Coherence and control of molecular dynamics in rare gas matrices

Bargheer, Matias; Borowski, Alexander; Cohen, Arik; Fushitani, Mizuho; Gerber, R. Benny; Gühr, Markus; Hamm, Peter; Ibrahim, Heide; Kiljunen, Toni; Korolkov, M. V.; Kühn, Oliver; Manz, J.; Schmidt, Burkhard; Schröder, M.; Schwentner, N.

doi:10.1007/978-3-540-68038-3_4

Cited by 12 publications

(14 citation statements)

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“…During the last few decades, the structure and dynamics of molecules, most notably hydrogen halides and dihalides, in rare-gas environments have been studied extensively [1][2][3]. These systems are often considered as simple models for condensed phase dynamics, where the 'solvation' can range from clusters of increasing size up to bulk liquid or crystals [3].…”

Section: Introductionmentioning

confidence: 99%

“…These systems are often considered as simple models for condensed phase dynamics, where the 'solvation' can range from clusters of increasing size up to bulk liquid or crystals [3]. In addition, owing to the simple electronic structure, molecules in rare gases are very suitable for theoretical modelling, particularly because simple pair potential or 'diatomics in molecules' models have often been found to be sufficiently accurate [4].…”

Section: Introductionmentioning

confidence: 99%

“…In addition, owing to the simple electronic structure, molecules in rare gases are very suitable for theoretical modelling, particularly because simple pair potential or 'diatomics in molecules' models have often been found to be sufficiently accurate [4]. Apart from the rotational and vibrational dynamics of the guest molecules [1], many studies on molecules in rare-gas hosts are concerned with light-induced electronic excitation and the subsequent dynamics of the photodissociation fragments [2,3]. Interesting topics include the cage effect [2,[5][6][7][8] and matrix-induced non-adiabatic electronic transitions [9,10], possibly leading to spin-flips [11][12][13][14] and/or to recombination of the fragments [15].…”

Section: Introductionmentioning

confidence: 99%

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RETRACTED ARTICLE: Quantum effects on translation and rotation of molecular chlorine in solid para-hydrogen

Accardi

Schmidt

2013

Molecular Physics

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Structure and quantum effects of a Cl 2 molecule embedded in fcc and hcp para-hydrogen (pH 2 ) crystals are investigated in the zero-temperature limit. The interaction is modelled in terms of Cl 2 -pH 2 and pH 2 -pH 2 pair potentials from ab initio CCSD(T) and MP2 calculations. Translational and rotational motions of the molecules are described within three-dimensional anharmonic Einstein and Devonshire models, respectively, where the crystals are either treated as rigid or allowed to relax. The pH 2 molecules, as well as the heavier Cl 2 molecule, show large translational zero-point energies (ZPEs) and undergo large-amplitude translational motions. This gives rise to substantial reductions in the cohesive energies and expansions of the lattices, in agreement with experimental results for pure hydrogen crystals. The rotational dynamics of the Cl 2 impurity is restricted to small-amplitude librations, again with high librational ZPEs, which are described in terms of two-dimensional non-degenerate anharmonic oscillators. The lattice relaxation causes qualitative changes of the rotational energy surfaces, which finally favour librations around the crystallographic directions pointing towards the nearest neighbours, both for fcc and hcp lattices. Implications on the reactant orientation in the experimentally observed laser-induced chemical reaction, Cl + H 2 → HCl + H, are discussed.

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Section: Introductionmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

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RETRACTED ARTICLE: Quantum effects on translation and rotation of molecular chlorine in solid para-hydrogen

Accardi

Schmidt

2013

Molecular Physics

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“…A more in-depth analysis of the quality of the G-MCTDH approximations and the discrepancies with the MCTDH results is provided by the comparison of the densities of Eq. (26), which are depicted in Fig. 6(b) for the bath degrees of freedom, as resulting from the G-MCTDH calculation III.…”

Section: A Autocorrelation Function Spectra and Dissipation Dynamicsmentioning

confidence: 99%

Quantum dynamics and spectroscopy of dihalogens in solid matrices. I. Efficient simulation of the photodynamics of the embedded I2Kr18 cluster using the G-MCTDH method

Picconi

Cina

Burghardt

2019

The Journal of Chemical Physics

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The molecular dynamics following the electronic B 3 Π u (0 + ) ←− X 1 Σ + g photoexcitation of the iodine molecule embedded in solid krypton are studied quantum mechanically using the Gaussian variant of the multiconfigurational time-dependent Hartree method (G-MCTDH). The accuracy of the Gaussian wave packet approximation is validated against numerically exact MCTDH simulations for a fully anharmonic seven-dimensional model of the I 2 Kr 18 cluster in a crystal Kr cage. The linear absorption spectrum, time-evolving vibrational probability densities, and I 2 energy expectation value are accurately reproduced by the numerically efficient G-MCTDH approach. The reduced density matrix of the chromophore is analyzed in the coordinate, Wigner and energy representations, so as to obtain a multifaceted dynamical view of the guest-host interactions. Vibrational coherences extending over the bond distance range 2.7Å < R I−I < 4.0Å are found to survive for several vibrational periods, despite extensive dissipation. The present results prepare the ground for the simulation of time-resolved coherent Raman spectroscopy of the I 2 -krypton system addressed in a companion paper.

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“…In a general context, doped rare gas clusters or solids have long been used as model systems. In particular, experimental and theoretical studies of dihalogens such as Cl 2 , Br 2 , I 2 , F 2 , or ClF in rare-gas matrices [17][18][19][20][21][22][23][24][25] have revealed many interesting effects, such as the coherent motion of the surrounding rare gas atoms upon photoexcitation of the dopant, 21,[27][28][29]48 and its dephasing, 26,27 or even ultrafast spin-flip transitions. 20,23,31 The group of Chergui has performed extended femtosecond pump-probe studies of NO in various rare gas matrices [33][34][35][36][37][38] and in para-H 2 , 39-44 which makes this system an ideal candidate to test the methodology to be presented.…”

Section: Introductionmentioning

confidence: 99%

Quantum dynamics of solid Ne upon photo-excitation of a NO impurity: A Gaussian wave packet approach

Unn-Toc

Uranga-Piña

Meier

et al. 2012

The Journal of Chemical Physics

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A high-dimensional quantum wave packet approach based on Gaussian wave packets in Cartesian coordinates is presented. In this method, the high-dimensional wave packet is expressed as a product of time-dependent complex Gaussian functions, which describe the motion of individual atoms. It is applied to the ultrafast geometrical rearrangement dynamics of NO doped cryogenic Ne matrices after femtosecond laser pulse excitation. The static deformation of the solid due to the impurity as well as the dynamical response after femtosecond excitation are analyzed and compared to reduced dimensionality studies. The advantages and limitations of this method are analyzed in the perspective of future applications to other quantum solids.

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Coherence and control of molecular dynamics in rare gas matrices

Cited by 12 publications

References 256 publications

RETRACTED ARTICLE: Quantum effects on translation and rotation of molecular chlorine in solid para-hydrogen

RETRACTED ARTICLE: Quantum effects on translation and rotation of molecular chlorine in solid para-hydrogen

Quantum dynamics and spectroscopy of dihalogens in solid matrices. I. Efficient simulation of the photodynamics of the embedded I2Kr18 cluster using the G-MCTDH method

Quantum dynamics of solid Ne upon photo-excitation of a NO impurity: A Gaussian wave packet approach

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