The amount of information trafficking internet nowadays is enormous and will increase further in the near future. It can be expected that in the next decennia the current technologies to store and process data will no longer suffice and that other strategies to handle information have to be developed. One approach is to explore chemical routes, which nature has also followed during evolution: our brain can store and handle very large amounts of data and process them in a way silicon-based computers cannot do. Although brain-like chemical computers are still far beyond reach, it is of interest to explore how atom and molecule-based systems that can write, read, and store information might be designed and constructed.


In our group we aim at developing a new technology to write, store, and read information, i.e. on single polymer chains with the help of a molecular machine that is inspired by the hypothetical device (Turing machine) proposed by the British mathematician Alan Turing in 1936 as the general basis for the operation of a computer.

The molecular machine (shown in green in the image) is composed of a chiral catalytic cage compound (tape-head) that moves unidirectionally along a chiral polymer chain (yellow) while writing a binary code in the form of (R)- (symbol 0, red) and (S)- (symbol 1, purple) epoxide functions. This writing process is controlled by light or electrons.




Previous Research


Over the years, research in the group has focused on the development of supramolecular catalysts and materials using nature as a guide. Our research interests are wide-spread, covering many topics including chiral polymers, host-guest chemistry, liquid-crystals, surfactants, enzymes, viruses, single molecule spectroscopy, and single molecule catalysis.
We have developed a new type of chiral polymers, i.e. polyisocyanopeptides, which are mimics of naturally occurring beta-sheet helices, see Science, 270, 966 (1995), Science, 280, 1427 (1998), and Science, 293, 676 (2001). These polymers are stiffer than DNA and can be used as scaffolds for the assembly of functional groups. They self-assemble in water to form super helical architectures. We have pioneered the self-assembly of dye molecules (porphyrins and phthalocyanines) to generate helical architectures by a process of stepwise information transfer, see Science, 284, 785 (1999). In the field of host-guest chemistry we have developed a new type of building block, i.e. glycoluril, for the construction of guest binding supramolecular systems, see for a summary of research activities Acc.Chem. Res., 32, 995 (1999). Glycoluril cages provided with a catalytically active function have been synthesized as a new type of catalyst that can glide along a polymer chain and modify this chain, see Nature, 424, 915 (2003) and Science, 322, 1668 (2008). Such so-called processive systems have not been reported before and are modelled after the naturally occurring DNA polymerases. Liquid-crystalline compounds have been a topic of intense research in our research group, in particular compounds that form discotic mesophases. We have developed new methods for the preparation of command layers for the alignment of liquid-crystalline compounds by self-assembly processes, see Angew. Chem. Int. Ed. 42, 1812 (2003) and Science, 314, 1433 (2006). As part of our studies on self-assembling supramolecular systems we have worked on different types of amphiphilic molecules, not only traditional low molecular ones, but also block copolymers (super amphiphiles), and polymer-enzyme constructs, for which we have coined the name giant amphiphiles. The latter systems form unusual self-assembled architectures in water, e.g. toroids. For an overview, see Acc. Chem. Res., 42, 681 (2009). As part of our studies on amphiphilic polymer-enzyme biohybrids we have measured the activity of single enzymes, see Proc. Natl. Acad. Science, 102, 2368 (2005) and Nature Nanotechn., 2, 635 (2007). In recent years we have focused our research on viruses as nanosized building blocks in supramolecular chemistry, e.g. as containers and scaffolds. For this new line of research we have proposed the name "Chemical Virology". We have used viruses as monodisperse containers for enzymes and as building blocks for the development of new materials, e.g. see Nature Chem., 2, 394 (2010). The work mentioned above has been published in circa 650 papers and book chapters.
After his retirement in 2010 Roeland Nolte continued to work as a Royal Netherlands Academy of Science Professor in Chemistry at the Radboud University Nijmegen. In 2011 he received an ERC Advanced grant allowing him to continue his work on processive catalytic systems. A summary of this program is presented below .

Research Highlights

M. Kauranen, T. Verbiest, C. Boutton, M.N. Teerenstra, K. Clays, A.J. Schouten, R.J.M. Nolte, and A. Persoons, “Supramolecular second-order nonlinearity of polymers with orientationally correlated chromophores”, Science, 270 (1995) 966

J.J.L.M. Cornelissen, M. Fischer, N.A.J.M. Sommerdijk, R.J.M. Nolte, “Helical superstructures from charged poly(styrene)-poly(isocyanodipeptide) block copolymers”, Science, 280 (1998) 1427

H. Engelkamp, S. Middelbeek, R.J.M. Nolte, “Self-assembly of disk-shaped molecules to coiled-coil aggregates with tunable helicity”, Science, 284 (1999) 785

