Our students have been involved in new and exciting interdisciplinary research and have published in leading high impact journals including Nature Chemistry, Nature Communications, JACS, Angewandte Chemie, Applied Physics Letters, ACS Nano, Nano Letters, Advanced Materials, Nature Protocols, PloS one, and many others.
A full list of the work published by our NanoDTC Students, Associates and others, acknowledging the NanoDTC grants EP/G037221, EP/L015978 and EP/S022953/1 is below. If you want to view the papers on google scholar, see here.
Some papers published by our students are also featured below with some additional contextual information.
Last updated: Mar 2021
Looking inside lithium-ion batteries
Spectroscopy and Electrocatalysis for a Sustainable Future
From waste to fuel: quantifying sustainability
Novel spin states discovered in silicon-based artificial atoms
A step forward in efficient artificial photosynthesis
Self-assembling hydrogels on microfluidic droplets that respond to light or chemical stimuli by disassembling
2014
52.
Venkateshvaran, Deepak; Nikolka, Mark; Sadhanala, Aditya; Lemaur, Vincent; Zelazny, Mateusz; Kepa, Michal; Hurhangee, Michael; Kronemeijer, Auke Jisk; Pecunia, Vincenzo; Nasrallah, Iyad; others,
Approaching disorder-free transport in high-mobility conjugated polymers Journal Article
In: Nature, vol. 515, no. 7527, pp. 384–388, 2014.
@article{venkateshvaran2014approaching,
title = {Approaching disorder-free transport in high-mobility conjugated polymers},
author = {Deepak Venkateshvaran and Mark Nikolka and Aditya Sadhanala and Vincent Lemaur and Mateusz Zelazny and Michal Kepa and Michael Hurhangee and Auke Jisk Kronemeijer and Vincenzo Pecunia and Iyad Nasrallah and others},
url = {https://www.nature.com/articles/nature13854},
year = {2014},
date = {2014-01-01},
journal = {Nature},
volume = {515},
number = {7527},
pages = {384--388},
publisher = {Nature Publishing Group},
abstract = {Conjugated polymers enable the production of flexible semiconductor devices that can be processed from solution at low temperatures. Over the past 25 years, device performance has improved greatly as a wide variety of molecular structures have been studied1. However, one major limitation has not been overcome; transport properties in polymer films are still limited by pervasive conformational and energetic disorder2,3,4,5. This not only limits the rational design of materials with higher performance, but also prevents the study of physical phenomena associated with an extended π-electron delocalization along the polymer backbone. Here we report a comparative transport study of several high-mobility conjugated polymers by field-effect-modulated Seebeck, transistor and sub-bandgap optical absorption measurements. We show that in several of these polymers, most notably in a recently reported, indacenodithiophene-based donor–acceptor copolymer with a near-amorphous microstructure6, the charge transport properties approach intrinsic disorder-free limits at which all molecular sites are thermally accessible. Molecular dynamics simulations identify the origin of this long sought-after regime as a planar, torsion-free backbone conformation that is surprisingly resilient to side-chain disorder. Our results provide molecular-design guidelines for ‘disorder-free’ conjugated polymers.},
keywords = {},
pubstate = {published},
tppubtype = {article}
}
Conjugated polymers enable the production of flexible semiconductor devices that can be processed from solution at low temperatures. Over the past 25 years, device performance has improved greatly as a wide variety of molecular structures have been studied1. However, one major limitation has not been overcome; transport properties in polymer films are still limited by pervasive conformational and energetic disorder2,3,4,5. This not only limits the rational design of materials with higher performance, but also prevents the study of physical phenomena associated with an extended π-electron delocalization along the polymer backbone. Here we report a comparative transport study of several high-mobility conjugated polymers by field-effect-modulated Seebeck, transistor and sub-bandgap optical absorption measurements. We show that in several of these polymers, most notably in a recently reported, indacenodithiophene-based donor–acceptor copolymer with a near-amorphous microstructure6, the charge transport properties approach intrinsic disorder-free limits at which all molecular sites are thermally accessible. Molecular dynamics simulations identify the origin of this long sought-after regime as a planar, torsion-free backbone conformation that is surprisingly resilient to side-chain disorder. Our results provide molecular-design guidelines for ‘disorder-free’ conjugated polymers.
51.
Lin, Chia-Yu; Mersch, Dirk; Jefferson, David A; Reisner, Erwin
Cobalt sulphide microtube array as cathode in photoelectrochemical water splitting with photoanodes Journal Article
In: Chem. Sci., vol. 5, pp. 4906–4913, 2014.
@article{lin2014cobalt,
title = {Cobalt sulphide microtube array as cathode in photoelectrochemical water splitting with photoanodes},
author = {Chia-Yu Lin and Dirk Mersch and David A Jefferson and Erwin Reisner},
url = {https://pubs.rsc.org/no/content/articlehtml/2014/sc/c4sc01811g},
year = {2014},
date = {2014-01-01},
journal = {Chem. Sci.},
volume = {5},
pages = {4906--4913},
abstract = {We report on a cobalt sulphide (CoS) electrode prepared by simple and scalable chemical bath deposition (CBD), which performs as a highly efficient and robust electrocatalyst for the H2 evolution reaction (HER) in both neutral and pH 13 electrolyte solution at a small overpotential (η < 90 mV). At η = 390 mV, turnover frequencies of 38.8 ± 1.9 and 52.1 ± 2.0 mol H2 (mol Co)−1 h−1 were achieved with high stability (Faradaic efficiency >95% for at least 72 h) and turnover numbers of approximately 2600 and 3400 in neutral and basic electrolyte solution, respectively. The rate of HER per geometric area is further enhanced by employing a CoS microtube array (microCoS), which is prepared by sulphurisation of a cobalt hydroxide carbonate nanorod array template using CBD. MicroCoS shows excellent HER activity when it is coupled with a cadmium sulphide sensitised zinc oxide photoanode in the presence of sodium sulphide and a nanostructured hematite (α-Fe2O3) photoanode from photoelectrochemical water splitting in basic electrolyte solution.},
keywords = {},
pubstate = {published},
tppubtype = {article}
}
We report on a cobalt sulphide (CoS) electrode prepared by simple and scalable chemical bath deposition (CBD), which performs as a highly efficient and robust electrocatalyst for the H2 evolution reaction (HER) in both neutral and pH 13 electrolyte solution at a small overpotential (η < 90 mV). At η = 390 mV, turnover frequencies of 38.8 ± 1.9 and 52.1 ± 2.0 mol H2 (mol Co)−1 h−1 were achieved with high stability (Faradaic efficiency >95% for at least 72 h) and turnover numbers of approximately 2600 and 3400 in neutral and basic electrolyte solution, respectively. The rate of HER per geometric area is further enhanced by employing a CoS microtube array (microCoS), which is prepared by sulphurisation of a cobalt hydroxide carbonate nanorod array template using CBD. MicroCoS shows excellent HER activity when it is coupled with a cadmium sulphide sensitised zinc oxide photoanode in the presence of sodium sulphide and a nanostructured hematite (α-Fe2O3) photoanode from photoelectrochemical water splitting in basic electrolyte solution.
