The Experts below are selected from a list of 5991 Experts worldwide ranked by ideXlab platform
David T. Limmer - One of the best experts on this subject based on the ideXlab platform.
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Studying rare nonadiabatic dynamics with transition path sampling Quantum Jump trajectories.
The Journal of chemical physics, 2018Co-Authors: Addison J. Schile, David T. LimmerAbstract:We present a method to study rare nonadiabatic dynamics in open Quantum systems using transition path sampling and Quantum Jump trajectories. As with applications of transition path sampling to classical dynamics, the method does not rely on prior knowledge of transition states or reactive pathways and thus can provide mechanistic insight into ultrafast relaxation processes in addition to their associated rates. In particular, we formulate a Quantum path ensemble using the stochastic realizations of an unravelled Quantum master equation, which results in trajectories that can be conditioned on starting and ending in particular Quantum states. Because the dynamics rigorously obeys detailed balance, rate constants can be evaluated from reversible work calculations in this conditioned ensemble, allowing for branching ratios and yields to be computed in an unbiased manner. We illustrate the utility of this method with three examples: energy transfer in a donor-bridge-acceptor model, and models of photo-induced proton-coupled electron transfer and thermally activated electron transfer. These examples demonstrate the efficacy of path ensemble methods and pave the way for their use in studying complex reactive Quantum dynamics.We present a method to study rare nonadiabatic dynamics in open Quantum systems using transition path sampling and Quantum Jump trajectories. As with applications of transition path sampling to classical dynamics, the method does not rely on prior knowledge of transition states or reactive pathways and thus can provide mechanistic insight into ultrafast relaxation processes in addition to their associated rates. In particular, we formulate a Quantum path ensemble using the stochastic realizations of an unravelled Quantum master equation, which results in trajectories that can be conditioned on starting and ending in particular Quantum states. Because the dynamics rigorously obeys detailed balance, rate constants can be evaluated from reversible work calculations in this conditioned ensemble, allowing for branching ratios and yields to be computed in an unbiased manner. We illustrate the utility of this method with three examples: energy transfer in a donor-bridge-acceptor model, and models of photo-induce...
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Studying rare nonadiabatic dynamics with transition path sampling Quantum Jump trajectories.
arXiv: Statistical Mechanics, 2018Co-Authors: Addison J. Schile, David T. LimmerAbstract:We present a method to study rare nonadiabatic dynamics in open Quantum systems using transition path sampling and Quantum Jump trajectories. As with applications of transition path sampling to classical dynamics, the method does not rely on prior knowledge of transition states or reactive pathways, and thus can provide mechanistic insight into ultrafast relaxation processes in addition to their associated rates. In particular, we formulate a Quantum path ensemble using the stochastic realizations of an unravelled Quantum master equation, which results in trajectories that can be conditioned on starting and ending in particular Quantum states. Because the dynamics rigorously obeys detailed balance, rate constants can be evaluated from reversible work calculations in this conditioned ensemble, allowing for branching ratios and yields to be computed in an unbiased manner. We illustrate the utility of this method with three examples: energy transfer in a donor-bridge-acceptor model, and models of photo-induced proton-coupled electron transfer and thermally activated electron transfer. These examples demonstrate the efficacy of path ensemble methods and pave the way for their use in studying of complex reactive Quantum dynamics.
Addison J. Schile - One of the best experts on this subject based on the ideXlab platform.
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Studying rare nonadiabatic dynamics with transition path sampling Quantum Jump trajectories.
The Journal of chemical physics, 2018Co-Authors: Addison J. Schile, David T. LimmerAbstract:We present a method to study rare nonadiabatic dynamics in open Quantum systems using transition path sampling and Quantum Jump trajectories. As with applications of transition path sampling to classical dynamics, the method does not rely on prior knowledge of transition states or reactive pathways and thus can provide mechanistic insight into ultrafast relaxation processes in addition to their associated rates. In particular, we formulate a Quantum path ensemble using the stochastic realizations of an unravelled Quantum master equation, which results in trajectories that can be conditioned on starting and ending in particular Quantum states. Because the dynamics rigorously obeys detailed balance, rate constants can be evaluated from reversible work calculations in this conditioned ensemble, allowing for branching ratios and yields to be computed in an unbiased manner. We illustrate the utility of this method with three examples: energy transfer in a donor-bridge-acceptor model, and models of photo-induced proton-coupled electron transfer and thermally activated electron transfer. These examples demonstrate the efficacy of path ensemble methods and pave the way for their use in studying complex reactive Quantum dynamics.We present a method to study rare nonadiabatic dynamics in open Quantum systems using transition path sampling and Quantum Jump trajectories. As with applications of transition path sampling to classical dynamics, the method does not rely on prior knowledge of transition states or reactive pathways and thus can provide mechanistic insight into ultrafast relaxation processes in addition to their associated rates. In particular, we formulate a Quantum path ensemble using the stochastic realizations of an unravelled Quantum master equation, which results in trajectories that can be conditioned on starting and ending in particular Quantum states. Because the dynamics rigorously obeys detailed balance, rate constants can be evaluated from reversible work calculations in this conditioned ensemble, allowing for branching ratios and yields to be computed in an unbiased manner. We illustrate the utility of this method with three examples: energy transfer in a donor-bridge-acceptor model, and models of photo-induce...
