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Tailored anharmonic–harmonic vibrational profiles for fluorescent biomarkers
Physical Chemistry Chemical Physics ( IF 2.9 ) Pub Date : 2022-06-13 , DOI: 10.1039/d2cp01486f
Nghia Nguyen Thi Minh 1 , Carolin König 1
Affiliation  

We propose a hybrid anharmonic–harmonic scheme for vibrational broadenings, which embeds a reduced-space vibrational configuration interaction (VCI) anharmonic wave function treatment in the independent-mode displaced harmonic oscillator (IMDHO) model. The resulting systematically-improvable VCI-in-IMDHO model allows including the vibronic effects of all vibrational degrees of freedom, while focusing the effort on the important degrees of freedom with minimal extra computational effort compared to a reduced-space VCI treatment. We show for oligothiophene examples that the VCI-in-IMDHO approach can yield accurate vibrational profiles employing smaller vibrational spaces in the VCI part than the reduced-space VCI approach. By this, the VCI-in-IMDHO model enables accurate calculation of vibrational profiles of common fluorescent dyes with more than 100 vibrational degrees of freedom. We illustrate this for three examples of fluorescent biomarkers of current interest. These are the oligothiophene-based fluorescent dye called HS84, 1,4-diphenylbutadiene, and an anthracene diimide. For all examples, we assess the impact of the anharmonic treatment on the vibrational broadening, which we find to be more pronounced for the intensities than for the peak positions.

中文翻译:

为荧光生物标志物量身定制的非谐波-谐波振动曲线

我们提出了一种用于振动展宽的混合非谐-谐方案,该方案在独立模式位移谐振子 (IMDHO) 模型中嵌入了缩减空间振动配置相互作用 (VCI) 非谐波函数处理。由此产生的可系统改进的 VCI-in-IMDHO 模型允许包括所有振动自由度的振动效应,同时将精力集中在重要的自由度上,与缩减空间的 VCI 处理相比,额外的计算工作量最少。我们针对低聚噻吩的例子表明,与缩小空间的 VCI 方法相比,VCI-in-IMDHO 方法可以产生准确的振动曲线,在 VCI 部分采用更小的振动空间。这样,VCI-in-IMDHO 模型能够准确计算常见荧光染料的振动曲线,具有超过 100 个振动自由度。我们用三个当前感兴趣的荧光生物标志物的例子来说明这一点。这些是称为 HS84 的基于低聚噻吩的荧光染料、1,4-二苯基丁二烯和蒽二亚胺。对于所有示例,我们评估了非谐处理对振动展宽的影响,我们发现强度比峰值位置更明显。
更新日期:2022-06-13
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