Highly sensitive chemiluminescence imaging of misfolded proteins in neurodegenerative models

B Biyue Zhu (Athinoula A. Martinos Center for Biomedical Imaging, Department of Radiology, Massachusetts General Hospital/Harvard Medical School) Z Zhenhua Liu (Shanghai Collaborative Innovation Center of Agri-Seeds, School of Agriculture and Biology, Shanghai Jiao Tong University) R Richard Van (Department of Chemistry and Biochemistry, Stephenson Life Sciences Research Center, University of Oklahoma) H Huizhe Wang (Athinoula A. Martinos Center for Biomedical Imaging, Department of Radiology, Massachusetts General Hospital/Harvard Medical School) S Shi Kuang (State Key Laboratory of Chemo and Biosensing, College of Chemistry and Chemical Engineering, Hunan Provincial Key Laboratory of Biomacromolecular Chemical Biology) Y Yuntao Jia (Department of Pharmacy, Children’s Hospital of Chongqing Medical University, National Clinical Research Center for Children and Adolescents’ Health and Diseases, Ministry of Education Key Laboratory of Child Development and Disorders, International Science and Technology Cooperation base of Child Development and Critical Disorders, Chongqing Key Laboratory of Child Neurodevelopment and Cognitive Disorders) E Erick Calderon Leon (Department of Chemistry and Biochemistry, Stephenson Life Sciences Research Center, University of Oklahoma) F Fan Yang J Jing Zhang J Jun Yang H Howard Hong (Athinoula A. Martinos Center for Biomedical Imaging, Department of Radiology, Massachusetts General Hospital/Harvard Medical School) F Fleur Lobo (Department of Chemistry and Biochemistry, Stephenson Life Sciences Research Center, University of Oklahoma) A Astra Yu (Athinoula A. Martinos Center for Biomedical Imaging, Department of Radiology, Massachusetts General Hospital/Harvard Medical School) J Johnson Wang (Athinoula A. Martinos Center for Biomedical Imaging, Department of Radiology, Massachusetts General Hospital/Harvard Medical School) R Rudolph E. Tanzi C Can Zhang (School of Integrated Circuits and Electronics, MIIT Key Laboratory for Low-Dimensional Quantum Structure and Devices) X Xiaobo Mao (Neuroregeneration and Stem Cell Programs, Institute for Cell Engineering, Department of Neurology, Johns Hopkins University School of Medicine) Y Yihan Shao (Department of Chemistry) C Chongzhao Ran (Athinoula A. Martinos Center for Biomedical Imaging, Department of Radiology, Massachusetts General Hospital/Harvard Medical School)

Abstract

Protein misfolding in the brain is a key pathological hallmark of neurodegenerative diseases. Optical imaging of misfolded proteins in disease models is essential for elucidating etiology and early diagnosis. However, developing specific optical imaging probes for each misfolded protein is time-consuming and challenging, leaving many pathological targets without effective detection tools, especially for in vivo imaging. Here, we present a dual-mode chemiluminescence strategy that enables both generic and specific detection of misfolded proteins using a single probe platform. In the generic mode, we demonstrate that ADLumin-1, a chemiluminescent probe, enables highly sensitive detection of diverse misfolded proteins in vitro, achieving up to 128-fold higher signal enhancement than Thioflavin T, and allows noninvasive imaging in mice models of Parkinson’s disease, Alzheimer’s disease, and amyotrophic lateral sclerosis. In the specific mode, ADLumin-1 combined with protein misfolding cyclic amplification allows femtomolar-level detection of α-synuclein in cerebrospinal fluid, while integration with a bio-orthogonal chemiluminescence resonance energy transfer technique enables in vivo discrimination of α-synuclein from Aβ. This dual-mode, modular approach offers a practical solution to the current probe limitations, with potential preclinical and clinical applications in neurodegenerative disorders.

Article Details

Volume / Issue Vol. 123, Issue 2
Published January 13, 2026
ISSN 0027-8424
Publisher National Academy of Sciences

Authors (19)

B

Biyue Zhu

Athinoula A. Martinos Center for Biomedical Imaging, Department of Radiology, Massachusetts General Hospital/Harvard Medical School

Z

Zhenhua Liu

Shanghai Collaborative Innovation Center of Agri-Seeds, School of Agriculture and Biology, Shanghai Jiao Tong University

R

Richard Van

Department of Chemistry and Biochemistry, Stephenson Life Sciences Research Center, University of Oklahoma

H

Huizhe Wang

Athinoula A. Martinos Center for Biomedical Imaging, Department of Radiology, Massachusetts General Hospital/Harvard Medical School

S

Shi Kuang

State Key Laboratory of Chemo and Biosensing, College of Chemistry and Chemical Engineering, Hunan Provincial Key Laboratory of Biomacromolecular Chemical Biology

Y

Yuntao Jia

Department of Pharmacy, Children’s Hospital of Chongqing Medical University, National Clinical Research Center for Children and Adolescents’ Health and Diseases, Ministry of Education Key Laboratory of Child Development and Disorders, International Science and Technology Cooperation base of Child Development and Critical Disorders, Chongqing Key Laboratory of Child Neurodevelopment and Cognitive Disorders

E

Erick Calderon Leon

Department of Chemistry and Biochemistry, Stephenson Life Sciences Research Center, University of Oklahoma

F

Fan Yang

J

Jing Zhang

J

Jun Yang

H

Howard Hong

Athinoula A. Martinos Center for Biomedical Imaging, Department of Radiology, Massachusetts General Hospital/Harvard Medical School

F

Fleur Lobo

Department of Chemistry and Biochemistry, Stephenson Life Sciences Research Center, University of Oklahoma

A

Astra Yu

Athinoula A. Martinos Center for Biomedical Imaging, Department of Radiology, Massachusetts General Hospital/Harvard Medical School

J

Johnson Wang

Athinoula A. Martinos Center for Biomedical Imaging, Department of Radiology, Massachusetts General Hospital/Harvard Medical School

R

Rudolph E. Tanzi

C

Can Zhang

School of Integrated Circuits and Electronics, MIIT Key Laboratory for Low-Dimensional Quantum Structure and Devices

X

Xiaobo Mao

Neuroregeneration and Stem Cell Programs, Institute for Cell Engineering, Department of Neurology, Johns Hopkins University School of Medicine

Y

Yihan Shao

Department of Chemistry

C

Chongzhao Ran

Athinoula A. Martinos Center for Biomedical Imaging, Department of Radiology, Massachusetts General Hospital/Harvard Medical School