Attosecond molecular quantum dynamics; Matricization of the wave function; Schmidt rank; Singular value decomposition; Time-resolved electron-nuclei entanglement in molecules; Attosecond molecular quantum dynamic; Attoseconds; Quantum dynamics; Schmidt; Time evolutions; Time-resolved; Time-resolved electron-nucleus entanglement in molecule; Vibronics; Physics and Astronomy (all)
Abstract :
[en] Atto pulses allow controlling the charge migration and the spatio-temporal beating of the electronic density on a purely electronic time scale by tailoring the parameters of the pump pulse to excite specific electronic coherences. As the nuclei begin to move, the electronic and nuclear motions are entangled and the engineered electronic coherences can be usefully exploited for steering the vibronic density to specific products through the network of non adiabatic interactions. Three recent examples for which we demonstrate such a control by fully quantum dynamical computations are discussed. Two diatomic molecules, LiH and N2 excited by a 2 fs deep UV pulse and the ultrafast structural Jahn-Teller rearrangement in CH4+. The entanglement between electronic and nuclear degrees of freedom arises from the optical excitation and from non adiabatic coupling induced by the nuclear motion. We provide insight of the coherence control mechanism by analyzing the time evolution of the entanglement using a singular valued decomposition (SVD) of the matricized wave function.
Disciplines :
Chemistry
Author, co-author :
Blavier, Martin ; Université de Liège - ULiège > Molecular Systems (MolSys) ; Fritz Haber Research Center, Institute of Chemistry, The Hebrew University of Jerusalem, Jerusalem, Israel
Gelfand, Natalia; Fritz Haber Research Center, Institute of Chemistry, The Hebrew University of Jerusalem, Jerusalem, Israel
Levine, R.D.; Fritz Haber Research Center, Institute of Chemistry, The Hebrew University of Jerusalem, Jerusalem, Israel ; Department of Chemistry and Biochemistry, Department of Molecular and Medical Pharmacology, David Geffen School of Medicine, University of California, Los Angeles, United States
Remacle, Françoise ; Université de Liège - ULiège > Département de chimie (sciences) > Laboratoire de chimie physique théorique ; Fritz Haber Research Center, Institute of Chemistry, The Hebrew University of Jerusalem, Jerusalem, Israel
Language :
English
Title :
Controlling the Time Evolution of Electron-Nuclei Entanglement for Steering Vibronic Coherences Dynamics Induced by Short 1–2 fs Optical Pulses
Publication date :
2024
Event name :
Atto 2023
Event organizer :
Luca Argentini
Event place :
Orlando, Usa
Event date :
10-07-2023 => 15-07-2023
Audience :
International
Main work title :
Proceedings of the 8th International Conference on Attosecond Science and Technology
Editor :
Argenti, Luca
Chini, Michael
Fang, Li
Publisher :
Springer Science and Business Media Deutschland GmbH
ISBN/EAN :
978-3-03-147937-3
Pages :
83-100
Peer reviewed :
Peer reviewed
Tags :
CÉCI : Consortium des Équipements de Calcul Intensif
Nisoli, M., Decleva, P., Calegari, F., Palacios, A., Martín, F.: Attosecond electron dynamics in molecules. Chem. Rev. 117(16), 10760–10825 (2017)
Calegari, F., Ayuso, D., Trabattoni, A., Belshaw, L., De Camillis, S., Anumula, S., Frassetto, F., Poletto, L., Palacios, A., Decleva, P., Greenwood, J.B., Martín, F., Nisoli, M.: Ultrafast electron dynamics in phenylalanine initiated by attosecond pulses. Science. 346(6207), 336–339 (2014)
Perfetto, E., Trabattoni, A., Calegari, F., Nisoli, M., Marini, A., Stefanucci, G.: Ultrafast quantum interference in the charge migration of tryptophan. J. Phys. Chem. Lett. 11, 891–899 (2020)
Despré, V., Marciniak, A., Loriot, V., Galbraith, M.C.E., Rouzée, A., Vrakking, M.J.J., Lépine, F., Kuleff, A.I.: Attosecond hole migration in benzene molecules surviving nuclear motion. J. Phys. Chem. Lett. 6(3), 426–431 (2015)
Kling, M.F., Siedschlag, C., Verhoef, A.J., Khan, J.I., Schultze, M., Uphues, T., Ni, Y., Uiberacker, M., Drescher, M., Krausz, F., Vrakking, M.J.J.: Control of electron localization in molecular dissociation. Science. 312(5771), 246–248 (2006)
