Amorphous Quantum Nanomaterials.
Ferdinand F E KohleJoshua A HinckleySongying LiNikhil DhawanWilliam P KattJacob A ErstlingUlrike Werner-ZwanzigerJosef ZwanzigerRichard A CerioneUlrich B WiesnerPublished in: Advanced materials (Deerfield Beach, Fla.) (2018)
In quantum materials, macroscopic behavior is governed in nontrivial ways by quantum phenomena. This is usually achieved by exquisite control over atomic positions in crystalline solids. Here, it is demonstrated that the use of disordered glassy materials provides unique opportunities to tailor quantum material properties. By borrowing ideas from single-molecule spectroscopy, single delocalized π-electron dye systems are isolated in relatively rigid ultrasmall (<10 nm diameter) amorphous silica nanoparticles. It is demonstrated that chemically tuning the local amorphous silica environment around the dye over a range of compositions enables exquisite control over dye quantum behavior, leading to efficient probes for photodynamic therapy (PDT) and stochastic optical reconstruction microscopy (STORM). The results suggest that efficient fine-tuning of light-induced quantum behavior mediated via effects like spin-orbit coupling can be effectively achieved by systematically varying averaged local environments in glassy amorphous materials as opposed to tailoring well-defined neighboring atomic lattice positions in crystalline solids. The resulting nanoprobes exhibit features proven to enable clinical translation.
Keyphrases
- single molecule
- room temperature
- molecular dynamics
- photodynamic therapy
- energy transfer
- living cells
- high resolution
- fluorescence imaging
- monte carlo
- highly efficient
- density functional theory
- ionic liquid
- solid state
- air pollution
- small molecule
- walled carbon nanotubes
- high speed
- fluorescent probe
- electron microscopy
- quantum dots