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We present momentum resolved covariance measurements of entangled electronic-nuclear wave packets created and probed with octave spanning phaselocked ultrafast pulses. We launch vibrational wave packets on multiple electronic states via…

Quantum Physics · Physics 2023-11-20 Gonenc Mogol , Brian Kaufman , Chuan Cheng , Itzik Ben-Itzhak , Thomas Weinacht

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…

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 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

Free electrons provide a powerful tool to probe material properties at atomic-scale spatial resolution. Recent advances in ultrafast electron microscopy enable the manipulation of free electron wavefunctions using laser pulses. It would be…

Quantum Physics · Physics 2021-06-16 Ron Ruimy , Alexey Gorlach , Chen Mechel , Nicholas Rivera , Ido Kaminer

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

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…

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

We present various types of reduced models including five vibrational modes and three electronic states for the pyrazine molecule in order to investigate the lifetime of electronic coherence in a rigid and neutral system. Using an ultrafast…

Chemical Physics · Physics 2020-08-26 A. Csehi , P. Badankó , G. J. Halász , Á. Vibók , B. Lasorne

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

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 origin of the coherences in two-dimensional spectroscopy of photosynthetic complexes remains disputed. Recently it has been shown that in the ultrashort-pulse limit, oscillations in a frequency-integrated pump-probe signal correspond…

Quantum Physics · Physics 2015-06-22 Allan S. Johnson , Joel Yuen-Zhou , Alán Aspuru-Guzik , Jacob J. Krich

We study the conditions for coherent radiation of an electron bunch driven by a counterpropagating strong pulsed electromagnetic plane wave. We derive the spectrum of the coherent radiation and show that it is emitted backwards with respect…

Plasma Physics · Physics 2024-04-17 Evgeny Gelfer , Alexander Fedotov , Ondrej Klimo , Stefan Weber

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 behavior of a twisted electron colliding with a linearly polarized laser pulse is investigated within relativistic quantum mechanics. In order to better fit the real experimental conditions, we introduce a Gaussian spatial profile for…

Quantum Physics · Physics 2022-10-12 I. A. Aleksandrov , D. A. Tumakov , A. Kudlis , V. A. Zaytsev , N. N. Rosanov

Nonstationary molecular states which contain electronic coherences can be impulsively created and manipulated by using recently-developed ultrashort optical and X-ray pulses via photoexcitation, photoionization and Auger processes. We…

Chemical Physics · Physics 2015-09-02 Konstantin E. Dorfman , Kochise Bennett , Shaul Mukamel

Coherent control of ultrafast quantum phenomena benefits from pulse-shaping capabilities allowing to modulate the envelope and instantaneous phase of optical fields on femtosecond time scales. While such control is available for optical…

Optics · Physics 2026-02-05 Nelin Laštovičková Streshkova , Martin Kozák

We develop an ultrafast frequency-resolved Raman spectroscopy with entangled photons for polyatomic molecules in condensed phases, to probe the electronic and vibrational coherences. Using quantum correlation between the photons, the signal…

Quantum Physics · Physics 2021-06-23 Zhedong Zhang , Tao Peng , Xiaoyu Nie , Girish S. Agarwal , Marlan O. Scully

Here we experimentally map the dynamics of electron plasma waves in laser solid interaction. We do time resolved measurements of second harmonic and hard X-ray generation from interaction of intense ($10^{16} W cm^{-2}$, 100 fs, 800nm)…

Plasma Physics · Physics 2007-05-23 Arvinder S. Sandhu , G. Ravindra Kumar , S. Sengupta , A. Das , P. K. Kaw

We characterize both entanglement and quantum coherence in a molecular system by connecting the linear entropy of electronic-nuclear entanglement with Wigner-Yanase skew information measuring vibronic coherence and local quantum uncertainty…

Quantum Physics · Physics 2018-11-21 Mihaela Vatasescu
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