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Light-induced nonadiabatic effects can arise from the interaction of a molecule with the quantized electromagnetic field of a Fabry--P\'erot or plasmonic nanocavity. In this context, the quantized radiation field mixes the vibrational,…

Atomic and Molecular Clusters · Physics 2025-03-17 Krisztián Szabó , Csaba Fábri , Gábor J. Halász , Ágnes Vibók

Imaging in real time the complete dynamics of a process as fundamental as photoemission has long been out of reach due to the difficulty of combining attosecond temporal resolution with fine spectral and angular resolutions. Here, we…

Collective optical excitations, such as localized surface plasmons in metallic nanoparticles and Mie resonances in high-index dielectrics, play a central role in nanoscale light--matter interactions. When such optical modes interact with…

Molecular adsorbates on metal surfaces exchange energy with substrate phonons and low-lying electron-hole pair excitations. In the limit of weak coupling, electron-hole pair excitations can be seen as exerting frictional forces on…

Materials Science · Physics 2016-09-28 Reinhard J. Maurer , Mikhail Askerka , Victor S. Batista , John C. Tully

We demonstrate coherent control of motional dynamics in trapped Rydberg ions engineered to exhibit a conical intersection between adiabatic potential-energy surfaces. Using quantum optimal control, an optimally shaped electric field drives…

Quantum Physics · Physics 2025-09-16 Abdessamad Belfakir , Yousra Bouasria , Herschel Rabitz , Ahmed Ratnani

Geometric phases play a crucial role in diverse fields. In chemistry they appear when a reaction path encircles an intersection between adiabatic potential energy surfaces and the molecular wavefunction experiences quantum-mechanical…

Quantum Physics · Physics 2024-02-05 Rocco Martinazzo , Irene Burghardt

Ultrafast wavepacket dynamics of electron-phonon-photon systems is studied by numerical calculations. When nonadiabaticity of electron-phonon systems is taken into account, Raman scattering process plays an important role in the dynamics of…

Mesoscale and Nanoscale Physics · Physics 2019-06-26 Kunio Ishida

Attochemistry aims to exploit the properties of coherent electronic wavepackets excited via attosecond pulses, to control the formation of photoproducts. Such molecular processes can in principle be simulated with various nonadiabatic…

Chemical Physics · Physics 2024-05-28 Thierry Tran , Anthony Ferté , Morgane Vacher

In this paper, we investigate coherent control of nonadiabatic dynamics at a conical intersection (CI) using engineered ultrafast laser pulses. Within a model vibronic system, we tailor pulse chirp and temporal profile and compute the…

Nonadiabatic molecular dynamics simulations aim to describe the coupled electron-nuclear dynamics of molecules in excited electronic states. These simulations have been applied to understand a plethora of photochemical and photophysical…

Modern X-ray spectroscopy has proven itself as a robust tool for probing the electronic structure of atoms in complex environments. Despite working on energy scales that are much larger than those corresponding to nuclear motions, taking…

Chemical Physics · Physics 2017-06-28 Sven Karsten , Sergey I. Bokarev , Saadullah G. Aziz , Sergei D. Ivanov , Oliver Kühn

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

The basic properties of atoms, molecules and solids are governed by electron dynamics which take place on extremely short time scales. To measure and control these dynamics therefore requires ultrafast sources of radiation combined with…

Atomic Physics · Physics 2008-02-27 J. Mauritsson , P. Johnsson , E. Gustafsson , M. Swoboda , T. Ruchon , A. LHuillier , K. J. Schafer

We describe an experiment to measure the emitted real-time electric field from an ultrafast third-order nonlinear optical interaction in molecules, using a phase-tracked spectral interferometry scheme. By combining a software lock-in…

Optics · Physics 2025-03-11 Siddhant Pandey , Francis Walz , Niranjan Shivaram

The coherent interaction with ultrashort light pulses is a powerful strategy for monitoring and controlling the dynamics of wave packets in all states of matter. As light presents an oscillation period of a few femtoseconds ($T=2.6$~fs in…

The attosecond ultrafast ionization dynamics of correlated two- or many-electron systems have, so far, been mainly addressed investigating atomic systems. In the case of single ionization, it is well known that electron-electron correlation…

We introduce and demonstrate a new approach to measuring coherent electron wave packets using high-harmonic spectroscopy. By preparing a molecule in a coherent superposition of electronic states, we show that electronic coherence opens…

Chemical Physics · Physics 2014-07-09 P. M. Kraus , S. B. Zhang , A. Gijsbertsen , R. R. Lucchese , N. Rohringer , H. J. Wörner

Coherent light pulses of few to hundreds of femtoseconds (fs) duration have prolifically served the field of ultrafast phenomena. While fs pulses address mainly dynamics of nuclear motion in molecules or lattices in the gas, liquid or…

Chemical Physics · Physics 2013-04-26 P. A. Carpeggiani , P. Tzallas , A. Palacios , D. Gray , F. Martín , D. Charalambidis

Isotopic substitution in molecular systems can affect fundamental molecular properties including the energy position and spacing of electronic, vibrational and rotational levels, thus modifying the dynamics associated to their coherent…

Nonadiabatic effects are ubiquitous in physics, chemistry and biology. They are strongly amplified by conical intersections (CIs) which are degeneracies between electronic states of triatomic or larger molecules. A few years ago it has been…

Atomic and Molecular Clusters · Physics 2014-11-25 Gábor J. Halász , Ágnes Vibók , Lorenz S. Cederbaum