Time gated Fourier transform spectroscopy with burst excitation for time-resolved spectral maps from the nano- to millisecond range

Liisberg, Mikkel B.; Rück, Vanessa; Vosch, Tom

doi:10.1039/d3cc03961g

Cited by 4 publications

(4 citation statements)

References 22 publications

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“…A recent paper uses a similar approach, burst-mode Time Gated Fourier Transform Spectroscopy (bmTG-FTS), where multiple pulsed excitation is combined with a Fourier spectroscopy method, Translating Wedge-based Identical pulses eNcoding System (TWINS), in order to obtain correlated timescale spanning spectral information. 17 It is important to note that we resolve non steady-state dynamics during multi-pulsed excitation, yielding additional rich photophysical information in the form of often neglected nonradiative rates, such as intersystem crossing rates.…”

Section: Total Photophysics Of [Pt(thpy)(dppm)] + From Foc and Qy Mea...mentioning

confidence: 99%

Measuring the Total Photon Economy of Molecular Species through Fluorescent Optical Cycling (FOC)

Sica,

Hua,

Coffey

et al. 2024

Preprint

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The total photon economy of a molecule/material is a measure of how light input is converted to light and heat output across energies and timescales. We describe a technique, Fluorescent Optical Cycling (FOC), which allows for simultaneous observation of prompt and delayed emission during and after multiple pulsed excitation, ultimately granting access to multi-state photophysical rates. We exercise control over the excitation pulse train, which allows us to “optically shelve” long-lived intermediate states without the use of diode or flashlamp excitation. By recording all photon arrival times in the visible and shortwave infrared, we can simultaneously resolve fluorescence, phosphorescence, and singlet oxygen sensitization in a single experiment. We use FOC to examine the photophysics of dual emitting bis(di-R-phosphino)alkanethiophene-pyridine-platinum ([Pt(thpy)(dppm)]+) under different solvation conditions, revealing changes in intersystem crossing and phosphorescent rates induced by the external heavy atom effect. Coupling FOC with Decay Associated Fourier Spectroscopy (DAFS), we demonstrate simultaneous correlated spectral and lifetime data in this dual emitting complex. Finally, FOC combined with superconducting nanowire single photon detectors (SNSPDs) allows us to observe the shortwave infrared region (SWIR) phosphorescence of singlet oxygen sensitized by Rose Bengal. Overall, FOC provides a powerful tool to simultaneously study multiple photophysics across timescales, even in weakly populated electronic states.

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Section: Total Photophysics Of [Pt(thpy)(dppm)] + From Foc and Qy Mea...mentioning

confidence: 99%

Measuring the Total Photon Economy of Molecular Species through Fluorescent Optical Cycling (FOC)

Sica,

Hua,

Coffey

et al. 2024

Preprint

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“…From the time-resolved interferometric map (TRIM), it is possible by Fourier transformation (FT, along with a number of corrections) to obtain a time-resolved emission map (TREM), that shows the fluorescence decay at every wavelength within the probed 500–1000 nm range (see the Supporting Information for details regarding data analysis). As we have previously described in detail, it is possible to time gate the signal and obtain spectra of short- and long-lived emitters, and even get rid of scatter from the IRF. , We decided to add a 900 nm short-pass filter in the excitation path in order to limit the white light to the 490–900 nm range. This is because, first, the detection efficiency of the detector used quickly diminishes upon advancing into the NIR II region (1000–1700 nm), and second, the white light continuum still contains an intense 1064 nm line, which gave rise to an unnecessary high scatter contribution.…”

Section: Principle Of White Light Excitation For Screening Of Dna-agncsmentioning

confidence: 99%

“…As we have previously described in detail, it is possible to time gate the signal and obtain spectra of short-and long-lived emitters, and even get rid of scatter from the IRF. 34,35 We decided to add a 900 nm shortpass filter in the excitation path in order to limit the white light to the 490−900 nm range. This is because, first, the detection efficiency of the detector used quickly diminishes upon advancing into the NIR II region (1000−1700 nm), and second, the white light continuum still contains an intense 1064 nm line, which gave rise to an unnecessary high scatter contribution.…”

mentioning

confidence: 99%

Fluorescence Screening of DNA-AgNCs with Pulsed White Light Excitation

Liisberg,

Vosch

2024

Nano Lett.

