---
_id: '13216'
abstract:
- lang: eng
text: Physical catalysts often have multiple sites where reactions can take place.
One prominent example is single-atom alloys, where the reactive dopant atoms can
preferentially locate in the bulk or at different sites on the surface of the
nanoparticle. However, ab initio modeling of catalysts usually only considers
one site of the catalyst, neglecting the effects of multiple sites. Here, nanoparticles
of copper doped with single-atom rhodium or palladium are modeled for the dehydrogenation
of propane. Single-atom alloy nanoparticles are simulated at 400–600 K, using
machine learning potentials trained on density functional theory calculations,
and then the occupation of different single-atom active sites is identified using
a similarity kernel. Further, the turnover frequency for all possible sites is
calculated for propane dehydrogenation to propene through microkinetic modeling
using density functional theory calculations. The total turnover frequencies of
the whole nanoparticle are then described from both the population and the individual
turnover frequency of each site. Under operating conditions, rhodium as a dopant
is found to almost exclusively occupy (111) surface sites while palladium as a
dopant occupies a greater variety of facets. Undercoordinated dopant surface sites
are found to tend to be more reactive for propane dehydrogenation compared to
the (111) surface. It is found that considering the dynamics of the single-atom
alloy nanoparticle has a profound effect on the calculated catalytic activity
of single-atom alloys by several orders of magnitude.
acknowledgement: "B.C. acknowledges resources provided by the Cambridge Tier2 system
operated by the University of Cambridge Research\r\nComputing Service funded by
EPSRC Tier-2 capital grant EP/\r\nP020259/1."
article_processing_charge: Yes (via OA deal)
article_type: original
author:
- first_name: Rhys
full_name: Bunting, Rhys
id: 91deeae8-1207-11ec-b130-c194ad5b50c6
last_name: Bunting
orcid: 0000-0001-6928-074X
- first_name: Felix
full_name: Wodaczek, Felix
id: 8b4b6a9f-32b0-11ee-9fa8-bbe85e26258e
last_name: Wodaczek
orcid: 0009-0000-1457-795X
- first_name: Tina
full_name: Torabi, Tina
last_name: Torabi
- first_name: Bingqing
full_name: Cheng, Bingqing
id: cbe3cda4-d82c-11eb-8dc7-8ff94289fcc9
last_name: Cheng
orcid: 0000-0002-3584-9632
citation:
ama: 'Bunting R, Wodaczek F, Torabi T, Cheng B. Reactivity of single-atom alloy
nanoparticles: Modeling the dehydrogenation of propane. Journal of the American
Chemical Society. 2023;145(27):14894-14902. doi:10.1021/jacs.3c04030'
apa: 'Bunting, R., Wodaczek, F., Torabi, T., & Cheng, B. (2023). Reactivity
of single-atom alloy nanoparticles: Modeling the dehydrogenation of propane. Journal
of the American Chemical Society. American Chemical Society. https://doi.org/10.1021/jacs.3c04030'
chicago: 'Bunting, Rhys, Felix Wodaczek, Tina Torabi, and Bingqing Cheng. “Reactivity
of Single-Atom Alloy Nanoparticles: Modeling the Dehydrogenation of Propane.”
Journal of the American Chemical Society. American Chemical Society, 2023.
https://doi.org/10.1021/jacs.3c04030.'
ieee: 'R. Bunting, F. Wodaczek, T. Torabi, and B. Cheng, “Reactivity of single-atom
alloy nanoparticles: Modeling the dehydrogenation of propane,” Journal of the
American Chemical Society, vol. 145, no. 27. American Chemical Society, pp.
