Bond-selective fluorescence imaging with single-molecule sensitivity

Wang, Haomin; Lee, Dongkwan; Cao, Yulu; Bi, Xiaotian; Du, Jiajun; Miao, Kun; Lu, Wei

doi:10.1038/s41566-023-01243-8

Cited by 20 publications

(20 citation statements)

References 41 publications

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“…Recently, an experiment similar to the encoding mechanism 1 shown here has been reported using the confocal imaging mode or with a limited field of view of ∼3 μm using picosecond 80 MHz optical parametric oscillator (OPO) systems. 61 Since the photon flux of IR excitation is inversely proportional to the size of the illuminated area, widefield imaging requires high energy for each IR pulse that modules the PL intensity. Our MD-WISE experiments benefit from the usage of kHz optical parametric amplifier (OPA) systems.…”

Section: ■ Concluding Remarksmentioning

confidence: 99%

Multidimensional Widefield Infrared-Encoded Spontaneous Emission Microscopy: Distinguishing Chromophores by Ultrashort Infrared Pulses

Yan,

Wang,

Wagner

et al. 2023

J. Am. Chem. Soc.

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Photoluminescence (PL) imaging has broad applications in visualizing biological activities, detecting chemical species, and characterizing materials. However, the chemical information encoded in the PL images is often limited by the overlapping emission spectra of chromophores. Here, we report a PL microscopy based on the nonlinear interactions between mid-infrared and visible excitations on matters, which we termed MultiDimensional Widefield Infrared-encoded Spontaneous Emission (MD-WISE) microscopy. MD-WISE microscopy can distinguish chromophores that possess nearly identical emission spectra via conditions in a multidimensional space formed by three independent variables: the temporal delay between the infrared and the visible pulses (t), the wavelength of visible pulses (λ vis ), and the frequencies of the infrared pulses (ω IR ). This method is enabled by two mechanisms: (1) modulating the optical absorption cross sections of molecular dyes by exciting specific vibrational functional groups and (2) reducing the PL quantum yield of semiconductor nanocrystals, which was achieved through strong field ionization of excitons. Importantly, MD-WISE microscopy operates under widefield imaging conditions with a field of view of tens of microns, other than the confocal configuration adopted by most nonlinear optical microscopies, which require focusing the optical beams tightly. By demonstrating the capacity of registering multidimensional information into PL images, MD-WISE microscopy has the potential of expanding the number of species and processes that can be simultaneously tracked in high-speed widefield imaging applications.

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Section: ■ Concluding Remarksmentioning

confidence: 99%

Multidimensional Widefield Infrared-Encoded Spontaneous Emission Microscopy: Distinguishing Chromophores by Ultrashort Infrared Pulses

Yan,

Wang,

Wagner

et al. 2023

J. Am. Chem. Soc.

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“…26,27 Continuous and pulsed mid-infrared lights are also applied to modulate fluorescence by exciting molecular vibrations. 28−41 Very recently, a femtosecond (fs) visible and mid-IR double resonance approach 42 and a picosecond (ps) visible and mid-IR double resonance approach 43 have been able to, respectively, achieve single-molecule sensitivity with chemical bond information encoded in fluorescence, opening a new avenue for fluorescence modulation.…”

Section: Introductionmentioning

confidence: 99%

“…Physical methods, usually optical manipulations, are also often used to modulate the fluorescence. For instance, the two-photon fluorescence using two near-infrared pulses to produce fluorescence to avoid sample damage caused by direct absorption of visible photons. , Continuous and pulsed mid-infrared lights are also applied to modulate fluorescence by exciting molecular vibrations. − Very recently, a femtosecond (fs) visible and mid-IR double resonance approach and a picosecond (ps) visible and mid-IR double resonance approach have been able to, respectively, achieve single-molecule sensitivity with chemical bond information encoded in fluorescence, opening a new avenue for fluorescence modulation.…”

