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Journal of Optics B Quantum and Semiclassical Optics

Control of molecular decoherence and entanglement

Gershon Kurizki, Abraham G. Kofman, David Petrosyan, T Opatrn yacute

Published Aug 1, 2002• 6 citations
Publisher

Abstract

The impediment towards the successful development of the field of quantum information (QI) is decoherence , i.e., the loss of entanglement by the effect of the environment on the systems of interest. An important challenge is that of QI engineering, by entanglement and decoherence control, in complex systems, such as unimolecular and bimolecular systems, that can simultaneously handle large amounts of QI. Progress towards this goal can be achieved by: (a) decay modification and decoherence suppression in molecules, using laser-induced phase and amplitude modulation of rovibrational levels and inter-mode couplings; (b) transfer of internal-translational entanglement and teleportation of wavepackets via molecular dissociation and collisions.

DOI
10.1088/1464-4266/4/4/309

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How to control decoherence and entanglement in quantum complex systems?

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Theory and experiment have not fully resolved the apparent dichotomy , which has agonized physics for the past eighty years: on the one hand, the description of microsystems by quantum mechanics and, on the other, the description of macrosystems by classical dynamics or statistical mechanics. Derivations of the time-irreversible Liouville equation for an open quantum system, based on projecting out its environment, have narrowed the gap between the quantum and classical descriptions. Yet our `classical' intuition continues to be confronted by quantum-mechanical results like the Einstein--Podolsky--Rosen paradox that challenges the classical notion of locality, or the quantum Zeno effect which suggests that the isolation of a system is not the only way to preserve its quantum state. There are two key concepts in any discussion of such issues. 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At what stage does system--meter entanglement give rise to a classical readout of the meter? Is there an upper limit on the size or complexity of systems displaying entanglement? Major developments have opened new vistas into controlled entanglement , which is the resource of quantum information processing. However, these developments have mainly focused on ensembles of simple two- and three-level systems that are thoroughly isolated from their environments. Treatments of coherence in quantum computing have mostly assumed that only a single or a few the elements of the quantum ensemble may simultaneously undergo an uncontrolled intervention---a quantum error. Decoherence-control protocols for more general types of errors are still incomplete. In order to resolve the outstanding issues of the quantum--classical transition, and study the control of entanglement and decoherence without the foregoing restrictions, we must venture into the domain of Quantum Complex Systems (QUACS), either consisting of a large number of inseparable elements or having many coupled degrees of freedom. Our conviction is that fundamental understanding and manipulation of entanglement within QUACS or their entanglement with the environment or a meter, call for the creation of a new conceptual framework or paradigm, that would encompass phenomena common to cold atoms in laser fields, large molecules, Josephson junctions, quantum gases and solids, with the view of employing these systems for quantum information processing and computing. Progress within this paradigm should allow us to answer the questions: does entanglement play an essential role in the evolution of large collections of complex systems? 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Decoherence and decay of quantum states in open systems is the main obstacle towards the realization of quantum computing and communications and a major impediment for coherent control (of atomic, molecular and condensed-phase processes) and quantum state engineering (of fields and atoms in cavities and trapped ions). This Focus Issue is an attempt to highlight the development of schemes for the control of quantum decay and decoherence, by presenting the major trends in this area. To this end, I have solicited a number of articles from groups that have been particularly active in the pursuit of these trends.