14894–14902, 2023.'
ista: 'Bunting R, Wodaczek F, Torabi T, Cheng B. 2023. Reactivity of single-atom
alloy nanoparticles: Modeling the dehydrogenation of propane. Journal of the American
Chemical Society. 145(27), 14894–14902.'
mla: 'Bunting, Rhys, et al. “Reactivity of Single-Atom Alloy Nanoparticles: Modeling
the Dehydrogenation of Propane.” Journal of the American Chemical Society,
vol. 145, no. 27, American Chemical Society, 2023, pp. 14894–902, doi:10.1021/jacs.3c04030.'
short: R. Bunting, F. Wodaczek, T. Torabi, B. Cheng, Journal of the American Chemical
Society 145 (2023) 14894–14902.
date_created: 2023-07-12T09:16:40Z
date_published: 2023-06-30T00:00:00Z
date_updated: 2023-10-11T08:45:10Z
day: '30'
ddc:
- '540'
department:
- _id: MaIb
- _id: BiCh
doi: 10.1021/jacs.3c04030
external_id:
isi:
- '001020623900001'
pmid:
- '37390457'
file:
- access_level: open_access
checksum: e07d5323f9c0e5cbd1ad6453f29440ab
content_type: application/pdf
creator: cchlebak
date_created: 2023-07-12T10:22:04Z
date_updated: 2023-07-12T10:22:04Z
file_id: '13219'
file_name: 2023_JACS_Bunting.pdf
file_size: 3155843
relation: main_file
success: 1
file_date_updated: 2023-07-12T10:22:04Z
has_accepted_license: '1'
intvolume: ' 145'
isi: 1
issue: '27'
keyword:
- Colloid and Surface Chemistry
- Biochemistry
- General Chemistry
- Catalysis
language:
- iso: eng
month: '06'
oa: 1
oa_version: Published Version
page: 14894-14902
pmid: 1
publication: Journal of the American Chemical Society
publication_identifier:
eissn:
- 1520-5126
issn:
- 0002-7863
publication_status: published
publisher: American Chemical Society
quality_controlled: '1'
status: public
title: 'Reactivity of single-atom alloy nanoparticles: Modeling the dehydrogenation
of propane'
tmp:
image: /images/cc_by.png
legal_code_url: https://creativecommons.org/licenses/by/4.0/legalcode
name: Creative Commons Attribution 4.0 International Public License (CC-BY 4.0)
short: CC BY (4.0)
type: journal_article
user_id: 8b945eb4-e2f2-11eb-945a-df72226e66a9
volume: 145
year: '2023'
...
---
_id: '13354'
abstract:
- lang: eng
text: 'Integrating light-sensitive molecules within nanoparticle (NP) assemblies
is an attractive approach to fabricate new photoresponsive nanomaterials. Here,
we describe the concept of photocleavable anionic glue (PAG): small trianions
capable of mediating interactions between (and inducing the aggregation of) cationic
NPs by means of electrostatic interactions. Exposure to light converts PAGs into
dianionic products incapable of maintaining the NPs in an assembled state, resulting
in light-triggered disassembly of NP aggregates. To demonstrate the proof-of-concept,
we work with an organic PAG incorporating the UV-cleavable o-nitrobenzyl moiety
and an inorganic PAG, the photosensitive trioxalatocobaltate(III) complex, which
absorbs light across the entire visible spectrum. Both PAGs were used to prepare
either amorphous NP assemblies or regular superlattices with a long-range NP order.
These NP aggregates disassembled rapidly upon light exposure for a specific time,
which could be tuned by the incident light wavelength or the amount of PAG used.
Selective excitation of the inorganic PAG in a system combining the two PAGs results
in a photodecomposition product that deactivates the organic PAG, enabling nontrivial
disassembly profiles under a single type of external stimulus.'
article_processing_charge: No
article_type: original
author:
- first_name: Jinhua
full_name: Wang, Jinhua
last_name: Wang
- first_name: Tzuf Shay
full_name: Peled, Tzuf Shay
last_name: Peled
- first_name: Rafal
full_name: Klajn, Rafal
id: 8e84690e-1e48-11ed-a02b-a1e6fb8bb53b
last_name: Klajn
citation:
ama: Wang J, Peled TS, Klajn R. Photocleavable anionic glues for light-responsive
nanoparticle aggregates. Journal of the American Chemical Society. 2023;145(7):4098-4108.
