High-throughput UV-photofragmentation studies of thymine and guanine

Wang, Siwen; Dauletyarov, Yerbolat; Krüger, Peter; Horke, Daniel A.

doi:10.1039/d3cp00328k

Cited by 4 publications

(8 citation statements)

References 52 publications

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“…35 The continuous nature of this molecular source furthermore allows for very high-throughput experiments if high repetitionrate lasers are used. 18 Finally, decoupling the vaporization step from the ionization step allows for greater control and flexibility over the latter.…”

Section: ■ Results and Discussionmentioning

confidence: 99%

“…Since the produced samples are clean and free from contamination, they also allow the use of “universal probes”, such as ultrafast lasers for time-resolved dynamics studies or X-ray/electron beams for scattering experiments . The continuous nature of this molecular source furthermore allows for very high-throughput experiments if high repetition-rate lasers are used . Finally, decoupling the vaporization step from the ionization step allows for greater control and flexibility over the latter.…”

Section: Discussionmentioning

confidence: 99%

“…While LBTD is clearly a form of soft thermal vaporization, 14,15 the mechanism for LIAD, initially thought to be purely acoustic, is still actively debated. 16,17 The LBTD approach has now been implemented by a number of groups around the world, and has successfully vaporized nucleobases, 14,18 amino acids, 19−21 and nucleosides. 7,22 Related approaches that use a glass surface instead of a metal substrate have also been demonstrated for desorption of nanoparticles 23 or phthalocyanine molecules.…”

Section: ■ Introductionmentioning

confidence: 99%

“…The LBTD approach has now been implemented by a number of groups around the world, and has successfully vaporized nucleobases, , amino acids, − and nucleosides. , Related approaches that use a glass surface instead of a metal substrate have also been demonstrated for desorption of nanoparticles or phthalocyanine molecules …”

Section: Introductionmentioning

confidence: 99%

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Vaporization of Intact Neutral Biomolecules Using Laser-Based Thermal Desorption

Dauletyarov¹,

Wang²,

Horke³

2023

J. Am. Soc. Mass Spectrom.

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The production of a clean neutral molecular sample is a crucial step in many gas-phase spectroscopy and reaction dynamics experiments investigating neutral species. Unfortunately, conventional methods based on heating cannot be used with most nonvolatile biomolecules due to their thermal instability. In this paper, we demonstrate the application of laser-based thermal desorption (LBTD) to produce neutral molecular plumes of biomolecules such as dipeptides and lipids. Specifically, we report mass spectra of glycylglycine, glycyl-l-alanine, and cholesterol obtained using LBTD vaporization, followed by soft femtosecond multiphoton ionization (fs-MPI) at 400 nm. For all molecules, the signal from the intact precursor ion was observed, highlighting the softness and applicability of the LBTD and fs-MPI approach. In more detail, cholesterol underwent hardly any fragmentation. Both dipeptides fragmented significantly, although mostly through only a single channel, which we attribute to the fs-MPI process.

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Section: ■ Results and Discussionmentioning

confidence: 99%

Section: Discussionmentioning

confidence: 99%

Section: ■ Introductionmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

See 2 more Smart Citations

Vaporization of Intact Neutral Biomolecules Using Laser-Based Thermal Desorption

Dauletyarov¹,

Wang²,

Horke³

2023

J. Am. Soc. Mass Spectrom.

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“…This involves the application of sample to a thin (10

m) Titanium substrate, which is subsequently heated in a controlled manner from the back side, leading to sample release into the gas phase. This leads to the production of intact neutral biomolecules as a high density and continuous molecular plume into the gas phase, enabling high repetition rate measurements on these samples with much-reduced vacuum pumping requirements [ 21 ]. The LBTD approach has now been successfully used for the desorption of nucleobases [ 21 , 22 ], nucleosides [ 20 , 23 ] and amino acids [ 17 , 24 , 25 ].…”

Section: Introductionmentioning

confidence: 99%

High-Throughput UV Photoionization and Fragmentation of Neutral Biomolecules as a Structural Fingerprint

Wang¹,

Dauletyarov²,

Horke³

2023

Molecules

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We present UV photofragmentation studies of the structural isomers paracetamol, 3-Pyridinepropionic acid (3-PPIA) and (R)-(-)-2-Phenylglycine. In particular, we utilized a new laser-based thermal desorption source in combination with femtosecond multiphoton ionization at 343 nm and 257 nm. The continuous nature of our molecule source, combined with the 50 kHz repetition rate of the laser, allowed us to perform these experiments at high throughput. In particular, we present detailed laser intensity dependence studies at both wavelengths, producing 2D mass spectra with highly differential information about the underlying fragmentation processes. We show that UV photofragmentation produces highly isomer-specific mass spectra, and assign all major fragmentation pathways observed. The intensity-dependence measurements, furthermore, allowed us to evaluate the appearance intensities for each fragmentation channel, which helped to distinguish competing from consecutive fragmentation pathways.

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Design and characterization of an optical-fiber-coupled laser-induced desorption source for gas-phase dynamics experiments

Milešević,

Popat,

Gellersen

et al. 2023

Review of Scientific Instruments

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Preparation of neutral non-volatile molecules intact in the gas phase for mass spectrometry or chemical dynamics experiments remains a challenge for many classes of molecules. Here, we report the design and characterization of a fiber-coupled laser-based thermal desorption source capable of preparing intact neutral molecules at high molecular densities in the gas phase for use in velocity-map imaging experiments. Within this source, the sample is deposited onto a thin tantalum foil. Irradiation of the foil from the reverse side by a focused laser beam leads to highly localized heating of the sample, resulting in desorption of a plume of molecules into the gas phase. The fiber-coupled design simplifies the alignment of the desorption laser beam, and the ability to rotate the foil relative to the fixed laser beam allows the sample to be continually refreshed under vacuum. We use 118 nm photoionization of three test molecules—uracil, adenine, and phenylalanine—to characterize the source and to demonstrate various aspects of its performance. These include the dependence of the velocity-map imaging performance on the size of the interaction region and the dependence of the laser-induced desorption source emission on desorption laser power and heating time. Signal levels recorded in these measurements are comparable to those we typically obtain in similar experiments using a pulsed supersonic molecular beam, and we, therefore, believe that the source has considerable potential for use in a wide range of chemical dynamics and other experiments.

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High-throughput UV-photofragmentation studies of thymine and guanine

Abstract: High-throughput photofragmentation studies of thymine and guanine were performed at 257 and 343 nm and for a wide range of ionisation laser intensities. Combining a continuous laser-based thermal desorption source...

Cited by 4 publications

References 52 publications

Vaporization of Intact Neutral Biomolecules Using Laser-Based Thermal Desorption

Vaporization of Intact Neutral Biomolecules Using Laser-Based Thermal Desorption

High-Throughput UV Photoionization and Fragmentation of Neutral Biomolecules as a Structural Fingerprint

Design and characterization of an optical-fiber-coupled laser-induced desorption source for gas-phase dynamics experiments

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