Rossini Mirko, Ammerpohl Ole, Siebert Reiner, Ankerhold Joachim
Ulm University, Institute for Complex Quantum Systems, 89069, Ulm, Germany.
Center for Integrated Quantum Science and Technology (IQST), Ulm, Germany.
Sci Rep. 2025 May 20;15(1):17543. doi: 10.1038/s41598-025-02819-w.
Charge fluctuations along stacked nucleobases in the DNA double helix play a key role in processes such as DNA repair and replication. While classical charge transfer mechanisms between adjacent bases due to energetic excitations are well established, quantum effects can also contribute significantly. Specifically, the overlap of π-orbitals in well-stacked nucleobases can enable charge delocalization along the DNA double-strand. However, the cellular environment, including water, surrounding molecules, and thermal noise, is thought to induce rapid decoherence, limiting quantum-enhanced charge transport under physiological conditions. To explore charge mobility in such noisy environments, we model quantum diffusion in DNA-inspired two-dimensional tight-binding lattices, considering intrinsic and environmental fluctuations and revealing, via atomistic parametrization, a complex network of charge transport pathways. Our results show that long-range quantum phenomena depend on the carrier type (electrons or holes), base sequence, and noise/disorder characteristics. Notably, spatially correlated low-frequency fluctuations can sustain coherent charge transfer across several bases, whereas moderate vibrational noise can enhance rather than suppress quantum coherence by facilitating tunneling effects. These findings suggest that even under physiological conditions, the DNA structure can support non-classical charge dynamics, offering insights into its potential role in bioelectronic processes and inspiring future models of quantum transport in biological systems.
DNA双螺旋中沿堆叠核碱基的电荷涨落在DNA修复和复制等过程中起着关键作用。虽然由于能量激发导致的相邻碱基之间的经典电荷转移机制已得到充分确立,但量子效应也可能有显著贡献。具体而言,排列良好的核碱基中π轨道的重叠能够使电荷沿DNA双链离域。然而,包括水、周围分子和热噪声在内的细胞环境被认为会引发快速退相干,限制生理条件下量子增强的电荷传输。为了探索这种嘈杂环境中的电荷迁移率,我们在受DNA启发的二维紧束缚晶格中对量子扩散进行建模,考虑内在和环境涨落,并通过原子参数化揭示了一个复杂的电荷传输路径网络。我们的结果表明,长程量子现象取决于载流子类型(电子或空穴)、碱基序列以及噪声/无序特征。值得注意的是,空间相关的低频涨落能够维持跨越多个碱基的相干电荷转移,而适度的振动噪声可以通过促进隧穿效应增强而非抑制量子相干。这些发现表明,即使在生理条件下,DNA结构也能够支持非经典电荷动力学,为其在生物电子过程中的潜在作用提供了见解,并启发了未来生物系统中量子传输的模型。