First‐principles dynamics of photoexcited molecules and materials towards a quantum description

You, Peiwei; Chen, Daqiang; Lian, Chao; Zhang, Cui; Meng, Sheng

doi:10.1002/wcms.1492

Cited by 20 publications

(20 citation statements)

References 104 publications

(187 reference statements)

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“…A Monkhorst–Pack k-point mesh of 1 × 1×1 was adopted for the calculations. There are other methods which can also deal with the excited state dynamics including plasmon excitations of metal nanoparticles and their couplings with molecules ( Shao et al, 2006 ; Guan et al, 2018 ; Lian et al, 2018 ; You et al, 2021 ).…”

Section: Methodsmentioning

confidence: 99%

Plasmon-Induced Water Splitting on Ag-Alloyed Pt Single-Atom Catalysts

et al. 2021

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A promising route to realize solar-to-chemical energy conversion resorts to water splitting using plasmon photocatalysis. However, the ultrafast carrier dynamics and underlying mechanism in such processes has seldom been investigated, especially when the single-atom catalyst is introduced. Here, from the perspective of quantum dynamics at the atomic length scale and femtosecond time scale, we probe the carrier and structural dynamics of plasmon-assisted water splitting on an Ag-alloyed Pt single-atom catalyst, represented by the Ag19Pt nanocluster. The substitution of an Ag atom by the Pt atom at the tip of the tetrahedron Ag20 enhances the interaction between water and the nanoparticle. The excitation of localized surface plasmons in the Ag19Pt cluster strengthens the charge separation and electron transfer upon illumination. These facts cooperatively turn on more than one charge transfer channels and give rise to enhanced charge transfer from the metal nanoparticle to the water molecule, resulting in rapid plasmon-induced water splitting. These results provide atomistic insights and guidelines for the design of efficient single-atom photocatalysts for plasmon-assisted water splitting.

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Section: Methodsmentioning

confidence: 99%

Plasmon-Induced Water Splitting on Ag-Alloyed Pt Single-Atom Catalysts

et al. 2021

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“…In this work, we review the implementation of firstprinciple rt-TDDFT algorithms with a numerical atomic orbital formalism, which is named as time-dependent ab initio propagation (TDAP) approach [35][36][37]. The timedomain quantum evolution of electronic states with the classical approximations of nuclear motions are treated concurrently in the scheme of Ehrenfest dynamics, which has enabled real-time tracking of coupled electron-nuclear dynamics in large-scale systems.…”

Section: Introductionmentioning

confidence: 99%

Theoretical Insights into Ultrafast Dynamics in Quantum Materials

Guan

Chen

et al. 2022

Ultrafast Sci

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The last few decades have witnessed the extraordinary advances in theoretical and experimental tools, which have enabled the manipulation and monitoring of ultrafast dynamics with high precisions. For modeling dynamical responses beyond the perturbative regime, computational methods based on time-dependent density functional theory (TDDFT) are the optimal choices. Here, we introduce TDAP (time-dependent ab initio propagation), a first-principle approach that is aimed at providing robust dynamic simulations of light-induced, highly nonlinear phenomena by real-time calculation of combined photonic, electronic, and ionic quantum mechanical effects within a TDDFT framework. We review the implementation of real-time TDDFT with numerical atomic orbital formalisms, which has enabled high-accuracy, large-scale simulations with moderate computational cost. The newly added features, i.e., the time-dependent electric field gauges and controllable ionic motion make the method especially suitable for investigating ultrafast electron-nuclear dynamics in complex periodic and semiperiodic systems. An overview of the capabilities of this first-principle method is provided by showcasing several representative applications including high-harmonic generation, tunable phase transitions, and new emergent states of matter. The method demonstrates a great potential in obtaining a predictive and comprehensive understanding of quantum dynamics and interactions in a wide range of materials at the atomic and attosecond space-time scale.

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“…This has allowed us to increase the time step by two orders of magnitude, for example, from 0.001 to 0.2 fs 51 . This algorithm has now been implemented in PWmat, 31,52 as well as in TDAP 30,53 and ELK 54,55 …”

Section: Introductionmentioning

confidence: 99%

“…35,51 This has allowed us to increase the time step by two orders of magnitude, for example, from 0.001 to 0.2 fs. 51 This algorithm has now been implemented in PWmat, 31,52 as well as in TDAP 30,53 and ELK. 54,55 Based on the above rt-TDDFT method, we have implemented the electron-light interaction, spin-orbit coupling (SOC), and noncollinear magnetic moment in the plane-wave Hamiltonian, to study the ultrafast demagnetization mechanism in ferromagnetic metals and semiconductors.…”

Section: Introductionmentioning

confidence: 99%

Algorithm advances and applications of time‐dependent first‐principles simulations for ultrafast dynamics

Liu

Wang

Chen

et al. 2021

WIREs Comput Mol Sci

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Far from equilibrium phenomenon is a central theme of contemporary material research. Such phenomenon can exhibit itself in atomic structure and dynamics, but very often it also happens as non-equilibrium phenomenon in the electronic structure. In ab initio material simulation, density functional theory (DFT) has played an essential role in studying electronic ground state problems. For excited states, besides many-body perturbation theory, another powerful tool is the time dependent DFT (TDDFT) method. In particular, the real-time TDDFT (rt-TDDFT) method can be used to simulate many non-equilibrium phenomena directly. Here we introduce our works on some algorithm advances based on our recently rt-TDDFT method. This method uses the plane-wave basis set, and significantly accelerates its efficiency by increasing the time step from 0.1-1 as in traditional methods to 0.2-0.5 fs. The noncollinear magnetic moments and spin-orbit coupling have also been included in our rt-TDDFT method. Furthermore, a Boltzmann-TDDFT algorithm has been developed to solve the hot carrier overheating problem in Ehrenfest dynamics, and a natural orbital branching algorithm has been developed to overcome the mean-field approximation in Ehrenfest dynamics nuclear trajectory, thus allows stochastic multiple paths in chemical reactions. Utilizing these methods, we have studied the photoinduced ultrafast demagnetization, ultrafast phase transition, energy transfer between plasmon and hot carriers, as well as the high-energy ion implantation and low-energy atomic diffusion in semiconductors.We believe the tools as the ones introduced here can enable us to study a wide range of phenomena which are of great interest in modern day material research.

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First‐principles dynamics of photoexcited molecules and materials towards a quantum description

Cited by 20 publications

References 104 publications

Plasmon-Induced Water Splitting on Ag-Alloyed Pt Single-Atom Catalysts

Plasmon-Induced Water Splitting on Ag-Alloyed Pt Single-Atom Catalysts

Theoretical Insights into Ultrafast Dynamics in Quantum Materials

Algorithm advances and applications of time‐dependent first‐principles simulations for ultrafast dynamics

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