doi:10.1021/jacs.2c11973
apa: Wang, J., Peled, T. S., & Klajn, R. (2023). Photocleavable anionic glues
for light-responsive nanoparticle aggregates. Journal of the American Chemical
Society. American Chemical Society. https://doi.org/10.1021/jacs.2c11973
chicago: Wang, Jinhua, Tzuf Shay Peled, and Rafal Klajn. “Photocleavable Anionic
Glues for Light-Responsive Nanoparticle Aggregates.” Journal of the American
Chemical Society. American Chemical Society, 2023. https://doi.org/10.1021/jacs.2c11973.
ieee: J. Wang, T. S. Peled, and R. Klajn, “Photocleavable anionic glues for light-responsive
nanoparticle aggregates,” Journal of the American Chemical Society, vol.
145, no. 7. American Chemical Society, pp. 4098–4108, 2023.
ista: Wang J, Peled TS, Klajn R. 2023. Photocleavable anionic glues for light-responsive
nanoparticle aggregates. Journal of the American Chemical Society. 145(7), 4098–4108.
mla: Wang, Jinhua, et al. “Photocleavable Anionic Glues for Light-Responsive Nanoparticle
Aggregates.” Journal of the American Chemical Society, vol. 145, no. 7,
American Chemical Society, 2023, pp. 4098–108, doi:10.1021/jacs.2c11973.
short: J. Wang, T.S. Peled, R. Klajn, Journal of the American Chemical Society 145
(2023) 4098–4108.
date_created: 2023-08-01T09:33:08Z
date_published: 2023-02-09T00:00:00Z
date_updated: 2023-08-02T10:44:22Z
day: '09'
doi: 10.1021/jacs.2c11973
extern: '1'
external_id:
pmid:
- '36757850'
intvolume: ' 145'
issue: '7'
keyword:
- Colloid and Surface Chemistry
- Biochemistry
- General Chemistry
- Catalysis
language:
- iso: eng
main_file_link:
- open_access: '1'
url: https://doi.org/10.1021/jacs.2c11973
month: '02'
oa: 1
oa_version: Published Version
page: 4098-4108
pmid: 1
publication: Journal of the American Chemical Society
publication_identifier:
eissn:
- 1520-5126
issn:
- 0002-7863
publication_status: published
publisher: American Chemical Society
quality_controlled: '1'
scopus_import: '1'
status: public
title: Photocleavable anionic glues for light-responsive nanoparticle aggregates
type: journal_article
user_id: 2DF688A6-F248-11E8-B48F-1D18A9856A87
volume: 145
year: '2023'
...
---
_id: '13348'
abstract:
- lang: eng
text: Molecular confinement effects can profoundly alter the physicochemical properties
of the confined species. A plethora of organic molecules were encapsulated within
the cavities of supramolecular hosts, and the impact of the cavity size and polarity
was widely investigated. However, the extent to which the properties of the confined
guests can be affected by the symmetry of the cage─which dictates the shape of
the cavity─remains to be understood. Here we show that cage symmetry has a dramatic
effect on the equilibrium between two isomers of the encapsulated spiropyran guests.
Working with two Pd-based coordination cages featuring similarly sized but differently
shaped hydrophobic cavities, we found a highly selective stabilization of the
isomer whose shape matches that of the cavity of the cage. A Td-symmetric cage
stabilized the spiropyrans’ colorless form and rendered them photochemically inert.
In contrast, a D2h-symmetric cage favored the colored isomer, while maintaining
reversible photoswitching between the two states of the encapsulated spiropyrans.
