Dual-Comb Coherent Raman Spectroscopy with near 100% Duty Cycle

Kameyama, Risako; Takizawa, Shigeo; Hiramatsu, Kazumasa; Goda, Keisuke

doi:10.1021/acsphotonics.0c01656

Cited by 25 publications

(22 citation statements)

References 32 publications

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“…For sorting other cell types (mammalian, yeast, and bacteria) that do not feature the same high concentration of target analytes, sensitivity enhancements to our machine are necessary. Sensitivity enhancements have been demonstrated for coherent Raman measurement using heterodyne detection, [55,56] Sagnac interferometry, [57] polarization-selective measurement, [58,59] and quasi-dual comb laser systems, [60] all of which could be integrated into our system. Sensitivity for Raman-inactive molecules can also be enabled by stepping out of the label-free regime and employing Raman tags.…”

Section: Discussionmentioning

confidence: 99%

High‐Throughput Raman‐Activated Cell Sorting in the Fingerprint Region

Lindley

Pablo

Peterson

et al. 2022

Adv Materials Technologies

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Cell sorting is the workhorse of biological research and medicine. [1] Cell sorters are commonly used to sort heterogeneous populations of cells based on their intrinsic features and have numerous applications in microbiology, immunology, virology, stem cell biology, and metabolic engineering. [2][3][4][5][6] While several schemes have been developed for sorting cells based on features such as size, [7] morphology, [8][9][10] viability, [11,12] and surface antigens, [13] those able to sort at high throughput for intracellular chemical content are limited to fluorescence-activated and Raman-activated cell sorting (FACS and RACS, respectively). [1,14] In both methods, sorting is accomplished by a stepwise automatic process: 1) measurement of chemical content with single-cell resolution, 2) analysis of the measurement data to identify cells of interest, and 3) mechanical separation of target cells from the original sample. [1] FACS machines commonly identify molecular targets by signals from attached exogenous fluorophores or coexpressed transgenic fluorescent proteins. This indirect detection scheme is often referred to as labeled detection. [1] Although fluorescent labeling is essential for microbiological research, the use of labels has inherrent drawbacks. These include reduced cellular vitality due to the cytotoxicity of labels themselves, nonspecific binding of labels, a lack of labels or transfection methods for many molecular targets and species, incompatibility with human-targeted cell therapies, and increased experimental complexity imposed by labeling protocols. [14] On the other hand, RACS machines directly identify target molecules in a label-free manner via Raman spectroscopy, which measures the inelastic scattering of incident photons by characteristic molecular vibrations. [14] The chemical specificity of this optical measurement contrasts with non-chemically-specific label-free methods such as impedance-based sorting for cell viability and image-based sorting for morphology or deformability. [10][11][12] To date, FACS technology is well developed, commercialized, and broadly adopted, while RACS is nascent and comprised of a small number of lab-based demonstrations. [14][15][16][17][18][19][20][21][22][23][24][25][26] A major hurdle in the broad deployment of RACS for biomedical applications is the weak signal produced by the Raman scattering process. This necessitates comparatively Cell sorting is the workhorse of biological research and medicine. Cell sorters are commonly used to sort heterogeneous cell populations based on their intrinsic features. Raman-activated cell sorting (RACS) has recently received considerable interest by virtue of its ability to discriminate cells by their intracellular chemical content, in a label-free manner. However, the broad deployment of RACS beyond lab-based demonstrations is hindered by a fundamental trade-off between throughput and measurement bandwidth (i.e., cellular information content). Here this trade-off is overcome and broadband RACS in the fingerprint reg...

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Section: Discussionmentioning

confidence: 99%

High‐Throughput Raman‐Activated Cell Sorting in the Fingerprint Region

Lindley

Pablo

Peterson

et al. 2022

Adv Materials Technologies

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“…This change would also increase the spectral acquisition rate in DIVS, limited in our system by the speed of mechanical scanning of the probe delay. In principle, DIVS is also fully compatible with the faster method of pumpprobe group delay scanning used in quasi-dual-comb CARS spectroscopy 41 (100,000 spectra∕s).…”

Section: Discussionmentioning

confidence: 99%

Ultrafast impulsive Raman spectroscopy across the terahertz–fingerprint region

et al. 2022

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Broadband Raman spectroscopy (detection bandwidth >1000 cm −1 ) is a valuable and widely used tool for understanding samples via label-free measurements of their molecular vibrations. Two important Raman spectral regions are the chemically specific "fingerprint" (200 to 1800 cm −1 ) and "low-frequency" or "terahertz" (THz) (<200 cm −1 ; <6 THz) regions, which mostly contain intramolecular and intermolecular vibrations, respectively. These two regions are highly complementary; broadband simultaneous measurement of both regions can provide a big picture comprising information about molecular structures and interactions. Although techniques for acquiring broadband Raman spectra covering both regions have been demonstrated, these methods tend to have spectral acquisition rates <10 spectra∕s, prohibiting high-speed applications, such as Raman imaging or vibrational detection of transient phenomena. Here, we demonstrate a single-laser method for ultrafast (24,000 spectra∕s) broadband Raman spectroscopy covering both THz and fingerprint regions. This is achieved by simultaneous detection of Sagnac-enhanced impulsive stimulated Raman scattering (SE-ISRS; THz-sensitive) and Fourier-transform coherent anti-Stokes Raman scattering (FT-CARS; fingerprint-sensitive). With dual-detection impulsive vibrational spectroscopy, the SE-ISRS signal shows a >500× enhancement of <6.5 THz sensitivity compared with that of FT-CARS, and the FT-CARS signal shows a >10× enhancement of fingerprint sensitivity above 1000 cm −1 compared with that of SE-ISRS.

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“…88 Outside of the microscope, even higher spectral acquisition rates have been reached, 89 up to 100;000 spectra∕s in the form of dual-comb coherent Raman spectroscopy. 90,91 6 Taking Stock and Looking Ahead…”

Section: Speedmentioning

confidence: 99%

Coherent Raman scattering microscopy: capable solution in search of a larger audience

Prince

Potma

2021

J. Biomed. Opt.

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Significance: Coherent Raman scattering (CRS) microscopy is an optical imaging technique with capabilities that could benefit a broad range of biomedical research studies.Aim: We reflect on the birth, rapid rise, and inescapable growing pains of the technique and look back on nearly four decades of developments to examine where the CRS imaging approach might be headed in the next decade to come.Approach: We provide a brief historical account of CRS microscopy, followed by a discussion of the challenges to disseminate the technique to a larger audience. We then highlight recent progress in expanding the capabilities of the CRS microscope and assess its current appeal as a practical imaging tool.Results: New developments in Raman tagging have improved the specificity and sensitivity of the CRS technique. In addition, technical advances have led to CRS microscopes that can capture hyperspectral data cubes at practical acquisition times. These improvements have broadened the application space of the technique. Conclusion:The technical performance of the CRS microscope has improved dramatically since its inception, but these advances have not yet translated into a substantial user base beyond a strong core of enthusiasts. Nonetheless, new developments are poised to move the unique capabilities of the technique into the hands of more users.

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Dual-Comb Coherent Raman Spectroscopy with near 100% Duty Cycle

Cited by 25 publications

References 32 publications

High‐Throughput Raman‐Activated Cell Sorting in the Fingerprint Region

High‐Throughput Raman‐Activated Cell Sorting in the Fingerprint Region

Ultrafast impulsive Raman spectroscopy across the terahertz–fingerprint region

Coherent Raman scattering microscopy: capable solution in search of a larger audience

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