50.
Hoye, Robert LZ; Heffernan, Shane; Ievskaya, Yulia; Sadhanala, Aditya; Flewitt, Andrew; Friend, Richard H; MacManus-Driscoll, Judith L; Musselman, Kevin P
Engineering Schottky contacts in open-air fabricated heterojunction solar cells to enable high performance and ohmic charge transport Journal Article
In: ACS applied materials & interfaces, vol. 6, no. 24, pp. 22192–22198, 2014.
@article{hoye2014engineering,
title = {Engineering Schottky contacts in open-air fabricated heterojunction solar cells to enable high performance and ohmic charge transport},
author = {Robert LZ Hoye and Shane Heffernan and Yulia Ievskaya and Aditya Sadhanala and Andrew Flewitt and Richard H Friend and Judith L MacManus-Driscoll and Kevin P Musselman},
url = {https://pubs.acs.org/doi/abs/10.1021/am5058663},
year = {2014},
date = {2014-01-01},
journal = {ACS applied materials & interfaces},
volume = {6},
number = {24},
pages = {22192--22198},
publisher = {American Chemical Society},
abstract = {The efficiencies of open-air processed Cu2O/Zn1–xMgxO heterojunction solar cells are doubled by reducing the effect of the Schottky barrier between Zn1–xMgxO and the indium tin oxide (ITO) top contact. By depositing Zn1–xMgxO with a long band-tail, charge flows through the Zn1–xMgxO/ITO Schottky barrier without rectification by hopping between the sub-bandgap states. High current densities are obtained by controlling the Zn1–xMgxO thickness to ensure that the Schottky barrier is spatially removed from the p–n junction, allowing the full built-in potential to form, in addition to taking advantage of the increased electrical conductivity of the Zn1–xMgxO films with increasing thickness. This work therefore shows that the Zn1–xMgxO window layer sub-bandgap state density and thickness are critical parameters that can be engineered to minimize the effect of Schottky barriers on device performance. More generally, these findings show how to improve the performance of other photovoltaic system reliant on transparent top contacts, e.g., CZTS and CIGS.},
keywords = {},
pubstate = {published},
tppubtype = {article}
}
The efficiencies of open-air processed Cu2O/Zn1–xMgxO heterojunction solar cells are doubled by reducing the effect of the Schottky barrier between Zn1–xMgxO and the indium tin oxide (ITO) top contact. By depositing Zn1–xMgxO with a long band-tail, charge flows through the Zn1–xMgxO/ITO Schottky barrier without rectification by hopping between the sub-bandgap states. High current densities are obtained by controlling the Zn1–xMgxO thickness to ensure that the Schottky barrier is spatially removed from the p–n junction, allowing the full built-in potential to form, in addition to taking advantage of the increased electrical conductivity of the Zn1–xMgxO films with increasing thickness. This work therefore shows that the Zn1–xMgxO window layer sub-bandgap state density and thickness are critical parameters that can be engineered to minimize the effect of Schottky barriers on device performance. More generally, these findings show how to improve the performance of other photovoltaic system reliant on transparent top contacts, e.g., CZTS and CIGS.
49.
Heffernan, Shane; Flewitt, Andrew J
Electrodeposited Cu2O| ZnO Heterostructures With High Built-In Voltages For Photovoltaic Applications Journal Article
In: MRS Online Proceedings Library, vol. 1675, no. 1, pp. 27–32, 2014.
@article{heffernan2014electrodeposited,
title = {Electrodeposited Cu2O| ZnO Heterostructures With High Built-In Voltages For Photovoltaic Applications},
author = {Shane Heffernan and Andrew J Flewitt},
url = {https://link.springer.com/article/10.1557/opl.2014.830},
year = {2014},
date = {2014-01-01},
journal = {MRS Online Proceedings Library},
volume = {1675},
number = {1},
pages = {27--32},
publisher = {Springer International Publishing},
abstract = {Methods of improving low-cost Cu2O|ZnO heterojunction diodes fabricated through galvanostatic deposition of Cu2O are presented. Improved processing parameters responsible for maximizing built-in voltage (Vbi) are determined. The relationship between pH, deposition current, temperature, and diode quality is analyzed and a process window for optimal Cu2O deposition on ZnO is obtained with a pH range between 12.0 and 12.1 and a current density range which is determined by the effect of both pH and deposition current (Jdep) on grain size. The pH window is found to be narrower than previously reported1 and much narrower than the processing window for the deposition of Cu2O films. A two-step approach deposition based on the use of different Jdep is presented for the first time. A Vbi of 0.6 V is achieved, which is the highest reported for cells produced using low temperature processing routes involving electrodeposition and reactive sputtering.},
keywords = {},
pubstate = {published},
tppubtype = {article}
}
Methods of improving low-cost Cu2O|ZnO heterojunction diodes fabricated through galvanostatic deposition of Cu2O are presented. Improved processing parameters responsible for maximizing built-in voltage (Vbi) are determined. The relationship between pH, deposition current, temperature, and diode quality is analyzed and a process window for optimal Cu2O deposition on ZnO is obtained with a pH range between 12.0 and 12.1 and a current density range which is determined by the effect of both pH and deposition current (Jdep) on grain size. The pH window is found to be narrower than previously reported1 and much narrower than the processing window for the deposition of Cu2O films. A two-step approach deposition based on the use of different Jdep is presented for the first time. A Vbi of 0.6 V is achieved, which is the highest reported for cells produced using low temperature processing routes involving electrodeposition and reactive sputtering.