We also show that the switching kinetics strongly depend on the substitution pattern
on the spiropyran scaffold. This finding was used to fabricate a time-sensitive
information storage medium with tunable lifetimes of the encoded messages.
article_processing_charge: No
article_type: original
author:
- first_name: Jinhua
full_name: Wang, Jinhua
last_name: Wang
- first_name: Liat
full_name: Avram, Liat
last_name: Avram
- first_name: Yael
full_name: Diskin-Posner, Yael
last_name: Diskin-Posner
- first_name: Michał J.
full_name: Białek, Michał J.
last_name: Białek
- first_name: Wojciech
full_name: Stawski, Wojciech
last_name: Stawski
- first_name: Moran
full_name: Feller, Moran
last_name: Feller
- first_name: Rafal
full_name: Klajn, Rafal
id: 8e84690e-1e48-11ed-a02b-a1e6fb8bb53b
last_name: Klajn
citation:
ama: Wang J, Avram L, Diskin-Posner Y, et al. Altering the properties of spiropyran
switches using coordination cages with different symmetries. Journal of the
American Chemical Society. 2022;144(46):21244-21254. doi:10.1021/jacs.2c08901
apa: Wang, J., Avram, L., Diskin-Posner, Y., Białek, M. J., Stawski, W., Feller,
M., & Klajn, R. (2022). Altering the properties of spiropyran switches using
coordination cages with different symmetries. Journal of the American Chemical
Society. American Chemical Society. https://doi.org/10.1021/jacs.2c08901
chicago: Wang, Jinhua, Liat Avram, Yael Diskin-Posner, Michał J. Białek, Wojciech
Stawski, Moran Feller, and Rafal Klajn. “Altering the Properties of Spiropyran
Switches Using Coordination Cages with Different Symmetries.” Journal of the
American Chemical Society. American Chemical Society, 2022. https://doi.org/10.1021/jacs.2c08901.
ieee: J. Wang et al., “Altering the properties of spiropyran switches using
coordination cages with different symmetries,” Journal of the American Chemical
Society, vol. 144, no. 46. American Chemical Society, pp. 21244–21254, 2022.
ista: Wang J, Avram L, Diskin-Posner Y, Białek MJ, Stawski W, Feller M, Klajn R.
2022. Altering the properties of spiropyran switches using coordination cages
with different symmetries. Journal of the American Chemical Society. 144(46),
21244–21254.
mla: Wang, Jinhua, et al. “Altering the Properties of Spiropyran Switches Using
Coordination Cages with Different Symmetries.” Journal of the American Chemical
Society, vol. 144, no. 46, American Chemical Society, 2022, pp. 21244–54,
doi:10.1021/jacs.2c08901.
short: J. Wang, L. Avram, Y. Diskin-Posner, M.J. Białek, W. Stawski, M. Feller,
R. Klajn, Journal of the American Chemical Society 144 (2022) 21244–21254.
date_created: 2023-08-01T09:31:01Z
date_published: 2022-11-15T00:00:00Z
date_updated: 2023-08-02T06:39:50Z
day: '15'
doi: 10.1021/jacs.2c08901
extern: '1'
intvolume: ' 144'
issue: '46'
keyword:
- Colloid and Surface Chemistry
- Biochemistry
- General Chemistry
- Catalysis
language:
- iso: eng
main_file_link:
- open_access: '1'
url: https://doi.org/10.1021/jacs.2c08901
month: '11'
oa: 1
oa_version: Published Version
page: 21244-21254
publication: Journal of the American Chemical Society
publication_identifier:
eissn:
- 1520-5126
issn:
- 0002-7863
publication_status: published
publisher: American Chemical Society
quality_controlled: '1'
scopus_import: '1'
status: public
title: Altering the properties of spiropyran switches using coordination cages with
different symmetries
type: journal_article
user_id: 2DF688A6-F248-11E8-B48F-1D18A9856A87
volume: 144
year: '2022'
...
