relaxation2. An accurate description of the ultrafast vibrational motion of water molecules is essential for understanding the nature of hydrogen bonds and many solution-phase chemical reactions. Most existing knowledge of vibrational relaxation in water is built upon ultrafast spectroscopy experiments. However, these experiments cannot directly resolve the motion of the atomic positions and require difficult translation of spectral dynamics into hydrogen bond dynamics. Here, we measure the ultrafast structural response to the excitation of the OH stretching vibration in liquid water with femtosecond temporal and atomic spatial resolution using liquid ultrafast electron scattering. We observed a transient hydrogen bond contraction of roughly 0.04 Å on a timescale of 80 femtoseconds, followed by a thermalization on a timescale of approximately 1 picosecond. Molecular dynamics simulations reveal the need to treat the distribution of the shared proton in the hydrogen bond quantum mechanically to capture the structural dynamics on femtosecond timescales. Our experiment and simulations unveil the intermolecular character of the water vibration preceding the relaxation of the OH stretch.

Water is one of the most important, yet least understood, liquids in nature. Many anomalous properties of liquid water originate from its well-connected hydrogen bond network1, including unusually efficient vibrational energy redistribution and relaxation2. An accurate description of the ultrafast vibrational motion of water molecules is essential for understanding the nature of hydrogen bonds and many solution-phase chemical reactions. Most existing knowledge of vibrational relaxation in water is built upon ultrafast spectroscopy experiments2-7. However, these experiments cannot directly resolve the motion of the atomic positions and require difficult translation of spectral dynamics into hydrogen bond dynamics. Here, we measure the ultrafast structural response to the excitation of the OH stretching vibration in liquid water with femtosecond temporal and atomic spatial resolution using liquid ultrafast electron scattering. We observed a transient hydrogen bond contraction of roughly 0.04 Å on a timescale of 80 femtoseconds, followed by a thermalization on a timescale of approximately 1 picosecond. Molecular dynamics simulations reveal the need to treat the distribution of the shared proton in the hydrogen bond quantum mechanically to capture the structural dynamics on femtosecond timescales. Our experiment and simulations unveil the intermolecular character of the water vibration preceding the relaxation of the OH stretch.

The development of ultrafast gas electron diffraction with nonrelativistic electrons has enabled the determination of molecular structures with atomic spatial resolution. It has, however, been challenging to break the picosecond temporal resolution barrier and achieve the goal that has long been envisioned—making space- and-time resolved molecular movies of chemical reaction in the gas-phase. Recently, an ultrafast electron diffraction (UED) apparatus using mega-electron-volt (MeV) electrons was developed at the SLAC National Accelerator Laboratory for imaging ultrafast structural dynamics of molecules in the gas phase. The SLAC gas-phase MeV UED has achieved 65 fs root mean square temporal resolution, 0.63A˚ spatial resolution, and 0.22A˚-1 reciprocal-space resolution. Such high spatial-temporal resolution has enabled the capturing of real-time molecular movies of fundamental photochemical mechanisms, such as chemical bond breaking, ring opening, and a nuclear wave packet crossing a conical intersection. In this paper, the design that enables the high spatial-temporal resolution of the SLAC gas phase MeV UED is presented. The compact design of the differential pump section of the SLAC gas phase MeV UED realized five orders-of-magnitude vacuum isolation between the electron source and gas sample chamber. The spatial resolution, temporal resolution, and long-term stability of the apparatus are systematically characterized.

We resolve the structural dynamics of the ultrafast photoinduced ring opening reaction of 1,3-cyclohexadiene in space and time employing megaelectronvolt gas phase ultrafast electron diffraction. We, furthermore, observe coherent large amplitude motions of the photoproduct.