48.
Tan, Zhi-Kuang; Moghaddam, Reza Saberi; Lai, May Ling; Docampo, Pablo; Higler, Ruben; Deschler, Felix; Price, Michael; Sadhanala, Aditya; Pazos, Luis M; Credgington, Dan; others,
Bright light-emitting diodes based on organometal halide perovskite Journal Article
In: Nature nanotechnology, vol. 9, no. 9, pp. 687–692, 2014.
@article{tan2014bright,
title = {Bright light-emitting diodes based on organometal halide perovskite},
author = {Zhi-Kuang Tan and Reza Saberi Moghaddam and May Ling Lai and Pablo Docampo and Ruben Higler and Felix Deschler and Michael Price and Aditya Sadhanala and Luis M Pazos and Dan Credgington and others},
url = {https://www.nature.com/articles/nnano.2014.149},
year = {2014},
date = {2014-01-01},
journal = {Nature nanotechnology},
volume = {9},
number = {9},
pages = {687--692},
publisher = {Nature Publishing Group},
abstract = {Solid-state light-emitting devices based on direct-bandgap semiconductors have, over the past two decades, been utilized as energy-efficient sources of lighting. However, fabrication of these devices typically relies on expensive high-temperature and high-vacuum processes, rendering them uneconomical for use in large-area displays1,2. Here, we report high-brightness light-emitting diodes based on solution-processed organometal halide perovskites. We demonstrate electroluminescence in the near-infrared, green and red by tuning the halide compositions in the perovskite. In our infrared device, a thin 15 nm layer of CH3NH3PbI3–xClx perovskite emitter is sandwiched between larger-bandgap titanium dioxide (TiO2) and poly(9,9′-dioctylfluorene) (F8) layers, effectively confining electrons and holes in the perovskite layer for radiative recombination. We report an infrared radiance of 13.2 W sr−1 m−2 at a current density of 363 mA cm−2, with highest external and internal quantum efficiencies of 0.76% and 3.4%, respectively. In our green light-emitting device with an ITO/PEDOT:PSS/CH3NH3PbBr3/F8/Ca/Ag structure, we achieved a luminance of 364 cd m−2 at a current density of 123 mA cm−2, giving external and internal quantum efficiencies of 0.1% and 0.4%, respectively. We show, using photoluminescence studies, that radiative bimolecular recombination is dominant at higher excitation densities. Hence, the quantum efficiencies of the perovskite light-emitting diodes increase at higher current densities. This demonstration of effective perovskite electroluminescence offers scope for developing this unique class of materials into efficient and colour-tunable light emitters for low-cost display, lighting and optical communication applications.},
keywords = {},
pubstate = {published},
tppubtype = {article}
}
Solid-state light-emitting devices based on direct-bandgap semiconductors have, over the past two decades, been utilized as energy-efficient sources of lighting. However, fabrication of these devices typically relies on expensive high-temperature and high-vacuum processes, rendering them uneconomical for use in large-area displays1,2. Here, we report high-brightness light-emitting diodes based on solution-processed organometal halide perovskites. We demonstrate electroluminescence in the near-infrared, green and red by tuning the halide compositions in the perovskite. In our infrared device, a thin 15 nm layer of CH3NH3PbI3–xClx perovskite emitter is sandwiched between larger-bandgap titanium dioxide (TiO2) and poly(9,9′-dioctylfluorene) (F8) layers, effectively confining electrons and holes in the perovskite layer for radiative recombination. We report an infrared radiance of 13.2 W sr−1 m−2 at a current density of 363 mA cm−2, with highest external and internal quantum efficiencies of 0.76% and 3.4%, respectively. In our green light-emitting device with an ITO/PEDOT:PSS/CH3NH3PbBr3/F8/Ca/Ag structure, we achieved a luminance of 364 cd m−2 at a current density of 123 mA cm−2, giving external and internal quantum efficiencies of 0.1% and 0.4%, respectively. We show, using photoluminescence studies, that radiative bimolecular recombination is dominant at higher excitation densities. Hence, the quantum efficiencies of the perovskite light-emitting diodes increase at higher current densities. This demonstration of effective perovskite electroluminescence offers scope for developing this unique class of materials into efficient and colour-tunable light emitters for low-cost display, lighting and optical communication applications.
47.
Wang, XL; Bernardo, Angelo Di; Banerjee, Niladri; Wells, A; Bergeret, Sebastian F; Blamire, Mark Giffard; Robinson, Jason WA
Giant triplet proximity effect in superconducting pseudo spin valves with engineered anisotropy Journal Article
In: Physical Review B, vol. 89, no. 14, pp. 140508, 2014.
