Crystalline Small Molecule-Polymer Superlattice for Spatially Isolated Tetrathiafulvalene Spin Qubit Arrays

Linkuo Li; Zhecheng Sun; Xin Wang; Lei Zhang; Zihao Chen; Qianfeng Gu; Jinglun Yang; Yifan Cui; Yung-Kang Peng; Lei Sun; Qichun Zhang

doi:10.1002/anie.7183450

Crystalline Small Molecule-Polymer Superlattice for Spatially Isolated Tetrathiafulvalene Spin Qubit Arrays

Linkuo Li (Co-first Author)
, Zhecheng Sun (Co-first Author)
, Xin Wang (Co-first Author)
, Lei Zhang
, Zihao Chen
, Qianfeng Gu
, Jinglun Yang
, Yifan Cui
, Yung-Kang Peng
, Lei Sun^*
, Qichun Zhang^*

^*Corresponding author for this work

Research output: Journal Publications and Reviews › RGC 21 - Publication in refereed journal › peer-review

2 Citations (Scopus)

Abstract

Molecular electron spins are compelling qubit candidates; however, mitigating their rapid relaxation and decoherence driven by structural disorder and phonon coupling remains a central challenge. Constructing molecular qubit frameworks (MQFs) represents a promising strategy to preserve quantum coherence by embedding spin centers in a rigid and ordered microenvironment. Here, we report a host–guest superlattice MQF by cocrystallizing tetrathiafulvalene (TTF) with a one-dimensional B←N coordination polymer (CityU-65). Encaging TTF radical spins within this highly ordered lattice establishes a rigid and magnetically dilute environment, effectively suppressing spin-lattice relaxation and partially mitigating spin decoherence. Consequently, CityU-65 preserves coherent spin addressability even under ambient conditions. At room temperature, the superlattice exhibits a prolonged spin–lattice relaxation time (T₁ = 9.6 µs) and a modestly improved phase-memory time (T_m = 0.9 µs) compared to pristine crystalline TTF. Our work establishes B←N superlattice cocrystallization as a powerful strategy for engineering designer quantum materials, providing a general guideline for the development of high-performance organic qubits through structural and phononic modulation. © 2026 Wiley-VCH GmbH.

Original language	English
Article number	e7183450
Number of pages	10
Journal	Angewandte Chemie - International Edition
Volume	65
Issue number	33
Online published	23 Jun 2026
DOIs	https://doi.org/10.1002/anie.7183450
Publication status	Published - 10 Aug 2026

Funding

Qichun Zhang acknowledges financial support from the City University of Hong Kong (9380117 and 7020089) and the Hong Kong Branch of the National Precious Metals Material Engineering Research Center(NPMM), Hong Kong, People’s Republic of China. Qichun Zhang also acknowledges funding support from the Innovation and Technology Fund(ITF, ITS/322/22), the National Natural Science Foundation of China(NSFC, 22475183), and the Shenzhen Science and Technology Program(JCYJ20240813153135046). Zhecheng Sun and Lei Sun acknowledge sup-port from the National Natural Science Foundation of China (NSFC No.22273078) and the Hangzhou Municipal Funding, Team of Innovation(TD2022004), and thank the Instrumentation and Service Center for Molecular Sciences at Westlake University for the support with CW and pulse EPR measurements.

Research Keywords

B ← N coordination polymer
molecular spin qubits
organic qubits
superlattice cocrystal
tetrathiafulvalene (TTF)

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title = "Crystalline Small Molecule-Polymer Superlattice for Spatially Isolated Tetrathiafulvalene Spin Qubit Arrays",

abstract = "Molecular electron spins are compelling qubit candidates; however, mitigating their rapid relaxation and decoherence driven by structural disorder and phonon coupling remains a central challenge. Constructing molecular qubit frameworks (MQFs) represents a promising strategy to preserve quantum coherence by embedding spin centers in a rigid and ordered microenvironment. Here, we report a host–guest superlattice MQF by cocrystallizing tetrathiafulvalene (TTF) with a one-dimensional B←N coordination polymer (CityU-65). Encaging TTF radical spins within this highly ordered lattice establishes a rigid and magnetically dilute environment, effectively suppressing spin-lattice relaxation and partially mitigating spin decoherence. Consequently, CityU-65 preserves coherent spin addressability even under ambient conditions. At room temperature, the superlattice exhibits a prolonged spin–lattice relaxation time (T1 = 9.6 µs) and a modestly improved phase-memory time (Tm = 0.9 µs) compared to pristine crystalline TTF. Our work establishes B←N superlattice cocrystallization as a powerful strategy for engineering designer quantum materials, providing a general guideline for the development of high-performance organic qubits through structural and phononic modulation. {\textcopyright} 2026 Wiley-VCH GmbH.",

keywords = "B ← N coordination polymer, molecular spin qubits, organic qubits, superlattice cocrystal, tetrathiafulvalene (TTF)",

author = "Linkuo Li and Zhecheng Sun and Xin Wang and Lei Zhang and Zihao Chen and Qianfeng Gu and Jinglun Yang and Yifan Cui and Yung-Kang Peng and Lei Sun and Qichun Zhang",