QC 20170301

The process of second harmonic generation (SHG) has a unique property of forming a sharp optical contrast between noncentrosymmetric crystalline materials and other types of material, which is a highly valuable asset for contrast microscopy. The coherent signal obtained through SHG also allows for the recording of holograms at high spatial and temporal resolution, enabling whole-field four-dimensional microscopy for highly dynamic microsystems and nanosystems. Here we describe a new holographic principle, harmonic holography (H2), which records holograms between independently generated second harmonic signals and reference. We experimentally demonstrate this technique with digital holographic recording of second harmonic signals upconverted from an ensemble of second harmonic generating nanocrystal clusters under femtosecond laser excitation. Our results show that harmonic holography is uniquely suited for ultrafast four-dimensional contrast microscopy.

The process of second harmonic generation (SHG) has a unique property of forming a sharp optical contrast between noncentrosymmetric crystalline materials and other types of material, which is a highly valuable asset for contrast microscopy. The coherent signal obtained through SHG also allows for the recording of holograms at high spatial and temporal resolution, enabling whole-field four-dimensional microscopy for highly dynamic microsystems and nanosystems. Here we describe a new holographic principle, harmonic holography (H2), which records holograms between independently generated second harmonic signals and reference. We experimentally demonstrate this technique with digital holographic recording of second harmonic signals upconverted from an ensemble of second harmonic generating nanocrystal clusters under femtosecond laser excitation. Our results show that harmonic holography is uniquely suited for ultrafast four-dimensional contrast microscopy.

We investigate analytically, numerically, and experimentally the modulational instability in a layered, cubically nonlinear (Kerr) optical medium that consists of alternating layers of glass and air. We model this setting using a nonlinear Schrödinger (NLS) equation with a piecewise constant nonlinearity coefficient and conduct a theoretical analysis of its linear stability, obtaining a Kronig-Penney equation whose forbidden bands correspond to the modulationally unstable regimes. We find very good quantitative agreement between the theoretical analysis of the Kronig-Penney equation, numerical simulations of the NLS equation, and the experimental results for the modulational instability. Because of the periodicity in the evolution variable arising from the layered medium, we find multiple instability regions rather than just the one that would occur in uniform media.

We investigate analytically, numerically, and experimentally the modulational instability in a layered, cubically nonlinear (Kerr) optical medium that consists of alternating layers of glass and air. We model this setting using a nonlinear Schrödinger (NLS) equation with a piecewise constant nonlinearity coefficient and conduct a theoretical analysis of its linear stability, obtaining a Kronig-Penney equation whose forbidden bands correspond to the modulationally unstable regimes. We find very good quantitative agreement between the theoretical analysis of the Kronig-Penney equation, numerical simulations of the NLS equation, and the experimental results for the modulational instability. Because of the periodicity in the evolution variable arising from the layered medium, we find multiple instability regions rather than just the one that would occur in uniform media.

We conduct an experimental investigation of nonlinearity management in optics using femtosecond pulses and layered Kerr media consisting of glass and air. By examining the propagation properties over several diffraction lengths, we show that wave collapse can be prevented. We corroborate these experimental results with numerical simulations of the (2+1)-dimensional focusing cubic nonlinear Schrödinger equation with piecewise constant coefficients and a theoretical analysis of this setting using a moment method.

We present the first experimental investigation of modulational instability in a layered Kerr medium. The particularly interesting and appealing feature of our configuration, consisting of alternating glass-air layers, is the piecewise-constant nature of the material properties, which allows a theoretical linear stability analysis leading to a Kronig-Penney equation whose forbidden bands correspond to the modulationally unstable regimes. We find very good quantitative agreement between theoretical, numerical, and experimental diagnostics of the modulational instability. Because of the periodicity in the evolution variable arising from the layered medium, there are multiple instability regions rather than just one as in a uniform medium.

We have implemented a holographic system to study the propagation of femtosecond laser pulses with high temporal (150 fs) and spatial resolutions (4 µm). The phase information in the holograms allows us to reconstruct both positive and negative index changes due to the Kerr nonlinearity (positive) and plasma formation (negative), and to reconstruct three-dimensional structure. Dramatic differences were observed in the interaction of focused femtosecond pulses with air, water, and carbon disulfide. The air becomes ionized in the focal region, while in water long plasma filaments appear before the light reaches a tight focus. In contrast, in carbon disulfide the optical beam breaks up into multiple filaments but no plasma is measured. We explain these different propagation regimes in terms of the different nonlinear material properties.

