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Mechanical tuning of molecular machines for nucleotide recognition at the air-water interface.

Mori T, Okamoto K, Endo H, Sakakibara K, Hill JP, Shinoda S, Matsukura M, Tsukube H, Suzuki Y, Kanekiyo Y, Ariga K - Nanoscale Res Lett (2011)

Bottom Line: Molecular machines embedded in a Langmuir monolayer at the air-water interface can be operated by application of lateral pressure.As part of the challenge associated with versatile sensing of biologically important substances, we here demonstrate discrimination of nucleotides by applying a cholesterol-armed-triazacyclononane host molecule.The concept of mechanical tuning of the host structure for optimization of molecular recognition should become a novel methodology in bio-related nanotechnology as an alternative to traditional strategies based on increasingly complex and inconvenient molecular design strategies.

View Article: PubMed Central - HTML - PubMed

Affiliation: World Premier International (WPI) Research Center for Materials Nanoarchitectonics (MANA), National Institute for Materials Science (NIMS), 1-1 Namiki, Tsukuba, Ibaraki 305-0044, Japan. ARIGA.Katsuhiko@nims.go.jp.

ABSTRACT
Molecular machines embedded in a Langmuir monolayer at the air-water interface can be operated by application of lateral pressure. As part of the challenge associated with versatile sensing of biologically important substances, we here demonstrate discrimination of nucleotides by applying a cholesterol-armed-triazacyclononane host molecule. This molecular machine can discriminate ribonucleotides based on a twofold to tenfold difference in binding constants under optimized conditions including accompanying ions in the subphase and lateral surface pressures of its Langmuir monolayer. The concept of mechanical tuning of the host structure for optimization of molecular recognition should become a novel methodology in bio-related nanotechnology as an alternative to traditional strategies based on increasingly complex and inconvenient molecular design strategies.

No MeSH data available.


Related in: MedlinePlus

Structures and schematic drawing of host 1 and guest nucleotides.
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Figure 1: Structures and schematic drawing of host 1 and guest nucleotides.

Mentions: Supramolecular structures constructed through bottom-up processes play crucial roles in nanoscience and nanotechnology [1,2]. In particular, those structures can be applied in bio-related nanotechnologies such as drug discrimination. Molecular assemblies immobilized at the air-water interface are appropriate media for incorporation of the sensing and diagnostic modules of aqueous biological molecules, since they provide great opportunities for molecular recognition of water-soluble guests by designer hosts in an insoluble floating monolayer [3]. Enhanced binding efficiencies of host-guest recognition at the air-water interface are in accord with theoretical simulations [4,5] and are supported experimentally as seen in selective sensing of aqueous peptides [6-8]. We have recently applied the concept of nanotechnology to these interfacial molecular recognition systems by embedding molecular machines in a Langmuir monolayer at the air-water interface where their mechanical operation can be operated by compressive surface pressure applied laterally [9]. The morphologies of the molecular machines can be controlled by macroscopic mechanical forces, resulting in optimization of structure for molecular sensing. We have previously demonstrated the (i) capture and release of fluorescent molecules upon cavity closure-opening motions of molecular machines [10-13], (ii) control of enantioselective binding of amino acids upon twisting motion of molecular machines [14,15], and (iii) discrimination of single-methyl-group difference between nucleobases (thymine and uracil) by control of macroscopic lateral pressures [16]. In our next demonstration of the utility of host molecules at the air-water interface, we show discrimination of some naturally occurring nucleotides, which are important in biological activities such as energy storage and signal transduction, using cholesterol-armed-triazacyclononane (1) as a molecular machine (see Figure 1 for recognition system). Using this strategy, we were able to discriminate between several ribonucleotides based on the twofold to tenfold difference in their binding constants under optimized conditions.


Mechanical tuning of molecular machines for nucleotide recognition at the air-water interface.

Mori T, Okamoto K, Endo H, Sakakibara K, Hill JP, Shinoda S, Matsukura M, Tsukube H, Suzuki Y, Kanekiyo Y, Ariga K - Nanoscale Res Lett (2011)

Structures and schematic drawing of host 1 and guest nucleotides.
© Copyright Policy - open-access
Related In: Results  -  Collection

License
Show All Figures
getmorefigures.php?uid=PMC3211390&req=5

Figure 1: Structures and schematic drawing of host 1 and guest nucleotides.
Mentions: Supramolecular structures constructed through bottom-up processes play crucial roles in nanoscience and nanotechnology [1,2]. In particular, those structures can be applied in bio-related nanotechnologies such as drug discrimination. Molecular assemblies immobilized at the air-water interface are appropriate media for incorporation of the sensing and diagnostic modules of aqueous biological molecules, since they provide great opportunities for molecular recognition of water-soluble guests by designer hosts in an insoluble floating monolayer [3]. Enhanced binding efficiencies of host-guest recognition at the air-water interface are in accord with theoretical simulations [4,5] and are supported experimentally as seen in selective sensing of aqueous peptides [6-8]. We have recently applied the concept of nanotechnology to these interfacial molecular recognition systems by embedding molecular machines in a Langmuir monolayer at the air-water interface where their mechanical operation can be operated by compressive surface pressure applied laterally [9]. The morphologies of the molecular machines can be controlled by macroscopic mechanical forces, resulting in optimization of structure for molecular sensing. We have previously demonstrated the (i) capture and release of fluorescent molecules upon cavity closure-opening motions of molecular machines [10-13], (ii) control of enantioselective binding of amino acids upon twisting motion of molecular machines [14,15], and (iii) discrimination of single-methyl-group difference between nucleobases (thymine and uracil) by control of macroscopic lateral pressures [16]. In our next demonstration of the utility of host molecules at the air-water interface, we show discrimination of some naturally occurring nucleotides, which are important in biological activities such as energy storage and signal transduction, using cholesterol-armed-triazacyclononane (1) as a molecular machine (see Figure 1 for recognition system). Using this strategy, we were able to discriminate between several ribonucleotides based on the twofold to tenfold difference in their binding constants under optimized conditions.

Bottom Line: Molecular machines embedded in a Langmuir monolayer at the air-water interface can be operated by application of lateral pressure.As part of the challenge associated with versatile sensing of biologically important substances, we here demonstrate discrimination of nucleotides by applying a cholesterol-armed-triazacyclononane host molecule.The concept of mechanical tuning of the host structure for optimization of molecular recognition should become a novel methodology in bio-related nanotechnology as an alternative to traditional strategies based on increasingly complex and inconvenient molecular design strategies.

View Article: PubMed Central - HTML - PubMed

Affiliation: World Premier International (WPI) Research Center for Materials Nanoarchitectonics (MANA), National Institute for Materials Science (NIMS), 1-1 Namiki, Tsukuba, Ibaraki 305-0044, Japan. ARIGA.Katsuhiko@nims.go.jp.

ABSTRACT
Molecular machines embedded in a Langmuir monolayer at the air-water interface can be operated by application of lateral pressure. As part of the challenge associated with versatile sensing of biologically important substances, we here demonstrate discrimination of nucleotides by applying a cholesterol-armed-triazacyclononane host molecule. This molecular machine can discriminate ribonucleotides based on a twofold to tenfold difference in binding constants under optimized conditions including accompanying ions in the subphase and lateral surface pressures of its Langmuir monolayer. The concept of mechanical tuning of the host structure for optimization of molecular recognition should become a novel methodology in bio-related nanotechnology as an alternative to traditional strategies based on increasingly complex and inconvenient molecular design strategies.

No MeSH data available.


Related in: MedlinePlus