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The impediment towards the successful development of the field of quantum information (QI) is decoherence , i.e., the loss of entanglement by the effect of the environment on the systems of interest. An important challenge is that of QI engineering, by entanglement and decoherence control, in complex systems, such as unimolecular and bimolecular systems, that can simultaneously handle large amounts of QI. Progress towards this goal can be achieved by: (a) decay modification and decoherence suppression in molecules, using laser-induced phase and amplitude modulation of rovibrational levels and inter-mode couplings; (b) transfer of internal-translational entanglement and teleportation of wavepackets via molecular dissociation and collisions.
Theory and experiment have not fully resolved the apparent dichotomy , which has agonized physics for the past eighty years: on the one hand, the description of microsystems by quantum mechanics and, on the other, the description of macrosystems by classical dynamics or statistical mechanics. Derivations of the time-irreversible Liouville equation for an open quantum system, based on projecting out its environment, have narrowed the gap between the quantum and classical descriptions. Yet our `classical' intuition continues to be confronted by quantum-mechanical results like the Einstein--Podolsky--Rosen paradox that challenges the classical notion of locality, or the quantum Zeno effect which suggests that the isolation of a system is not the only way to preserve its quantum state. There are two key concepts in any discussion of such issues. The first, which is responsible for the most salient nonclassical properties, is entanglement , that is partial or complete correlation or, more generally, inseparability of the elements comprising a quantum ensemble . Even after their interaction has ceased, this inseparability, originating from their past interaction, can affect the state of one element when another element is subject to a nonunitary action, such as its measurement, tracing- out, or thermalization. The second key concept is decoherence of open quantum systems, which is the consequence of their entanglement with their environment, a `meter' or a thermal `reservoir', followed by the tracing-out of the latter. Despite new insights into entanglement and decoherence, there are still no complete, unequivocal answers to the fundamental questions of the transition from quantal to classical behaviour: how do irreversibility and classicality emerge from unitarity as systems and their environments become increasingly complex ? At what stage does system--meter entanglement give rise to a classical readout of the meter? Is there an upper limit on the size or complexity of systems displaying entanglement? Major developments have opened new vistas into controlled entanglement , which is the resource of quantum information processing. However, these developments have mainly focused on ensembles of simple two- and three-level systems that are thoroughly isolated from their environments. Treatments of coherence in quantum computing have mostly assumed that only a single or a few the elements of the quantum ensemble may simultaneously undergo an uncontrolled intervention---a quantum error. Decoherence-control protocols for more general types of errors are still incomplete. In order to resolve the outstanding issues of the quantum--classical transition, and study the control of entanglement and decoherence without the foregoing restrictions, we must venture into the domain of Quantum Complex Systems (QUACS), either consisting of a large number of inseparable elements or having many coupled degrees of freedom. Our conviction is that fundamental understanding and manipulation of entanglement within QUACS or their entanglement with the environment or a meter, call for the creation of a new conceptual framework or paradigm, that would encompass phenomena common to cold atoms in laser fields, large molecules, Josephson junctions, quantum gases and solids, with the view of employing these systems for quantum information processing and computing. Progress within this paradigm should allow us to answer the questions: does entanglement play an essential role in the evolution of large collections of complex systems? What are the size and complexity limits of systems and ensembles still controllable by an external intervention? What are the most appropriate decoherence protection schemes and control algorithms? This special issue addresses the challenge of understanding in depth and manipulating the basic quantum properties of optical, atomic, molecular and condensed-matter QUACS, and large ensembles thereof. In view of the interdisciplinary character of this issue, we find it expedient to look at the presented articles not only according to the physical objects they describe, but also from a unifying standpoint. Several unifying themes may be discerned: memory effects in dephasing and relaxation; protection of quantum information by its distribution throughout the ensemble; control of decoherence and entanglement by time-dependent interventions or measurements; manifestations of entanglement in scattering off statistical ensembles; measurment-induced dynamics. The concerted discussion of the topics outlined above should help us advance the new paradigm that addresses our abilities to diagnose and manipulate the entangled states of complex quantum objects and their robustness against decoherence. These abilities are required for quantum information (QI) applications in matter--wave interferometry in molecular, semiconducting or superconducting systems. On the fundamental level, this book may help establish the notion of dynamical information exchange between quantum systems and chart in detail the route from unitarity to classicality. Further developments within the outlined paradigm should yield novel, advantageous QI processing schemes and high-sensitivity interferometers, owing to decoherence suppression and effective control of many degrees of freedom. In the long run, these strategies may prove to be the first step towards the (hitherto unattempted) use of entanglement in nanotechnology, metrology and chemistry, with potentially remarkable novel applications.