@article{wang2014giant,
title = {Giant triplet proximity effect in superconducting pseudo spin valves with engineered anisotropy},
author = {XL Wang and Angelo Di Bernardo and Niladri Banerjee and A Wells and Sebastian F Bergeret and Mark Giffard Blamire and Jason WA Robinson},
url = {https://journals.aps.org/prb/abstract/10.1103/PhysRevB.89.140508},
year = {2014},
date = {2014-01-01},
journal = {Physical Review B},
volume = {89},
number = {14},
pages = {140508},
publisher = {American Physical Society},
abstract = {The proximity coupling of a thin superconducting layer and an inhomogeneous ferromagnet can lead to a significant reduction of the critical temperature due to the generation of spin-polarized triplet Cooper pairs. We report critical temperature measurements of Co/Cu/NiFe(Py)/Cu/Nb superconducting pseudo spin valves (PSVs) in which the magnetization of the soft layer (Py) can be independently rotated in-plane with a magnetic field to create an angle (θ) between it and the magnetization of Co. Here we observe results consistent with spin-triplet theory and demonstrate large changes in ΔTC up to −120 mK as the Py layer is rotated from 0° (Co and Py are parallel) to 90° (Co and Py are orthogonal), which offers the potential for active control of the superconducting state. The key to this achievement is engineered magnetic anisotropy in Py, which enables well-defined control over the magnetization configuration of the PSV.},
keywords = {},
pubstate = {published},
tppubtype = {article}
}
The proximity coupling of a thin superconducting layer and an inhomogeneous ferromagnet can lead to a significant reduction of the critical temperature due to the generation of spin-polarized triplet Cooper pairs. We report critical temperature measurements of Co/Cu/NiFe(Py)/Cu/Nb superconducting pseudo spin valves (PSVs) in which the magnetization of the soft layer (Py) can be independently rotated in-plane with a magnetic field to create an angle (θ) between it and the magnetization of Co. Here we observe results consistent with spin-triplet theory and demonstrate large changes in ΔTC up to −120 mK as the Py layer is rotated from 0° (Co and Py are parallel) to 90° (Co and Py are orthogonal), which offers the potential for active control of the superconducting state. The key to this achievement is engineered magnetic anisotropy in Py, which enables well-defined control over the magnetization configuration of the PSV.
46.
Kalcheim, Yoav; Felner, Israel; Millo, Oded; Kirzhner, Tal; Koren, Gad; Bernardo, Angelo Di; Egilmez, Mehmet; Blamire, Mark G; Robinson, Jason WA
Magnetic field dependence of the proximity-induced triplet superconductivity at ferromagnet/superconductor interfaces Journal Article
In: Physical Review B, vol. 89, no. 18, pp. 180506, 2014.
@article{kalcheim2014magnetic,
title = {Magnetic field dependence of the proximity-induced triplet superconductivity at ferromagnet/superconductor interfaces},
author = {Yoav Kalcheim and Israel Felner and Oded Millo and Tal Kirzhner and Gad Koren and Angelo Di Bernardo and Mehmet Egilmez and Mark G Blamire and Jason WA Robinson},
url = {https://journals.aps.org/prb/abstract/10.1103/PhysRevB.89.180506},
year = {2014},
date = {2014-01-01},
journal = {Physical Review B},
volume = {89},
number = {18},
pages = {180506},
publisher = {APS},
abstract = {Long-ranged superconductor proximity effects recently found in superconductor-ferromagnetic (S-F) systems are generally attributed to the formation of triplet-pairing correlations due to various forms of magnetic inhomogeneities at the S-F interface. In order to investigate this conjecture within a single F layer coupled to a superconductor, we performed scanning tunneling spectroscopy on bilayers of La2/3Ca1/3MnO3 (LCMO) ferromagnetic thin films grown on high-temperature superconducting films of YBa2Cu3O7−δ or Pr1.85Ce0.15CuO4 under various magnetic fields. We find a strong correlation between the magnitude of superconductor-related spectral features measured on the LCMO layer and the degree of magnetic inhomogeneity controlled by the external magnetic field. This corroborates theoretical predictions regarding the role played by magnetic inhomogeneities in inducing triplet pairing at S-F interfaces.},
keywords = {},
pubstate = {published},
tppubtype = {article}
}
Long-ranged superconductor proximity effects recently found in superconductor-ferromagnetic (S-F) systems are generally attributed to the formation of triplet-pairing correlations due to various forms of magnetic inhomogeneities at the S-F interface. In order to investigate this conjecture within a single F layer coupled to a superconductor, we performed scanning tunneling spectroscopy on bilayers of La2/3Ca1/3MnO3 (LCMO) ferromagnetic thin films grown on high-temperature superconducting films of YBa2Cu3O7−δ or Pr1.85Ce0.15CuO4 under various magnetic fields. We find a strong correlation between the magnitude of superconductor-related spectral features measured on the LCMO layer and the degree of magnetic inhomogeneity controlled by the external magnetic field. This corroborates theoretical predictions regarding the role played by magnetic inhomogeneities in inducing triplet pairing at S-F interfaces.
45.
Bell, Nicholas Andrew William
DNA origami nanopores and single molecule transport through nanocapillaries PhD Thesis
University of Cambridge, 2014.
@phdthesis{bell2014dna,
title = {DNA origami nanopores and single molecule transport through nanocapillaries},
author = {Nicholas Andrew William Bell},
url = {https://ethos.bl.uk/OrderDetails.do?uin=uk.bl.ethos.648810},
year = {2014},
date = {2014-01-01},
school = {University of Cambridge},
keywords = {},
pubstate = {published},
tppubtype = {phdthesis}
}
2013
44.
Mertens, Jan; Eiden, Anna L; Sigle, Daniel O; Lombardo, Antonio; Sun, Zhipei; Sundaram, Ravi S; Colli, Alan; Tserkezis, Christos; Aizpurua, Javier; Milana, Silvia; others,
Controlling Sub-nm Gaps in Plasmonic Dimers using Graphene Journal Article
In: 2013.