---
_id: '13362'
abstract:
- lang: eng
text: Aggregation of organic molecules can drastically affect their physicochemical
properties. For instance, the optical properties of BODIPY dyes are inherently
related to the degree of aggregation and the mutual orientation of BODIPY units
within these aggregates. Whereas the noncovalent aggregation of various BODIPY
dyes has been studied in diverse media, the ill-defined nature of these aggregates
has made it difficult to elucidate the structure–property relationships. Here,
we studied the encapsulation of three structurally simple BODIPY derivatives within
the hydrophobic cavity of a water-soluble, flexible PdII6L4 coordination cage.
The cavity size allowed for the selective encapsulation of two dye molecules,
irrespective of the substitution pattern on the BODIPY core. Working with a model,
a pentamethyl-substituted derivative, we found that the mutual orientation of
two BODIPY units in the cage’s cavity was remarkably similar to that in the crystalline
state of the free dye, allowing us to isolate and characterize the smallest possible
noncovalent H-type BODIPY aggregate, namely, an H-dimer. Interestingly, a CF3-substituted
BODIPY, known for forming J-type aggregates, was also encapsulated as an H-dimer.
Taking advantage of the dynamic nature of encapsulation, we developed a system
in which reversible switching between H- and J-aggregates can be induced for multiple
cycles simply by addition and subsequent destruction of the cage. We expect that
the ability to rapidly and reversibly manipulate the optical properties of supramolecular
inclusion complexes in aqueous media will open up avenues for developing detection
systems that operate within biological environments.
article_processing_charge: No
article_type: original
author:
- first_name: Julius
full_name: Gemen, Julius
last_name: Gemen
- first_name: Johannes
full_name: Ahrens, Johannes
last_name: Ahrens
- first_name: Linda J. W.
full_name: Shimon, Linda J. W.
last_name: Shimon
- first_name: Rafal
full_name: Klajn, Rafal
id: 8e84690e-1e48-11ed-a02b-a1e6fb8bb53b
last_name: Klajn
citation:
ama: Gemen J, Ahrens J, Shimon LJW, Klajn R. Modulating the optical properties of
BODIPY dyes by noncovalent dimerization within a flexible coordination cage. Journal
of the American Chemical Society. 2020;142(41):17721-17729. doi:10.1021/jacs.0c08589
apa: Gemen, J., Ahrens, J., Shimon, L. J. W., & Klajn, R. (2020). Modulating
the optical properties of BODIPY dyes by noncovalent dimerization within a flexible
coordination cage. Journal of the American Chemical Society. American Chemical
Society. https://doi.org/10.1021/jacs.0c08589
chicago: Gemen, Julius, Johannes Ahrens, Linda J. W. Shimon, and Rafal Klajn. “Modulating
the Optical Properties of BODIPY Dyes by Noncovalent Dimerization within a Flexible
Coordination Cage.” Journal of the American Chemical Society. American
Chemical Society, 2020. https://doi.org/10.1021/jacs.0c08589.
ieee: J. Gemen, J. Ahrens, L. J. W. Shimon, and R. Klajn, “Modulating the optical
properties of BODIPY dyes by noncovalent dimerization within a flexible coordination
cage,” Journal of the American Chemical Society, vol. 142, no. 41. American
Chemical Society, pp. 17721–17729, 2020.
ista: Gemen J, Ahrens J, Shimon LJW, Klajn R. 2020. Modulating the optical properties
of BODIPY dyes by noncovalent dimerization within a flexible coordination cage.
