Laser control over the ultrafast Coulomb explosion of 
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 after Auger decay: A quantum-dynamics investigation

Hanna, Athiya Mahmud; Vendrell, Oriol; Ourmazd, A.; Santra, Robin

doi:10.1103/physreva.95.043419

Cited by 12 publications

(54 citation statements)

References 43 publications

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“…In a recent quantum dynamics (QD) [20] investigation, the interaction of the IR pulse with the dicationic system * Corresponding author: murali.krishna@cfel.de as a function of time delay of the IR pulse has been investigated using the multiconfiguration time-dependent Hartree (MCTDH) [21][22][23] method and similar trends as in the experiment have been observed [20]. Additionally, the dependence of unfragmented N 2 2+ on intensity and width of the IR pulse was investigated.…”

Section: Introductionmentioning

confidence: 73%

“…Please note that the harmonic approximation is employed in this work for sampling the ground vibrational state of N 2 . The average energy of the initial trajectories is thus E = 1 2h ω = 0.14 eV, which is larger than the exact energy expectation value of 0.12 eV [20], the energy of the wave packet employed in the quantum dynamics calculations [20].…”

Section: B Initial Conditions Photoionization and Auger Decaymentioning

confidence: 80%

“…II, the basic expressions underlying the theory and the computational methods used in this work are presented. Section III discusses the Auger spectrum and unfragmented-N 2 2+ yield, in a quasidiabatic representation from FSSH simulations, and compares to previous QD simulations [20]. Section IV gives a detailed discussion of the fragmentation dynamics in the adiabatic representation in comparison to the dynamics in the quasidiabatic representation and discusses the impact of nonadiabatic couplings.…”

Section: Introductionmentioning

confidence: 93%

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Infrared-laser-pulse-enhanced ultrafast fragmentation of N22+ following Auger decay: Mixed quantum-classical simulations

2018

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We employ mixed quantum-classical molecular dynamics simulations to investigate the fragmentation of N 2 molecules after core-level photoionization by an x-ray laser, subsequent Auger decay, and followed by a femtosecond IR pulse that interacts with N 2 2+. The delayed IR pulse couples the dissociative electronic states of N 2 2+ with electronic states that can support long-lived vibrational resonances. We compare our simulations with previous quantum dynamics calculations in a quasidiabatic representation, which employed a small number of electronic states. Good agreement for both the Auger spectrum as well as the influence of the delayed IR pulse is found. By employing the mixed quantum-classical treatment, we can greatly reduce the computational cost to simulate the fragmentation dynamics compared to the quantum dynamics simulations. Furthermore, we reinvestigate the title process by employing an extended set of adiabatic potential energy surfaces and also investigate the role of nonadiabatic coupling in the process. The use of the full set of adiabatic potentials increases the dissociation probability and changes the details of the interaction with the IR pulse, but no effect due to the nonadiabatic coupling is found.

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Section: Introductionmentioning

confidence: 73%

Section: B Initial Conditions Photoionization and Auger Decaymentioning

confidence: 80%

Section: Introductionmentioning

confidence: 93%

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Infrared-laser-pulse-enhanced ultrafast fragmentation of N22+ following Auger decay: Mixed quantum-classical simulations

2018

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“…[9,10,11,12,13,14,15]. Even optical laser control Email address: christian.buth@web.de (Christian Buth) URL: http://www.christianbuth.name (Christian Buth) of the dissociation of N 2+ 2 can be realized [16,17]. When emitted photons and electrons are not considered, an open quantum-system approach based on a master equation in Lindblad form [18,19,20,21,22,23] needs to be employed.…”

Section: Introductionmentioning

confidence: 99%

Dissociating diatomic molecules in ultrafast and intense light

Buth

2019

Chemical Physics

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An ab initio theory is devised for the quantum dynamics of molecules undergoing (multiple) ionization in ultrafast and intense light. Specifically, the intertwined problem of photoionization, radiative, and electronic transitions in the course of dissociation is addressed which arises, e.g., when molecules are exposed to xuv light or x rays from free electron lasers or attosecond light sources, but the approach is equally useful in optical strong-field physics. The coherent interaction of the molecule with the light in a specific charge state is also treated. I set out from an abstract formulation in terms of the quantum optical notion of system-reservoir interaction using a master equation in Lindblad form and analyze its short-time approximation. First, I express it in a direct sum rigged Hilbert space for an efficient solution with numerical methods for systems of differential equations. Second, I derive a treatment via quantum Monte Carlo wave packet (MCWP) propagation. The formalism is concretized to diatomic molecules in Born-Oppenheimer approximation whereby molecular rotation is disregarded. The numerical integration of the master equation is carried out with a suitably factored density matrix that exploits the locality of the Hamiltonian and the Lindblad superoperator with respect to the internuclear distance. The formulation of the MCWP for molecules requires a thorough analysis of the quantum jump process; namely, the dependence on the continuous distance renders a straight wave packet promotion useless and, instead, a projected outer product needs to be employed involving an integrated quantum jump operator.

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“…One of the most successful strategies to track electron dynamics to date uses a pump-probe setup combining an attosecond x-ray or XUV pulse to excite or ionize the system, followed by a femtosecond IR probe to retrieve an image of electronic processes in time or to drive the reaction [8,9]. Recent experiments at the Linac Coherent Light Source FEL have demonstrated coherent control over the ultrafast Coulomb explosion of N 2 2+ using x-ray and IR pulses [10]. Similar experiments combining x-rays with optical-frequency pulses were also successfully performed to explore ultrafast dynamics in more complex molecular targets [11,12].…”

Section: Introductionmentioning

confidence: 99%

A pump–probe scheme with a single chirped pulse to image electron and nuclear dynamics in molecules

et al. 2018

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A single chirped few-femtosecond pulse can be used to control and image coupled electron-nuclear dynamics. Using full ab initio simulations of the simplest molecule, H , 2 + as a prototype target, we show that for intermediate values of the chirp, interference between sequential and direct contributions enables significant control over ionization yields, even when taking into account the effective decoherence introduced by nuclear motion and the presence of an electronic continuum. For larger values of the chirp, the single chirped pulse reproduces a classical pump-probe setup, with the chirp parameter mapping an effective time delay between the pumping and probing frequencies of the pulse. After demonstrating this numerically, we present a full analytical solution for the two-photon ionization amplitudes that provides an intuitive analogy between the molecular dynamics induced by a single chirped pulse and a traditional pump-probe setup.

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Laser control over the ultrafast Coulomb explosion of N22+ after Auger decay: A quantum-dynamics investigation

Cited by 12 publications

References 43 publications

Infrared-laser-pulse-enhanced ultrafast fragmentation of N22+ following Auger decay: Mixed quantum-classical simulations

Infrared-laser-pulse-enhanced ultrafast fragmentation of N22+ following Auger decay: Mixed quantum-classical simulations

Dissociating diatomic molecules in ultrafast and intense light

A pump–probe scheme with a single chirped pulse to image electron and nuclear dynamics in molecules

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