@article{13412, abstract = {Nanoparticles (NPs) and molecular/supramolecular switches have attracted considerable interest during the past decade on account of their unique properties and prominent roles in the fields of organic chemistry and materials science. Materials derived from the combination of these two components are now emerging in the literature. This critical review evaluates materials which comprise NPs functionalised with well-defined self-assembled monolayers of molecular and supramolecular switches. We draw attention to the fact that immobilisation of switches on NPs does not, in general, hamper their switching ability, although it can impart new properties on the supporting particles. This premise leads us to the discussion of systems in which switching on the surfaces of NPs can be used to modulate reversibly a range of NP properties—optical, fluorescent, electrical, magnetic—as well as the controlled release of small molecules. Finally, we discuss examples in which molecular switches direct reversible self-assembly of NPs (308 references).}, author = {Klajn, Rafal and Stoddart, J. Fraser and Grzybowski, Bartosz A.}, issn = {1460-4744}, journal = {Chemical Society Reviews}, keywords = {General Chemistry}, number = {6}, pages = {2203--2237}, publisher = {Royal Society of Chemistry}, title = {{Nanoparticles functionalised with reversible molecular and supramolecular switches}}, doi = {10.1039/b920377j}, volume = {39}, year = {2010}, } @article{10127, abstract = {We use numerical simulations to show how noninteracting hard particles binding to a deformable elastic shell may self-assemble into a variety of linear patterns. This is a result of the nontrivial elastic response to deformations of shells. The morphology of the patterns can be controlled by the mechanical properties of the surface, and can be fine-tuned by varying the binding energy of the particles. We also repeat our calculations for a fully flexible chain and find that the chain conformations follow patterns similar to those formed by the nanoparticles under analogous conditions. We propose a simple way of understanding and sorting the different structures and relate it to the underlying shape transition of the shell. Finally, we discuss the implications of our results.}, author = {Šarić, Anđela and Cacciuto, Angelo}, issn = {1744-683X}, journal = {Soft Matter}, keywords = {condensed matter physics, general chemistry}, number = {5}, pages = {1874--1878}, publisher = {Royal Society of Chemistry (RSC)}, title = {{Particle self-assembly on soft elastic shells}}, doi = {10.1039/c0sm01143f}, volume = {7}, year = {2010}, } @article{8474, abstract = {Hydrogen bonds are ubiquitous interactions in proteins, and are important for their folding and functionality. Scalar coupling constants across hydrogen bonds in the protein backbone, some as small as 0.5 Hz, can be directly measured in the solid state by NMR spectroscopy (see figure). The nuclei on both sides of the hydrogen bond can be identified and the size of the coupling constant can be measured accurately.}, author = {Schanda, Paul and Huber, Matthias and Verel, René and Ernst, Matthias and Meier, Beat H.}, issn = {1433-7851}, journal = {Angewandte Chemie International Edition}, keywords = {General Chemistry, Catalysis}, number = {49}, pages = {9322--9325}, publisher = {Wiley}, title = {{Direct detection of 3hJN' hydrogen-bond scalar couplings in proteins by solid-state NMR spectroscopy}}, doi = {10.1002/anie.200904411}, volume = {48}, year = {2009}, } @article{13414, abstract = {Supraspherical aggregates of crosslinked metal nanoparticles are transformed into pancakes and nanorods by mechanical stresses and shears imparted by macroscopic objects (see image). The dimensions of both types of nanostructures can be controlled by the pressures applied.}, author = {Browne, Kevin P. and Klajn, Rafal and Villa, JulieAnn and Grzybowski, Bartosz A.}, issn = {1613-6829}, journal = {Small}, keywords = {Biomaterials, Biotechnology, General Materials Science, General Chemistry}, number = {23}, pages = {2656--2658}, publisher = {Wiley}, title = {{Mechanofabrication of pancake and rodlike nanostructures from deformable nanoparticle aggregates}}, doi = {10.1002/smll.200900902}, volume = {5}, year = {2009}, } @article{13415, abstract = {Systems in which nanoscale components of different types can be captured and/or released from organic scaffolds provide a fertile basis for the construction of dynamic, exchangeable functional materials. In such heterogeneous systems, the components interact with one another by means of programmable, noncovalent bonding interactions. Herein, we describe polymers that capture and release functionalized nanoparticles selectively during redox-controlled aggregation and disaggregation, respectively. The interactions between the polymer and the NPs are mediated by the reversible formation of polypseudorotaxanes, and give rise to architectures ranging from short chains composed of few nanoparticles to extended networks of nanoparticles crosslinked by the polymer. In the latter case, the polymer/nanoparticle aggregates precipitate from solution such that the polymer acts as a selective ‘sponge’ for the capture/release of the nanoparticles of different types.