Kraus, P.M., Mignolet, B., Baykusheva, D., Rupenyan, A., Horný, L., Penka, E.F., Grassi, G., Tolstikhin, O.I., Schneider, J., Jensen, F., Madsen, L.B., Bandrauk, A.D., Remacle, F., Wörner, H.J.: Measurement and laser control of attosecond charge migration in ionized iodoacetylene. Science. 350(6262), 790–795 (2015)
Matselyukh, D.T., Despré, V., Golubev, N.V., Kuleff, A.I., Wörner, H.J.: Decoherence and revival in attosecond charge migration driven by non-adiabatic dynamics. Nat. Phys. 18, 1206– 1213 (2022)
Baldini, E., Palmieri, T., Pomarico, E., Auböck, G., Chergui, M.: Clocking the ultrafast electron cooling in Anatase titanium dioxide nanoparticles. ACS Photo. 5(4), 1241–1249 (2018)
Borrego-Varillas, R., Lucchini, M., Nisoli, M.: Attosecond spectroscopy for the investigation of ultrafast dynamics in atomic, molecular and solid-state physics. Rep. Prog. Phys. 85(6), 066401 (2022)
Lucchini, M., Sato, S.A., Lucarelli, G.D., Moio, B., Inzani, G., Borrego-Varillas, R., Frassetto, F., Poletto, L., Hübener, H., De Giovannini, U., Rubio, A., Nisoli, M.: Unravelling the intertwined atomic and bulk nature of localised excitons by attosecond spectroscopy. Nat. Commun. 12(1), 1021 (2021)
Mignolet, B., Levine, R.D., Remacle, F.: Charge migration in the bifunctional PENNA cation induced and probed by ultrafast ionization: a dynamical study. J. Phys. B Atomic Mol. Phys. 47(12), 124011 (2014)
Remacle, F., Nest, M., Levine, R.D.: Laser steered ultrafast quantum dynamics of electrons in LiH. Phys. Rev. Lett. 99(18), 183902 (2007)
Remacle, F., Levine, R.D.: An electronic time scale in chemistry. Proc. Natl. Acad. Sci. U. S. A. 103(18), 6793–6798 (2006)
Valentini, A., van den Wildenberg, S., Remacle, F.: Selective bond formation triggered by short optical pulses: quantum dynamics of a four-center ring closure. Phys. Chem. Chem. Phys. 22(39), 22302–22313 (2020)
Nikodem, A., Levine, R.D., Remacle, F.: Spatial and temporal control of populations, branching ratios, and electronic coherences in LiH by a single one-cycle infrared pulse. Phys. Rev. A. 95(5), 053404 (2017)
Muskatel, B.H., Remacle, F., Levine, R.D.: AttoPhotoChemistry: probing ultrafast electron dynamics by the induced nuclear motion: the prompt and delayed predissociation of N2. Chem. Phys. Lett. 601(0), 45–48 (2014)
Ekert, A., Knight, P.L.: Entangled quantum systems and the Schmidt decomposition. Am. J. Phys. 63(5), 415–423 (1995)
Horodecki, R., Horodecki, P., Horodecki, M., Horodecki, K.: Quantum entanglement. Rev. Mod. Phys. 81(2), 865–942 (2009)
Nielsen, M.A., Chuang, I.L.: Quantum Computation and Quantum Information. Cambridge University Press, Cambridge (2010)
Sanz-Vicario, J.L., Pérez-Torres, J.F., Moreno-Polo, G.: Electronic-nuclear entanglement in ${{\mathrm{H}}_{2}}ˆ{+}$: schmidt decomposition of non-born-oppenheimer wave functions expanded in nonorthogonal basis sets. Phys. Rev. A. 96(2), 022503 (2017)
McKemmish, L.K., McKenzie, R.H., Hush, N.S., Reimers, J.R.: Quantum entanglement between electronic and vibrational degrees of freedom in molecules. J. Chem. Phys. 135(24), 244110 (2011)
Haxton, D.J., Lawler, K.V., McCurdy, C.W.: Multiconfiguration time-dependent Hartree-Fock treatment of electronic and nuclear dynamics in diatomic molecules. Phys. Rev. A. 83(6), 063416 (2011)
Haxton, D.J., Lawler, K.V., McCurdy, C.W.: Qualitative failure of a multiconfiguration method in prolate spheroidal coordinates in calculating dissociative photoionization of ${\mathrm{H}}_{2}{}ˆ{+}$. Phys. Rev. A. 91(6), 062502 (2015)
Vatasescu, M.: Entanglement between electronic and vibrational degrees of freedom in a laserdriven molecular system. Phys. Rev. A. 88(6), 063415 (2013)
Izmaylov, A.F., Franco, I.: Entanglement in the born–oppenheimer approximation. J. Chem. Theory Comput. 13(1), 20–28 (2017)
Hou, X.-W., Chen, J.-H., Ma, Z.-Q.: Dynamical entanglement of vibrations in an algebraic model. Phys. Rev. A. 74(6), 062513 (2006)
Li, J., Kais, S.: Entanglement classifier in chemical reactions. Sci. Adv. 5(8), eaax5283 (2019)