J.J.L.M. Cornelissen, J.J.J.M. Donners, R. de Gelder, W.S. Graswinckel, A.E. Rowan, N.A.J.M. Sommerdijk, and R.J.M. Nolte, “-Helical polymers from isocyanopeptides”, Science, 293 (2001) 676

P. Thordarson, E.J.A. Bijsterveld, A.E. Rowan, and R.J.M. Nolte, “Epoxidation of polybutadiene by a topologically-linked processive catalyst”, Nature, 424 (2003) 915

R. van Hameren, P. Schön, A. van Buul, J. Hoogboom, S.V. Lazarenko, J.W. Gerritsen, H. Engelkamp, P.C.M. Christianen, H.A. Heus, J.C. Maan, Th. Rasing, S. Speller, A.E. Rowan., J.A.A.W. Elemans, and R.J. M. Nolte, “Macroscopic, hierarchical surface patterning of porphyrin trimers via self-assembly and dewetting”, Science, 314 (2006) 1433

N. Carette, H. Engelkamp, E. Akpa, S.J. Pierre, N.R. Cameron, P.C.M. Christianen, J.C. Maan, J.C. Thies, R. Weberskirch, A.E. Rowan, R.J.M. Nolte, T. Michon, and J.C.M. van Hest, “A virus-based biocatalyst”, Nature Nanotechnology, 2 (2007) 226

B. Hulsken, R. van Hameren, J.W. Gerritsen, T. Khoury, P. Thordarson, M.J. Crossley, A.E. Rowan, R.J.M. Nolte, J.A.A.W. Elemans, and S. Speller, “Real-time single molecule imaging of alkene oxidation by manganese porphyrins at a liquid-solid interface”, Nature Nanotechnology, 2 (2007) 285

M.Comellas-Aragonès, H. Engelkamp, V.I. Claessen, N.A.J.M. Sommerdijk, A.E. Rowan, P.C.M. Christianen, J.C. Maan, B.J.M. Verduin, J.J.L.M. Cornelissen, and R.J.M. Nolte, “A virus-based single-enzyme nanoreactor”, Nature Nanotechnology, 2 (2007) 635

A.B.C. Deutman, C. Monnereau, J.A.A.W. Elemans, G. Ercolani, R.J.M. Nolte, and A.E. Rowan, “Mechanism of threading a polymer through a macrocyclic ring”, Science, 322 (2008) 1668

M.A. Kostiainen, O. Kasyutich, J.J.L.M. Cornelissen, and R.J.M.Nolte, “Self-assembly and optically triggered disassembly of dendron-virus complexes”, Nature Chem., 2 (2010) 394

D.A. Wilson, R.J.M. Nolte, and J.C.M. van Hest, “Autonomous movement of platinum loaded stomatocytes”, Nature Chem., 4 (2012), 268

P.H.J. Kouwer, M. Koepf, V.A.A. Le Sage, M. Jaspers, A.M. van Buul, Z.H. Eksteen-Akeroyed, T. Woltinge, E. Schwartz, H.J. Kitto, R. Hoogenboom, S.J. Picken, R.J.M. Nolte, E. Mendes, and A.E. Rowan, “Responsive biomimetic networks from polyisocyanopeptide hydrogels”, Nature, 493 (2013) 651

D. den Boer, M. Li, Th. Habets, P. Iavicoli, A.E. Rowan, R.J.M. Nolte, S. Speller, D.B. Amabilino, S. De Feyeter, and J.A.A.W. Elemans, “Detection of different oxidation states of individual manganese porphyrins during their reaction with oxygen at a solid/liquid interface”, Nature Chem., 5, 621 (2013)

S. F. M. van Dongen, J. Clerx, K. Nørgaard, T. G. Bloemberg, J. J. L. M. Cornelissen, M. A. Trakselis, S. W. Nelson, S. J. Benkovic, A. E. Rowan, and R. J. M. Nolte, “A clamp-like biohybrid catalyst for DNA oxidation”, Nature Chem., 5, 945-951 (2013)

P.G. van Rhee, R.S.M. Rikken, L.K.E.A. Abdelmohsen, J.C. Maan, R.J.M. Nolte, J.C.M. van Hest, P.C.M. Christianen, and D.A. Wilson, Polymersome magneto-valves for reversible capture and release of nanoparticles, Nature Communications, 5, article number 5010 (2014)

R.S.M. Rikken, H. Engelkamp, R.J.M. Nolte, J.C. Maan, J.C.M. van Hest, D.A. Wilson, and P.C.M. Christianen, “Shaping polymersomes into predictable morphologies  via out-of-equilibrium self-assembly”, Nature Commun., 7, article number 12606 (2016)