Any real system, no matter how well isolated, unavoidably interacts with the environment. This interaction makes the evolution of a quantum system nonunitary and destroys the coherence of quantum superpositions. This process, known as decoherence, is widely regarded as the most important and fundamental obstacle to the practical realization of quantum information processing. On the other hand, the objectives of quantum control are predicated on the ability to manipulate the system coherently over a period of time. Quantum control has been applied successfully to several experimental systems and coupling such a controlled system to an environment makes the study of coherence loss possible. The standard model of decoherence is formulated in terms of a system, defined by the observables that can be measured, and a reservoir, de¯ned by those degrees of freedom that are not accessed by observation. The vibrational and rotational degree of freedom of diatomic molecules form an experimental model of such a system and bath 1. The nature of the ro-vibrational coupling does not allow a Decoherence Free Subspace, instead we try to identify a Decoherence Resistant Subspace using closed loop control. We set up a learning control loop experiment to monitor the coherence in a vibrational wavepacket, consisting of about 6 vibrational states of the A(1Σ+g ) electronic state, excited by a shaped, ultrashort optical pulse, and then to determine the pulse shape that yielded the longest coherence lifetime. The coherence of the vibrational wavepacket was monitored by measuring the fluorescence quantum beats from the outer turning point of the wave packet's trajectory. The closed loop controller altered the shape of the driving optical pulse to maximize the the depth of modulation of the quantum beats at a prescribed time after excitation, within the constraints of the laser system. The outcome of this closed loop control experiment shows an improvement of the beat decay constant of about 60%, as shown in Fig. (1), a result which occurs for several di®erent pulse shapes. Our experiments show that a number of interesting decoherence-resistant excitations exist. The nature of the dephasing was examined theoretically. Using measured optical pulse shapes, we simulated numerically the molecular wavepacket in the limit of perturbation theory. The experiment and simulations show that there are di®erent mechanisms contributing to the decoherence resistant excitation. The shaped pulse reduces the °uctuations in the wave packet spatial extent, which in turn changes the system reservoir coupling. Other components of the optimal pulse are a sequence of pulses that creates constructive interference of the vibrational wavepacket at the desired time, and chirp which compensates for the anharmonicity of the adiabatic potential. The experimental results show general agreement with numerical simulations. We conclude that wavepackets resistant to dephasing do exist,and that learning algorithms provide an effcient means for finding them.
Decoherence and decay of quantum states in open systems is the main obstacle towards the realization of quantum computing and communications and a major impediment for coherent control (of atomic, molecular and condensed-phase processes) and quantum state engineering (of fields and atoms in cavities and trapped ions). This Focus Issue is an attempt to highlight the development of schemes for the control of quantum decay and decoherence, by presenting the major trends in this area. To this end, I have solicited a number of articles from groups that have been particularly active in the pursuit of these trends.
In this thesis, we discuss the possibilities for suppression of decoherence, the loss of purity in an open quantum system, and the related process of dephasing. In the first chapter, we review the literature on the subject of open system dynamics, decoherence and methods of decoherence suppression. In the second chapter, we focus on the specific case of a rotationally hot diatomic molecule as an example of an open quantum system, where molecular vibrational wavepackets are subject to dephasing due to rovibrational coupling. We report analytical and numerical results addressing whether the dephasing rate can be controlled by adjustment of the initial wavepacket phases. It appears that over long timescales, phase-only control is not possible, but for earlier timescales the possibility of phase-only control of dephasing remains. In addition, we point out that the time-dependence of the dephasing process depends significantly upon the degeneracy of the rotational environment states. In the final chapter, we discuss the same system, but apply a qualitatively different method of dephasing suppression based on the nonlinear resonance effect in a driving field. We extend previous work on the topic (Shapiro et al. [1]) by considering the effect of using a train of laser pulses as the driving field, in place of a two-colour continuous-wave laser field. We demonstrate that the pulse train method can be more effective at suppressing dephasing than the two-colour CW case.
We present a Physics-Informed Neural Quantum Control (PINQC) framework for rovibrational photoassociation in a Morse molecular system. The proposed method combines neural-network-based laser-field generation with differentiable quantum propagation, allowing optimized laser pulses to be obtained directly from the underlying quantum dynamics without requiring external training data. The optimized control fields efficiently transfer an initially continuum-like Gaussian wave packet into the vibrational ground-state level, promoting continuum-to-bound population transfer through coherent rovibrational dynamics. The resulting photoassociation process involves both vibrational stabilization and rotational redistribution arising naturally from dipole-induced couplings between neighboring rotational channels. A central result of the present work is the successful application of the PINQC framework to extended rovibrational models containing larger rotational levels than those previously accessible in our conventional photoassociation calculations. The optimization remains numerically stable despite the increased complexity of the molecular system, demonstrating that differentiable optimization provides an effective strategy for treating rovibrational models of increased dimensionality. These results establish the PINQC framework as a promising computational tool for molecular photoassociation and motivate future investigations of increasingly complex rovibrational quantum-control problems.