@article{mertenscontrolling,
title = {Controlling Sub-nm Gaps in Plasmonic Dimers using Graphene},
author = {Jan Mertens and Anna L Eiden and Daniel O Sigle and Antonio Lombardo and Zhipei Sun and Ravi S Sundaram and Alan Colli and Christos Tserkezis and Javier Aizpurua and Silvia Milana and others},
url = {http://www-g.eng.cam.ac.uk/nms/publications/pdf/1305.5367v1.pdf},
year = {2013},
date = {2013-05-23},
abstract = {Graphene is used as the thinnest possible spacer between gold nanoparticles and a gold substrate. This creates a robust, repeatable, and stable sub-nanometre gap for massive plasmonic field enhancements. White
light spectroscopy of single 80 nm gold nanoparticles reveals plasmonic coupling between the particle and its image within the gold substrate. While for a single graphene layer, spectral doublets from coupled dimer modes
are observed shifted into the near infra-red, these disappear for increasing numbers of layers. These doublets arise from plasmonic charge transfer, allowing the direct optical measurement of out-of-plane conductivity in such layered systems. Gating the graphene can thus directly produce plasmon tuning.},
keywords = {},
pubstate = {published},
tppubtype = {article}
}
Graphene is used as the thinnest possible spacer between gold nanoparticles and a gold substrate. This creates a robust, repeatable, and stable sub-nanometre gap for massive plasmonic field enhancements. White
light spectroscopy of single 80 nm gold nanoparticles reveals plasmonic coupling between the particle and its image within the gold substrate. While for a single graphene layer, spectral doublets from coupled dimer modes
are observed shifted into the near infra-red, these disappear for increasing numbers of layers. These doublets arise from plasmonic charge transfer, allowing the direct optical measurement of out-of-plane conductivity in such layered systems. Gating the graphene can thus directly produce plasmon tuning.
light spectroscopy of single 80 nm gold nanoparticles reveals plasmonic coupling between the particle and its image within the gold substrate. While for a single graphene layer, spectral doublets from coupled dimer modes
are observed shifted into the near infra-red, these disappear for increasing numbers of layers. These doublets arise from plasmonic charge transfer, allowing the direct optical measurement of out-of-plane conductivity in such layered systems. Gating the graphene can thus directly produce plasmon tuning.
43.
Hernández-Ainsa, Silvia; Bell, Nicholas AW; Thacker, Vivek V; Gopfrich, Kerstin; Misiunas, Karolis; Fuentes-Perez, Maria Eugenia; Moreno-Herrero, Fernando; Keyser, Ulrich F
DNA origami nanopores for controlling DNA translocation Journal Article
In: ACS nano, vol. 7, no. 7, pp. 6024–6030, 2013.
@article{hernandez2013dna,
title = {DNA origami nanopores for controlling DNA translocation},
author = {Silvia Hernández-Ainsa and Nicholas AW Bell and Vivek V Thacker and Kerstin Gopfrich and Karolis Misiunas and Maria Eugenia Fuentes-Perez and Fernando Moreno-Herrero and Ulrich F Keyser},
url = {https://pubs.acs.org/doi/abs/10.1021/nn401759r},
year = {2013},
date = {2013-01-01},
journal = {ACS nano},
volume = {7},
number = {7},
pages = {6024--6030},
publisher = {American Chemical Society},
abstract = {We combine DNA origami structures with glass nanocapillaries to reversibly form hybrid DNA origami nanopores. Trapping of the DNA origami onto the nanocapillary is proven by imaging fluorescently labeled DNA origami structures and simultaneous ionic current measurements of the trapping events. We then show two applications highlighting the versatility of these DNA origami nanopores. First, by tuning the pore size we can control the folding of dsDNA molecules (“physical control”). Second, we show that the specific introduction of binding sites in the DNA origami nanopore allows selective detection of ssDNA as a function of the DNA sequence (“chemical control”).},
keywords = {},
pubstate = {published},
tppubtype = {article}
}
We combine DNA origami structures with glass nanocapillaries to reversibly form hybrid DNA origami nanopores. Trapping of the DNA origami onto the nanocapillary is proven by imaging fluorescently labeled DNA origami structures and simultaneous ionic current measurements of the trapping events. We then show two applications highlighting the versatility of these DNA origami nanopores. First, by tuning the pore size we can control the folding of dsDNA molecules (“physical control”). Second, we show that the specific introduction of binding sites in the DNA origami nanopore allows selective detection of ssDNA as a function of the DNA sequence (“chemical control”).
42.
Hernández-Ainsa, Silvia; Muus, Christoph; Bell, Nicholas AW; Steinbock, Lorenz J; Thacker, Vivek V; Keyser, Ulrich F
Lipid-coated nanocapillaries for DNA sensing Journal Article
In: Analyst, vol. 138, no. 1, pp. 104–106, 2013.
@article{hernandez2013lipid,
title = {Lipid-coated nanocapillaries for DNA sensing},
author = {Silvia Hernández-Ainsa and Christoph Muus and Nicholas AW Bell and Lorenz J Steinbock and Vivek V Thacker and Ulrich F Keyser},
url = {https://pubs.rsc.org/en/content/articlehtml/2012/an/c2an36397f},
year = {2013},
date = {2013-01-01},
journal = {Analyst},
volume = {138},
number = {1},
pages = {104--106},
publisher = {Royal Society of Chemistry},
abstract = {We report a simple and efficient way to accomplish the chemical modification of glass nanopores by means of lipid self-assembly. Lipid coating improves the success rate of these glass nanopores as biosensors to detect λ-DNA.},
keywords = {},
pubstate = {published},
tppubtype = {article}
}
We report a simple and efficient way to accomplish the chemical modification of glass nanopores by means of lipid self-assembly. Lipid coating improves the success rate of these glass nanopores as biosensors to detect λ-DNA.
41.
Bell, Nicholas AW; Thacker, Vivek V; Hernández-Ainsa, Silvia; Fuentes-Perez, Maria E; Moreno-Herrero, Fernando; Liedl, Tim; Keyser, Ulrich F
Multiplexed ionic current sensing with glass nanopores Journal Article
In: Lab on a Chip, vol. 13, no. 10, pp. 1859–1862, 2013.
