Charge migration and attosecond solitons in conjugated organic molecules

Mauger, F.; S., Folorunso, Aderonke; Hamer, Kyle; Chandre, Cristel; Gaarde, Mette B.; Lopata, Kenneth A.; Schafer, Kenneth J.

doi:10.1103/physrevresearch.4.013073

Cited by 23 publications

(23 citation statements)

References 46 publications

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“…[50]. An appealing application for ME-WFAT may come to the study of particle-like charge migration [9,10,35] where it is shown that an initial localized hole can sustain its locality throughout the periodic dynamics. Given the coupled time-space sensitivity of such a dynamic, IR ME-WFAT opens up a promising avenue in the modeling of tunnel ionization as a probe of charge migration.…”

Section: Discussionmentioning

confidence: 99%

“…In the adiabatic approximation, the exchange-correlation potential V XC and the electron mean field repulsion V H depend only on the instantaneous density denoted by ρ(r, t) [34]. Typically, RT-TDDFT simulations start from a ground state density matrix converged with DFT, but a superposition of non-stationary density matrices can also be used to emulate a sudden excitation [9,10,35,36].…”

Section: A Rt-tddft With Capmentioning

confidence: 99%

“…Tunnel ionization, wherein an electron driven by an external field moves through the barrier formed by the combination of the molecular and external field potentials, is the ionization process that forms the initial step in many strong field processes. The study of a range of important physical processes in ultrafast science, such as orientation-dependent strong field ionization (SFI), high-harmonic generation [1,2], the measurement of time delays in tunnel ionization via the attoclock [3], lightinduced electron diffraction [4,5], and ionization-based probes of charge migration [6][7][8][9][10], are expected to benefit from an efficient and accurate theoretical method of calculating SFI in a variety of molecules. In light of this overarching influence of tunnel ionization, it is therefore of paramount importance to have theoretical models that can reliably treat this ionization mechanism.…”

Section: Introductionmentioning

confidence: 99%

See 2 more Smart Citations

All-Electron, Density Functional-Based Method for Angle-Resolved Tunneling Ionization in the Adiabatic Regime

Wahyutama¹,

Jayasinghe²,

Mauger³

et al. 2022

Preprint

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We develop and test a method that integrates many-electron weak-field asymptotic theory (ME-WFAT) [Phys. Rev. A 89, 013421 (2014)] in the integral representation (IR) into the density functional theory (DFT) framework. In particular, we present modifications of the integral formula in the IR ME-WFAT to incorporate the potential terms unique to DFT. By solving an adiabatic rate equation for the angle-resolved ionization yield in our DFT-based ME-WFAT method, we show that the results are in excellent agreement with those of real-time time-dependent density functional theory (RT-TDDFT) simulations for NO, OCS, CH3Br, and CH3Cl interacting with one-and twocolor laser fields with a fundamental wavelength of 800 nm. This agreement is significant because the WFAT calculations take only a small fraction of the time of full TDDFT calculations. These results suggest that in the wavelength region commonly used in strong-field experiments (800 nm and longer), our DFT-based WFAT treatment can be used to rapidly screen for the ionization properties of a large number of molecules as a function of alignment or orientation between the molecule and the strong field.

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Section: Discussionmentioning

confidence: 99%

Section: A Rt-tddft With Capmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

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All-Electron, Density Functional-Based Method for Angle-Resolved Tunneling Ionization in the Adiabatic Regime

Wahyutama¹,

Jayasinghe²,

Mauger³

et al. 2022

Preprint

Self Cite

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“…XC [n(t)](r) which can be a useful analysis tool in cases where the exact groundstate xc potential can be computed (usually model 1D systems). Due to the lack of memory, the adiabatic approximation leads to large errors in some applications, sometimes failing completely [52][53][54][55][56][57][58][59][60], but in other cases it has been found to yield good predictions [5][6][7][8][9][10][11][12][13][14][15][16][17][18], even when the system is far from a ground-state. It is not completely understood why: possible reasons include, that the adiabatic approximation satisfies a number of exact conditions that are important in the time-dependent case [2], that in some applications a strong external field dominates over xc effects in driving the dynamics and that partial compensation of selfinteraction in the Hartree potential, even at the groundstate level, is enough, especially when the observables involve averaging over the details of the density distribution.…”

Section: A Memory: History and Initial-state Dependencementioning

confidence: 99%

“…While perturbations around the ground-state yields a formalism for excited states, their couplings, and response, it is particularly the generality and practical efficiency of the real-time formulation that has led to the possibility of applications on large systems which could not be done otherwise, e.g. [5][6][7][8][9][10][11][12][13][14][15][16][17][18].…”

Section: Introductionmentioning

confidence: 99%

The Exact Exchange-Correlation Potential in Time-Dependent Density Functional Theory: Choreographing Electrons with Steps and Peaks

Dar¹,

Lacombe²,

Maitra³

2022

Preprint

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The time-dependent exchange-correlation potential has an unusual task in directing fictitious noninteracting electrons to move with exactly the same probability density as true interacting electrons. This has intriguing implications for its structure, especially in the non-perturbative regime, leading to step and peak features that cannot be captured by bootstrapping any ground-state functional approximations. We review what has been learned about these features in the exact exchange-correlation potential in time-dependent density functional theory in the past decade or so, and implications for the performance of simulations when electrons are driven far from any ground-state.

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DFT Studies on the Molecular Structure, Regioisomerism, Ground and Excited state Charge Transfer Properties of Spiro‐heterocycles

Anumol¹,

Jose²,

Joy³

2022

ChemistrySelect

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The electronic structure, stereochemical aspects and charge transfer properties of the spiro compound (5S,8S) spiro‐{6‐phenyl‐1‐aza‐3‐oxa‐7‐thia‐bicyclo[3,3,0]‐octene‐8,3’(2’H)‐indol}‐2’‐one (spiro bicyclo adduct) synthesized using the multi‐component reaction via 1,3‐dipolar cycloaddition of isatin and thioproline with the dipolarophile phenylacetylene have been studied. The two lowest energy regio‐isomers of the spiro heterocycle formed from the stereospecific dipolar reaction have been analysed along with the electron‐withdrawing and releasing substituents using DFT method at the CAM‐B3LYP/6‐311++G(d,p) level of theory. The atomic charges and the stabilization energy due to the intramolecular charge delocalization process calculated using the natural orbitals at the different molecular sites reveal the different donor‐acceptor interactions occurring in the system. The intramolecular electronic transitions (specifically n to π* and π to π*) is found to occur from the localized donor end component to the acceptor end components in the multi‐component system. The hole produced by the ionization of the entities is found to migrate from the thioproline component to the phenyl acetylene part in a time scale of around 4 fs. The electron‐withdrawing and donating substituents on the spirobicyclo adduct have been proven to tune the excited and ground state charge transfer properties uniquely. The results can shed light on how multi‐component reactions can be directed to produce spiro adducts with versatile applications.

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Charge migration and attosecond solitons in conjugated organic molecules

Cited by 23 publications

References 46 publications

All-Electron, Density Functional-Based Method for Angle-Resolved Tunneling Ionization in the Adiabatic Regime

All-Electron, Density Functional-Based Method for Angle-Resolved Tunneling Ionization in the Adiabatic Regime

The Exact Exchange-Correlation Potential in Time-Dependent Density Functional Theory: Choreographing Electrons with Steps and Peaks

DFT Studies on the Molecular Structure, Regioisomerism, Ground and Excited state Charge Transfer Properties of Spiro‐heterocycles

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