}, author = {Klajn, Rafal and Olson, Mark A. and Wesson, Paul J. and Fang, Lei and Coskun, Ali and Trabolsi, Ali and Soh, Siowling and Stoddart, J. Fraser and Grzybowski, Bartosz A.}, issn = {1755-4349}, journal = {Nature Chemistry}, keywords = {General Chemical Engineering, General Chemistry}, pages = {733--738}, publisher = {Springer Nature}, title = {{Dynamic hook-and-eye nanoparticle sponges}}, doi = {10.1038/nchem.432}, volume = {1}, year = {2009}, } @article{13416, abstract = {The reversible molecular template-directed self-assembly of gold nanoparticles (AuNPs), a process which relies solely on noncovalent bonding interactions, has been demonstrated by high-resolution transmission electron microscopy (HR-TEM). By employing a well-known host−guest binding motif, the AuNPs have been systemized into discrete dimers, trimers, and tetramers. These nanoparticulate twins, triplets, and quadruplets, which can be disassembled and reassembled either chemically or electrochemically, can be coalesced into larger, permanent polygonal structures by thermal treatment using a focused HR-TEM electron beam.}, author = {Olson, Mark A. and Coskun, Ali and Klajn, Rafal and Fang, Lei and Dey, Sanjeev K. and Browne, Kevin P. and Grzybowski, Bartosz A. and Stoddart, J. Fraser}, issn = {1530-6992}, journal = {Nano Letters}, keywords = {Mechanical Engineering, Condensed Matter Physics, General Materials Science, General Chemistry, Bioengineering}, number = {9}, pages = {3185--3190}, publisher = {American Chemical Society}, title = {{Assembly of polygonal nanoparticle clusters directed by reversible noncovalent bonding interactions}}, doi = {10.1021/nl901385c}, volume = {9}, year = {2009}, } @article{13417, abstract = {Mission Impossible: Metal nanoparticles (NPs) coated with photoresponsive ligands are used as “inks” for self-erasing “paper” whereby light-induced self-assembly of the NPs is transduced into local color changes (see picture). Depending on the degree of self-assembly, multicolor images can be written using only one type of NP ink. Duration of image erasure is regulated by the surface concentration of photoactive groups and can range from seconds to days.}, author = {Klajn, Rafal and Wesson, Paul J. and Bishop, Kyle J. M. and Grzybowski, Bartosz A.}, issn = {1521-3773}, journal = {Angewandte Chemie International Edition}, keywords = {General Chemistry, Catalysis}, number = {38}, pages = {7035--7039}, publisher = {Wiley}, title = {{Writing self-erasing images using metastable nanoparticle “inks”}}, doi = {10.1002/anie.200901119}, volume = {48}, year = {2009}, } @article{13420, abstract = {Weakly protected metal nanoparticles (MNPs) are used as precursors for the preparation of catenane- and pseudorotaxane-decorated NPs of various compositions (gold, palladium, platinum). When attached to the surface of MNPs, the molecular switches retain their switching abilities. The redox potentials of these switches depend on and can be regulated by the composition of the mixed self-assembled monolayers covering the MNPs.}, author = {Klajn, Rafal and Fang, Lei and Coskun, Ali and Olson, Mark A. and Wesson, Paul J. and Stoddart, J. Fraser and Grzybowski, Bartosz A.}, issn = {1520-5126}, journal = {Journal of the American Chemical Society}, keywords = {Colloid and Surface Chemistry, Biochemistry, General Chemistry, Catalysis}, number = {12}, pages = {4233--4235}, publisher = {American Chemical Society}, title = {{Metal nanoparticles functionalized with molecular and supramolecular switches}}, doi = {10.1021/ja9001585}, volume = {131}, year = {2009}, } @article{13421, abstract = {Side-chain poly[2]catenanes at the click of a switch! A bistable side-chain poly[2]catenane has been synthesized and found to form hierarchical self-assembled hollow superstructures of nanoscale dimensions in solution. Molecular electromechanical switching (see picture) of the material is demonstrated, and the ground-state equilibrium thermodynamics and switching kinetics are examined as the initial steps towards processible molecular-based electronic devices and nanoelectromechanical systems.