189 research outputs found
Enhancement of Intermediate-Field Two-Photon Absorption by Rationally-Shaped Femtosecond Pulses
We extend the powerful frequency-domain analysis of femtosecond two-photon
absorption to the intermediate-field regime, which involves both two- and
four-photon transitions. Consequently, we find a broad family of shaped pulses
that enhance the absorption over the transform-limited pulse. It includes any
spectral phase that is anti-symmetric around half the transition frequency. The
spectrum is asymmetric around it. The theoretical framework and results for Na
are verified experimentally. This work opens the door for rational femtosecond
coherent control in a regime of considerable absorption yields
Pulse-Bandwidth Dependence of Coherent Phase Control of Resonance-Mediated (2+1) Three-Photon Absorption
We study in detail coherent phase control of femtosecond resonance-mediated
(2+1) three-photon absorption and its dependence on the spectral bandwidth of
the excitation pulse. The regime is the weak-field regime of third perturbative
order. The corresponding interference mechanism involves a group of
three-photon excitation pathways that are on resonance with the intermediate
state and a group of three-photon excitation pathways that are near resonant
with it. The model system of the study is atomic sodium (Na), for which
experimental and numerical-theoretical results are obtained. Prominent among
the results is our finding that with simple proper pulse shaping an increase in
the excitation bandwidth leads to a corresponding increase in the enhancement
of the three-photon absorption over the absorption induced by the (unshaped)
transform-limited pulse. For example, here, a 40-nm bandwidth leads to an
order-of-magnitude enhancement over the transform-limited absorption.Comment: 23 pages, 5 figure
Quantum control by von Neumann measurements
A general scheme is presented for controlling quantum systems using evolution
driven by non-selective von Neumann measurements, with or without an additional
tailored electromagnetic field. As an example, a 2-level quantum system
controlled by non-selective quantum measurements is considered. The control
goal is to find optimal system observables such that consecutive non-selective
measurement of these observables transforms the system from a given initial
state into a state which maximizes the expected value of a target operator (the
objective). A complete analytical solution is found including explicit
expressions for the optimal measured observables and for the maximal objective
value given any target operator, any initial system density matrix, and any
number of measurements. As an illustration, upper bounds on measurement-induced
population transfer between the ground and the excited states for any number of
measurements are found. The anti-Zeno effect is recovered in the limit of an
infinite number of measurements. In this limit the system becomes completely
controllable. The results establish the degree of control attainable by a
finite number of measurements
Reprint of: Femtosecond transition-state spectroscopy of iodine: From strongly bound to repulsive surface dynamics
The application of femtosecond transition-state spectroscopy (FTS) to molecular iodine is reported. The real-time motion of wave packets prepared coherently in the bound B state is observed. In addition, the motion is probed near and above the dissociation limit for the reaction: I_2 → I (^2P_(3/2)) + I∗(^2P_(1/2)). FTS measurements of the dynamics on repulsive surfaces are also reported
Femtosecond real-time probing of reactions. V. The reaction of IHgI
The dissociation reaction of HgI2 is examined experimentally using femtosecond transition-state spectroscopy (FTS). The reaction involves symmetric and antisymmetric coordinates and the transition-state is well-defined: IHgI*-->[IHgI][double-dagger]@B|Q[sub S[script ']]Q[sub a[script ']]q-->HgI+I. FTS is developed for this class of ABA-type reactions and recurrences are observed for the vibrating fragments (symmetric coordinate) along the reaction coordinate (antisymmetric coordinate). The translational motion is also observed as a "delay time" of the free fragments. Analysis of our FTS results indicates that the reaction wave packet proceeds through two pathways, yielding either I(2P3/2) or I*(2P1/2) as one of the final products. Dissociation into these two pathways leads to HgI fragments with different vibrational energy, resulting in distinct trajectories. Hence, oscillatory behaviors of different periods in the FTS transients are observed depending on the channel probed (~300 fs to ~1 ps). These results are analyzed using the standard FTS description, and by classical trajectory calculations performed on model potentials which include the two degrees of freedom of the reaction. Quantum calculations of the expected fluorescence of the fragment are also performed and are in excellent agreement with experiments
Pulse generation without gain-bandwidth limitation in a laser with self-similar evolution
With existing techniques for mode-locking, the bandwidth of ultrashort pulses from a laser is determined primarily by the spectrum of the gain medium. Lasers with self-similar evolution of the pulse in the gain medium can tolerate strong spectral breathing, which is stabilized by nonlinear attraction to the parabolic self-similar pulse. Here we show that this property can be exploited in a fiber laser to eliminate the gain-bandwidth limitation to the pulse duration. Broad (̃200 nm) spectra are generated through passive nonlinear propagation in a normal-dispersion laser, and these can be dechirped to ̃20-fs duration
Intravital Imaging Study on Photodamage Produced by Femtosecond Near-infrared Laser Pulses in Vivo
© 2016 The American Society of Photobiology.Ultrashort femtosecond pulsed lasers may provide indispensable benefits for medical bioimaging and diagnosis, particularly for noninvasive biopsy. However, the ability of femtosecond laser irradiation to produce biodamage in the living body is still a concern. To solve this biosafety issue, results of theoretical estimations as well as the in vitro and in situ experiments on femtosecond biodamage should be verified by experimental studies conducted in vivo. Here, we analyzed photodamage produced by femtosecond (19, 42 and 100 fs) near-infrared (NIR; ∼800 nm) laser pulses with an average power of 5 and 15 mW in living undissected Drosophila larvae (in vivo). These experimental data on photodamage in vivo agree with the results of theoretical modeling of other groups. Femtosecond NIR laser pulses may affect the concentration of fluorescent biomolecules localized in mitochondria of the cells of living undissected Drosophila larva. Our findings confirm that the results of the mathematical models of femtosecond laser ionization process in living tissues may have a practical value for development of noninvasive biopsy based on the use of femtosecond pulses
Historical perspective on: Femtosecond transition-state spectroscopy of iodine—From strongly bound to repulsive surface dynamics [Volume 161, Issues 4–5, 22 September 1989, Pages 297–302]
Summary by J.L. Herek. Nobel prize-winner: Professor Ahmed Zewail. In the spring of 1990, I was a young liberal arts student soon to graduate from Lawrence University in Wisconsin, dreaming of a career in chemical physics. Thanks to an elective course on applications of lasers in chemistry and physics, which also required a literature study and report, I had found that a revolution in chemical physics was underway, with many groups clamouring to conquer new territory in the study of chemical reactions: the elusive and fleeting transition state. My interest in this emerging field dictated my choices of potential graduate schools, with Caltech and the group of Ahmed Zewail at the top of my list
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