Dynamics of Electronic Transfer Processes at Metal/Insulator Interfaces

Guedde, J.; Berthold, W.; Hoefer, Ulrich

doi:10.1002/chin.200652228

Cited by 7 publications

(13 citation statements)

References 1 publication

Supporting

Mentioning

Contrasting

Order By: Relevance

“…We use the model potential developed by Chulkov et al , 103 successfully applied in the past to describe the dynamics of the excited states at metal surfaces. 13,[48][49][50]104 This model potential only depends on the electron coordinate z perpendicular to the surface:…”

Section: Interaction With the Metal Surfacementioning

confidence: 99%

“…From the experimental point of view the electron dynamics in excited states at surfaces has been thoroughly addressed using the proximal probe Scanning Tunneling Mi- 63,64 croscopy (STM) technique [43][44][45][46] as well as the Time-Resolved Two-Photon-Photoemission (TR-2PPE). 13,[47][48][49][50] These and other experiments triggered large theoretical interest. Among other theoretical approaches, the excited-state potential-energy surfaces for molecules adsorbed on metal substrates were obtained using the ∆ self-consistent field (∆SCF) method 51 and the ∆ self-consistent field density-functional theory (∆DFT).…”

Section: Introductionmentioning

confidence: 99%

See 1 more Smart Citation

Ultrafast Dynamics of Electronic Resonances in Molecules Adsorbed on Metal Surfaces: A Wave Packet Propagation Approach

Aguilar-Galindo

Borisov

Díaz‐Tendero

2021

J. Chem. Theory Comput.

View full text Add to dashboard Cite

We present a wave packet propagation-based method to study the electron dynamics in molecular species in the gas phase and adsorbed on metal surfaces. It is a very general method that can be employed to any system where the electron dynamics is dominated by an active electron and the coupling between the discrete and continuum electronic states is of importance. As an example one can consider resonant moleculesurface electron transfer or molecular photoionization. Our approach is based on a 1 computational strategy allowing to incorporate ab initio inputs from Quantum Chemistry methods, such as Density Functional Theory, Hartree-Fock and Coupled Cluster.Thus, the electronic structure of the molecule is fully taken into account. The electron wave function is represented on a 3D grid in spatial coordinates, and its temporal evolution is obtained from the solution of the time dependent Schrödinger equation. We illustrate our method with an example -electron dynamics of anionic states localized on organic molecules adsorbed on metal surfaces. In particular, we study resonant charge transfer from π * orbitals of three vinyl derivatives (acrylamide, acrylonitrile, and acrolein) adsorbed on a Cu(100) surface. Electron transfer between these lowest unoccupied molecular orbitals and the metal surface is extremely fast, leading to a decay of the population of the molecular anion on the femtosecond timescale. We detail how to analyze the time-dependent electronic wave function in order to obtain the relevant information on the system: the energies and lifetimes of the molecule-localized quasi-stationary states, their associated resonant wavefunctions, and the population decay channels. In particular, we demonstrate the effect of the electronic structure of the substrate on the energy and wave vector distribution of the hot electrons injected into the metal by the decaying molecular resonance.

show abstract

Section: Interaction With the Metal Surfacementioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

Ultrafast Dynamics of Electronic Resonances in Molecules Adsorbed on Metal Surfaces: A Wave Packet Propagation Approach

Aguilar-Galindo

Borisov

Díaz‐Tendero

2021

J. Chem. Theory Comput.

View full text Add to dashboard Cite

show abstract

“…Other possible applications exist regarding isomerization reactions of molecular switches at surfaces, 385 or the impact of surface electronic states on adsorbates. [46][47][48][437][438][439][440][441][442][443] We expect that third-order 2D IR is going to be advantageous as a starting point for implementing transient 2D IR over a broader range of sample systems, since 2D SFG is already a higher-order nonlinear method with even weaker signals.…”

Section: Figure 36 Comparison Of 2d Ir and Transient 2d Ir Signals Omentioning

confidence: 99%

Surface-Sensitive and Surface-Specific Ultrafast Two-Dimensional Vibrational Spectroscopy

