Application of the Time-Domain Multichromophoric Fluorescence Resonant Energy Transfer Method in the NISE Programme

Area of Science:

• Computational Chemistry
• Quantum Mechanics
• Biophysics

Background:

• Efficient simulation of energy transfer is crucial for understanding complex molecular systems.
• Existing methods may struggle with the scale and complexity of systems like photosynthetic complexes.

Purpose of the Study:

• To implement and validate a novel time-domain multichromophoric fluorescence resonant energy transfer (TD-MCFRET) approach within the numerical integration of the Schrödinger equation (NISE) program.
• To enable efficient and accurate simulation of incoherent energy transfer in large molecular systems.

Main Methods:

• Developed a segmentation protocol to divide complex systems into manageable parts.
• Incorporated a modified thermal correction to ensure detailed balance.
• Integrated the TD-MCFRET approach into the NISE program for systematic calculation of energy transfer rates.

Main Results:

• Successfully applied the TD-MCFRET method to various test cases, including linear aggregates and biological systems (B850 rings, Fenna-Matthews-Olson complex).
• Achieved excellent agreement between simulation results and previous experimental or theoretical studies.
• Demonstrated the accuracy and efficiency of the implemented TD-MCFRET approach.

Conclusions:

• The implemented TD-MCFRET method provides an accurate and efficient tool for calculating energy transfer rates in large molecular systems.
• This approach is expected to be broadly applicable to diverse systems and advance future simulations of multidimensional electronic spectra.