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Open Questions in Quantum Control of Chemical Reactions: A Guide to the Perplexed Is weak field control possible? Dwayne Miller, Shapiro, Brumer, Kosloff What are the limits on control of bimolecular reactions? Dantus, Shapiro, Brumer, de Vivie Riedle, Motzkus, Ohmori, Amitay, Koch, Kosloff Can attosecond pulses generate coherent control of electrons? Can electron correlation be controlled? Bucksbaum, Dudovich, Ivanov, Smirnova, Baumert Laser control of photodissociation products – where do we stand? Gerber, Levis, Dantus Can quantum control landscapes have traps? Rabitz, Pechen, Tannor What is responsible for the differences between theoretical vs. practical limits on controllability? Rabitz, Brixner, Khasin, Kosloff How does one elucidate mechanism? How can we learn from learning algorithms? Can one distinguish unambiguously between quantum coherent control and classical control? Gerber, Bucksbaum, Brumer, Weinacht, Rabitz, Brixner, Tannor, Meier, Kallush This is just a beginning --- what other open questions can you add? Open Questions in Quantum Control of Chemical Reactions: A Guide to the Perplexed Is weak field control possible? Dwayne Miller, Shapiro, Brumer, Kosloff… 1. Is Weak Field Control Possible? 1. Is Weak Field Control Possible? New Journal of Ph ys ics The open–access journal for physics Control by decoherence: weak field control of an excited state objective Gil Katz1 , Mark A Ratner2 and Ronnie Kosloff3 Coherent control employing a broadband excitation is applied to a branching reaction in the excited state. In a weak field for an isolated molecule, a control objective is only frequency dependent. This means that phase control of the pulse cannot improve the objective beyond the best frequency selection. Once the molecule is put into a dissipative environment a new timescale emerges. In this study, we demonstrate that the dissipation allows us to achieve coherent control of branching ratios in the excited state. The model studied contains a nuclear coordinate and three electronic states: the ground and two coupled diabatic excited states. The influence of the environment is modeled by the stochastic surrogate Hamiltonian. The excitation is generated by a Gaussian pulse where the phase control introduced a chirp to the pulse. For sufficient relaxation, we find significant control in the weak field depending on the chirp rate. The observed control is rationalized by a timing argument caused by a focused wavepacket. The initial non-adiabatic crossing is enhanced by the chirp. This is followed by energy relaxation which stabilizes the state by having an energy lower than the crossing point. Abstract. 1. Is Weak Field Control Possible? 1. Is Weak Field Control Possible? Open Questions in Quantum Control of Chemical Reactions: A Guide to the Perplexed What are the limits on control of bimolecular reactions? Dantus, Shapiro, Brumer, de Vivie Riedle, Motzkus, Ohmori, Amitay, Koch, Kosloff,… What are the limits on control of bimolecular reactions? What are the limits on control of bimolecular reactions? What are the limits on control of bimolecular reactions? What are the limits on control of bimolecular reactions? What are the limits on control of bimolecular reactions? Open Questions in Quantum Control of Chemical Reactions: A Guide to the Perplexed Can attosecond pulses generate coherent control of electrons? Can electron correlation be controlled? Bucksbaum, Dudovich, Ivanov, Smirnova, Baumert,… Can attosecond pulses generate coherent control of electrons? Can electron correlation be controlled? Can attosecond pulses generate coherent control of electrons? Can electron correlation be controlled? Open Questions in Quantum Control of Chemical Reactions: A Guide to the Perplexed Laser control of photodissociation products – where do we stand? Gerber, Levis, Dantus,… Laser control of photodissociation products – Where do we stand? Laser control of photodissociation products – Where do we stand? Laser control of photodissociation products – Where do we stand? Open Questions in Quantum Control of Chemical Reactions: A Guide to the Perplexed Can quantum control landscapes have traps? Rabitz, Schirmer, Pechen, Tannor,… Can quantum control landscapes have traps? Can quantum control landscapes have traps? Can quantum control landscapes have traps? Can quantum control landscapes have traps? Open Questions in Quantum Control of Chemical Reactions: A Guide to the Perplexed What is responsible for the differences between theoretical vs. practical limits on controllability? Rabitz, Brixner, Khasin, Kosloff,… What is responsible for the differences between theoretical vs. practical limits on controllability? Open Questions in Quantum Control of Chemical Reactions: A Guide to the Perplexed How does one elucidate mechanism? How can we learn from learning algorithms? Can one distinguish unambiguously between quantum coherent control and classical control? Weinacht, Sension, Bucksbaum, Rabitz, Brixner, Kallush,… How does one elucidate mechanism? How can we learn from learning algorithms? Can one distinguish unambiguously between quantum coherent control and classical control? How does one elucidate mechanism? How can we learn from learning algorithms? Can one distinguish unambiguously between quantum coherent control and classical control? How does one elucidate mechanism? How can we learn from learning algorithms? Can one distinguish unambiguously between quantum coherent control and classical control? How does one elucidate mechanism? How can we learn from learning algorithms? Can one distinguish unambiguously between quantum coherent control and classical control? How does one elucidate mechanism? How can we learn from learning algorithms? Can one distinguish unambiguously between quantum coherent control and classical control? How does one elucidate mechanism? How can we learn from learning algorithms? Can one distinguish unambiguously between quantum coherent control and classical control? How does one elucidate mechanism? How can we learn from learning algorithms? Can one distinguish unambiguously between quantum coherent control and classical control? How does one elucidate mechanism? How can we learn from learning algorithms? Can one distinguish unambiguously between quantum coherent control and classical control? How does one elucidate mechanism? How can we learn from learning algorithms? Can one distinguish unambiguously between quantum coherent control and classical control?