Optical Control of Crossing the Conical Intersection in β-Carotene

Liu, Na; Zhang, Yifei; Niu, Kangwei; Lu, Faming; Zhong, Dongping

doi:10.1021/acs.jpclett.3c01932

Cited by 2 publications

(1 citation statement)

References 51 publications

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“…Moreover, anharmonic couplings between the eigenmodes were estimated. Spectroscopy-based methods to measure the vibronic coupling or interstate coupling in a diabatic framework between PESs of selected systems have been presented. , Optical control schemes to target segments in the CI seam with favorable topographies have been proposed, and the dynamics of β-carotene crossing a CI has already been modulated via the phase of the excitation pulse …”

Section: Introductionmentioning

confidence: 99%

A Local Diabatisation Method for Two-State Adiabatic Conical Intersections

Vandaele,

Mališ,

Luber

2024

J. Chem. Theory Comput.

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A methodology to locally characterize conical intersections (CIs) between two adiabatic electronic states for which no nonadiabatic coupling (NAC) vectors are available is presented. Based on the Hessian and gradient at the CI, the branching space coordinates are identified. The potential energy surface around the CI in the branching space is expressed in the diabatic representation, from which the NAC vectors can be calculated in a wave-function-free, energy-based approach. To demonstrate the universality of the developed methodology, the minimum-energy CI (MECI) between the first (S1) and second (S2) singlet excited states of formamide is investigated at the stateaveraged complete active space self-consistent field (SA-CASSCF) and extended multistate complete active space second-order perturbation theory (XMS-CASPT2) levels of theory. In addition, the asymmetrical MECI between the ground state (S0) and S1 of cyclopropanone is evaluated using SA-CASSCF, as well as (ME)CIs between the S1 and S2 states of benzene using SA-CASSCF and time-dependent density functional theory (TDDFT). Finally, a CI between the S1 and S2 excited states of thiophene was analyzed using TDDFT.

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Section: Introductionmentioning

confidence: 99%

A Local Diabatisation Method for Two-State Adiabatic Conical Intersections

Vandaele,

Mališ,

Luber

2024

J. Chem. Theory Comput.

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Optical Quantum Control of the Electron Transfer Reactions in Protein Flavodoxin

Liu,

Zhang,

Wang

et al. 2024

J. Phys. Chem. B

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The optical quantum control has been successfully applied in modulating biological processes such as energy transfer and bond isomerization. Among the reactions in realizing biological functions, the electron transfer (ET) process is fundamental; hence, the quantum control over such an ET reaction is of far-reaching significance. Here, we realized optical quantum control over ultrafast ET processes in a protein, flavodoxin, by applying various chirped excitation pulses. We observed the wavepacket dynamics within a dephasing time of less than 1 ps. Within this time window, we found that the ultrafast photoinduced ET reaction can be controlled by different chirped excitations with a rate change by a factor of about 2. Furthermore, the control effect is propagated into the subsequent ultrafast back ET reaction, showing a variation of the BET dynamics with different excitation chirps. The underlying mechanism is the initial wavepacket dynamics; the differently prepared wavepackets with chirped excitation evolve along various pathways, resulting in the changes of ET rates. The successful demonstration of optical quantum control of ultrafast biological ET is significant and opens a new avenue to explore the quantum control of real biological ET reactions.

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Optical Control of Crossing the Conical Intersection in β-Carotene

Cited by 2 publications

References 51 publications

A Local Diabatisation Method for Two-State Adiabatic Conical Intersections

A Local Diabatisation Method for Two-State Adiabatic Conical Intersections

Optical Quantum Control of the Electron Transfer Reactions in Protein Flavodoxin

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