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Extended Dissipaton Theory with Application to Adatom-Graphene Composite.

Yu Su^1,2, Yao Wang^1,2, Zi-Fan Zhu^1,2

¹Hefei National Research Center for Physical Sciences at the Microscale, University of Science and Technology of China, Hefei, Anhui 230026, China.

Journal of Chemical Theory and Computation

|April 14, 2025

Summary

We introduce the extended dissipaton theory, an exact method for quantum systems with linear and quadratic environmental couplings. This approach reveals complex spectral behaviors in adatoms on graphene substrates.

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Area of Science:

Quantum mechanics
Condensed matter physics
Materials science

Background:

Strongly correlated electronic systems often exhibit complex interactions with their environment.
Existing theories struggle to accurately model both linear and quadratic environmental couplings.
Understanding these interactions is crucial for mesoscopic nanodevices and superconductors.

Purpose of the Study:

To present an extended dissipaton theory capable of handling complex environmental couplings.
To develop exact, non-Markovian, and nonperturbative theoretical formalisms.
To apply the theory to a relevant physical system and analyze its predictions.

Main Methods:

Developed the dissipaton-equation-of-motion formalism.
Formulated an equivalent dissipaton-embedded quantum master equation.
Applied these methods to simulate spectral functions of an adatom on a graphene substrate.

Main Results:

The extended dissipaton theory successfully models linear and quadratic environmental couplings.
Simulations revealed intricate spectral peak behaviors for an adatom on graphene.
Comparison with conventional metal environments highlighted unique graphene-substrate interactions.

Conclusions:

The extended dissipaton theory provides an accurate and versatile tool for studying quantum systems with strong environmental interactions.
The unique band structure of graphene significantly influences adatom spectral functions.
This work opens avenues for investigating complex phenomena in nanodevices and superconductors.