}, author = {Olson, Mark A. and Braunschweig, Adam B. and Fang, Lei and Ikeda, Taichi and Klajn, Rafal and Trabolsi, Ali and Wesson, Paul J. and Benítez, Diego and Mirkin, Chad A. and Grzybowski, Bartosz A. and Stoddart, J. Fraser}, issn = {1521-3773}, journal = {Angewandte Chemie International Edition}, keywords = {General Chemistry, Catalysis}, number = {10}, pages = {1792--1797}, publisher = {Wiley}, title = {{A bistable poly[2]catenane forms nanosuperstructures}}, doi = {10.1002/anie.200804558}, volume = {48}, year = {2009}, } @article{13422, abstract = {Make like a leaf: The synthesis and characterization of a family of “flowerlike” Au/Fe3O4 nanoparticles is described, whereby Fe3O4 “leaves” adhere to a gold core (see image). The size and numbers of iron oxide domains can be adjusted flexibly by changing the proportion of the starting materials and the reaction time.}, author = {Wei, Yanhu and Klajn, Rafal and Pinchuk, Anatoliy O. and Grzybowski, Bartosz A.}, issn = {1613-6829}, journal = {Small}, keywords = {Biomaterials, Biotechnology, General Materials Science, General Chemistry}, number = {10}, pages = {1635--1639}, publisher = {Wiley}, title = {{Synthesis, shape control, and optical properties of hybrid Au/Fe3O4 “nanoflowers”}}, doi = {10.1002/smll.200800511}, volume = {4}, year = {2008}, } @article{8486, abstract = {A technique is described that allows reducing acquisition times of multidimensional NMR experiments by extensive spectral folding. The method is simple and has many interesting applications for NMR studies of molecular structure, dynamics, and kinetics.}, author = {Lescop, Ewen and Schanda, Paul and Rasia, Rodolfo and Brutscher, Bernhard}, issn = {0002-7863}, journal = {Journal of the American Chemical Society}, keywords = {Colloid and Surface Chemistry, Biochemistry, General Chemistry, Catalysis}, number = {10}, pages = {2756--2757}, publisher = {American Chemical Society}, title = {{Automated spectral compression for fast multidimensional NMR and increased time resolution in real-time NMR spectroscopy}}, doi = {10.1021/ja068949u}, volume = {129}, year = {2007}, } @article{8487, abstract = {Following unidirectional biophysical events such as the folding of proteins or the equilibration of binding interactions, requires experimental methods that yield information at both atomic-level resolution and at high repetition rates. Toward this end a number of different approaches enabling the rapid acquisition of 2D NMR spectra have been recently introduced, including spatially encoded “ultrafast” 2D NMR spectroscopy and SOFAST HMQC NMR. Whereas the former accelerates acquisitions by reducing the number of scans that are necessary for completing arbitrary 2D NMR experiments, the latter operates by reducing the delay between consecutive scans while preserving sensitivity. Given the complementarities between these two approaches it seems natural to combine them into a single tool, enabling the acquisition of full 2D protein NMR spectra at high repetition rates. We demonstrate here this capability with the introduction of “ultraSOFAST” HMQC NMR, a spatially encoded and relaxation-optimized approach that can provide 2D protein correlation spectra at ∼1 s repetition rates for samples in the ∼2 mM concentration range. The principles, relative advantages, and current limitations of this new approach are discussed, and its application is exemplified with a study of the fast hydrogen−deuterium exchange characterizing amide sites in Ubiquitin.}, author = {Gal, Maayan and Schanda, Paul and Brutscher, Bernhard and Frydman, Lucio}, issn = {0002-7863}, journal = {Journal of the American Chemical Society}, keywords = {Colloid and Surface Chemistry, Biochemistry, General Chemistry, Catalysis}, number = {5}, pages = {1372--1377}, publisher = {American Chemical Society}, title = {{UltraSOFAST HMQC NMR and the repetitive acquisition of 2D protein spectra at Hz rates}}, doi = {10.1021/ja066915g}, volume = {129}, year = {2007}, } @article{13424, abstract = {Changing shapes: Metastable spherical aggregates of gold nanoparticles undergo a one-to-one, thermally induced transformation into heterodimers comprising connected plate and spherical domains. By controlling the reaction time, it is possible to isolate a variety of structures differing in the relative sizes of the domains and in the overall optical properties (see picture).}, author = {Klajn, Rafal and Pinchuk, Anatoliy O. and Schatz, George C. and Grzybowski, Bartosz A.}, issn = {1521-3773}, journal = {Angewandte Chemie International Edition}, keywords = {General Chemistry, Catalysis}, number = {44}, pages = {8363--8367}, publisher = {Wiley}, title = {{Synthesis of heterodimeric sphere–prism nanostructures via metastable gold supraspheres}}, doi = {10.1002/anie.200702570}, volume = {46}, year = {2007}, } @article{8488, abstract = {We demonstrate for different protein samples that three-dimensional HNCO and HNCA correlation spectra may be recorded in a few minutes acquisition time using the band-selective excitation short-transient sequences presented here. This opens new perspectives for the NMR structural investigation of unstable protein samples and real-time site-resolved studies of protein kinetics.