A helium nanodroplet setup for mid and far-infrared spectroscopy using pulsed-free-electron lasers: vibrational spectra of propargyl alcohol

Mani, Devendra; Fischer, Theo; Schwan, Raffael; Dey, Arghya; Redlich, Britta; Meer, A. F. G. van der; Schwaab, Gerhard; Havenith, Martina

doi:10.1039/c7ra08102b

Cited by 12 publications

(18 citation statements)

References 47 publications

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“…Thee xperimental setup BoHeNDI@FELIX, combining the helium nanodroplet isolation technique with the ultrabright radiation source FELIX and covering the entire frequency region from 66 to 3600 cm À1 ,i sd escribed in detail in ap revious publication. [40] In HeNDI spectroscopy,t he absorption is measured indirectly as the depletion of the ion current of ac ertain ionic fragment in the mass spectrum upon excitation of the embedded solute.I np resent study,w ei nvestigate water clusters,w hich are formed after sequential pick-up of single water molecules.I Ra bsorption results in an evaporation of helium atoms and thereby in ad ecrease of ionization cross section which is detected at al oss of signal on the ionic fragment [H 2 O] + and [(H 2 O)H] + at m/z = 18 and m/z = 19, respectively.Anoverview of the experimental low-frequency spectrum of water cluster in helium nanodroplets is shown in Figure 1a (lower trace) in gray.…”

Section: Resultsmentioning

confidence: 99%

Observation of the Low‐Frequency Spectrum of the Water Dimer as a Sensitive Test of the Water Dimer Potential and Dipole Moment Surfaces

Schwan

Mani

et al. 2019

Angew Chem Int Ed

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Using the helium nanodroplet isolation setup at the ultrabright free-electron laser source FELIX in Nijmegen (BoHeNDI@FELIX), the intermolecular modes of water dimer in the frequency region from 70 to 550 cm À1 were recorded. Observed bands were assigned to donor torsion, acceptor wag, acceptor twist, intermolecular stretch, donor torsion overtone,a nd in-plane and out-of-plane librational modes.T his experimental data set provides as ensitive test for state-of-the-art water potentials and dipole moment surfaces. Theoretical calculations of the IR spectrum are presented using high-level quantum and approximate quasiclassical molecular dynamics approaches.T hese calculations use the full-dimensional ab initio WHHB potential and dipole moment surfaces. Based on the experimental data, aconsiderable increase of the acceptor switch and ab ifurcation tunneling splitting in the librational mode is deduced, whichi saconsequence of the effective decrease in the tunneling barrier.Supportinginformation and the ORCID identification number(s) for the author(s) of this article can be found under: https://doi.

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Section: Resultsmentioning

confidence: 99%

Observation of the Low‐Frequency Spectrum of the Water Dimer as a Sensitive Test of the Water Dimer Potential and Dipole Moment Surfaces

Schwan

Mani

et al. 2019

Angew Chem Int Ed

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“…Our experimental setup is shown schematically in Fig. 4, which has earlier been described in detail ( 35 ). The helium droplet apparatus consists of four differentially pumped vacuum chambers.…”

Section: Methodsmentioning

confidence: 99%

“…While the FELIX-macropulses are of the order of microsecond time duration, the radiation-induced depletion signal is present for ~3-ms duration, which corresponds to the flight time of the droplets in the machine (typical droplet velocity, ~400 m/s). For each measurement, the average ion current before the arrival of the laser pulse (0- to 10-ms time window) served as a “reference.” The ion current in a time window of ~10 to 13 ms contains the depletion signal [see also ( 35 )].…”

Section: Methodsmentioning

confidence: 99%

“…Here, we report the results of a joint experimental/theoretical study of the generic HCl-water system in superfluid helium nanodroplets, which are known to enable the controlled formation of H-bonded molecular aggregates at ultracold conditions of 0.37 K ( 34 ). Using the high-intensity pulsed free-electron lasers (FELs) at FELIX in Nijmegen, our measurements were performed in the IR fingerprint region (about 1000 to 1700 cm −1 ) based on the recently developed BoHeNDI@FELIX end station ( 35 ).…”

Section: Introductionmentioning

confidence: 99%

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Acid solvation versus dissociation at “stardust conditions”: Reaction sequence matters

et al. 2019

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Chemical reactions at ultralow temperatures are of fundamental importance to primordial molecular evolution as it occurs on icy mantles of dust nanoparticles or on ultracold water clusters in dense interstellar clouds. As we show, studying reactions in a stepwise manner in ultracold helium nanodroplets by mass-selective infrared (IR) spectroscopy provides an avenue to mimic these “stardust conditions” in the laboratory. In our joint experimental/theoretical study, in which we successively add H2O molecules to HCl, we disclose a unique IR fingerprint at 1337 cm−1 that heralds hydronium (H3O+) formation and, thus, acid dissociation generating solvated protons. In stark contrast, no reaction is observed when reversing the sequence by allowing HCl to interact with preformed small embryonic ice-like clusters. Our ab initio simulations demonstrate that not only reaction stoichiometry but also the reaction sequence needs to be explicitly considered to rationalize ultracold chemistry.

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“…This shift appears to be smaller in larger ions, as compared to smaller ions, presumably because of a larger separation of the charge center from the helium atoms in the former [198]. With the advent of FEL IR facilities, which offer wide spectral tunability and large photon flux, spectroscopic studies of charged species have become more facile [195,198,[201][202][203][204]. Aside from cations, anions have recently been investigated in He droplets [205,206].…”

Section: Molecular Ionsmentioning

confidence: 99%

Infrared spectroscopy in superfluid helium droplets

Verma

Tanyag

O’Connell

et al. 2018

Advances in Physics: X

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For more than two decades, encapsulation in superfluid helium nanodroplets has served as a reliable technique for probing the structure and dynamics of molecules and clusters at a low temperature of ≈0.37 K. Due to weak interactions between molecules and the host liquid helium, good spectral resolution can usually be achieved, making helium droplets an ideal matrix for spectroscopy in a wide spectral range from infrared to ultraviolet. Furthermore, rotational structure in the spectra of small molecules provides a unique probe for interactions with the superfluid on an atomic scale. This review presents a summary of results and a discussion of recent experimental developments in helium droplet spectroscopy with the emphasis laid on infrared studies. Initially, studies focused on single molecules and have been expanded to larger species, such as metal-molecular clusters, biomolecules, free radicals, ions, and proteins. ARTICLE HISTORY

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A helium nanodroplet setup for mid and far-infrared spectroscopy using pulsed-free-electron lasers: vibrational spectra of propargyl alcohol

Abstract: Helium nanodroplets spectroscopy in combination with free electron laser. The combination is suitable for studying molecular clusters in 66–3600 cm−1 spectral range, covering the important low-frequency large amplitude intra and inter-molecular motions.

Cited by 12 publications

References 47 publications

Observation of the Low‐Frequency Spectrum of the Water Dimer as a Sensitive Test of the Water Dimer Potential and Dipole Moment Surfaces

Observation of the Low‐Frequency Spectrum of the Water Dimer as a Sensitive Test of the Water Dimer Potential and Dipole Moment Surfaces

Acid solvation versus dissociation at “stardust conditions”: Reaction sequence matters

Infrared spectroscopy in superfluid helium droplets

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