We present the first experimental investigation of modulational instability in a layered Kerr medium. The particularly interesting and appealing feature of our configuration, consisting of alternating glass-air layers, is the piecewise-constant nature of the material properties, which allows a theoretical linear stability analysis leading to a Kronig-Penney equation whose forbidden bands correspond to the modulationally unstable regimes. We find very good quantitative agreement between theoretical, numerical, and experimental diagnostics of the modulational instability. Because of the periodicity in the evolution variable arising from the layered medium, there are multiple instability regions rather than just one as in a uniform medium.

We have implemented a holographic system to study the propagation of femtosecond laser pulses with high temporal (150 fs) and spatial resolutions (4 µm). The phase information in the holograms allows us to reconstruct both positive and negative index changes due to the Kerr nonlinearity (positive) and plasma formation (negative), and to reconstruct three-dimensional structure. Dramatic differences were observed in the interaction of focused femtosecond pulses with air, water, and carbon disulfide. The air becomes ionized in the focal region, while in water long plasma filaments appear before the light reaches a tight focus. In contrast, in carbon disulfide the optical beam breaks up into multiple filaments but no plasma is measured. We explain these different propagation regimes in terms of the different nonlinear material properties.

We conduct an experimental investigation of nonlinearity management in optics using femtosecond pulses and layered Kerr media consisting of glass and air. By examining the propagation properties over several diffraction lengths, we show that wave collapse can be prevented. We corroborate these experimental results with numerical simulations of the (2+1)-dimensional focusing cubic nonlinear Schrödinger equation with piecewise constant coefficients and a theoretical analysis of this setting using a moment method.

We have studied the large-scale beam breakup and filamentation of femtosecond pulses in a Kerr medium. We have experimentally monitored the formation of stable light filaments, conical emission, and interactions between filaments. Three major stages lead to the formation of stable light filaments: First the beam breaks up into a pattern of connected lines (constellation), then filaments form on the constellations, and finally the filaments release a fraction of their energy through conical emission. We observed a phase transition to a faster filamentation rate at the onset of conical emission. We attribute this to the interaction of conical emissions with the constellation which creates additional filaments. Numerical simulations show good agreement with the experimental results.

We present experimental results on the transverse modulation instability of an elliptical beam propagating in a bulk nonlinear Kerr medium, and the formation and self-organization of spatial solitons. We have observed the emergence of order, self organization and a transition to an unstable state. Order emerges through the formation of spatial solitons in a periodic array. If the initial period of the array is unstable the solitons will tend to self-organize into a larger (more stable) period. Finally the system transitions to a disordered state where most of the solitons disappear and the beam profile becomes unstable to small changes in the input energy.

This paper studies the propagation of femtosecond pulses in a Kerr medium both experimentally and numerically. This work also investigates the similarities between the propagation of light pulses in a Kerr medium and the evolution of fluid dynamical systems, and proposes the use of an optical system to simulate fluid dynamics.

The paper reports on the generation of spatial solitons with carbon disulfide (CS_2) as the nonlinear material, which has a critical power of 190 kW for the laser wavelength of 800 nm. A 150-femtosecond pulse with a maximum energy of 1 mJ is also used. Each pulse from the laser is split into pump and probe pulses. The pump pulse is focused into a line (using a cylindrical lens) at the entrance face of a 10 mm glass cell filled with CS_2.

We present experimental results on the transverse modulation instability of an elliptical beam propagating in a bulk nonlinear Kerr medium, and the formation and self-organization of spatial solitons. We have observed the emergence of order, self organization and a transition to an unstable state. Order emerges through the formation of spatial solitons in a periodic array. If the initial period of the array is unstable the solitons will tend to self-organize into a larger (more stable) period. Finally the system transitions to a disordered state where most of the solitons disappear and the beam profile becomes unstable to small changes in the input energy.

