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Abstract Electron transfer is a fundamental process in chemistry, biology, and physics. One of the most intriguing questions concerns the realization of the transitions between nonadiabatic and adiabatic regimes of electron transfer. Using colloidal quantum dot molecules, we computationally demonstrate how the hybridization energy (electronic coupling) can be tuned by changing the neck dimensions and/or the quantum dot sizes. This provides a handle to tune the electron transfer from the incoherent nonadiabatic regime to the coherent adiabatic regime in a single system. We develop an atomistic model to account for several states and couplings to the lattice vibrations and utilize the mean-field mixed quantum-classical method to describe the charge transfer dynamics. Here, we show that charge transfer rates increase by several orders of magnitude as the system is driven to the coherent, adiabatic limit, even at elevated temperatures, and delineate the inter-dot and torsional acoustic modes that couple most strongly to the charge transfer dynamics.
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This content will become publicly available on July 25, 2026
Electrons in Quantum Dots on Helium: From Charge Qubits to Synthetic Color Centers
Electrons trapped above the surface of helium provide a means to study many-body physics free from the randomness that comes from defects in other condensed-matter systems. Localizing an electron in an electrostatic quantum dot makes its energy spectrum discrete, with controlled level spacing. The lowest two states can act as charge qubit states. In this paper, we study how the coupling to the quantum field of capillary waves on helium—known as ripplons—affects electron dynamics. As we show, the coupling can be strong. This bounds the parameter range where electron-based charge qubits can be implemented. The constraint is different from the conventional relaxation time constraint. The electron–ripplon system in a dot is similar to a color center formed by an electron defect coupled to phonons in a solid. In contrast to solids, the coupling in the electron on helium system can be varied from strong to weak. This enables a qualitatively new approach to studying color center physics. We analyze the spectroscopy of the pertinent synthetic color centers in a broad range of the coupling strength.
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- Award ID(s):
- 2003815
- PAR ID:
- 10618500
- Publisher / Repository:
- MDPI
- Date Published:
- Journal Name:
- Entropy
- Volume:
- 27
- Issue:
- 8
- ISSN:
- 1099-4300
- Page Range / eLocation ID:
- 787
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
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