@article{bell2013multiplexed,
title = {Multiplexed ionic current sensing with glass nanopores},
author = {Nicholas AW Bell and Vivek V Thacker and Silvia Hernández-Ainsa and Maria E Fuentes-Perez and Fernando Moreno-Herrero and Tim Liedl and Ulrich F Keyser},
url = {https://pdfs.semanticscholar.org/0b99/a0158f957c4c40c9c8e4b298b906acb0301e.pdf},
year = {2013},
date = {2013-01-01},
journal = {Lab on a Chip},
volume = {13},
number = {10},
pages = {1859--1862},
publisher = {Royal Society of Chemistry},
abstract = {We report a method for simultaneous ionic current measurements of single molecules across up to 16 solid state nanopore channels. Each device, costing less than $20, contains 16 glass nanopores made by laser assisted capillary pulling. We demonstrate simultaneous multichannel detection of double stranded DNA and trapping of DNA origami nanostructures to form hybrid nanopores.},
keywords = {},
pubstate = {published},
tppubtype = {article}
}
We report a method for simultaneous ionic current measurements of single molecules across up to 16 solid state nanopore channels. Each device, costing less than $20, contains 16 glass nanopores made by laser assisted capillary pulling. We demonstrate simultaneous multichannel detection of double stranded DNA and trapping of DNA origami nanostructures to form hybrid nanopores.
40.
Bell, Nicholas AW; Thacker, Vivek V; Hernández-Ainsa, Silvia; Fuentes-Perez, Maria E; Moreno-Herrero, Fernando; Liedlc, Tim; Keyser, Ulrich F
TECHNICAL INNOVATION Journal Article
In: Lab Chip, vol. 13, pp. 1859–1862, 2013.
@article{bell2013technical,
title = {TECHNICAL INNOVATION},
author = {Nicholas AW Bell and Vivek V Thacker and Silvia Hernández-Ainsa and Maria E Fuentes-Perez and Fernando Moreno-Herrero and Tim Liedlc and Ulrich F Keyser},
year = {2013},
date = {2013-01-01},
journal = {Lab Chip},
volume = {13},
pages = {1859--1862},
keywords = {},
pubstate = {published},
tppubtype = {article}
}
39.
Sha, Jingjie; Hasan, Tawfique; Milana, Silvia; Bertulli, Cristina; Bell, Nicholas AW; Privitera, Giulia; Ni, Zhonghua; Chen, Yunfei; Bonaccorso, Francesco; Ferrari, Andrea C; others,
Nanotubes complexed with DNA and proteins for resistive-pulse sensing Journal Article
In: ACS nano, vol. 7, no. 10, pp. 8857–8869, 2013.
@article{sha2013nanotubes,
title = {Nanotubes complexed with DNA and proteins for resistive-pulse sensing},
author = {Jingjie Sha and Tawfique Hasan and Silvia Milana and Cristina Bertulli and Nicholas AW Bell and Giulia Privitera and Zhonghua Ni and Yunfei Chen and Francesco Bonaccorso and Andrea C Ferrari and others},
url = {https://pubs.acs.org/doi/abs/10.1021/nn403323k},
year = {2013},
date = {2013-01-01},
journal = {ACS nano},
volume = {7},
number = {10},
pages = {8857--8869},
publisher = {American Chemical Society},
abstract = {We use a resistive-pulse technique to analyze molecular hybrids of single-wall carbon nanotubes (SWNTs) wrapped in either single-stranded DNA or protein. Electric fields confined in a glass capillary nanopore allow us to probe the physical size and surface properties of molecular hybrids at the single-molecule level. We find that the translocation duration of a macromolecular hybrid is determined by its hydrodynamic size and solution mobility. The event current reveals the effects of ion exclusion by the rod-shaped hybrids and possible effects due to temporary polarization of the SWNT core. Our results pave the way to direct sensing of small DNA or protein molecules in a large unmodified solid-state nanopore by using nanofilaments as carriers.},
keywords = {},
pubstate = {published},
tppubtype = {article}
}
We use a resistive-pulse technique to analyze molecular hybrids of single-wall carbon nanotubes (SWNTs) wrapped in either single-stranded DNA or protein. Electric fields confined in a glass capillary nanopore allow us to probe the physical size and surface properties of molecular hybrids at the single-molecule level. We find that the translocation duration of a macromolecular hybrid is determined by its hydrodynamic size and solution mobility. The event current reveals the effects of ion exclusion by the rod-shaped hybrids and possible effects due to temporary polarization of the SWNT core. Our results pave the way to direct sensing of small DNA or protein molecules in a large unmodified solid-state nanopore by using nanofilaments as carriers.
38.
Michaelis, Benjamin; Snoswell, David RE; Bell, Nicholas AW; Spahn, Peter; Hellmann, Goetz P; Finlayson, Chris E; Baumberg, Jeremy J
Generating Lithographically-D efined Tunable Printed Structural Color Journal Article
In: Advanced Engineering Materials, vol. 15, no. 10, pp. 948–953, 2013.
@article{michaelis2013generating,
title = {Generating Lithographically-D efined Tunable Printed Structural Color},
author = {Benjamin Michaelis and David RE Snoswell and Nicholas AW Bell and Peter Spahn and Goetz P Hellmann and Chris E Finlayson and Jeremy J Baumberg},
url = {https://onlinelibrary.wiley.com/doi/abs/10.1002/adem.201300089},
year = {2013},
date = {2013-01-01},
journal = {Advanced Engineering Materials},
volume = {15},
number = {10},
pages = {948--953},
abstract = {A tunable method for generating non‐fading printed structural color is demonstrated. The process involves the rapid generation and self‐assembly of particle strings, using standard colloidal polymeric particles and AC electric fields, with no requirement for a “wash‐out” step. By using an organic UV‐curable medium, we demonstrate that these tunable structures can be permanently fixed in a flexible polymer matrix and thus are suitable for printing applications.},
keywords = {},
pubstate = {published},
tppubtype = {article}
}
A tunable method for generating non‐fading printed structural color is demonstrated. The process involves the rapid generation and self‐assembly of particle strings, using standard colloidal polymeric particles and AC electric fields, with no requirement for a “wash‐out” step. By using an organic UV‐curable medium, we demonstrate that these tunable structures can be permanently fixed in a flexible polymer matrix and thus are suitable for printing applications.
37.