Journal of the American Chemical Society. 142(41), 17721–17729.
mla: Gemen, Julius, et al. “Modulating the Optical Properties of BODIPY Dyes by
Noncovalent Dimerization within a Flexible Coordination Cage.” Journal of the
American Chemical Society, vol. 142, no. 41, American Chemical Society, 2020,
pp. 17721–29, doi:10.1021/jacs.0c08589.
short: J. Gemen, J. Ahrens, L.J.W. Shimon, R. Klajn, Journal of the American Chemical
Society 142 (2020) 17721–17729.
date_created: 2023-08-01T09:36:10Z
date_published: 2020-10-04T00:00:00Z
date_updated: 2023-08-07T10:09:54Z
day: '04'
doi: 10.1021/jacs.0c08589
extern: '1'
external_id:
pmid:
- '33006898'
intvolume: ' 142'
issue: '41'
keyword:
- Colloid and Surface Chemistry
- Biochemistry
- General Chemistry
- Catalysis
language:
- iso: eng
main_file_link:
- open_access: '1'
url: https://doi.org/10.1021/jacs.0c08589
month: '10'
oa: 1
oa_version: Published Version
page: 17721-17729
pmid: 1
publication: Journal of the American Chemical Society
publication_identifier:
eissn:
- 1520-5126
issn:
- 0002-7863
publication_status: published
publisher: American Chemical Society
quality_controlled: '1'
scopus_import: '1'
status: public
title: Modulating the optical properties of BODIPY dyes by noncovalent dimerization
within a flexible coordination cage
type: journal_article
user_id: 2DF688A6-F248-11E8-B48F-1D18A9856A87
volume: 142
year: '2020'
...
---
_id: '13364'
abstract:
- lang: eng
text: Photochromic molecules undergo reversible isomerization upon irradiation with
light at different wavelengths, a process that can alter their physical and chemical
properties. For instance, dihydropyrene (DHP) is a deep-colored compound that
isomerizes to light-brown cyclophanediene (CPD) upon irradiation with visible
light. CPD can then isomerize back to DHP upon irradiation with UV light or thermally
in the dark. Conversion between DHP and CPD is thought to proceed via a biradical
intermediate; bimolecular events involving this unstable intermediate thus result
in rapid decomposition and poor cycling performance. Here, we show that the reversible
isomerization of DHP can be stabilized upon confinement within a PdII6L4 coordination
cage. By protecting this reactive intermediate using the cage, each isomerization
reaction proceeds to higher yield, which significantly decreases the fatigue experienced
by the system upon repeated photocycling. Although molecular confinement is known
to help stabilize reactive species, this effect is not typically employed to protect
reactive intermediates and thus improve reaction yields. We envisage that performing
reactions under confinement will not only improve the cyclic performance of photochromic
molecules, but may also increase the amount of product obtainable from traditionally
low-yielding organic reactions.
article_processing_charge: No
article_type: original
author:
- first_name: Martina
full_name: Canton, Martina
last_name: Canton
- first_name: Angela B.
full_name: Grommet, Angela B.
last_name: Grommet
- first_name: Luca
full_name: Pesce, Luca
last_name: Pesce
- first_name: Julius
full_name: Gemen, Julius
last_name: Gemen
- first_name: Shiming
full_name: Li, Shiming
last_name: Li
- first_name: Yael
full_name: Diskin-Posner, Yael
last_name: Diskin-Posner
- first_name: Alberto
full_name: Credi, Alberto
last_name: Credi
- first_name: Giovanni M.
full_name: Pavan, Giovanni M.
last_name: Pavan
- first_name: Joakim
full_name: Andréasson, Joakim
last_name: Andréasson
- first_name: Rafal
full_name: Klajn, Rafal
id: 8e84690e-1e48-11ed-a02b-a1e6fb8bb53b
last_name: Klajn
citation:
ama: Canton M, Grommet AB, Pesce L, et al. Improving fatigue resistance of dihydropyrene
by encapsulation within a coordination cage. Journal of the American Chemical
Society. 2020;142(34):14557-14565. doi:10.1021/jacs.0c06146
apa: Canton, M., Grommet, A. B., Pesce, L., Gemen, J., Li, S., Diskin-Posner, Y.,
… Klajn, R. (2020). Improving fatigue resistance of dihydropyrene by encapsulation
within a coordination cage. Journal of the American Chemical Society. American
Chemical Society. https://doi.org/10.1021/jacs.0c06146
chicago: Canton, Martina, Angela B. Grommet, Luca Pesce, Julius Gemen, Shiming Li,
Yael Diskin-Posner, Alberto Credi, Giovanni M. Pavan, Joakim Andréasson, and Rafal
Klajn. “Improving Fatigue Resistance of Dihydropyrene by Encapsulation within
a Coordination Cage.” Journal of the American Chemical Society. American
Chemical Society, 2020. https://doi.org/10.1021/jacs.0c06146.
