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Quantum coherence between electronic states of a photoionized molecule and the resulting process of ultrafast electron-hole migration have been put forward as a possible quantum mechanism of charge-directed reactivity governing the…

Conical intersections (CI) between molecular potential energy surfaces with non-vanishing non-adiabatic couplings generally occur in any molecule consisting of at least three atoms. They play a fundamental role in describing the molecular…

Using a combination of high-level ab initio electronic structure methods with efficient on-the-fly semiclassical evaluation of nuclear dynamics, we performed a massive scan of small polyatomic molecules searching for a long lasting…

Chemical Physics · Physics 2024-09-26 Alan Scheidegger , Jiří Vaníček , Nikolay V. Golubev

Short-in-time, broad-in-energy attosecond or few-femtosecond pulses can excite coherent superpositions of several electronic states in molecules. This results in ultrafast charge oscillations known as charge migration. A key open question…

Chemical Physics · Physics 2025-09-12 Lina Fransén , Sandra Gomez , Morgane Vacher

Electronic coherences can be leveraged to control molecular dynamics, but such control is limited by ultrafast decoherence driven by coupling between electronic excitations and molecular vibrations. With the goal of understanding and…

Chemical Physics · Physics 2025-05-27 Jiří Suchan , Benjamin G. Levine

The effect of nuclear dynamics and conical intersections on electronic coherences is investigated employing a two-state, two-mode linear vibronic coupling model. Exact quantum dynamical calculations are performed using the…

Chemical Physics · Physics 2018-08-22 Caroline Arnold , Oriol Vendrell , Ralph Welsch , Robin Santra

The rates and outcomes of virtually all photophysical and photochemical processes are determined by Conical Intersections. These are regions of degeneracy between electronic states on the nuclear landscape of molecules where electrons and…

Chemical Physics · Physics 2022-05-25 Daniel Keefer , Thomas Schnappinger , Regina de Vivie-Riedle , Shaul Mukamel

The development of attosecond technology has enabled the real-time observation of coherent electron motion in atoms, molecules and condensed phases. Experimentally, it is now possible to generate laser pulses of durations of only a few tens…

Chemical Physics · Physics 2017-05-18 David Ayuso

Due to the electron correlation, a fast removal of an electron from a molecule may create a coherent superposition of cationic states and in this way initiate pure electronic dynamics in which the hole-charge left by ionization migrates…

Chemical Physics · Physics 2023-04-03 J. Vester , V. Despré , A. I. Kuleff

Recently it was demonstrated that long-lived quantum coherence exists during excitation energy transport in photosynthesis. It is a valid question up to which length, time and mass scales quantum coherence may extend, how to one may detect…

Quantum Physics · Physics 2015-05-19 A. Vaziri , M. B. Plenio

The light-harvesting efficiency of a photoactive molecular complex is largely determined by the properties of its electronic quantum states. Those, in turn, are influenced by molecular vibrational states of the nuclear degrees of freedom.…

Biological Physics · Physics 2019-10-23 Hong-Guang Duan , Michael Thorwart , R. J. Dwayne Miller

Ultrafast laser excitation can trigger multiplex coherent dynamics in molecules. Here, we report attosecond transient absorption experiments addressing simultaneous probing of electronic and vibrational dynamics in a prototype molecule,…

Quantum states are described by wave functions whose phases cannot be directly measured, but which play a vital role in quantum effects such as interference and entanglement. The loss of the relative phase information, termed decoherence,…

Chemical Physics · Physics 2019-12-20 Jia Chen , Cong Hu , John F. Stanton , Stephen Hill , Hai-Ping Cheng , Xiao-Guang Zhang

Attosecond pulses can ionize atoms in a coherent process. Since the emerging fragments are entangled, however, each preserves only a fraction of the initial coherence, thus limiting the chance of guiding the ion subsequent evolution. In…

Atomic Physics · Physics 2021-06-30 Saad Mehmood , Eva Lindroth , Luca Argenti

Conical intersections between electronic states often dictate the chemistry of photoexcited molecules. Recently developed sources of ultrashort extreme ultraviolet (XUV) pulses tuned to element-specific transitions in molecules allow for…

Conical intersections (CoIn) dominate the pathways and outcomes of virtually all photophysical and photochemical molecular processes. Despite extensive experimental and theoretical effort, CoIns have not been directly observed yet and the…

Chemical Physics · Physics 2015-11-16 Markus Kowalewski , Kochise Bennett , Konstantin E. Dorfman , Shaul Mukamel

Exposing a molecule to intense light pulses may bring this molecule to a nonstationary quantum state, thus launching correlated dynamics of electronic and nuclear subsystems. Although much had been achieved in the understanding of…

Chemical Physics · Physics 2024-04-11 Nikolay V. Golubev , Jiří Vaníček

Photoionization using attosecond pulses can lead to the formation of coherent superpositions of the electronic states of the parent ion. However, ultrafast electron ejection triggers not only electronic but also nuclear dynamics---leading…

Chemical Physics · Physics 2017-03-29 Caroline Arnold , Oriol Vendrell , Robin Santra

We identify an intriguing feature of the electron-vibrational dynamics of molecular systems via a computational examination of \emph{trans}-polyacetylene oligomers. Here, via the vibronic interactions, the decay of an electron in the…

Quantum Physics · Physics 2013-04-09 Ignacio Franco , Angel Rubio , Paul Brumer

The direct observation of non-adiabatic dynamics at conical intersections is a long-standing goal of molecular physics. Novel time-resolved spectroscopies have been proposed which are sensitive to electronic coherences induced by the…

Chemical Physics · Physics 2020-11-16 Simon P. Neville , Albert Stolow , Michael S. Schuurman
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