Section: Introductionmentioning

confidence: 99%

Blue-Shifted and Broadened Fluorescence Enhancement by Visible and Mode-Selective Infrared Double Excitations

Yu,

Li,

Shen

et al. 2024

J. Phys. Chem. A

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Mode-selective vibrational excitations to modify the electronic states of fluorescein dianion in methanol solutions are carried out with a femtosecond visible pulse synchronized with a tunable high-power, narrow-band picosecond infrared (IR) pulse. In this work, simultaneous intensity enhancement, peak blueshift, and line width broadening of fluorescence are observed in the visible/IR double resonance experiments. Comprehensive investigations on the modulation mechanism with scanning the vibrational excitation frequencies, tuning the time delay between the two excitation pulses, theoretical calculations, and nonlinear and linear spectroscopic measurements suggest that the fluorescence intensity enhancement is caused by the increase of the Franck−Condon factor induced by the vibrational excitations at the electronic ground state. Various enhancement effects are observed as vibrations initially excited by the IR photons relax to populate the vibrational modes of lower frequencies. The peak blueshift and line width broadening are caused by both increasing the Franck−Condon factors among different subensembles because of IR pre-excitation and the long-lived processes induced by the initial IR excitation. The results demonstrate that the fluorescence from the visible/IR double resonance experiments is not a simple sum frequency effect, and vibrational relaxations can produce profound effects modifying luminescence.

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“…Absorption of light and the conversion of photons into other forms of energy, such as excitons and phonons, have been widely utilized for optical sensing, , imaging, and energy harvesting . Recently, rapid developments in wearable devices and emergence of the Internet of Things have further increased the demand for smaller photodetectors (PDs) with high absorption efficiency. , Compact integrated PDs could potentially provide several advantages for these applications, including high-resolution imaging thanks to the large pixel count, , reduced energy consumption, and high-speed operation .…”

mentioning

confidence: 99%

“…A bsorption of light and the conversion of photons into other forms of energy, such as excitons and phonons, have been widely utilized for optical sensing, 1,2 imaging, 3 and energy harvesting. 4 Recently, rapid developments in wearable devices and emergence of the Internet of Things have further increased the demand for smaller photodetectors (PDs) with high absorption efficiency.…”

mentioning

confidence: 99%

Nonlocal, Flat-Band Meta-Optics for Monolithic, High-Efficiency, Compact Photodetectors

Choi,

Munley,

Fröch

et al. 2024

Nano Lett.

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Miniaturized photodetectors are becoming increasingly sought-after components for next-generation technologies, such as autonomous vehicles, integrated wearable devices, or gadgets embedded on the Internet of Things. A major challenge, however, lies in shrinking the device footprint while maintaining high efficiency. This conundrum can be solved by realizing a nontrivial relation between the energy and momentum of photons, such as dispersion-free devices, known as flat bands. Here, we leverage flat-band meta-optics to simultaneously achieve critical absorption over a wide range of incidence angles. For a monolithic silicon meta-optical photodiode, we achieved an ∼10-fold enhancement in the photon-to-electron conversion efficiency. Such enhancement over a large angular range of ∼36°allows incoming light to be collected via a large-aperture lens and focused on a compact photodiode, potentially enabling high-speed and low-light operation. Our research unveils new possibilities for creating compact and efficient optoelectronic devices with far-reaching impact on various applications, including augmented reality and light detection and ranging.

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Bond-selective fluorescence imaging with single-molecule sensitivity

Cited by 20 publications

References 41 publications

Multidimensional Widefield Infrared-Encoded Spontaneous Emission Microscopy: Distinguishing Chromophores by Ultrashort Infrared Pulses

Multidimensional Widefield Infrared-Encoded Spontaneous Emission Microscopy: Distinguishing Chromophores by Ultrashort Infrared Pulses

Blue-Shifted and Broadened Fluorescence Enhancement by Visible and Mode-Selective Infrared Double Excitations

Nonlocal, Flat-Band Meta-Optics for Monolithic, High-Efficiency, Compact Photodetectors

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