We have studied the large-scale beam breakup and filamentation of femtosecond pulses in a Kerr medium. We have experimentally monitored the formation of stable light filaments, conical emission, and interactions between filaments. Three major stages lead to the formation of stable light filaments: First the beam breaks up into a pattern of connected lines (constellation), then filaments form on the constellations, and finally the filaments release a fraction of their energy through conical emission. We observed a phase transition to a faster filamentation rate at the onset of conical emission. We attribute this to the interaction of conical emissions with the constellation which creates additional filaments. Numerical simulations show good agreement with the experimental results.

We have observed the filamentation of optical pulses in carbon disulfide(CS2) using femtosecond time-resolved optical polarigraphy(FTOP). A pump-probe setup is used to capture the propagation of a 150 femtosecond laser pulse in CS2. The probe pulse propagates in a direction perpendicular to the pump. The high intensity of the pump pulse causes a transient index change in the material through the Kerr effect. The induced birefringence is proportional to the intensity of the pump and can be captured by monitoring the polarization of the probe. The probe pulse is imaged on a CCD camera to recover the intensity profile of the pump pulse. We have used this technique to observe the spatial evolution of the pulse as a function of power and propagation distance. Initially, the pulse propagation causes a coarse redistribution of the intensity. The beam then breaks up into stable light filaments which propagate for several millimeters, and finally the beam profile becomes unstable to small fluctuations in the input power.

We present a holographic recording technique with 150 femtosecond time resolution. This technique allows us to capture either a single hologram with fine spatial resolution (4 micrometers), or a time-sequence of multiple holograms with reduced spatial resolution in a single-shot experiment, while preserving amplitude and phase information. The time resolution and the frame rate are limited only by the duration of the laser pulses. The holograms are recorded on a CCD camera and digitally reconstructed. We have used the technique to study the nonlinear propagation of high energy femtosecond pulses through liquids. We have observed dramatic differences in the pulse propagation characteristics depending on the strength of the nonlinear coefficient of the material and it's time response. The fine spatial resolution allows us to zoom in and visualize the spatial profile of the pulses breaking up into multiple filaments while the phase recovered from the holograms helps us identify the nonlinear index changes in the material. We have measured both positive and negative index changes. Very fast positive index changes are generally attributable to the Kerr nonlinearity. The negative index changes can be caused by electron plasma generated by multiphoton absorption.

We report on a holographic probing technique that allows for measurement of free-electron distribution with fine spatial detail. Plasma is generated by focusing a femtosecond pulse in air. We also demonstrate the capability of the holographic technique of capturing the time evolution of the plasma-generation process.

We report on a holographic probing technique that allows for measurement of free-electron distribution with fine spatial detail. Plasma is generated by focusing a femtosecond pulse in air. We also demonstrate the capability of the holographic technique of capturing the time evolution of the plasma-generation process.

We report on holographic recording of nanosecond events on a conventional CCD camera. Three frames of an air-discharge event, with resolution of 5.9 ns and frame interval of 12 ns, are recorded in a single CCD frame. Each individual frame is reconstructed by digital filtering of the CCD frame, since successively recorded holograms are centered at different carrier frequencies in the spatial frequency domain.

We report on holographic recording of nanosecond events on a conventional CCD camera. Three frames of an air-discharge event, with resolution of 5.9 ns and frame interval of 12 ns, are recorded in a single CCD frame. Each individual frame is reconstructed by digital filtering of the CCD frame, since successively recorded holograms are centered at different carrier frequencies in the spatial frequency domain.

In this paper we report on a holographic method used to record fast events in the nanosecond time scale. Several frames of the expansion of shock waves in air and in a polymer sample are recorded holographically in a single shot experiment, using a pulse train generated with a single pulse from a Q-switched Nd:YAG laser. The time resolution is limited by the laser pulse width, which is 5.9 ns. The different frames are recorded on the holographic material using angle multiplexing. Two cavities are used to generate the signal and reference pulses at different angles. We also present a method in which the recording material is replaced by a CCD camera. In this method the holograms are recorded directly on the CCD and digitally reconstructed. The holograms are recorded on a single frame of the CCD camera and then digitally separated and reconstructed.