Li, J., Sajjan, M., Kale, S.S., Kais, S.: Statistical correlation between quantum entanglement and spin–orbit coupling in crossed beam molecular dynamics. Adv. Quant. Technol. 4, 2100098 (2021)
Vrakking, M.J.J.: Control of attosecond entanglement and coherence. Phys. Rev. Lett. 126(11), 113203 (2021)
Koll, L.-M., Maikowski, L., Drescher, L., Witting, T., Vrakking, M.J.J.: Experimental control of quantum-mechanical entanglement in an attosecond pump-probe experiment. Phys. Rev. Lett. 128(4), 043201 (2022)
Busto, D., Laurell, H., Finkelstein-Shapiro, D., Alexandridi, C., Isinger, M., Nandi, S., Squibb, R.J., Turconi, M., Zhong, S., Arnold, C.L., Feifel, R., Gisselbrecht, M., Salières, P., Pullerits, T., Martín, F., Argenti, L., L’Huillier, A.: Probing electronic decoherence with high-resolution attosecond photoelectron interferometry. Eur. Phys. J. D. 76(7), 112 (2022)
Blavier, M., Levine, R.D., Remacle, F.: Time evolution of entanglement of electrons and nuclei and partial traces in ultrafast photochemistry. Phys. Chem. Chem. Phys. 24(29), 17516–17525 (2022)
Blavier, M., Gelfand, N., Levine, R.D., Remacle, F.: Entanglement of electrons and nuclei: amost compact representation of the molecular wave function. Chem. Phys. Lett. 804, 139885 (2022)
Bradley, T.-D., Stoudenmire, E.M., Terilla, J.: Modeling sequences with quantum states: a look under the hood. Mach. Learn.: Sci. Technol. 1(3), 035008 (2020)
Blavier, M., Komarova, K., Gonçalves, C.E.M., Levine, R.D., Remacle, F.: Electronic coherences steer the strong isotope effect in the ultrafast Jahn–teller structural rearrangement of methane cation upon tunnel ionization. J. Phys. Chem. A. 125(43), 9495–9507 (2021)
van den Wildenberg, S., Mignolet, B., Levine, R.D., Remacle, F.: Temporal and spatially resolved imaging of the correlated nuclear-electronic dynamics and of the ionized photoelectron in a coherently electronically highly excited vibrating LiH molecule. J. Chem. Phys. 151(13), 134310 (2019)
Ajay, J.S., Komarova, K.G., Remacle, F., Levine, R.D.: Time-dependent view of an isotope effect in electron-nuclear nonequilibrium dynamics with applications to N2. Proc. Natl. Acad. Sci. U. S. A. 115, 5890–5895 (2018)
Golub, G.H., Reinsch, C.: Singular value decomposition and least squares solutions. In: Wilkinson, J.H., Reinsch, C., Bauer, F.L. (eds.) Linear Algebra, pp. 134–151. Springer, Berlin/Heidelberg (1971)
Baker, S., Robinson, J.S., Haworth, C.A., Teng, H., Smith, R.A., Chirilă, C.C., Lein, M., Tisch, J.W.G., Marangos, J.P.: Probing proton dynamics in molecules on an attosecond time scale. Science. 312(5772), 424–427 (2006)
Marangos, J.P., Baker, S., Kajumba, N., Robinson, J.S., Tisch, J.W.G., Torres, R.: Dynamic imaging of molecules using high order harmonic generation. Phys. Chem. Chem. Phys. 10(1), 35–48 (2008)
Mondal, T., Varandas, A.J.C.: The Jahn-teller effect in the triply degenerate electronic state of methane radical cation. J. Chem. Phys. 135(17), 174304 (2011)
Mondal, T., Varandas, A.J.C.: On extracting subfemtosecond data from femtosecond quantum dynamics calculations: the methane cation. J. Chem. Theory Comput. 10(9), 3606–3616 (2014)
Mondal, T., Varandas, A.J.C.: Structural evolution of the methane cation in subfemtosecond photodynamics. J. Chem. Phys. 143(1), 014304 (2015)
Gonçalves, C.E.M., Levine, R.D., Remacle, F.: Ultrafast geometrical reorganization of a methane cation upon sudden ionization: an isotope effect on electronic non-equilibrium quantum dynamics. Phys. Chem. Chem. Phys. 23(21), 12051–12059 (2021)
Zhang, T., Golub, G.H.: Rank-one approximation to high order tensors. Siam J. Matrix Anal. Appl. 23(2), 534–550 (2001)
Baiardi, A., Reiher, M.: Large-scale quantum dynamics with matrix product states. J. Chem. Theory Comput. 15(6), 3481–3498 (2019)
Larsson, H.R., Zhai, H., Gunst, K., Chan, G.K.-L.: Matrix product states with large sites. J. Chem. Theory Comput. 18(2), 749–762 (2022)
Schollwöck, U.: The density-matrix renormalization group in the age of matrix product states. Ann. Phys. 326(1), 96–192 (2011)
