Visible-super-resolution infrared microscopy using saturated transient fluorescence detected infrared spectroscopy

Bokor, Nándor; Inoue, Keiichi; Kogure, Satoshi; Fujii, Masaaki; Sakai, Makoto

doi:10.1016/j.optcom.2009.10.032

Cited by 5 publications

(5 citation statements)

References 24 publications

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“…We call this process encoding as information regarding a nuclear displacement is encoded into an excited electronic population. Although modern exploration of this technique has been limited, − it retains ongoing relevance as a strategy for super-resolution IR vibrational measurements. , More recently, we developed a modernized two-photon-excited fluorescence-encoded IR (TPE-FEIR) experiment using an ultrafast IR pulse followed by a near-IR (NIR) two-photon-transition encoding pulse . Using this technique, we observed difference frequency oscillations in the time delay between the short IR pulse and the NIR encoding pulse, which arise from vibrational coherences on the ground electronic state.…”

Section: Introductionmentioning

confidence: 99%

Fourier Transform Fluorescence-Encoded Infrared Spectroscopy

Mastron

Tokmakoff

2018

J. Phys. Chem. A

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While time-resolved infrared (IR) vibrational spectroscopy provides insight on structural dynamics of solution-phase systems, current techniques are limited to high concentrations. Fluorescence-encoded infrared spectroscopy (FEIR) can be used to encode IR-driven vibrational excitations into excited electronic states that fluoresce, which can be detected at lower concentrations than a coherently detected IR signal. Here, we report on the development of Fourier transform FEIR as an alternate approach for high-sensitivity IR spectroscopy. Upon driving vibrational excitation with a pair of IR fields with a variable time delay, an interferometric component was observed in the encoded fluorescence. This signal can be Fourier transformed to obtain a vibrational spectrum. By additionally varying the time delay of the encoding pulse following the second IR pulse, we observed frequency-difference oscillations, allowing us to construct a 2D correlation spectrum of coupled vibrations. Response functions for this experiment have been modeled, which reproduce the observed spectral features and relate them to excitation pathways using diagrammatic perturbation theory. The pathways observed in a 2D FEIR spectrum arise from the excitation of vibrational populations and coherences between coupled vibrations.

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Section: Introductionmentioning

confidence: 99%

Fourier Transform Fluorescence-Encoded Infrared Spectroscopy

Mastron

Tokmakoff

2018

J. Phys. Chem. A

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“…Fluorescence-encoded IR (FEIR) vibrational spectroscopy was originally investigated by Kaiser and co-workers in the 1970s as part of the emerging field of picosecond IR spectroscopy, − but few investigations have followed up on this concept using modern ultrafast laser technology. − More recently, fluorescence encoding has also been used as a strategy for super-resolution IR vibrational imaging. , Although a growing number of coherent mixed electronic–vibrational spectroscopies are currently being used to investigate coupled electronic–nuclear dynamics, , the motivation for our studies is vibrational spectroscopy on the ground electronic state . As an analogue to fluorescence-detected coherent electronic spectroscopies, − this technique also presents a similar possibility of detecting Fourier transform coherent multidimensional spectroscopy through fluorescence.…”

Section: Introductionmentioning

confidence: 99%

“…10−14 More recently, fluorescence encoding has also been used as a strategy for super-resolution IR vibrational imaging. 15,16 Although a growing number of coherent mixed electronic−vibrational spectroscopies are currently being used to investigate coupled electronic−nuclear dynamics, 17,18 the motivation for our studies is vibrational spectroscopy on the ground electronic state. 19 As an analogue to fluorescence-detected coherent electronic spectroscopies, 20−25 this technique also presents a similar possibility of detecting Fourier transform coherent multidimensional spectroscopy through fluorescence.…”

Section: Introductionmentioning

confidence: 99%

Two-Photon-Excited Fluorescence-Encoded Infrared Spectroscopy

Mastron

Tokmakoff

2016

J. Phys. Chem. A

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We report on a method for performing ultrafast infrared (IR) vibrational spectroscopy using fluorescence detection. Vibrational dynamics on the ground electronic state driven by femtosecond mid-infrared pulses are detected by changes in fluorescence amplitude resulting from modulation of a two-photon visible transition by nuclear motion. We examine a series of coumarin dyes and study the signals as a function of solvent and excitation pulse parameters. The measured signal characterizes the relaxation of vibrational populations and coherences but yields different information than conventional IR transient absorption measurements. These differences result from the manner in which the ground-state dynamics are projected by the two-photon detection step. Extensions of this method can be adapted for a variety of increased-sensitivity IR measurements.

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“…The first type is exciting molecular vibrations through the linear absorption of a mid-IR photon that further modulates the electronic absorptions. Linear mid-IR absorption typically has a much larger cross section than nonlinear vibrational excitation such as Raman-based processes. , The IR-visible double-resonance process, during which a dye molecule sequentially absorbs a mid-IR photon and then a visible photon, can encode PL signals in the widefield configuration. ,− The second type of IR-visible nonlinear interaction is based on the strong electric field of femtosecond mid-IR pulses, which can reach the order of megavolts per centimeter (MV/cm) due to the high peak power and the relatively long wavelength. , Such electric fields can ionize excitons in semiconductor materials, affecting the PL intensity of quantum dot (QD) emitters …”

Section: Introductionmentioning

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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Visible-super-resolution infrared microscopy using saturated transient fluorescence detected infrared spectroscopy

Cited by 5 publications

References 24 publications

Fourier Transform Fluorescence-Encoded Infrared Spectroscopy

Fourier Transform Fluorescence-Encoded Infrared Spectroscopy

Two-Photon-Excited Fluorescence-Encoded Infrared Spectroscopy

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

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