Super-resolution imaging of non-fluorescent molecules by photothermal relaxation localization microscopy

Fu, Pengcheng; Cao, Wanlin; Chen, Tianrun; Huang, Xiangjie; Le, Taoran; Zhu, Shi‐Yao; Wang, Da-Wei; Lee, Hyeon Jeong; Zhang, De‐Long

doi:10.1038/s41566-022-01143-3

Cited by 40 publications

(25 citation statements)

References 51 publications

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“…Optically detected photothermal microscopy has been well developed 27 and has reached the sensitivity down to a single molecule 28 . In photothermal spectroscopy, first reported in 1970s 29 , an optical absorption raises the local temperature, creating local change of refractive index, which is measured with a probing beam.…”

Section: Figmentioning

confidence: 99%

“…Early photothermal microscopy works focused on electronic absorption, targeting non-fluorescent dye molecules or metal nanostructures 27 . Recently developed mid-infrared photothermal (MIP) microscopy provides universal infrared active vibrational spectroscopic features, offers a detection sensitivity at micro-molar level, and creates a spatial resolution at the visible diffraction limit 30,31 or even higher by probing the high harmonic signals 32 . While MIP microscopy has allowed chemical imaging of living cells, strong water absorption in the infrared region remains a fundamental limitation, which diminishes the infrared pump at a high rate and creates a background at the protein amide I region.…”

Section: Introductionmentioning

confidence: 99%

“…While the future of this method is bright, it is 51 currently limited by the low squeeze efficiency and 52 decoherence in complex imaging systems. On the boost 53 of SRS signal, different photophysical processes have 54 been utilized to increase the cross-section, hence the 55 signal intensity, including electronic pre-resonance 56 SRS [21][22][23] , plasmon enhanced SRS 24 detection sensitivity at micro-molar level, and creates a spatial resolution at the visible diffraction limit 30,31 or even higher by probing the high harmonic signals 32 . While MIP microscopy has allowed chemical imaging of living cells, strong water absorption in the infrared region remains a fundamental limitation, which diminishes the infrared pump at a high rate and creates a background at the protein amide I region.…”

mentioning

confidence: 99%

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Photothermally Detected Stimulated Raman Microscopy towards Ultrasensitive Chemical Imaging

Zhu

et al. 2023

Preprint

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Stimulated Raman scattering (SRS) microscopy has shown enormous potential in revealing molecular structures, dynamics and coupling in a complex system. However, the bond-detection sensitivity of SRS microscopy is fundamentally limited to milli-molar level due to the shot noise and the small modulation depth in either pump or Stokes beam4. Here, to overcome this barrier, we revisit SRS from the perspective of energy deposition. The SRS process pumps molecules to their vibrational excited states. The thereafter relaxation heats up the surrounding and induces a change in refractive index. By probing the refractive index change with a continuous wave beam, we introduce stimulated Raman photothermal (SRP) microscopy, where a >500-fold boost of modulation depth is achieved on dimethyl sulfide with conserved average power. Versatile applications of SRP microscopy on viral particles, cells, and tissues are demonstrated. With much improved signal to noise ratio compared to SRS, SRP microscopy opens a new way to perform vibrational spectroscopic imaging with ultrahigh sensitivity and minimal water absorption.

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Section: Figmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

mentioning

confidence: 99%

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Photothermally Detected Stimulated Raman Microscopy towards Ultrasensitive Chemical Imaging

Zhu

et al. 2023

Preprint

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“…First, the spatial resolution in MIP is usually determined by the diffraction limit of the visible probe beam, which is much higher than the long-wavelength IR. The reported lateral and axial resolution in MIP have reached ∼300 nm and ∼1.5 μm, respectively. , The spatial resolution could be further improved to the super-resolution regime (∼120 nm) by differentiating the spatially heterogeneous photothermal response in the temporal domain through high-harmonic lock-in demodulation . Second, MIP provides reduced water background.…”

Section: Coherent Raman Scattering: Srs and Cars Microscopymentioning

confidence: 99%

“… 8 , 81 The spatial resolution could be further improved to the super-resolution regime (∼120 nm) by differentiating the spatially heterogeneous photothermal response in the temporal domain through high-harmonic lock-in demodulation. 82 Second, MIP provides reduced water background. As water holds a large heat capacity, only a small change in the temperature, reflected in a slight change in refractive index, can be induced by IR radiations.…”

Section: Coherent Raman Scattering: Srs and Cars Microscopymentioning

confidence: 99%

Toward the Next Frontiers of Vibrational Bioimaging

Wang

Lee

2023

Chemical & Biomedical Imaging

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Chemical imaging based on vibrational contrasts can extract molecular information entangled in complex biological systems. To this end, nonlinear Raman scattering microscopy, mid-infrared photothermal (MIP) microscopy, and atomic force microscopy (AFM)-based force-detected photothermal microscopies are emerging with better chemical sensitivity, molecular specificity, and spatial resolution than conventional vibrational methods. Their utilization in bioimaging applications has provided biological knowledge in unprecedented detail. This Perspective outlines key methodological developments, bioimaging applications, and recent technical innovations of the three techniques. Representative biological demonstrations are also highlighted to exemplify the unique advantages of obtaining vibrational contrasts. With years of effort, these three methods compose an expanding vibrational bioimaging toolbox to tackle specific bioimaging needs, benefiting many biological investigations with rich information in both label-free and labeling manners. Each technique will be discussed and compared in the outlook, leading to possible future directions to accommodate growing needs in vibrational bioimaging.

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Proton‐Assisted Assembly of Colloidal Nanoparticles into Wafer‐Scale Monolayers in Seconds

Kim,

Lee,

Kim

et al. 2024

Advanced Materials

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Underwater adhesion processes in nature promise controllable assembly of functional nanoparticles for industrial mass production. However, their artificial strategies have faced challenges to uniformly transfer nanoparticles into a monolayer, particularly those below 100 nm in size, over large areas. Here we present a scalable “one‐shot” self‐limiting nanoparticle transfer technique, enabling the efficient transport of nanoparticles from water in microscopic volumes to an entire 2‐inch wafer in a remarkably short time of 10 seconds to reach near‐maximal surface coverage (ca. 40%) in a 2D mono‐layered fashion. Employing proton engineering in electrostatic assembly accelerates the diffusion of nanoparticles (over 50 μm2/sec), resulting in a hundredfold faster coating speed than the previously reported results in the literature. This charge‐sensitive process further enables “pick‐and‐place” nanoparticle patterning at the wafer scale, with large flexibility in surface materials, including flexible metal oxides and 3D‐printed polymers. As a result, we successfully demonstrate the fastest fabrication of wafer‐scale disordered plasmonic metasurfaces in seconds. These metasurfaces exhibit consistent resonating colors across diverse material and geometrical platforms, showcasing their potential for applications in full‐color painting and optical encryption devices.This article is protected by copyright. All rights reserved

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Super-resolution imaging of non-fluorescent molecules by photothermal relaxation localization microscopy

Cited by 40 publications

References 51 publications

Photothermally Detected Stimulated Raman Microscopy towards Ultrasensitive Chemical Imaging

Photothermally Detected Stimulated Raman Microscopy towards Ultrasensitive Chemical Imaging

Toward the Next Frontiers of Vibrational Bioimaging

Proton‐Assisted Assembly of Colloidal Nanoparticles into Wafer‐Scale Monolayers in Seconds

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