2016

View full text Add to dashboard Cite

Ultrafast two-dimensional infrared spectroscopy (2D IR) has been advanced in recent years toward measuring signals from only a monolayer of sample molecules at solid-liquid and solid-gas interfaces. A series of experimental methods has been introduced, which in the chronological order of development are 2D sum-frequency-generation (2D SFG), transmission 2D IR, and reflection 2D IR, the latter in either internal, attenuated total reflection (ATR), or external reflection configuration. The different variants of 2D vibrational spectroscopy are based on either the even-order or the odd-order nonlinear susceptibility, and all allow resolving similar molecular temporal and spectral information. In this review, we introduce the basic principles of the different methods of 2D vibrational spectroscopy at surfaces along with a balanced overview on the technological aspects as well as benefits and shortcomings. We furthermore discuss the current scope of applications for 2D vibrational surface spectroscopy, which spans an impressively broad range of samples from biological molecules to heterogeneous catalysts. The emphasis is on the ultrafast structural dynamics of molecules at interfaces, environmental interactions, and intermolecular interactions. We furthermore consider important recent technological developments of 2D vibrational surface spectroscopy, which employ (i) surface enhancement, (ii) methods for studying electrochemical interfaces, and (iii) extensions for resolving nonequilibrium processes (transient 2D IR). A detailed outlook is finally given regarding important future applications and technological developments of 2D vibrational surface spectroscopy.

show abstract

“…For this reason, countless studies focused on this correlation between the ultrafast single particle electron dynamics and the (spin-dependent) interfacial band structure of ultrathin metallic or molecular films on metallic surfaces [7][8][9][10][11][12][13][14][15][16][17][18][19][20][21][22][23][24]. The most commonly used experimental technique for such studies is time-resolved two-photonphotoemission spectroscopy (tr-2PPE) [25][26][27][28][29][30], which allows one to characterize the ultrafast electron dynamics by the quasiparticle lifetime of the optically excited electrons in the so-called single-particle limit.…”

Section: Introductionmentioning

confidence: 99%

Adsorption-induced modification of the hot electron lifetime in a Pb/Ag111 quantum well system

Haag,

Eul,

Grad

et al. 2021

Preprint

View full text Add to dashboard Cite

The interfacial band structures of multilayer systems play a crucial role for the ultrafast charge and spin carrier dynamics at interfaces. Here, we study the energy-and momentum-dependent quasiparticle lifetimes of excited states of a lead monolayer film on Ag(111) prior and after the adsorption of a monolayer of 3,4,9,10-perylene-tetracarboxylic-dianhydride (PTCDA). Using time-resolved twophoton momentum microscopy, we show that the electron dynamics of the bare Pb/Ag(111) bilayer system is dominated by isotropic intraband scattering processes within the quantum well state as well as interband scattering processes from the QWS into the Pb sideband. After the adsorption of PTCDA on the Pb monolayer, the interband scattering is suppressed and the electron dynamics is solely determined by intraband or inelastic scattering processes. Our findings hence uncover a new possibility to selectively tune and control scattering processes of quantum well systems by the adsorption of organic molecules.

show abstract

Dynamics of Electronic Transfer Processes at Metal/Insulator Interfaces

Abstract: ChemInform is a weekly Abstracting Service, delivering concise information at a glance that was extracted from about 200 leading journals. To access a ChemInform Abstract, please click on HTML or PDF.

Cited by 7 publications

References 1 publication

Ultrafast Dynamics of Electronic Resonances in Molecules Adsorbed on Metal Surfaces: A Wave Packet Propagation Approach

Ultrafast Dynamics of Electronic Resonances in Molecules Adsorbed on Metal Surfaces: A Wave Packet Propagation Approach

Surface-Sensitive and Surface-Specific Ultrafast Two-Dimensional Vibrational Spectroscopy

Adsorption-induced modification of the hot electron lifetime in a Pb/Ag111 quantum well system

Contact Info

Product

Resources

About