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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

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

Electronic coherences are key to understanding and controlling photo-induced molecular transformations. We identify a crucial quantum-mechanical feature of electron-nuclear correlation, the projected nuclear quantum momenta, essential to…

Chemical Physics · Physics 2024-11-13 Evaristo Villaseco Arribas , Neepa T. Maitra

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

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

Electronic coherence is of utmost importance for the access and control of quantum-mechanical solid-state properties. Using a purely electronic observable, the photocurrent, we measure an electronic coherence time of 22 +/- 4 fs in…

Mesoscale and Nanoscale Physics · Physics 2021-12-08 Christian Heide , Timo Eckstein , Tobias Boolakee , Constanze Gerner , Heiko B. Weber , Ignacio Franco , Peter Hommelhoff

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

We analyze electronically excited nuclear wave functions and their coherence when subjecting a molecule to the action of natural, pulsed incoherent solar-like light, and to that of ultrashort coherent light assumed to have the same center…

Quantum Physics · Physics 2015-06-12 Alex C. Han , Moshe Shapiro , Paul Brumer

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 existence of electronic coherence can fundamentally change the scenario of nonlinear interaction of light with quantum systems such as atoms and molecules, which, however, has escaped from observation in the investigations of strong…

The coupling of electronic and nuclear motion in polyatomic molecules is at the heart of attochemistry. The molecular properties, transient structures and reaction mechanism of these many-body quantum objects are defined on the level of…

Chemical Physics · Physics 2024-03-12 David Schwickert , Andreas Przystawik , Dian Diaman , Detlef Kip , Jon P. Marangos , Tim Laarmann

Accessing coherences is key to fully understand and control ultrafast dynamics of complex quantum systems like molecules. Most photochemical processes are mediated by conical intersections (CIs), which generate coherences between electronic…

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

Minimizing decoherence due to coupling of a quantum system to its fluctuating environment is at the forefront of quantum information science and photonics research. Nature sets the ultimate limit, however, given by the strength of the…

Mesoscale and Nanoscale Physics · Physics 2016-01-27 Galan Moody , Corey McDonald , Ari Feldman , Todd Harvey , Richard P. Mirin , Kevin L. Silverman

A remarkable amount of theoretical research has been carried out to elucidate the physical origins of the recently observed long-lived quantum coherence in the electronic energy transfer process in biological photosynthetic systems.…

Quantum Physics · Physics 2015-03-19 Sangwoo Shim , Patrick Rebentrost , Stéphanie Valleau , Alan Aspuru-Guzik

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

When an atom or molecule absorbs a high-energy photon, an electron is emitted with a well-defined energy and a highly-symmetric angular distribution, ruled by energy quantization and parity conservation. These rules seemingly break down…

We discuss the various manifestations of quantum decoherence in the forms of dephasing, entanglement with the environment, and revelation of "which-path" information. As a specific example, we consider an electron interference experiment.…

Quantum Physics · Physics 2015-05-13 Jen-Tsung Hsiang , L. H. Ford

Tracking the coupled motion of electrons and nuclei on their intrinsic timescales is essential to understanding and controlling photochemical transformations. While attosecond techniques have provided unprecedented insight into electronic…

Quantum mechanical phenomena, such as electronic coherence and entanglement, play a key role in achieving the unrivalled efficiencies of light-energy conversion in natural photosynthetic light-harvesting complexes, and triggered the growing…

Quantum Physics · Physics 2011-02-02 Richard Hildner , Daan Brinks , Niek F. van Hulst
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