将当代理论计算方法用于计算当前科学及技术感兴趣的复杂体系的光谱时面临巨大挑战。本项目将致力于发展和改进与复杂体系光谱计算相关的电子结构理论及量子动力学计算方法，特别是发展快速的理论计算方法和程序去计算生物大分子、分子聚集体、分子/半导体-贵金属纳米粒子等体系的振动谱、振动精度的电子谱及共振拉曼谱等。在量子动力学方面，拟进一步发展包含FC、HT、模混合效果的时间相关函数方法去计算谱微分截面。在电子结构方面将进一步发展和改进基于DFT/TDDFT 的基态、激发态能量及跃迁偶极对核坐标的解析导数方法；将已建立的程序并行和实现线性标度算法；发展量子-经典组合方法去描述镶嵌于凝聚环境中体系的基、激发态几何和电子结构，电-声耦合强度等；构建激子-激子、激子-等离子激元间相互作用的有效模型哈密顿；建立高效的计算软件，并用于描述光合作用体系、有机太阳能电池、分子/半导体-金属纳米粒子等体系的光物理性质。

The progress of theoretical and computational methods for the optical spectra of complex systems falls largely behind the innovation of lasers and spectral instruments. Therefore, the current theoretical and computational methods present a substantial challenge when they are applied to calculate the spectra of complex systems which are interesting to the current scientific and technological research. This project aims to develop or improve the relevant electronic structure theory and quantum dynamics methods for the vibrational and vibronic spectra, such as the vibrationally-resolved electronic spectra and resonance Raman spectra, of biological systems, molecular aggregates, and hybird molecule/semiconductor–noble metal nanoparticles. In quantum dynamics, the project will derive the spectral differential cross sections in time domain with inclusion of the mode-mixing,Franck-Condon (FC) and Herzberg-Teller(HT) effects. In the electronic structure theory, the project will further develop or improve the analytic geometric derivative approaches for the ground- and excited-state energies and the one- or two-photon transition tensors within the framework of density functional theory (DFT) and time-dependent density functional theory (TDDFT); realize the pallelization of developed codes and linear scaling calculations; further develop the hybrid quantum-classical methods, especially those based on TDDFT, for the systems embodied in the condensed-phase environments; build the effective model Hamiltonian for the systems with exciton-exciton or exciton-plasmon interactions. At the end, the computationally efficient and user-friendly program packages for the computation of vibrarional and vibronic spectra will be constructed. Finally, the project will efficiently connects the developed quantum dynamics and electronic structure methods with the classical molecular mechanics or polarizable continuum solvent model or electromagnetic theory to achieve the multi-scale simulations for realistic biological systems, organic solar cells and molecule-noble metal nanoparticles, reveal their photophysical properties.