Infrared laser driven double proton transfer. An optimal control theory study

Abdel-Latif, Mahmoud K.; Kühn, Oliver

doi:10.1016/j.chemphys.2009.12.021

Cited by 11 publications

(14 citation statements)

References 30 publications

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“…Another study was carried out for infrared laser-driven double proton transfer (DPT) by a 2D model (Abdel-Latif and Kühn, 2010) using the stepwise and concerted transfer pathways. It was concluded that the driven wave packet is dependent on the parameters of the model Hamiltonian and the propagation time.…”

Section: Proton Transfer In Nucleobasesmentioning

confidence: 99%

The Role of Proton Transfer on Mutations

Srivastava

2019

Front. Chem.

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Hydrogen bonds play a critical role in nucleobase studies as they encode genes, map protein structures, provide stability to the base pairs, and are involved in spontaneous and induced mutations. Proton transfer mechanism is a critical phenomenon that is related to the acid–base characteristics of the nucleobases in Watson–Crick base pairs. The energetic and dynamical behavior of the proton can be depicted from these characteristics and their adjustment to the water molecules or the surrounding ions. Further, new pathways open up in which protonated nucleobases are generated by proton transfer from the ionized water molecules and elimination of a hydroxyl radical in this review, the analysis will be focused on understanding the mechanism of untargeted mutations in canonical, wobble, Hoogsteen pairs, and mutagenic tautomers through the non-covalent interactions. Further, rare tautomer formation through the single proton transfer (SPT) and the double proton transfer (DPT), quantum tunneling in nucleobases, radiation-induced bystander effects, role of water in proton transfer (PT) reactions, PT in anticancer drugs–DNA interaction, displacement and oriental polarization, possible models for mutations in DNA, genome instability, and role of proton transfer using kinetic parameters for RNA will be discussed.

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Section: Proton Transfer In Nucleobasesmentioning

confidence: 99%

The Role of Proton Transfer on Mutations

Srivastava

2019

Front. Chem.

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“…Furthermore, it is seen that the probability density has a higher weight in that part of the potential where x a < 0, implying that there is a preference for the Cis1 minimum to be visited during the dynamics. According to our previous study [22] this is due to the higher stability of Cis1 as compared with Cis2. Finally, we note that there are several states in the region of the chosen intermediate state ϕ 4 , thus state selective population will be more easily achieved using long pulses as compared, e.g., with the NH-vibrational stretching frequency.…”

Section: Laser Control Of Dpt In the Electronic Ground Statementioning

confidence: 79%

“…The chosen above-barrier transition state involves an excitation of the asymmetric stretching coordinate x a which triggers the reaction to occur mostly along the stepwise pathway (see also Ref. [22]). Furthermore, it is seen that the probability density has a higher weight in that part of the potential where x a < 0, implying that there is a preference for the Cis1 minimum to be visited during the dynamics.…”

Section: Laser Control Of Dpt In the Electronic Ground Statementioning

confidence: 99%

“…The aim of the present contribution is to extend the model study of Ref. [22] towards a specific molecular system and to show exemplarily to what extent laser-triggered DPT can influence the Förster transfer coupling. Specifically, we will focus on porphycene like structures, which have rather strong hydrogen bonds (HBs) whose properties are widely adjustable by the structural design [24].…”

Section: Introductionmentioning

confidence: 99%

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Laser control of double proton transfer in porphycenes: towards an ultrafast switch for photonic molecular wires

Abdel-Latif

Kühn

2010

Theor Chem Acc

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Electronic excitation energy transfer along a molecular wire depends on the relative orientation of the electronic transition dipole moments of neighboring chromophores. In porphycenes this orientation is changed upon double proton transfer in the electronic ground state. We explore the possibility to trigger such a double proton transfer reaction by means of an infrared pump-dump laser control scheme. To this end a quantum chemical characterization of an asymmetrically substituted porphycene is performed using density functional theory. Ground state geometries, the topology of the potential energy surface for double proton transfer, and S 0 →S 1 transition energies are compared with the parent compound porphycene and a symmetric derivative. Employing a simple two-dimensional model for the double proton transfer, which incorporates sequential and concerted motions, quantum dynamics simulations of the laser driven dynamics are performed which demonstrate tautomerization control. Based on the orientation of the transition dipole moments this tautomerization may lead to an estimated change in the Förster transfer coupling of about 60%.

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“…II, is a generalization of the Hamiltonian previously handled by instanton techniques, 10 which was restricted to dipole coupling. In its previous version, it has been applied by us 10 and others [11][12][13] to a number of such double-proton transfer processes with various arrangements of the two hydrogen bonds. Investigations of alternative 2D Hamiltonians with more than one transition state have been reported in the literature, [14][15][16] but these were limited to potentials with only one set of minima and thus without a stable intermediate; moreover, they do not (generally) decompose into two 1D Hamiltonians and a coupling, and thus fail to meet the fundamental assumption formulated above, expected to be required for application to a pair of weakly coupled hydrogen bonds.…”

Section: And References Therein)mentioning

confidence: 99%

Entanglement and co-tunneling of two equivalent protons in hydrogen bond pairs

Smedarchina

Siebrand

Fernández‐Ramos

2017

The Journal of Chemical Physics

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A theoretical study is reported of a system of two identical symmetric hydrogen bonds, weakly coupled such that the two mobile protons can move either separately (stepwise) or together (concerted). It is modeled by two equivalent quartic potentials interacting through dipolar and quadrupolar coupling terms. The tunneling Hamiltonian has two imaginary modes (reaction coordinates) and a potential with a single maximum that may turn into a saddle-point of second order and two sets of (inequivalent) minima. Diagonalization is achieved via a modified Jacobi-Davidson algorithm. From this Hamiltonian the mechanism of proton transfer is derived. To find out whether the two protons move stepwise or concerted, a new tool is introduced, based on the distribution of the probability flux in the dividing plane of the transfer mode. While stepwise transfer dominates for very weak coupling, it is found that concerted transfer (co-tunneling) always occurs, even when the coupling vanishes since the symmetry of the Hamiltonian imposes permanent entanglement on the motions of the two protons. We quantify this entanglement and show that, for a wide range of parameters of interest, the lowest pair of states of the Hamiltonian represents a perfect example of highly entangled quantum states in continuous variables. The method is applied to the molecule porphycene for which the observed tunneling splitting is calculated in satisfactory agreement with experiment, and the mechanism of double-proton tunneling is found to be predominantly concerted. We show that, under normal conditions, when they are in the ground state, the two porphycene protons are highly entangled, which may have interesting applications. The treatment also identifies the conditions under which such a system can be handled by conventional one-instanton techniques.

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Infrared laser driven double proton transfer. An optimal control theory study

Cited by 11 publications

References 30 publications

The Role of Proton Transfer on Mutations

The Role of Proton Transfer on Mutations

Laser control of double proton transfer in porphycenes: towards an ultrafast switch for photonic molecular wires

Entanglement and co-tunneling of two equivalent protons in hydrogen bond pairs

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