}, author = {Schanda, Paul and Van Melckebeke, Hélène and Brutscher, Bernhard}, issn = {0002-7863}, journal = {Journal of the American Chemical Society}, keywords = {Colloid and Surface Chemistry, Biochemistry, General Chemistry, Catalysis}, number = {28}, pages = {9042--9043}, publisher = {American Chemical Society}, title = {{Speeding up three-dimensional protein NMR experiments to a few minutes}}, doi = {10.1021/ja062025p}, volume = {128}, year = {2006}, } @article{13428, abstract = {Mixtures of oppositely charged nanoparticles of various sizes and charge ratios precipitate only at the point of electroneutrality. This phenomenonspecific to the nanoscale and reminiscent of threshold precipitation of ionsis a consequence of the formation of core-and-shell nanoparticle aggregates, in which the shells are composed of like-charged particles and are stabilized by efficient electrostatic screening.}, author = {Kalsin, Alexander M. and Kowalczyk, Bartlomiej and Smoukov, Stoyan K. and Klajn, Rafal and Grzybowski, Bartosz A.}, issn = {1520-5126}, journal = {Journal of the American Chemical Society}, keywords = {Colloid and Surface Chemistry, Biochemistry, General Chemistry, Catalysis}, number = {47}, pages = {15046--15047}, publisher = {American Chemical Society}, title = {{Ionic-like behavior of oppositely charged nanoparticles}}, doi = {10.1021/ja0642966}, volume = {128}, year = {2006}, } @article{13429, abstract = {The fruitful core: Organic syntheses reported in the literature from 1850 to 2004 are analyzed with mathematical tools from network theory and statistical physics. There is a set of substances (the core) from which the majority of other organic compounds can be made (see picture; red: core, blue: periphery, green: islands). Search algorithms are used to identify small optimal sets of maximally useful chemicals.}, author = {Bishop, Kyle J. M. and Klajn, Rafal and Grzybowski, Bartosz A.}, issn = {1521-3773}, journal = {Angewandte Chemie International Edition}, keywords = {General Chemistry, Catalysis}, number = {32}, pages = {5348--5354}, publisher = {Wiley}, title = {{The core and most useful molecules in organic chemistry}}, doi = {10.1002/anie.200600881}, volume = {45}, year = {2006}, } @article{8492, abstract = {We demonstrate for different protein samples that 2D 1H−15N correlation NMR spectra can be recorded in a few seconds of acquisition time using a new band-selective optimized flip-angle short-transient heteronuclear multiple quantum coherence experiment. This has enabled us to measure fast hydrogen−deuterium exchange rate constants along the backbone of a small globular protein fragment by real-time 2D NMR.}, author = {Schanda, Paul and Brutscher, Bernhard}, issn = {0002-7863}, journal = {Journal of the American Chemical Society}, keywords = {Colloid and Surface Chemistry, Biochemistry, General Chemistry, Catalysis}, number = {22}, pages = {8014--8015}, publisher = {American Chemical Society}, title = {{Very fast two-dimensional NMR spectroscopy for real-time investigation of dynamic events in proteins on the time scale of seconds}}, doi = {10.1021/ja051306e}, volume = {127}, year = {2005}, } @article{13435, abstract = {Micropatterning of surfaces with several chemicals at different spatial locations usually requires multiple stamping and registration steps. Here, we describe an experimental method based on reaction–diffusion phenomena that allows for simultaneous micropatterning of a substrate with several coloured chemicals. In this method, called wet stamping (WETS), aqueous solutions of two or more inorganic salts are delivered onto a film of dry, ionically doped gelatin from an agarose stamp patterned in bas relief. Once in conformal contact, these salts diffuse into the gelatin, where they react to give deeply coloured precipitates. Separation of colours in the plane of the surface is the consequence of the differences in the diffusion coefficients, the solubility products, and the amounts of different salts delivered from the stamp, and is faithfully reproduced by a theoretical model based on a system of reaction–diffusion partial differential equations. The multicolour micropatterns are useful as non-binary optical elements, and could potentially form the basis of new applications in microseparations and in controlled delivery.}, author = {Klajn, Rafal and Fialkowski, Marcin and Bensemann, Igor T. and Bitner, Agnieszka and Campbell, C. J. and Bishop, Kyle and Smoukov, Stoyan and Grzybowski, Bartosz A.}, issn = {1476-4660}, journal = {Nature Materials}, keywords = {Mechanical Engineering, Mechanics of Materials, Condensed Matter Physics, General Materials Science, General Chemistry}, pages = {729--735}, publisher = {Springer Nature}, title = {{Multicolour micropatterning of thin films of dry gels}}, doi = {10.1038/nmat1231}, volume = {3}, year = {2004}, }