Bell, Nicholas; Hernandez-Ainsa, Silvia; Engst, Christian; Liedl, Tim; Keyser, Ulrich
DNA Origami Nanopores Journal Article
In: Biophysical Journal, vol. 104, no. 2, pp. 517a, 2013.
@article{bell2013dna,
title = {DNA Origami Nanopores},
author = {Nicholas Bell and Silvia Hernandez-Ainsa and Christian Engst and Tim Liedl and Ulrich Keyser},
year = {2013},
date = {2013-01-01},
journal = {Biophysical Journal},
volume = {104},
number = {2},
pages = {517a},
publisher = {Elsevier},
keywords = {},
pubstate = {published},
tppubtype = {article}
}
36.
Frišči'c, Tomislav; Halasz, Ivan; Beldon, Patrick J; Belenguer, Ana M; Adams, Frank; Kimber, Simon AJ; Honkimäki, Veijo; Dinnebier, Robert E
Real-time and in situ monitoring of mechanochemical milling reactions Journal Article
In: Nature chemistry, vol. 5, no. 1, pp. 66, 2013.
@article{frivsvcic2013real,
title = {Real-time and in situ monitoring of mechanochemical milling reactions},
author = {Tomislav Friš{č}i{'c} and Ivan Halasz and Patrick J Beldon and Ana M Belenguer and Frank Adams and Simon AJ Kimber and Veijo Honkimäki and Robert E Dinnebier},
url = {https://www.nature.com/articles/nchem.1505.pdf?origin=ppub},
year = {2013},
date = {2013-01-01},
journal = {Nature chemistry},
volume = {5},
number = {1},
pages = {66},
publisher = {Nature Publishing Group},
abstract = {Chemical and structural transformations have long been carried out by milling. Such mechanochemical steps are now ubiquitous in a number of industries (such as the pharmaceutical, chemical and metallurgical industries), and are emerging as excellent environmentally friendly alternatives to solution-based syntheses. However, mechanochemical transformations are typically difficult to monitor in real time, which leaves a large gap in the mechanistic understanding required for their development. We now report the real-time study of mechanochemical transformations in a ball mill by means of in situ diffraction of high-energy synchrotron X-rays. Focusing on the mechanosynthesis of metal–organic frameworks, we have directly monitored reaction profiles, the formation of intermediates, and interconversions of framework topologies. Our results reveal that mechanochemistry is highly dynamic, with reaction rates comparable to or greater than those in solution. The technique also enabled us to probe directly how catalytic additives recently introduced in the mechanosynthesis of metal–organic frameworks, such as organic liquids or ionic species, change the reactivity pathways and kinetics.},
keywords = {},
pubstate = {published},
tppubtype = {article}
}
Chemical and structural transformations have long been carried out by milling. Such mechanochemical steps are now ubiquitous in a number of industries (such as the pharmaceutical, chemical and metallurgical industries), and are emerging as excellent environmentally friendly alternatives to solution-based syntheses. However, mechanochemical transformations are typically difficult to monitor in real time, which leaves a large gap in the mechanistic understanding required for their development. We now report the real-time study of mechanochemical transformations in a ball mill by means of in situ diffraction of high-energy synchrotron X-rays. Focusing on the mechanosynthesis of metal–organic frameworks, we have directly monitored reaction profiles, the formation of intermediates, and interconversions of framework topologies. Our results reveal that mechanochemistry is highly dynamic, with reaction rates comparable to or greater than those in solution. The technique also enabled us to probe directly how catalytic additives recently introduced in the mechanosynthesis of metal–organic frameworks, such as organic liquids or ionic species, change the reactivity pathways and kinetics.
35.
Halasz, Ivan; Kimber, Simon AJ; Beldon, Patrick J; Belenguer, Ana M; Adams, Frank; Honkimäki, Veijo; Nightingale, Richard C; Dinnebier, Robert E; Frišči'c, Tomislav
In situ and real-time monitoring of mechanochemical milling reactions using synchrotron X-ray diffraction Journal Article
In: Nature protocols, vol. 8, no. 9, pp. 1718, 2013.
@article{halasz2013situ,
title = {In situ and real-time monitoring of mechanochemical milling reactions using synchrotron X-ray diffraction},
author = {Ivan Halasz and Simon AJ Kimber and Patrick J Beldon and Ana M Belenguer and Frank Adams and Veijo Honkimäki and Richard C Nightingale and Robert E Dinnebier and Tomislav Friš{č}i{'c}},
url = {https://www.nature.com/articles/nprot.2013.100.pdf?origin=ppub},
year = {2013},
date = {2013-01-01},
journal = {Nature protocols},
volume = {8},
number = {9},
pages = {1718},
publisher = {Nature Publishing Group},
abstract = {We describe the only currently available protocol for in situ, real-time monitoring of mechanochemical reactions and intermediates
by X-ray powder diffraction. Although mechanochemical reactions (inducing transformations by mechanical forces such as grinding
and milling) are normally performed in commercially available milling assemblies, such equipment does not permit direct reaction
monitoring. We now describe the design and in-house modification of milling equipment that allows the reaction jars of the
operating mill to be placed in the path of a high-energy (~90 keV) synchrotron X-ray beam while the reaction is taking place.
Resulting data are analyzed using conventional software, such as TOPAS. Reaction intermediates and products are identified using
the Cambridge Structural Database or Inorganic Crystal Structure Database. Reactions are analyzed by fitting the time-resolved
diffractograms using structureless Pawley refinement for crystalline phases that are not fully structurally characterized
(such as porous frameworks with disordered guests), or the Rietveld method for solids with fully determined crystal structures
(metal oxides, coordination polymers).},
keywords = {},
pubstate = {published},
tppubtype = {article}
}
We describe the only currently available protocol for in situ, real-time monitoring of mechanochemical reactions and intermediates
by X-ray powder diffraction. Although mechanochemical reactions (inducing transformations by mechanical forces such as grinding
and milling) are normally performed in commercially available milling assemblies, such equipment does not permit direct reaction
monitoring. We now describe the design and in-house modification of milling equipment that allows the reaction jars of the
operating mill to be placed in the path of a high-energy (~90 keV) synchrotron X-ray beam while the reaction is taking place.