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Studying rare nonadiabatic dynamics with transition path sampling Quantum Jump trajectories.
arXiv: Statistical Mechanics, 2018Co-Authors: Addison J. Schile, David T. LimmerAbstract:We present a method to study rare nonadiabatic dynamics in open Quantum systems using transition path sampling and Quantum Jump trajectories. As with applications of transition path sampling to classical dynamics, the method does not rely on prior knowledge of transition states or reactive pathways, and thus can provide mechanistic insight into ultrafast relaxation processes in addition to their associated rates. In particular, we formulate a Quantum path ensemble using the stochastic realizations of an unravelled Quantum master equation, which results in trajectories that can be conditioned on starting and ending in particular Quantum states. Because the dynamics rigorously obeys detailed balance, rate constants can be evaluated from reversible work calculations in this conditioned ensemble, allowing for branching ratios and yields to be computed in an unbiased manner. We illustrate the utility of this method with three examples: energy transfer in a donor-bridge-acceptor model, and models of photo-induced proton-coupled electron transfer and thermally activated electron transfer. These examples demonstrate the efficacy of path ensemble methods and pave the way for their use in studying of complex reactive Quantum dynamics.
Jean-françois Roch - One of the best experts on this subject based on the ideXlab platform.
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Enhancing single-molecule photostability by optical feedback from Quantum Jump detection
Applied Physics Letters, 2008Co-Authors: Vincent Jacques, John D. Murray, François Marquier, Dominique Chauvat, Frédéric Grosshans, François Treussart, Jean-françois RochAbstract:We report an optical technique that yields an enhancement of single-molecule photostability by greatly suppressing photobleaching pathways which involve photoexcitation from the triplet state. This is accomplished by dynamically switching off the excitation laser when a Quantum Jump of the molecule to the triplet state is optically detected. The resulting improvement in photostability unambiguously confirms the importance of photoexcitation from the triplet state in photobleaching dynamics and will allow the investigation of new phenomena at the single-molecule level.
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Enhancing single-molecule photostability by optical feedback from Quantum-Jump detection
2007Co-Authors: Vincent Jacques, François Marquier, Dominique Chauvat, Frédéric Grosshans, François Treussart, John Murray, Jean-françois RochAbstract:We report an optical technique that yields an enhancement of single-molecule photostability, by greatly suppressing photobleaching pathways which involve photoexcitation from the triplet state. This is accomplished by dynamically switching off the excitation laser when a Quantum-Jump of the molecule to the triplet state is optically detected. This procedure leads to a lengthened single-molecule observation time and an increased total number of detected photons. The resulting improvement in photostability unambiguously confirms the importance of photoexcitation from the triplet state in photobleaching dynamics, and may allow the investigation of new phenomena at the single-molecule level.
Michel H. Devoret - One of the best experts on this subject based on the ideXlab platform.
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To catch and reverse a Quantum Jump mid-flight
Nature, 2019Co-Authors: Zlatko K. Minev, R. Gutierrez-jauregui, Robert J. Schoelkopf, S. Shankar, Shantanu O. Mundhada, Philip Reinhold, Mazyar Mirrahimi, H. j. Carmichael, Michel H. DevoretAbstract:In Quantum physics, measurements can fundamentally yield discrete and random results. Emblematic of this feature is Bohr’s 1913 proposal of Quantum Jumps between two discrete energy levels of an atom^ 1 . Experimentally, Quantum Jumps were first observed in an atomic ion driven by a weak deterministic force while under strong continuous energy measurement^ 2 – 4 . The times at which the discontinuous Jump transitions occur are reputed to be fundamentally unpredictable. Despite the non-deterministic character of Quantum physics, is it possible to know if a Quantum Jump is about to occur? Here we answer this question affirmatively: we experimentally demonstrate that the Jump from the ground state to an excited state of a superconducting artificial three-level atom can be tracked as it follows a predictable ‘flight’, by monitoring the population of an auxiliary energy level coupled to the ground state. The experimental results demonstrate that the evolution of each completed Jump is continuous, coherent and deterministic. We exploit these features, using real-time monitoring and feedback, to catch and reverse Quantum Jumps mid-flight—thus deterministically preventing their completion. Our findings, which agree with theoretical predictions essentially without adjustable parameters, support the modern Quantum trajectory theory^ 5 – 9 and should provide new ground for the exploration of real-time intervention techniques in the control of Quantum systems, such as the early detection of error syndromes in Quantum error correction. Experiment overturns Bohr’s view of Quantum Jumps, demonstrating that they possess a degree of predictability and when completed are continuous, coherent and even deterministic.
