Attosecond spectroscopy of size-resolved water clusters

Gong, Xiaochun; Heck, Saijoscha; Jelovina, Denis; Perry, Conaill; Zinchenko, Kristina; Lucchese, Robert R.; Wörner, Hans Jakob

doi:10.1038/s41586-022-05039-8

Cited by 46 publications

(29 citation statements)

References 40 publications

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“…The water–solute interactions and the different ways in which water molecules bind themselves together in highly dynamic and complex networks lie at the heart of solvation chemistry as well as biomolecular folding and assembly. The accurate description of different forms and the intermolecular potential of water–solute interactions has been one of the most important subjects in chemistry, which is now receiving increased attention. − …”

Section: Introductionmentioning

confidence: 99%

Evolution of Solute–Water Interactions in the Benzaldehyde-(H₂O)_1–6Clusters by Rotational Spectroscopy

Pérez

Steber

et al. 2023

J. Am. Chem. Soc.

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The investigation on the preferred arrangement and intermolecular interactions of gas phase solute−water clusters gives insights into the intermolecular potentials that govern the structure and dynamics of the aqueous solutions. Here, we report the investigation of hydrated coordination networks of benzaldehyde-(water) n (n = 1−6) clusters in a pulsed supersonic expansion using broadband rotational spectroscopy. Benzaldehyde (PhCHO) is the simplest aromatic aldehyde that involves both hydrophilic (CHO) and hydrophobic (phenyl ring) functional groups, which can mimic molecules of biological significance. For the n = 1−3 clusters, the water molecules are connected around the hydrophilic CHO moiety of benzaldehyde through a strong CO•••HO hydrogen bond and weak CH•••OH hydrogen bond(s). For the larger clusters, the spectra are consistent with the structures in which the water clusters are coordinated on the surface of PhCHO with both the hydrophilic CHO and hydrophobic phenyl ring groups being involved in the bonding interactions. The presence of benzaldehyde does not strongly interfere with the cyclic water tetramer and pentamer, which retain the same structure as in the pure water cluster. The book isomer instead of cage or prism isomers of the water hexamer is incorporated into the microsolvated cluster. The PhCHO molecule deviates from the planar structure upon sequential addition of water molecules. The PhCHO−(H 2 O) 1−6 clusters may serve as a simple model system in understanding the solute−water interactions of biologically relevant molecules in an aqueous environment.

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Section: Introductionmentioning

confidence: 99%

Evolution of Solute–Water Interactions in the Benzaldehyde-(H₂O)_1–6Clusters by Rotational Spectroscopy

Pérez

Steber

et al. 2023

J. Am. Chem. Soc.

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“…H-bonded water systems fit the bill because they allow for a multitude of arrangements of H atoms giving rise to residual entropy; [7] the H-bond topologies represent local energy minima. Water clusters draw interest in both theoretical [8][9][10][11][12][13][14][15][16][17] and experimental [18][19][20][21][22] studies because of their relevance to condensed phases of water, water structures within crystals, atmospheric and astrophysical chemistry. The (H 2 O) 20 structure, detected by infrared spectroscopy, [18,21] has been studied extensively.…”

Section: Introductionmentioning

confidence: 99%

Statistical Equivalence of Quantum Chemical Methods for Energy Distribution in Water Clusters

Tokmachev

2023

ChemPhysChem

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Methods of quantum chemistry are instrumental in understanding molecular structures and properties. However, the results demonstrate significant variability, which is difficult to predict and rationalize. The fundamental question is whether some molecular systems exhibit properties invariant with respect to the computational method. The idea explored here is that collective properties of statistical ensembles should be more robust than characteristics of individual molecules and their arbitrary sets. This effect is demonstrated for the complete set of hydrogen-bond topologies of the dodecahedral water cluster (H 2 O) 20 . Non-Gaussian energy distributions produced by various methods have the same functional form despite strong differences in mean values and standard deviations. The conclusion is tested on methods of different complexity and origin employing a number of criteria. A linear mapping between the energies produced by different methods is discussed. The significance of the results is in establishing a collective equivalence property of quantum chemical methods.

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“…In addition, their ultrasmall size results in systems with distinctive properties such as strong photoluminescence, , superparamagnetism, and high catalytic performance . Notably, clusters possess a notable characteristic compared to bulk materials; their properties depend on the number of particles involved. − For instance, gold clusters can emit fluorescence of various colors with different core sizes. Au 31 , Au 23 , Au 13 , Au 8 , and Au 5 emit light in the near-infrared, red, green, blue, and ultraviolet regions, respectively .…”

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confidence: 99%

Lone Pair Electrons with Weak Nuclear Binding Inducing Sensitive Nonlinear Optical Responses in Phosphorus Clusters

Zhong

2023

J. Phys. Chem. Lett.

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Phosphorus clusters have broadband optical responses, adjustable geometries, and electronic structures, potentially balancing transparency and nonlinearity. In this study, the optical properties of phosphorus clusters are analyzed by using first-principles calculations. Phosphorus clusters exhibit strong light absorption in the ultraviolet region while remaining transparent in the visible to far-infrared bands. Importantly, the third-order nonlinear optical performance of phosphorus clusters surpasses that of p-nitroaniline with a D−π−A structure. The analysis reveals that lone pair electrons with weak nuclear binding induce sensitive nonlinear optical responses of phosphorus clusters. Furthermore, a practical approach for enhancing nonlinear optical effects in a medium via atom replacement and its application to hydride systems are discussed. Lone pair electron materials provide an alternative to conventional organic π-conjugated molecules for nonlinear optical devices, while potentially achieving a better trade-off of nonlinearity versus transparency. This study provides a novel concept for the development of high-performance nonlinear optical materials.

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Attosecond spectroscopy of size-resolved water clusters

Cited by 46 publications

References 40 publications

Evolution of Solute–Water Interactions in the Benzaldehyde-(H₂O)_1–6Clusters by Rotational Spectroscopy

Evolution of Solute–Water Interactions in the Benzaldehyde-(H₂O)_1–6Clusters by Rotational Spectroscopy

Statistical Equivalence of Quantum Chemical Methods for Energy Distribution in Water Clusters

Lone Pair Electrons with Weak Nuclear Binding Inducing Sensitive Nonlinear Optical Responses in Phosphorus Clusters

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Attosecond spectroscopy of size-resolved water clusters

Cited by 46 publications

References 40 publications

Evolution of Solute–Water Interactions in the Benzaldehyde-(H2O)1–6Clusters by Rotational Spectroscopy

Evolution of Solute–Water Interactions in the Benzaldehyde-(H2O)1–6Clusters by Rotational Spectroscopy

Statistical Equivalence of Quantum Chemical Methods for Energy Distribution in Water Clusters

Lone Pair Electrons with Weak Nuclear Binding Inducing Sensitive Nonlinear Optical Responses in Phosphorus Clusters

Contact Info

Product

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Evolution of Solute–Water Interactions in the Benzaldehyde-(H₂O)_1–6Clusters by Rotational Spectroscopy

Evolution of Solute–Water Interactions in the Benzaldehyde-(H₂O)_1–6Clusters by Rotational Spectroscopy