Tunable spin-phonon polarons in a chiral molecular qubit framework

• URL: http://arxiv.org/abs/2506.04885v1
• Date: Thu, 05 Jun 2025 11:03:51 GMT
• Title: Tunable spin-phonon polarons in a chiral molecular qubit framework
• Authors: Aimei Zhou, Ruihao Bi, Zhenghan Zhang, Luming Yang, Xudong Tian, Denan Li, Mingshu Tan, Weibin Ni, Haozhou Sun, Jinkun Guo, Xinxing Zhao, Zhifu Shi, Wei Tong, Zhitao Zhang, Jin-Hu Dou, Feng Jin, Shi Liu, Mircea Dinca, Tijana Rajh, Jian Li, Wenjie Dou, Lei Sun,
• Abstract summary: Chiral structures that produce asymmetric spin-phonon coupling can theoretically generate spin-phonon polarons.<n>We report spin dynamic signatures that clearly indicate the formation of spin-phonon polarons for the first time.
• Score: 7.313504149765732
• License: http://creativecommons.org/licenses/by-nc-nd/4.0/
• Abstract: Chiral structures that produce asymmetric spin-phonon coupling can theoretically generate spin-phonon polarons -- quasiparticles exhibiting non-degenerate spin states with phonon displacements. However, direct experimental evidence has been lacking. Using a chiral molecular qubit framework embedding stable semiquinone-like radicals, we report spin dynamic signatures that clearly indicate the formation of spin-phonon polarons for the first time. Our non-adiabatic model reveals that these quasiparticles introduce an active spin relaxation channel when polaron reorganization energy approaches Zeeman splitting. This new channel manifests as anomalous, temperature-independent spin relaxation, which can be suppressed by high magnetic fields or pore-filling solvents (e.g. CH2Cl2, CS2). Such field- and guest-tunable relaxation is unattainable in conventional spin systems. Harnessing this mechanism could boost repetition rates in spin-based quantum information technologies without compromising coherence.

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