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Abstract
Plasmon-driven molecular machines with ultrafast motion at the femtosecond scale are effective for treatment of cancer and other diseases. We recently showed that cyanine dyes act as molecular jackhammers (MJH) through vibronic (vibrational and electronic mode coupling) driven activation that causes the molecule to stretch longitudinally and axially through concerted whole molecule vibrations. However, the theoretical and experimental underpinnings of these plasmon-driven motions in molecules are difficult to assess. Here we describe the use of near-infrared (NIR) light activated plasmons in a broad array of MJH that mechanically disassemble membranes and cytoskeletons in human melanoma A375 cells. The characteristics of plasmon-driven molecular mechanical disassembly of supramolecular biological structures are observed and recorded using real-time fluorescence confocal microscopy. Molecular plasmon resonances in MJH are quantified through a new experimental plasmonicity index method. This is done through the measurement of the UV-vis-NIR spectra in various solvents, and quantification of the optical response as a function of the solvent polarity. Structure-activity relationships were used to optimize the synthesis of plasmon-driven MJH, applying them to eradicate human melanoma A375 cells at low lethal concentrations of 75 nM and 80 mWcm-2 of 730 nm NIR-light for 10 min.
Supplementary materials
Title
Supplementary Materials for How to build plasmon-driven molecular jackhammers that disassemble cell membranes and cytoskeletons in cancer
Description
The PDF file includes:
Materials and Methods
Figure S1 to S47
Caption for Movie S1
Materials and methods for the chemical synthesis of MJH library
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Title
Movie S1. Plasmon-driven MJH Cy5.5-amine disassembles and breaks plasma membranes upon light activation
Description
Movie S1. Plasmon-driven MJH Cy5.5-amine disassembles and breaks plasma membranes upon light activation. A375 cells are recorded in the confocal microscope while under treatment with MJH Cy5.5-amine and 640 nm light-exposure (exposure time = 10 min). Loading concentration of Cy5.5-amine: Cloading = 4 µM for 30 min. CellMask Green is added to visualize the plasma membrane in green, loading concentration Cloading = 5 µgmL-1 for 30 min, λex = 488 nm, and λem = 500-550 nm. The DAPI staining indicates the permeabilization of the plasma membrane. Loading concentration of DAPI: Cloading = 1 µM, λex = 405 nm, and λem = 425-475 nm.
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