Multimodal Metabolic Imaging Reveals Pigment Reduction and Lipid Accumulation in Metastatic Melanoma
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Objective and Impact Statement . Molecular signatures are needed for early diagnosis and improved treatment of metastatic melanoma. By high-resolution multimodal chemical imaging of human melanoma samples, we identify a metabolic reprogramming from pigmentation to lipid droplet (LD) accumulation in metastatic melanoma. Introduction . Metabolic plasticity promotes cancer survival and metastasis, which promises to serve as a prognostic marker and/or therapeutic target. However, identifying metabolic alterations has been challenged by difficulties in mapping localized metabolites with high spatial resolution. Methods . We developed a multimodal stimulated Raman scattering and pump-probe imaging platform. By time-domain measurement and phasor analysis, our platform allows simultaneous mapping of lipids and pigments at a subcellular level. Furthermore, we identify the sources of these metabolic signatures by tracking deuterium metabolites at a subcellular level. By validation with mass spectrometry, a specific fatty acid desaturase pathway was identified. Results . We identified metabolic reprogramming from a pigment-containing phenotype in low-grade melanoma to an LD-rich phenotype in metastatic melanoma. The LDs contain high levels of cholesteryl ester and unsaturated fatty acids. Elevated fatty acid uptake, but not de novo lipogenesis, contributes to the LD-rich phenotype. Monounsaturated sapienate, mediated by FADS2, is identified as an essential fatty acid that promotes cancer migration. Blocking such metabolic signatures effectively suppresses the migration capacity both in vitro and in vivo . Conclusion . By multimodal spectroscopic imaging and lipidomic analysis, the current study reveals lipid accumulation, mediated by fatty acid uptake, as a metabolic signature that can be harnessed for early diagnosis and improved treatment of metastatic melanoma.
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The drug-resistant U cancer cell state displays increased activity of enzymes promoting the synthesis and uptake of PUFAs such as arachidonic acid and linolenic acid.
“The drug-resistant, U cancer cell state displays increased activity of enzymes promoting the synthesis and uptake of PUFAs (16, 17), such as arachidonic acid (AA, C20:4) and linolenic acid (C18:2), which are major substrates for ROS attack.”
From Secreted Apoe rewires melanoma cell state vulnerability to ferroptosis (2024) · cites this paper as [17]
Results §2.3 reports increased fatty-acid uptake in MITFlow/AXLhigh melanoma cells, and the Discussion says FADS2 can generate polyunsaturated fatty acids. The paper does not show increased uptake or synthesis of the named PUFAs in a drug-resistant U state; its measured uptake concerns palmitate and oleate, and its principal desaturation finding concerns monounsaturated sapienate. (LLM, conf=0.86)
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Stimulated Raman Scattering Imaging Enabled Biomarker Discovery for Precision Medicine
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BINGO: a blind unmixing algorithm for ultra-multiplexing fluorescence images
Huang, X., Gao, X., & Fu, L. (2024) · Bioinformatics · doi:10.1093/bioinformatics/btae052 · Cited by 4 · see citing works
Genetic Insight into Expression-Defined Melanoma Subtypes and Network Mechanisms: An in Silico Study
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Raman metabolic imaging: an emerging tool for the study of drug resistance in cancer
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Photothermally Detected Stimulated Raman Microscopy towards Ultrasensitive Chemical ImagingPreprint
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Targeting de novo lipogenesis improves gemcitabine efficacy in pancreatic ductal adenocarcinomaPreprint
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Self-citationStimulated Raman scattering imaging for studying sterol synthesis
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Self-citationIn Situ Lipid Profiling at Submicron Resolution by Hyperspectral Stimulated Raman Imaging
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Self-citationLipid profiling at submicron resolution by hyperspectral stimulated Raman imaging
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Molecular Histology for Azoospermia by Submicron-Resolution Mid-IR Photothermal Spectroscopy
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Self-citationCholesteryl Ester as a Prognostic Biomarker In IDH-wildtype GlioblastomaPreprint
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- Authors
- Lee, H. J., Chen, Z., Collard, M., Chen, F., Chen, J. G., Wu, M., Alani, R. M., & Cheng, J.-X.
- Affiliations
- Boston University (US)
- Corresponding author
- Alani, Rhoda M.
- Cheng, Ji-Xin
- ORCID
- Venue
- BME Frontiers
- Published
- 2021-01
- Volume
- 2021
- Pages
- 9860123-9860123
- ISSN
- 2765-8031 (ISSN-L)
- PMC
- PMC10521760
- OpenAlex
- W3204110732
- Cited by
- 38
- References
- 66
- Citations by year
- 2026: 4 · 2025: 9 · 2024: 10 · 2023: 11 · 2022: 4
- FWCI
- 2.49
- Type
- journal article
- Language
- en
- Open access
- diamond
- doi.org
- Locations
- BME Frontiers (publishedVersion, cc-by)
- PubMed Central (publishedVersion, cc-by)
- PubMed (publishedVersion)
- DOAJ (DOAJ: Directory of Open Access Journals) (submittedVersion, cc-by-sa)
- Funders
- National Institutes of Health (R35 GM136223, R33 CA223581, S10OD024993)
- Boston University
- IU Simon Cancer Center (P30 CA082709)
- Topics
- Life Sciences › Biochemistry, Genetics and Molecular Biology › Cancer Research › Cancer, Lipids, and Metabolism
- Life Sciences › Biochemistry, Genetics and Molecular Biology › Biophysics › Spectroscopy Techniques in Biomedical and Chemical Research
- Life Sciences › Biochemistry, Genetics and Molecular Biology › Molecular Biology › Metabolomics and Mass Spectrometry Studies
- Keywords
- metastatic melanoma, lipid droplet accumulation, pigment reduction, metabolic reprogramming, stimulated Raman scattering microscopy, pump-probe imaging, phasor analysis, fatty acid desaturase, FADS2, fatty acid uptake, cholesterol esters, unsaturated fatty acids, tumor cell migration, deuterium labeling
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