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To catch and reverse a Quantum Jump mid-flight
Nature, 2019Co-Authors: Zlatko K. Minev, R. Gutierrez-jauregui, H. J. Carmichael, Robert J. Schoelkopf, S. Shankar, Shantanu O. Mundhada, Philip Reinhold, Mazyar Mirrahimi, Michel H. DevoretAbstract:Quantum physics was invented to account for two fundamental features of measurement results -- their discreetness and randomness. Emblematic of these features is Bohr's idea of Quantum Jumps between two discrete energy levels of an atom. Experimentally, Quantum Jumps were first observed in an atomic ion driven by a weak deterministic force while under strong continuous energy measurement. The times at which the discontinuous Jump transitions occur are reputed to be fundamentally unpredictable. Can there be, despite the indeterminism of Quantum physics, a possibility to know if a Quantum Jump is about to occur or not? Here, we answer this question affirmatively by experimentally demonstrating that the Jump from the ground to an excited state of a superconducting artificial three-level atom can be tracked as it follows a predictable "flight," by monitoring the population of an auxiliary energy level coupled to the ground state. The experimental results demonstrate that the Jump evolution when completed is continuous, coherent, and deterministic. Furthermore, exploiting these features and using real-time monitoring and feedback, we catch and reverse a Quantum Jump mid-flight, thus deterministically preventing its completion. Our results, which agree with theoretical predictions essentially without adjustable parameters, support the modern Quantum trajectory theory and provide new ground for the exploration of real-time intervention techniques in the control of Quantum systems, such as early detection of error syndromes.
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To catch and reverse a Quantum Jump mid-flight
2018Co-Authors: Zlatko K. Minev, R. Gutierrez-jauregui, Mazyar Mirahimi, H. J. Carmichael, Robert J. Schoelkopf, S. Shankar, Shantanu O. Mundhada, Philip Reinhold, Michel H. DevoretAbstract:A Quantum system driven by a weak deterministic force while under strong continuous energy measurement exhibits Quantum Jumps between its energy levels. This celebrated phenomenon is emblematic of the special nature of randomness in Quantum physics. The times at which the Jumps occur are reputed to be fundamentally unpredictable. However, certain classical phenomena, like tsunamis, while unpredictable in the long term, may possess a degree of predictability in the short term, and in some cases it may be possible to prevent a disaster by detecting an advance warning signal. Can there be, despite the indeterminism of Quantum physics, a possibility to know if a Quantum Jump is about to occur or not? In this paper, we answer this question affirmatively by experimentally demonstrating that the completed Jump from the ground to an excited state of a superconducting artificial atom can be tracked, as it follows its predictable "flight," by monitoring the population of an auxiliary level coupled to the ground state. Furthermore, we show that the completed Jump is continuous, deterministic, and coherent. Exploiting this coherence, we catch and reverse a Quantum Jump mid-flight, thus preventing its completion. This real-time intervention is based on a particular lull period in the population of the auxiliary level, which serves as our advance warning signal. Our results, which agree with theoretical predictions essentially without adjustable parameters, support the modern Quantum trajectory theory and provide new ground for the exploration of real-time intervention techniques in the control of Quantum systems, such as early detection of error syndromes.
Vincent Jacques - One of the best experts on this subject based on the ideXlab platform.
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Enhancing single-molecule photostability by optical feedback from Quantum Jump detection
Applied Physics Letters, 2008Co-Authors: Vincent Jacques, John D. Murray, François Marquier, Dominique Chauvat, Frédéric Grosshans, François Treussart, Jean-françois RochAbstract:We report an optical technique that yields an enhancement of single-molecule photostability by greatly suppressing photobleaching pathways which involve photoexcitation from the triplet state. This is accomplished by dynamically switching off the excitation laser when a Quantum Jump of the molecule to the triplet state is optically detected. The resulting improvement in photostability unambiguously confirms the importance of photoexcitation from the triplet state in photobleaching dynamics and will allow the investigation of new phenomena at the single-molecule level.
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Enhancing single-molecule photostability by optical feedback from Quantum-Jump detection
2007Co-Authors: Vincent Jacques, François Marquier, Dominique Chauvat, Frédéric Grosshans, François Treussart, John Murray, Jean-françois RochAbstract:We report an optical technique that yields an enhancement of single-molecule photostability, by greatly suppressing photobleaching pathways which involve photoexcitation from the triplet state. This is accomplished by dynamically switching off the excitation laser when a Quantum-Jump of the molecule to the triplet state is optically detected. This procedure leads to a lengthened single-molecule observation time and an increased total number of detected photons. The resulting improvement in photostability unambiguously confirms the importance of photoexcitation from the triplet state in photobleaching dynamics, and may allow the investigation of new phenomena at the single-molecule level.
