Far-Red Emission of mPlum Fluorescent Protein Results from Excited-State Interconversion between Chromophore Hydrogen-Bonding States

J Phys Chem Lett. 2016 Jun 16;7(12):2170-4. doi: 10.1021/acs.jpclett.6b00823. Epub 2016 May 26.

Abstract

Fluorescent proteins with large Stokes shifted emission beyond 600 nm are actively sought for live-cell imaging applications. The mechanism of excited-state relaxation leading to the Stokes shift in the mPlum fluorescent protein, which emits at a peak wavelength of 650 nm, has been previously investigated by both ultrafast spectroscopy and theoretical methods. Here, we report that femtosecond time-resolved area-normalized emission spectra of mPlum show a clear isoemissive point. This feature can only result from a system with two emitting states, rather than a system that undergoes a continuous spectral red shift, for example, as expected from typical solvation. Global analysis of the femtosecond time-resolved fluorescence spectra reveals time constants associated with chromophore relaxation, excited-state population transfer, and an excited-state lifetime of the final state. The observations confirm the findings of recent quantum chemical calculations on mPlum.

Publication types

  • Letter

MeSH terms

  • Green Fluorescent Proteins / chemistry*
  • Hydrogen Bonding
  • Molecular Dynamics Simulation
  • Quantum Theory
  • Spectrometry, Fluorescence / methods*

Substances

  • Green Fluorescent Proteins