Structural and electrostatic effects at the surfaces of size- and charge-selected aqueous nanodrops

Abstract

The effects of ion charge, polarity and size on the surface morphology of size-selected aqueous nanodrops containing a single ion and up to 550 water molecules are investigated with infrared photodissociation (IRPD) spectroscopy and theory.

Infrared Multiphoton Dissociation Spectroscopy with Free‐Electron Lasers: On the Road from Small Molecules to Biomolecules

“…2018, 24,3374 -3390 www.chemeurj.org light sources, such as opticalp arametric oscilators (OPOs)a nd meanwhilem any laboratories use this approach to record IR spectra of ions. [64] Thec hallenge for IRMPD spectroscopy at free-electron laser facilities is, therefore, to find and explore research fields that are not accessible in laboratory setups.…”

Strategy for Modeling the Infrared Spectra of Ion-Containing Water Drops

“…In recent years, several groups have been able to produce gaseous size-selected nanodrops of hydrated ions containing dozens to hundreds of water molecules, and to record their IRPD spectra 7,[9][10][11][12][13][14][15][16][17][18][19][20][21][22][23] Table S3. It can be seen that the extended feature in the 3100-3650 cm −1 range, corresponding to bonded O-H stretches, is well reproduced qualitatively by simulations.…”

“…Analogous computations were carried out for [M(H 2 O) 100 ] x , including 11 ions with x = -2 to +3. Experiments are not systematically available for this size 23 , however trends can be compared to measurements for clusters with 245-255 water molecules 13 . As can be seen in Figure 10, there is much more relative intensity in the red part of the hydrogen-bonded massif (3200-3350 cm −1 ) than for n=36, in agreement with the experimental trend.…”

“…Thus this regime may be of great interest. It has only been recently, however, that several research groups have been able to form and structurally characterize such species experimentally [7][8][9][10][11][12][13][14][15][16][17][18][19][20][21][22][23][24][25][26] . Their modelling is also a challenge, and it is the purpose of the present paper to put forth a method to generate infrared (IR) spectra of such species as vibrational spectroscopy has been shown to carry rather useful structural information [7][8][9][10][11][12][13][14][15][16][17][18][19][20][21][22][23] .…”

Photodynamics and Luminescence of Mono‐ and Tri‐Nuclear Lanthanide Complexes in the Gas Phase and in Solution

“…The lack of systematic physicochemical investigations of such type motivated us to study here the correlation between ultrafast excited state dynamics and lanthanide luminescence activity in acetonitrile by transient absorption spectroscopy (TA) for the recently synthesized metal complexes [Ln{H 3 L} 2 ](NO 3 ) (Ln=Dy ( 1 ), Eu ( 3 )) (Scheme , left)(H 4 L=2,2′‐{[(2‐aminoethyl)imino]bis[2,1‐ethanediyl‐nitriloethylidyne]}bis‐2‐hydroxy‐benzoic acid) providing two pockets for optional Mn II binding . Moreover, we performed very similar experiments on the same species isolated in the gas phase, i. e. in an ion trap of an electrospray ionization mass spectrometer (ESI‐MS) under mass and charge controlled conditions by pump‐probe fragmentation action spectroscopy and gas phase luminescence detection, in order to determine intrinsic properties and evaluate the influence of the solvent ,. Eventually, we compare for both, gas phase and solution, the properties of the related tri‐nuclear complexes (NHEt 3 ) 2 [Ln{MnL} 2 ](ClO 4 ) (Ln=Dy ( 2 ), Eu ( 4 )) (Scheme , right), in order to discern how an aggregated transition metal (TM) ion affects the lanthanide emission via ligand‐TM interaction.…”