Molekulare Erkennung in chemischen und biologischen Systemen

Persch, Elke; Dumele, Oliver; Diederich, François

doi:10.1002/ange.201408487

Cited by 112 publications

(8 citation statements)

References 484 publications

(266 reference statements)

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“…Such systems can nevertheless be investigated with surface-enhanced 2D IR. Applications may be found in label-free diagnostic tools for chemical sensing − or molecular recognition. ,, …”

Section: Resultsmentioning

confidence: 99%

“…Applications may be found in label-free diagnostic tools for chemical sensing 409−411 or molecular recognition. 319,412,413 Surface-enhanced 2D IR spectroscopy is currently applied in transmission and ATR geometry. However, similar electro- magnetic signal enhancement effects can contribute in SFG as well, 259 but have not been discussed so far in multidimensional signals.…”

Section: Surface Sensitivity Through Surface Enhancementmentioning

confidence: 99%

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Surface-Sensitive and Surface-Specific Ultrafast Two-Dimensional Vibrational Spectroscopy

2016

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Ultrafast two-dimensional infrared spectroscopy (2D IR) has been advanced in recent years toward measuring signals from only a monolayer of sample molecules at solid-liquid and solid-gas interfaces. A series of experimental methods has been introduced, which in the chronological order of development are 2D sum-frequency-generation (2D SFG), transmission 2D IR, and reflection 2D IR, the latter in either internal, attenuated total reflection (ATR), or external reflection configuration. The different variants of 2D vibrational spectroscopy are based on either the even-order or the odd-order nonlinear susceptibility, and all allow resolving similar molecular temporal and spectral information. In this review, we introduce the basic principles of the different methods of 2D vibrational spectroscopy at surfaces along with a balanced overview on the technological aspects as well as benefits and shortcomings. We furthermore discuss the current scope of applications for 2D vibrational surface spectroscopy, which spans an impressively broad range of samples from biological molecules to heterogeneous catalysts. The emphasis is on the ultrafast structural dynamics of molecules at interfaces, environmental interactions, and intermolecular interactions. We furthermore consider important recent technological developments of 2D vibrational surface spectroscopy, which employ (i) surface enhancement, (ii) methods for studying electrochemical interfaces, and (iii) extensions for resolving nonequilibrium processes (transient 2D IR). A detailed outlook is finally given regarding important future applications and technological developments of 2D vibrational surface spectroscopy.

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“…Such systems can nevertheless be investigated with surface-enhanced 2D IR. Applications may be found in label-free diagnostic tools for chemical sensing − or molecular recognition. ,, …”

Section: Resultsmentioning

confidence: 99%

Section: Surface Sensitivity Through Surface Enhancementmentioning

confidence: 99%

Surface-Sensitive and Surface-Specific Ultrafast Two-Dimensional Vibrational Spectroscopy

2016

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“…Non‐covalent interactions play a crucial role in chemistry, having been studied across a broad range of areas such as crystal engineering, catalysis, material design, and molecular biology [1–8] . Unlike covalent bonds which are generally described as a sharing of electrons between nuclei to form an overall attractive interaction, [9] non‐covalent interactions are primarily driven by electrostatics, dispersion, polarisation, Pauli repulsion, and charge transfer, each factor of which affects the overall stability of the interaction [10–13] …”

Section: Introductionmentioning

confidence: 99%

Hydrogen Bonding versus Halogen Bonding: Spectroscopic Investigation of Gas‐Phase Complexes Involving Bromide and Chloromethanes

et al. 2023

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Hydrogen bonding and halogen bonding are important noncovalent interactions that are known to occur in large molecular systems, such as in proteins and crystal structures. Although these interactions are important on a large scale, studying hydrogen and halogen bonding in small, gas-phase chemical species allows for the binding strengths to be determined and compared at a fundamental level. In this study, anion photoelectron spectra are presented for the gas-phase complexes involving bromide and the four chloromethanes, CH 3 Cl, CH 2 Cl 2 , CHCl 3 , and CCl 4 . The stabilisation energy and electron binding energy associated with each complex are determined experimentally, and the spectra are rationalised by high-level CCSD(T) calculations to determine the non-covalent interactions binding the complexes. These calculations involve nucleophilic bromide and electrophilic bromine interactions with chloromethanes, where the binding motifs, dissociation energies and vertical detachment energies are compared in terms of hydrogen bonding and halogen bonding.

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“…The interest in designing artificial molecules and assemblies for supramolecular recognition has endured for several decades since the discovery of the archetypal Watson-Crick DNAd uplex, which is sustained by nucleobase pairing. [1] Successful examples implemented include the use of natural and non-natural bases,c anonical and noncanonical basepairing patterns,a nd an expanding diversity of supramolecular motifs that have proved effective,s uch as hydrogen bonding,m etal binding,d ipolar interactions,a nd DNA bonding. [1] Many designs exploit one or af ew specific motifs for binding,b ut the molecular entities inevitably reside in three-dimensional space (i.e.with aspatial degree of freedom of 3).…”

mentioning

confidence: 99%

“…[1] Successful examples implemented include the use of natural and non-natural bases,c anonical and noncanonical basepairing patterns,a nd an expanding diversity of supramolecular motifs that have proved effective,s uch as hydrogen bonding,m etal binding,d ipolar interactions,a nd DNA bonding. [1] Many designs exploit one or af ew specific motifs for binding,b ut the molecular entities inevitably reside in three-dimensional space (i.e.with aspatial degree of freedom of 3). [1h] Thea vailable empty room thus endorses coexisting supramolecular interactions,such as p-p stacking and hydrophobic forces,w hich may hamper the recognition abilities of the host-guest systems in liquid media.…”

mentioning

confidence: 99%

Spatial, Hysteretic, and Adaptive Host–Guest Chemistry in a Metal–Organic Framework with Open Watson–Crick Sites

Cai¹,

Li²,

Lin³

et al. 2015

Angew Chem Int Ed

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Biological and artificial molecules and assemblies capable of supramolecular recognition, especially those with nucleobase pairing, usually rely on autonomous or collective binding to function. Advanced site-specific recognition takes advantage of cooperative spatial effects, as in local folding in protein-DNA binding. Herein, we report a new nucleobase-tagged metal-organic framework (MOF), namely ZnBTCA (BTC=benzene-1,3,5-tricarboxyl, A=adenine), in which the exposed Watson-Crick faces of adenine residues are immobilized periodically on the interior crystalline surface. Systematic control experiments demonstrated the cooperation of the open Watson-Crick sites and spatial effects within the nanopores, and thermodynamic and kinetic studies revealed a hysteretic host-guest interaction attributed to mild chemisorption. We further exploited this behavior for adenine-thymine binding within the constrained pores, and a globally adaptive response of the MOF host was observed.

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Molekulare Erkennung in chemischen und biologischen Systemen

Cited by 112 publications

References 484 publications

Surface-Sensitive and Surface-Specific Ultrafast Two-Dimensional Vibrational Spectroscopy

Surface-Sensitive and Surface-Specific Ultrafast Two-Dimensional Vibrational Spectroscopy

Hydrogen Bonding versus Halogen Bonding: Spectroscopic Investigation of Gas‐Phase Complexes Involving Bromide and Chloromethanes

Spatial, Hysteretic, and Adaptive Host–Guest Chemistry in a Metal–Organic Framework with Open Watson–Crick Sites

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