191 research outputs found
Extracting molecular Hamiltonian structure from time-dependent fluorescence intensity data
We propose a formalism for extracting molecular Hamiltonian structure from
inversion of time-dependent fluorescence intensity data. The proposed method
requires a minimum of \emph{a priori} knowledge about the system and allows for
extracting a complete set of information about the Hamiltonian for a pair of
molecular electronic surfaces.Comment: 7pages, no figures, LaTeX2
Coherent Optimal Control of Multiphoton Molecular Excitation
We give a framework for molecular multiphoton excitation process induced by
an optimally designed electric field. The molecule is initially prepared in a
coherent superposition state of two of its eigenfunctions. The relative phase
of the two superposed eigenfunctions has been shown to control the optimally
designed electric field which triggers the multiphoton excitation in the
molecule. This brings forth flexibility in desiging the optimal field in the
laboratory by suitably tuning the molecular phase and hence by choosing the
most favorable interfering routes that the system follows to reach the target.
We follow the quantum fluid dynamical formulation for desiging the electric
field with application to HBr molecule.Comment: 5 figure
Beable trajectories for revealing quantum control mechanisms
The dynamics induced while controlling quantum systems by optimally shaped
laser pulses have often been difficult to understand in detail. A method is
presented for quantifying the importance of specific sequences of quantum
transitions involved in the control process. The method is based on a
``beable'' formulation of quantum mechanics due to John Bell that rigorously
maps the quantum evolution onto an ensemble of stochastic trajectories over a
classical state space. Detailed mechanism identification is illustrated with a
model 7-level system. A general procedure is presented to extract mechanism
information directly from closed-loop control experiments. Application to
simulated experimental data for the model system proves robust with up to 25%
noise.Comment: Latex, 20 pages, 13 figure
Optimal Control of Molecular Motion Expressed Through Quantum Fluid Dynamics
A quantum fluid dynamic control formulation is presented for optimally
manipulating atomic and molecular systems. In quantum fluid dynamic the control
quantum system is expressed in terms of the probability density and the quantum
current. This choice of variables is motivated by the generally expected slowly
varying spatial-temporal dependence of the fluid dynamical variables. The
quantum fluid dynamic approach is illustrated for manipulation of the ground
electronic state dynamics of HCl induced by an external electric field.Comment: 18 pages, latex, 3 figure
Transform-limited pulses are not optimal for resonant multiphoton transitions
Maximizing nonlinear light-matter interactions is a primary motive for
compressing laser pulses to achieve ultrashort transform limited pulses. Here
we show how, by appropriately shaping the pulses, resonant multiphoton
transitions can be enhanced significantly beyond the level achieved by
maximizing the pulse's peak intensity. We demonstrate the counterintuitive
nature of this effect with an experiment in a resonant two-photon absorption,
in which, by selectively removing certain spectral bands, the peak intensity of
the pulse is reduced by a factor of 40, yet the absorption rate is doubled.
Furthermore, by suitably designing the spectral phase of the pulse, we increase
the absorption rate by a factor of 7.Comment: 4 pages, 3 figure
FAST CARS: Engineering a Laser Spectroscopic Technique for Rapid Identification of Bacterial Spores
Airborne contaminants, e.g., bacterial spores, are usually analyzed by time
consuming microscopic, chemical and biological assays. Current research into
real time laser spectroscopic detectors of such contaminants is based on e.g.
resonant Raman spectroscopy. The present approach derives from recent
experiments in which atoms and molecules are prepared by one (or more) coherent
laser(s) and probed by another set of lasers. The connection with previous
studies based on "Coherent Anti-Stokes Raman Spectroscopy" (CARS) is to be
noted. However generating and utilizing maximally coherent oscillation in
macromolecules having an enormous number of degrees of freedom is much more
challenging. This extension of the CARS technique is called FAST CARS
(Femtosecond Adaptive Spectroscopic Techniques for Coherent Anti-Stokes Raman
Spectroscopy), and the present paper proposes and analyses ways in which it
could be used to rapidly identify pre-selected molecules in real time.Comment: 43 pages, 21 figures; replacement with references added. Submitted to
the Proceedings of National Academy of Science
Optimal use of time dependent probability density data to extract potential energy surfaces
A novel algorithm was recently presented to utilize emerging time dependent
probability density data to extract molecular potential energy surfaces. This
paper builds on the previous work and seeks to enhance the capabilities of the
extraction algorithm: An improved method of removing the generally ill-posed
nature of the inverse problem is introduced via an extended Tikhonov
regularization and methods for choosing the optimal regularization parameters
are discussed. Several ways to incorporate multiple data sets are investigated,
including the means to optimally combine data from many experiments exploring
different portions of the potential. Results are presented on the stability of
the inversion procedure, including the optimal combination scheme, under the
influence of data noise. The method is applied to the simulated inversion of a
double well system.Comment: 34 pages, 5 figures, LaTeX with REVTeX and Graphicx-Package;
submitted to PhysRevA; several descriptions and explanations extended in Sec.
I
Coherent control using adaptive learning algorithms
We have constructed an automated learning apparatus to control quantum
systems. By directing intense shaped ultrafast laser pulses into a variety of
samples and using a measurement of the system as a feedback signal, we are able
to reshape the laser pulses to direct the system into a desired state. The
feedback signal is the input to an adaptive learning algorithm. This algorithm
programs a computer-controlled, acousto-optic modulator pulse shaper. The
learning algorithm generates new shaped laser pulses based on the success of
previous pulses in achieving a predetermined goal.Comment: 19 pages (including 14 figures), REVTeX 3.1, updated conten
Focusing and Compression of Ultrashort Pulses through Scattering Media
Light scattering in inhomogeneous media induces wavefront distortions which
pose an inherent limitation in many optical applications. Examples range from
microscopy and nanosurgery to astronomy. In recent years, ongoing efforts have
made the correction of spatial distortions possible by wavefront shaping
techniques. However, when ultrashort pulses are employed scattering induces
temporal distortions which hinder their use in nonlinear processes such as in
multiphoton microscopy and quantum control experiments. Here we show that
correction of both spatial and temporal distortions can be attained by
manipulating only the spatial degrees of freedom of the incident wavefront.
Moreover, by optimizing a nonlinear signal the refocused pulse can be shorter
than the input pulse. We demonstrate focusing of 100fs pulses through a 1mm
thick brain tissue, and 1000-fold enhancement of a localized two-photon
fluorescence signal. Our results open up new possibilities for optical
manipulation and nonlinear imaging in scattering media
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