369 research outputs found
Transform-Limited-Pulse Representation of Excitation with Natural Incoherent Light
We study the natural excitation of molecular systems, applicable to, for
example, photosynthetic light-harvesting complexes, by natural incoherent
light. In contrast with the conventional classical models, we show that the
light need not have random character to properly represent the resultant linear
excitation. Rather, thermal excitation can be interpreted as a collection of
individual events resulting from the system's interaction with individual,
deterministic pulsed realizations that constitute the field. The derived
expressions for the individual field realizations and excitation events allow
for a wave function formalism, and therefore constitute a useful calculational
tool to study dynamics following thermal-light excitation. Further, they
provide a route to the experimental determination of natural incoherent
excitation using pulsed laser techniques.Comment: 5 pages, 3 figures, 1 page supplementary information. Comments
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Decoherence Effects in Reactive Scattering
Decoherence effects on quantum and classical dynamics in reactive scattering
are examined using a Caldeira-Leggett type model. Through a study of dynamics
of the collinear H+H2 reaction and the transmission over simple one-dimensional
barrier potentials, we show that decoherence leads to improved agreement
between quantum and classical reaction and transmission probabilities,
primarily by increasing the energy dispersion in a well defined way. Increased
potential nonlinearity is seen to require larger decoherence in order to attain
comparable quantum-classical agreement.Comment: 25 pages, 6 figures, to be published in J. Chem. Phy
Coherent Control of Quantum Chaotic Diffusion
Extensive coherent control over quantum chaotic diffusion using the kicked
rotor model is demonstrated and its origin in deviations from random matrix
theory is identified. Further, the extent of control in the presence of
external decoherence is established. The results are relevant to both areas of
quantum chaos and coherent control.Comment: 4 pages, 4 figures, to appear in Phys. Rev. Let
Coherent Control and Entanglement in the Attosecond Electron Recollision Dissociation of D2+
We examine the attosecond electron recollision dissociation of D2+ recently
demonstrated experimentally [H. Niikura et al., Nature (London) 421, 826
(2003)] from a coherent control perspective. In this process, a strong laser
field incident on D2 ionizes an electron, accelerates the electron in the laser
field to eV energies, and then drives the electron to recollide with the parent
ion, causing D2+ dissociation. A number of results are demonstrated. First, a
full dimensional Strong Field Approximation (SFA) model is constructed and
shown to be in agreement with the original experiment. This is then used to
rigorously demonstrate that the experiment is an example of coherent pump-dump
control. Second, extensions to bichromatic coherent control are proposed by
considering dissociative recollision of molecules prepared in a coherent
superposition of vibrational states. Third, by comparing the results to similar
scenarios involving field-free attosecond scattering of independently prepared
D2+ and electron wave packets, recollision dissociation is shown to provide an
example of wave-packet coherent control of reactive scattering. Fourth, this
analysis makes clear that it is the temporal correlations between the continuum
electron and D2+ wave packet, and not entanglement, that are crucial for the
sub-femtosecond probing resolution demonstrated in the experiment. This result
clarifies some misconceptions regarding the importance of entanglement in the
recollision probing of D2+. Finally, signatures of entanglement between the
recollision electron and the atomic fragments, detectable via coincidence
measurements, are identified
Dynamic interference of photoelectrons produced by high-frequency laser pulses
The ionization of an atom by a high-frequency intense laser pulse, where the
energy of a single-photon is sufficient to ionize the system, is investigated
from first principles. It is shown that as a consequence of an AC Stark effect
in the continuum, the energy of the photoelectron follows the envelope of the
laser pulse. This is demonstrated to result in strong dynamic interference of
the photoelectrons of the same kinetic energy emitted at different times.