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DNA-stabilized silver nanoclusters (DNA-AgNCs) are a class of fluorophores with interesting photophysical properties dominated by the choice of DNA sequence. Screening methods with ultraviolet excitation and steady state well plate readers have previously been used for deepening the understanding between DNA sequence and emission color of the resulting DNA-AgNCs. Here, we present a new method for screening DNA-AgNCs by using pulsed white light excitation (λ ex ≈ 490−900 nm). By subtraction and time gating we are able to circumvent the dominating scatter of the white excitation light and extract both temporally and spectrally resolved emission of DNA-AgNCs over the visible to near-infrared range. Additionally, we are able to identify weak long-lived emission, which is often buried underneath the intense nanosecond fluorescence. This new approach will be useful for future screening of DNA-AgNCs (or other novel emissive materials) and aid machine-learning models by providing a richer training data set.

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“…[7] Machine learning algorithms have been developed for the design of new DNA-AgNCs based on emission color spearheaded by Copp et al [8] Since current machine learning algorithms are only based on steady-state emission spectra for classification, dual emissive DNA-AgNCs can lead to erroneous classifications; supplementing the training data with time-resolved information should improve the accuracy of the models. [9] Recently, Gonzàlez et al presented a new sub-class of DNA-AgNCs that only has microsecond emission; both the number of reduced silver atoms (8) and the congested nature of the absorption spectra seem to suggest that these DNA-AgNCs have a more spherical shape. [10] Although a triplet state seems like a plausible candidate for the electronic nature of the microsecond-lived state, there has not yet been any conclusive experimental evidence to support this.…”

Section: Introductionmentioning

confidence: 99%

Hydration Sensitive Orthogonal Dual Emission of a DNA‐Stabilized Silver Nanocluster

Liisberg,

Rück,

Romolini

et al. 2024

Advanced Optical Materials

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DNA‐stabilized silver nanoclusters (DNA‐AgNCs) are a class of emitters that have primarily been studied for their molecular‐like photophysical properties with ns‐lived fluorescence. However, µs‐lived luminescence has recently been reported for an increasing number of DNA‐AgNCs, but little is still known about the origin of the long‐lived emission. To deepen the understanding of the long‐lived state, (DNA)2‐[Ag11]7+, an emitter with short‐ and long‐lived dual emission, is studied. By examining crystals of (DNA)2‐[Ag11]7+, it is found that the fluorescence and luminescence transitions are orthogonal to each other, which implies that components orthogonal to the long axis of the AgNC, such as the nucleobases, contribute significantly to the polarization character of the long‐lived luminescent state. The effect of the hydration level on the dual emission of dried (DNA)2‐[Ag11]7+ droplets is also investigated, and it is found that water drastically reduces emission from the long‐lived state and causes a redshift of the emission. Finally, an unusual excitation intensity‐dependent response of dried (DNA)2‐[Ag11]7+ droplets is noticed. This is ascribed to the heterogeneous local environment of the amorphous solid resulting in different conformations of (DNA)2‐[Ag11]7+ with different optically activated delayed fluorescence probabilities. The presented results provide new key insights into the nature of the long‐lived state of DNA‐AgNCs.

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Time gated Fourier transform spectroscopy with burst excitation for time-resolved spectral maps from the nano- to millisecond range

Abstract: We demonstrate burst-mode Time Gated Fourier Transform Spectroscopy (bmTG-FTS), a technique for simultaneously capturing and disentangling emission signals from short- (ns) and long-lived (μs–ms) states.

Cited by 4 publications

References 22 publications

Measuring the Total Photon Economy of Molecular Species through Fluorescent Optical Cycling (FOC)

Measuring the Total Photon Economy of Molecular Species through Fluorescent Optical Cycling (FOC)

Fluorescence Screening of DNA-AgNCs with Pulsed White Light Excitation

Hydration Sensitive Orthogonal Dual Emission of a DNA‐Stabilized Silver Nanocluster

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