Quantum Biology Laboratory, Howard University, Washington, D.C. 20060, United States.
Institute of Physics, Benemérita Universidad Autónoma de Puebla, Puebla 72570, Mexico.
J Phys Chem B. 2024 May 2;128(17):4035-4046. doi: 10.1021/acs.jpcb.3c07936. Epub 2024 Apr 19.
Networks of tryptophan (Trp)─an aromatic amino acid with strong fluorescence response─are ubiquitous in biological systems, forming diverse architectures in transmembrane proteins, cytoskeletal filaments, subneuronal elements, photoreceptor complexes, virion capsids, and other cellular structures. We analyze the cooperative effects induced by ultraviolet (UV) excitation of several biologically relevant Trp mega-networks, thus giving insights into novel mechanisms for cellular signaling and control. Our theoretical analysis in the single-excitation manifold predicts the formation of strongly superradiant states due to collective interactions among organized arrangements of up to >10 Trp UV-excited transition dipoles in microtubule architectures, which leads to an enhancement of the fluorescence quantum yield (QY) that is confirmed by our experiments. We demonstrate the observed consequences of this superradiant behavior in the fluorescence QY for hierarchically organized tubulin structures, which increases in different geometric regimes at thermal equilibrium before saturation, highlighting the effect's persistence in the presence of disorder. Our work thus showcases the many orders of magnitude across which the brightest (hundreds of femtoseconds) and darkest (tens of seconds) states can coexist in these Trp lattices.
色氨酸(Trp)网络——一种具有强荧光响应的芳香族氨基酸——在生物系统中无处不在,在跨膜蛋白、细胞骨架丝、亚神经元元件、光受体复合物、病毒衣壳和其他细胞结构中形成多种结构。我们分析了几种与生物相关的 Trp 超网络紫外(UV)激发引起的协同效应,从而深入了解细胞信号转导和控制的新机制。我们在单激发态下的理论分析预测了由于微管结构中组织排列的高达 >10 个 Trp UV 激发跃迁偶极子之间的集体相互作用而形成的强超辐射态,这导致荧光量子产率(QY)的增强,实验证实了这一点。我们通过实验证明了这种超辐射行为在分层组织的微管结构的荧光 QY 中观察到的后果,在热平衡下,在达到饱和之前,不同的几何区域的 QY 增加,突出了在存在无序的情况下这种效应的持久性。因此,我们的工作展示了在这些 Trp 晶格中,最亮(数百飞秒)和最暗(数十秒)状态可以共存的多个数量级。