99 Semesters of Chemistry - A Personal Retrospective on the Molecular State Approach by Preparative Chemists

1997 ◽  
Vol 62 (1) ◽  
pp. 1-41 ◽  
Author(s):  
Hans Bock

Molecular states are the real building blocks of the chemist, because the structure of a molecule can change considerably as its energy and thus its electron distribution varies within the time-domain of dynamic relaxation. The ever increasing use of measuring methods from the armory of physics to characterize molecules by their molecular state fingerprints and, above all, of computers to rationalize both their properties and their microscopic reaction pathways, provides a wealth of information for the development of chemistry. To deal with the complexity of molecular states, a qualitative model based on the topology and symmetry of their structures as well as of their energies resulting from the electron distribution over the respective effective nuclear potentials is presented and is illustrated by examples of our own efforts to elucidate molecular state properties including time-dependent dynamics, microscopic reaction pathways both in the gas phase and in solution, and the self-assembly of molecules on crystallization. In conclusion, a personal retrospective is summarized and some prospects for the future are outlined.

Soft Matter ◽  
2018 ◽  
Vol 14 (31) ◽  
pp. 6415-6418 ◽  
Author(s):  
Guido Panzarasa ◽  
Alina Osypova ◽  
Alba Sicher ◽  
Arie Bruinink ◽  
Eric R. Dufresne

Directed self-assembly of chitosan as tunable-size particles is achieved in the time domain by means of the formaldehyde clock reaction.


2015 ◽  
Vol 11 ◽  
pp. 748-762 ◽  
Author(s):  
Mirko Lohse ◽  
Larissa K S von Krbek ◽  
Sebastian Radunz ◽  
Suresh Moorthy ◽  
Christoph A Schalley ◽  
...  

Two pairs of divalent and tetravalent porphyrin building blocks carrying the complementary supramolecular crown ether/secondary ammonium ion binding motif have been synthesized and their derived pseudorotaxanes have been studied by a combination of NMR spectroscopy in solution and ESI mass spectrometry in the gas phase. By simple mixing of the components the formation of discrete dimeric and trimeric (metallo)porphyrin complexes predominates, in accordance to binding stoichiometry, while the amount of alternative structures can be neglected. Our results illustrate the power of multivalency to program the multicomponent self-assembly of specific entities into discrete functional nanostructures.


2020 ◽  
Vol 11 (6) ◽  
pp. 1518-1522 ◽  
Author(s):  
Maria A. Cardona ◽  
Leonard J. Prins

The addition of ATP under dissipative conditions to a complex mixture causes the transient upregulation of hydrazone-bond formation.


1996 ◽  
Vol 61 (10) ◽  
pp. 1464-1472 ◽  
Author(s):  
Daniel Alexander ◽  
Petr Holý ◽  
Pavel Fiedler ◽  
Zdeněk Havlas ◽  
Jiří Závada

Concise synthesis of the tris(pyrimidones) 1a,b is described. Molecular modeling study demonstrated that both the prepared models 1a,b are capable of self-assembling under formation of spherical dimers locked by 18 hydrogen bonds. Extreme insolubility in all common solvents precluded investigation of the self-assembly in solution. Circumstantial evidence in favor of the self-assembly has been provided in the solid and gas phase.


Author(s):  
Guido Panzarasa ◽  
Alexandre L. Torzynski ◽  
Tianqi Sai ◽  
Katrina Smith-Mannschott ◽  
Eric R. Dufresne

<div>Transient self-assembly is a necessary step towards the development of life-like materials. Our approach allows to program pH-driven supramolecular assembly in the time domain with tailorable lag- and life-times, overcoming the limitations of previously described approaches and setting a new standard for active materials design.<br></div><div><br></div>


2020 ◽  
Vol 5 (2) ◽  
pp. 445-448 ◽  
Author(s):  
Guido Panzarasa ◽  
Tianqi Sai ◽  
Alexandre L. Torzynski ◽  
Katrina Smith-Mannschott ◽  
Eric R. Dufresne

Coupling an acid-autocatalyzed clock reaction with the hydrolysis of a cyclic ester enables the time-domain programming of supramolecular pH-driven self-assembly.


2019 ◽  
Author(s):  
Guido Panzarasa ◽  
Alexandre L. Torzynski ◽  
Tianqi Sai ◽  
Katrina Smith-Mannschott ◽  
Eric R. Dufresne

<div>Transient self-assembly is a necessary step towards the development of life-like materials. Our approach allows to program pH-driven supramolecular assembly in the time domain with tailorable lag- and life-times, overcoming the limitations of previously described approaches and setting a new standard for active materials design.<br></div><div><br></div>


2017 ◽  
Vol 19 (30) ◽  
pp. 19815-19821 ◽  
Author(s):  
E. P. Månsson ◽  
S. De Camillis ◽  
M. C. Castrovilli ◽  
M. Galli ◽  
M. Nisoli ◽  
...  

Ultrafast dynamics and fragmentation of thymidine and thymine after ionization by attosecond extreme ultraviolet radiation studied in the time-domain.


2019 ◽  
Vol 213 ◽  
pp. 02105 ◽  
Author(s):  
Marcin Zych ◽  
Robert Hanus ◽  
Marek Jaszczur ◽  
Anna Golijanek-Jędrzejczyk ◽  
Dariusz Świsulski ◽  
...  

The article presents the analysis of signals from a radiometric system consisting of two scintillation probes and two gamma radiation sealed sources. Calculations and interpretation were carried out for the bubble flow of the water-air mixture in the horizontal pipeline. The analysis of the obtained signals was done in time and frequency domain. In the frequency domain, a range of usable frequencies was identified, which were associated with changes in gamma-ray intensity recorded in the time domain. The gas phase velocity, void fraction and statistical parameters of the signal were also calculated.


1992 ◽  
Vol 2 (4) ◽  
pp. 615-620
Author(s):  
G. W. Series
Keyword(s):  

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