TY - JOUR
T1 - Quantum Defect Sensitization via Phase-Changing Supercharged Antibody Fragments
AU - Kim, Mijin
AU - McCann, James J.
AU - Fortner, Jacob
AU - Randall, Ewelina
AU - Chen, Chen
AU - Chen, Yu
AU - Yaari, Zvi
AU - Wang, Yu Huang
AU - Koder, Ronald L.
AU - Heller, Daniel A.
N1 - Publisher Copyright:
© 2024 American Chemical Society
PY - 2024/5
Y1 - 2024/5
N2 - Quantum defects in single-walled carbon nanotubes promote exciton localization, which enables potential applications in biodevices and quantum light sources. However, the effects of local electric fields on the emissive energy states of quantum defects and how they can be controlled are unexplored. Here, we investigate quantum defect sensitization by engineering an intrinsically disordered protein to undergo a phase change at a quantum defect site. We designed a supercharged single-chain antibody fragment (scFv) to enable a full ligand-induced folding transition from an intrinsically disordered state to a compact folded state in the presence of a cytokine. The supercharged scFv was conjugated to a quantum defect to induce a substantial local electric change upon ligand binding. Employing the detection of a proinflammatory biomarker, interleukin-6, as a representative model system, supercharged scFv-coupled quantum defects exhibited robust fluorescence wavelength shifts concomitant with the protein folding transition. Quantum chemical simulations suggest that the quantum defects amplify the optical response to the localization of charges produced upon the antigen-induced folding of the proteins, which is difficult to achieve in unmodified nanotubes. These findings portend new approaches to modulate quantum defect emission for biomarker sensing and protein biophysics and to engineer proteins to modulate binding signal transduction (Figure Presented).
AB - Quantum defects in single-walled carbon nanotubes promote exciton localization, which enables potential applications in biodevices and quantum light sources. However, the effects of local electric fields on the emissive energy states of quantum defects and how they can be controlled are unexplored. Here, we investigate quantum defect sensitization by engineering an intrinsically disordered protein to undergo a phase change at a quantum defect site. We designed a supercharged single-chain antibody fragment (scFv) to enable a full ligand-induced folding transition from an intrinsically disordered state to a compact folded state in the presence of a cytokine. The supercharged scFv was conjugated to a quantum defect to induce a substantial local electric change upon ligand binding. Employing the detection of a proinflammatory biomarker, interleukin-6, as a representative model system, supercharged scFv-coupled quantum defects exhibited robust fluorescence wavelength shifts concomitant with the protein folding transition. Quantum chemical simulations suggest that the quantum defects amplify the optical response to the localization of charges produced upon the antigen-induced folding of the proteins, which is difficult to achieve in unmodified nanotubes. These findings portend new approaches to modulate quantum defect emission for biomarker sensing and protein biophysics and to engineer proteins to modulate binding signal transduction (Figure Presented).
UR - https://www.scopus.com/pages/publications/85192049504
U2 - 10.1021/jacs.4c00149
DO - 10.1021/jacs.4c00149
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C2 - 38687180
AN - SCOPUS:85192049504
SN - 0002-7863
VL - 146
SP - 12454
EP - 12462
JO - Journal of the American Chemical Society
JF - Journal of the American Chemical Society
IS - 18
ER -