Resulting data are analyzed using conventional software, such as TOPAS. Reaction intermediates and products are identified using
the Cambridge Structural Database or Inorganic Crystal Structure Database. Reactions are analyzed by fitting the time-resolved
diffractograms using structureless Pawley refinement for crystalline phases that are not fully structurally characterized
(such as porous frameworks with disordered guests), or the Rietveld method for solids with fully determined crystal structures
(metal oxides, coordination polymers).
by X-ray powder diffraction. Although mechanochemical reactions (inducing transformations by mechanical forces such as grinding
and milling) are normally performed in commercially available milling assemblies, such equipment does not permit direct reaction
monitoring. We now describe the design and in-house modification of milling equipment that allows the reaction jars of the
operating mill to be placed in the path of a high-energy (~90 keV) synchrotron X-ray beam while the reaction is taking place.
Resulting data are analyzed using conventional software, such as TOPAS. Reaction intermediates and products are identified using
the Cambridge Structural Database or Inorganic Crystal Structure Database. Reactions are analyzed by fitting the time-resolved
diffractograms using structureless Pawley refinement for crystalline phases that are not fully structurally characterized
(such as porous frameworks with disordered guests), or the Rietveld method for solids with fully determined crystal structures
(metal oxides, coordination polymers).
34.
Halasz, Ivan; Puškari'c, Andreas; Kimber, Simon AJ; Beldon, Patrick J; Belenguer, Ana M; Adams, Frank; Honkimäki, Veijo; Dinnebier, Robert E; Patel, Bhavnita; Jones, William; others,
Real-Time In Situ Powder X-ray Diffraction Monitoring of Mechanochemical Synthesis of Pharmaceutical Cocrystals (Angew. Chem. Int. Ed. 44/2013) Journal Article
In: Angewandte Chemie International Edition, vol. 52, no. 44, pp. 11665–11665, 2013.
@article{halasz2013real,
title = {Real-Time In Situ Powder X-ray Diffraction Monitoring of Mechanochemical Synthesis of Pharmaceutical Cocrystals (Angew. Chem. Int. Ed. 44/2013)},
author = {Ivan Halasz and Andreas Puškari{'c} and Simon AJ Kimber and Patrick J Beldon and Ana M Belenguer and Frank Adams and Veijo Honkimäki and Robert E Dinnebier and Bhavnita Patel and William Jones and others},
url = {https://onlinelibrary.wiley.com/doi/full/10.1002/ange.201305928},
year = {2013},
date = {2013-01-01},
journal = {Angewandte Chemie International Edition},
volume = {52},
number = {44},
pages = {11665--11665},
publisher = {WILEY-VCH Verlag},
keywords = {},
pubstate = {published},
tppubtype = {article}
}
33.
Bertulli, Cristina; Beeson, Harry J; Hasan, Tawfique; Huang, Yan Yan S
In: Nanotechnology, vol. 24, no. 26, pp. 265102, 2013.
@article{bertulli2013spectroscopic,
title = {Spectroscopic characterization of protein-wrapped single-wall carbon nanotubes and quantification of their cellular uptake in multiple cell generations},
author = {Cristina Bertulli and Harry J Beeson and Tawfique Hasan and Yan Yan S Huang},
url = {https://iopscience.iop.org/article/10.1088/0957-4484/24/26/265102/meta},
year = {2013},
date = {2013-01-01},
journal = {Nanotechnology},
volume = {24},
number = {26},
pages = {265102},
publisher = {IOP Publishing},
abstract = {We study the spectral characteristics of bovine serum albumin (BSA) protein conjugated single-wall carbon nanotubes (SWNTs), and quantify their uptake by macrophages. The binding of BSA onto the SWNT surface is found to change the protein structure and to increase the doping of the nanotubes. The G-band Raman intensity follows a well-defined power law for SWNT concentrations of up to 33 μg ml−1 in aqueous solutions. Subsequently, in vitro experiments demonstrate that incubation of BSA-SWNT complexes with macrophages affects neither the cellular growth nor the cellular viability over multiple cell generations. Using wide spot Raman spectroscopy as a fast, non-destructive method for statistical quantification, we observe that macrophages effectively uptake BSA-SWNT complexes, with the average number of nanotubes internalized per cell remaining relatively constant over consecutive cell generations. The number of internalized SWNTs is found to be ~30 × 106 SWNTs/cell for a 60 mm−2 seeding density and ~100 × 106 SWNTs/cell for a 200 mm−2 seeding density. Our results show that BSA-functionalized SWNTs are an efficient molecular transport system with low cytotoxicity maintained over multiple cell generations.},
keywords = {},
pubstate = {published},
tppubtype = {article}
}
We study the spectral characteristics of bovine serum albumin (BSA) protein conjugated single-wall carbon nanotubes (SWNTs), and quantify their uptake by macrophages. The binding of BSA onto the SWNT surface is found to change the protein structure and to increase the doping of the nanotubes. The G-band Raman intensity follows a well-defined power law for SWNT concentrations of up to 33 μg ml−1 in aqueous solutions. Subsequently, in vitro experiments demonstrate that incubation of BSA-SWNT complexes with macrophages affects neither the cellular growth nor the cellular viability over multiple cell generations. Using wide spot Raman spectroscopy as a fast, non-destructive method for statistical quantification, we observe that macrophages effectively uptake BSA-SWNT complexes, with the average number of nanotubes internalized per cell remaining relatively constant over consecutive cell generations. The number of internalized SWNTs is found to be ~30 × 106 SWNTs/cell for a 60 mm−2 seeding density and ~100 × 106 SWNTs/cell for a 200 mm−2 seeding density. Our results show that BSA-functionalized SWNTs are an efficient molecular transport system with low cytotoxicity maintained over multiple cell generations.