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Lu-Lu键中的稳定未配对电子态导致Lu@C晶体管近藤效应中奇偶宇称的缺失。

Stable Unpaired Electron States in the Lu-Lu Bond Leading to the Absence of Odd-Even Parity in the Kondo Effect of Lu@C Transistors.

作者信息

Chen Jun, Shui Yuan, Shen Wangqiang, Wang Feng, Mao Yifu, Qi Haoran, Liu Xinrong, Du Yu, Fei Fucong, Qin Yuyuan, Wan Jianguo, Bao Lipiao, Zhang Minhao, Yang Tao, Lu Xing, Song Fengqi

机构信息

National Laboratory of Solid State Microstructures, Collaborative Innovation Center of Advanced Microstructures, School of Physics, Nanjing University, Nanjing 210093, China.

Institute of Atom Manufacturing, Nanjing University, Suzhou 215163, China.

出版信息

Nano Lett. 2025 Apr 9;25(14):5762-5769. doi: 10.1021/acs.nanolett.5c00365. Epub 2025 Mar 27.

DOI:10.1021/acs.nanolett.5c00365
PMID:40145565
原文链接:https://pmc.ncbi.nlm.nih.gov/articles/PMC12005644/
Abstract

Spin qubits constructed in endohedral fullerenes benefit from the protective shielding of the carbon cage, which effectively mitigates external decoherence and enables ultralong coherence times. However, endohedral fullerene spin qubits face the challenge of charge transfer in complex electrical environments, such as during qubit readout or large-scale integration, which can induce spin state modifications. In this study, we developed transistors based on the endohedral fullerene Lu@C and observed the absence of parity dependence in the Kondo effect; this result was contradictory to the typical behavior of the Kondo effect observed in C. Density functional theory calculations revealed that upon electron loss, a spin-1/2 electron predominantly from the -orbitals formed in the Lu-Lu bond and its orbital energy was significantly lower than that of the highest occupied molecular orbital. Based on these results, Lu@C held stable unpaired electron states across multiple charge states and has potential applications in spin quantum devices.

摘要

内嵌富勒烯中构建的自旋量子比特受益于碳笼的保护屏蔽,这有效地减轻了外部退相干并实现了超长的相干时间。然而,内嵌富勒烯自旋量子比特面临着复杂电环境中电荷转移的挑战,例如在量子比特读出或大规模集成期间,这可能会引起自旋态的改变。在本研究中,我们开发了基于内嵌富勒烯Lu@C的晶体管,并观察到近藤效应中不存在宇称依赖性;这一结果与在C中观察到的近藤效应的典型行为相矛盾。密度泛函理论计算表明,在电子损失时,一个主要来自Lu-Lu键中形成的 -轨道的自旋1/2电子,其轨道能量明显低于最高占据分子轨道的能量。基于这些结果,Lu@C在多个电荷态下保持稳定的未配对电子态,并在自旋量子器件中具有潜在应用。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/4ba6/12005644/3f49d7b88656/nl5c00365_0004.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/4ba6/12005644/ecda78d56277/nl5c00365_0001.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/4ba6/12005644/cc935866ac95/nl5c00365_0002.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/4ba6/12005644/bb1d639e6d5a/nl5c00365_0003.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/4ba6/12005644/3f49d7b88656/nl5c00365_0004.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/4ba6/12005644/ecda78d56277/nl5c00365_0001.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/4ba6/12005644/cc935866ac95/nl5c00365_0002.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/4ba6/12005644/bb1d639e6d5a/nl5c00365_0003.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/4ba6/12005644/3f49d7b88656/nl5c00365_0004.jpg

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Parity-independent Kondo effect of correlated electrons in electrostatically defined ZnO quantum dots.静电定义的ZnO量子点中关联电子的与奇偶性无关的近藤效应
Nat Commun. 2024 Nov 7;15(1):9556. doi: 10.1038/s41467-024-53890-2.
3
CaY@C: Exploring Molecular Qubits with Ca-Y Metal-Metal Bonds.
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J Am Chem Soc. 2024 Sep 4;146(35):24310-24319. doi: 10.1021/jacs.4c04720. Epub 2024 Aug 20.
4
Element effects in endohedral metal-metal-bonding fullerenes M2@C82 (M = Sc, Y, La, Lu).内嵌金属-金属键合富勒烯M2@C82(M = Sc、Y、La、Lu)中的元素效应
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5
Improving the molecular spin qubit performance in zirconium MOF composites by mechanochemical dilution and fullerene encapsulation.通过机械化学稀释和富勒烯封装提高锆基金属有机框架复合材料中的分子自旋量子比特性能。
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