Stochastic Schrödinger equation for hot-carrier dynamics in plasmonic systems
These videos have been matched automatically. Contact us if they are not relevant.
These videos have been matched automatically. Contact us if they are not relevant.
View abstract on PubMed
Summary
This summary is machine-generated.We developed a multiscale method to simulate hot-carrier dynamics in plasmonic systems. This approach reveals how nanoparticle effects enhance charge generation and how relaxation times influence these processes.
Area Of Science
- Computational chemistry
- Quantum mechanics
- Materials science
Background
- Hot-carrier dynamics in photoexcited plasmonic systems are crucial for applications like CO2 photoreduction.
- Understanding the interplay between quantum and classical effects is essential for designing efficient photocatalysts.
Purpose Of The Study
- To develop and apply a multiscale computational method for studying hot-carrier dynamics.
- To investigate the influence of relaxation (T1) and dephasing (T2) times on charge dynamics.
- To elucidate the role of a metallic nanoparticle in plasmon-driven photoreduction.
Main Methods
- Coupling open quantum systems theory with real-time ab initio electronic structure calculations.
- Utilizing the Markovian Stochastic Schrödinger equation and ab initio GW/Bethe-Salpeter (BSE) equation.
- Modeling the metallic nanoparticle classically using the polarizable continuum model.
Main Results
- Observed net hole injection from rhodium to a CHO fragment, enhanced by two orders of magnitude due to the nanocube.
- Demonstrated that nonradiative decay (T1) rapidly decreases charge population.
- Showed that pure dephasing (T2) erases coherent charge injection dynamics.
Conclusions
- The multiscale method accurately captures hot-carrier dynamics in photoexcited plasmonic systems.
- Metallic nanoparticles significantly enhance charge generation in plasmon-driven reactions.
- Both relaxation and dephasing times play critical roles in controlling charge dynamics and photoreduction efficiency.
These videos have been matched automatically. Contact us if they are not relevant.
These videos have been matched automatically. Contact us if they are not relevant.
Related Concept Videos
The generation of electrical current in semiconductors is fundamentally driven by two mechanisms: drift and diffusion. These processes are essential for the functionality and performance of semiconductor-based devices.
Drift Current:
The drift of charge carriers is started by an external electric field (E). Charged particles, such as electrons and holes, experience an acceleration between collisions with lattice atoms. For electrons, this results in a drift velocity (vd) given by:
Where...
Carrier generation is the process by which electron-hole pairs (EHPs) are created within the semiconductor. In direct-bandgap semiconductors, such as gallium arsenide (GaAs), this occurs efficiently when energy absorption prompts valence electrons to leap into the conduction band, leaving behind holes.
This process is given by the generation rate G and is efficient due to the conservation of momentum between the valence band maximum and conduction band minimum.
Indirect generation involves an...
Shortly after de Broglie published his ideas that the electron in a hydrogen atom could be better thought of as being a circular standing wave instead of a particle moving in quantized circular orbits, Erwin Schrödinger extended de Broglie’s work by deriving what is now known as the Schrödinger equation. When Schrödinger applied his equation to hydrogen-like atoms, he was able to reproduce Bohr’s expression for the energy and, thus, the Rydberg formula governing hydrogen spectra.
The electric potential of the system can be calculated by relating it to the electric charge densities that give rise to the electric potential. The differential form of Gauss's law expresses the electric field's divergence in terms of the electric charge density.
On the other hand, the electric field is expressed as the gradient of the electric potential.
Combining the above two equations, an electric potential is expressed in terms of the electric charge density.
This equation is called...
Anyone who has used a microwave oven knows there is energy in electromagnetic waves. Sometimes, this energy is obvious, such as in the summer sun's warmth. At other times, it is subtle, such as the unfelt energy of gamma rays, which can destroy living cells. Electromagnetic waves bring energy into a system through their electric and magnetic fields. These fields can exert forces and move charges in the system and, thus, do work on them. However, there is energy in an electromagnetic wave,...
In the macroscopic world, objects that are large enough to be seen by the naked eye follow the rules of classical physics. A billiard ball moving on a table will behave like a particle; it will continue traveling in a straight line unless it collides with another ball, or it is acted on by some other force, such as friction. The ball has a well-defined position and velocity or well-defined momentum, p = mv, which is defined by mass m and velocity v at any given moment. This is the typical...