Numerically exact computations on the hydrogen atom demonstrate that the
dynamic interference spectacularly modifies the photoionization process and is
prominently manifested in the photoelectron spectrum by the appearance of a
distinct multi-peak pattern. The general theory is shown to be well
approximated by explicit analytical expressions which allow for a transparent
understanding of the discovered phenomena and for making predictions on the
dependence of the measured spectrum on the properties of the pulse.Comment: 5 figure
Aspects of quantum coherence in the optical Bloch equations
Aspects of coherence and decoherence are analyzed within the optical Bloch
equations. By rewriting the analytic solution in an alternate form, we are able
to emphasize a number of unusual features: (a) despite the Markovian nature of
the bath, coherence at long times can be retained; (b) the long-time asymptotic
degree of coherence in the system is intertwined with the asymptotic difference
in level populations; (c) the traditional population-relaxation and decoherence
times, and , lose their meaning when the system is in the presence
of an external field, and are replaced by more general overall timescales; (d)
increasing the field strength, quantified by the Rabi frequency, ,
increases the rate of decoherence rather than reducing it, as one might expect;
and (e) maximum asymptotic coherence is reached when the system parameters
satisfy .Comment: 18 pages, 6 figures; to appear in J Chem Phy
Chaos and Correspondence in Classical and Quantum Hamiltonian Ratchets: A Heisenberg Approach
Previous work [Gong and Brumer, Phys. Rev. Lett., 97, 240602 (2006)]
motivates this study as to how asymmetry-driven quantum ratchet effects can
persist despite a corresponding fully chaotic classical phase space. A simple
perspective of ratchet dynamics, based on the Heisenberg picture, is
introduced. We show that ratchet effects are in principle of common origin in
classical and quantum mechanics, though full chaos suppresses these effects in
the former but not necessarily the latter. The relationship between ratchet
effects and coherent dynamical control is noted.Comment: 21 pages, 7 figures, to appear in Phys. Rev.
Directed deterministic classical transport: symmetry breaking and beyond
We consider transport properties of a double delta-kicked system, in a regime
where all the symmetries (spatial and temporal) that could prevent directed
transport are removed. We analytically investigate the (non trivial) behavior
of the classical current and diffusion properties and show that the results are
in good agreement with numerical computations. The role of dissipation for a
meaningful classical ratchet behavior is also discussed.Comment: 10 pages, 20 figure
Intermittency of glassy relaxation and the emergence of a non-equilibrium spontaneous measure in the aging regime
We consider heat exchange processes between non-equilibrium aging systems (in
their activated regime) and the thermal bath in contact. We discuss a scenario
where two different heat exchange processes concur in the overall heat
dissipation: a stimulated fast process determined by the temperature of the
bath and a spontaneous intermittent process determined by the fact that the
system has been prepared in a non-equilibrium state. The latter is described by
a probability distribution function (PDF) that has an exponential tail of width
given by a parameter , and satisfies a fluctuation theorem (FT)
governed by that parameter. The value of is proportional to the
so-called effective temperature, thereby providing a practical way to
experimentally measure it by analyzing the PDF of intermittent events.Comment: Latex file, 8 pages + 5 postscript figure
Entanglement and Timing-Based Mechanisms in the Coherent Control of Scattering Processes
The coherent control of scattering processes is considered, with electron
impact dissociation of H used as an example. The physical mechanism
underlying coherently controlled stationary state scattering is exposed by
analyzing a control scenario that relies on previously established entanglement
requirements between the scattering partners. Specifically, initial state
entanglement assures that all collisions in the scattering volume yield the
desirable scattering configuration. Scattering is controlled by preparing the
particular internal state wave function that leads to the favored collisional
configuration in the collision volume. This insight allows coherent control to
be extended to the case of time-dependent scattering. Specifically, we identify
reactive scattering scenarios using incident wave packets of translational
motion where coherent control is operational and initial state entanglement is
unnecessary. Both the stationary and time-dependent scenarios incorporate
extended coherence features, making them physically distinct. From a
theoretical point of view, this work represents a large step forward in the
qualitative understanding of coherently controlled reactive scattering. From an
experimental viewpoint, it offers an alternative to entanglement-based control
schemes. However, both methods present significant challenges to existing
experimental technologies
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