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Crystalline Small Molecule-Polymer Superlattice for Spatially Isolated Tetrathiafulvalene Spin Qubit Arrays. / Li, Linkuo (Co-first Author); Sun, Zhecheng (Co-first Author); Wang, Xin (Co-first Author) et al.
In: Angewandte Chemie - International Edition, Vol. 65, No. 33, e7183450, 10.08.2026.

Research output: Journal Publications and Reviews › RGC 21 - Publication in refereed journal › peer-review

TY - JOUR

T1 - Crystalline Small Molecule-Polymer Superlattice for Spatially Isolated Tetrathiafulvalene Spin Qubit Arrays

AU - Li, Linkuo

AU - Sun, Zhecheng

AU - Wang, Xin

AU - Zhang, Lei

AU - Chen, Zihao

AU - Gu, Qianfeng

AU - Yang, Jinglun

AU - Cui, Yifan

AU - Peng, Yung-Kang

AU - Sun, Lei

AU - Zhang, Qichun

PY - 2026/8/10

Y1 - 2026/8/10

N2 - Molecular electron spins are compelling qubit candidates; however, mitigating their rapid relaxation and decoherence driven by structural disorder and phonon coupling remains a central challenge. Constructing molecular qubit frameworks (MQFs) represents a promising strategy to preserve quantum coherence by embedding spin centers in a rigid and ordered microenvironment. Here, we report a host–guest superlattice MQF by cocrystallizing tetrathiafulvalene (TTF) with a one-dimensional B←N coordination polymer (CityU-65). Encaging TTF radical spins within this highly ordered lattice establishes a rigid and magnetically dilute environment, effectively suppressing spin-lattice relaxation and partially mitigating spin decoherence. Consequently, CityU-65 preserves coherent spin addressability even under ambient conditions. At room temperature, the superlattice exhibits a prolonged spin–lattice relaxation time (T1 = 9.6 µs) and a modestly improved phase-memory time (Tm = 0.9 µs) compared to pristine crystalline TTF. Our work establishes B←N superlattice cocrystallization as a powerful strategy for engineering designer quantum materials, providing a general guideline for the development of high-performance organic qubits through structural and phononic modulation. © 2026 Wiley-VCH GmbH.

AB - Molecular electron spins are compelling qubit candidates; however, mitigating their rapid relaxation and decoherence driven by structural disorder and phonon coupling remains a central challenge. Constructing molecular qubit frameworks (MQFs) represents a promising strategy to preserve quantum coherence by embedding spin centers in a rigid and ordered microenvironment. Here, we report a host–guest superlattice MQF by cocrystallizing tetrathiafulvalene (TTF) with a one-dimensional B←N coordination polymer (CityU-65). Encaging TTF radical spins within this highly ordered lattice establishes a rigid and magnetically dilute environment, effectively suppressing spin-lattice relaxation and partially mitigating spin decoherence. Consequently, CityU-65 preserves coherent spin addressability even under ambient conditions. At room temperature, the superlattice exhibits a prolonged spin–lattice relaxation time (T1 = 9.6 µs) and a modestly improved phase-memory time (Tm = 0.9 µs) compared to pristine crystalline TTF. Our work establishes B←N superlattice cocrystallization as a powerful strategy for engineering designer quantum materials, providing a general guideline for the development of high-performance organic qubits through structural and phononic modulation. © 2026 Wiley-VCH GmbH.

KW - B ← N coordination polymer

KW - molecular spin qubits

KW - organic qubits

KW - superlattice cocrystal

KW - tetrathiafulvalene (TTF)

UR - https://www.scopus.com/pages/publications/105042550822

UR - https://www.scopus.com/pages/publications/105042550822#tab=impact

U2 - 10.1002/anie.7183450

DO - 10.1002/anie.7183450

M3 - RGC 21 - Publication in refereed journal

SN - 1433-7851

VL - 65

JO - Angewandte Chemie - International Edition

JF - Angewandte Chemie - International Edition

IS - 33

M1 - e7183450

ER -

Crystalline Small Molecule-Polymer Superlattice for Spatially Isolated Tetrathiafulvalene Spin Qubit Arrays

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Crystalline Small Molecule-Polymer Superlattice for Spatially Isolated Tetrathiafulvalene Spin Qubit Arrays

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