ieee: M. Canton et al., “Improving fatigue resistance of dihydropyrene by
encapsulation within a coordination cage,” Journal of the American Chemical
Society, vol. 142, no. 34. American Chemical Society, pp. 14557–14565, 2020.
ista: Canton M, Grommet AB, Pesce L, Gemen J, Li S, Diskin-Posner Y, Credi A, Pavan
GM, Andréasson J, Klajn R. 2020. Improving fatigue resistance of dihydropyrene
by encapsulation within a coordination cage. Journal of the American Chemical
Society. 142(34), 14557–14565.
mla: Canton, Martina, et al. “Improving Fatigue Resistance of Dihydropyrene by Encapsulation
within a Coordination Cage.” Journal of the American Chemical Society,
vol. 142, no. 34, American Chemical Society, 2020, pp. 14557–65, doi:10.1021/jacs.0c06146.
short: M. Canton, A.B. Grommet, L. Pesce, J. Gemen, S. Li, Y. Diskin-Posner, A.
Credi, G.M. Pavan, J. Andréasson, R. Klajn, Journal of the American Chemical Society
142 (2020) 14557–14565.
date_created: 2023-08-01T09:36:59Z
date_published: 2020-08-14T00:00:00Z
date_updated: 2023-08-07T10:15:38Z
day: '14'
doi: 10.1021/jacs.0c06146
extern: '1'
external_id:
pmid:
- '32791832'
intvolume: ' 142'
issue: '34'
keyword:
- Colloid and Surface Chemistry
- Biochemistry
- General Chemistry
- Catalysis
language:
- iso: eng
main_file_link:
- open_access: '1'
url: https://doi.org/10.1021/jacs.0c06146
month: '08'
oa: 1
oa_version: Published Version
page: 14557-14565
pmid: 1
publication: Journal of the American Chemical Society
publication_identifier:
eissn:
- 1520-5126
issn:
- 0002-7863
publication_status: published
publisher: American Chemical Society
quality_controlled: '1'
scopus_import: '1'
status: public
title: Improving fatigue resistance of dihydropyrene by encapsulation within a coordination
cage
type: journal_article
user_id: 2DF688A6-F248-11E8-B48F-1D18A9856A87
volume: 142
year: '2020'
...
---
_id: '13365'
abstract:
- lang: eng
text: Photoswitchable molecules are employed for many applications, from the development
of active materials to the design of stimuli-responsive molecular systems and
light-powered molecular machines. To fully exploit their potential, we must learn
ways to control the mechanism and kinetics of their photoinduced isomerization.
One possible strategy involves confinement of photoresponsive switches such as
azobenzenes or spiropyrans within crowded molecular environments, which may allow
control over their light-induced conversion. However, the molecular factors that
influence and control the switching process under realistic conditions and within
dynamic molecular regimes often remain difficult to ascertain. As a case study,
here we have employed molecular models to probe the isomerization of azobenzene
guests within a Pd(II)-based coordination cage host in water. Atomistic molecular
dynamics and metadynamics simulations allow us to characterize the flexibility
of the cage in the solvent, the (rare) guest encapsulation and release events,
and the relative probability/kinetics of light-induced isomerization of azobenzene
analogues in these host–guest systems. In this way, we can reconstruct the mechanism
of azobenzene switching inside the cage cavity and explore key molecular factors
that may control this event. We obtain a molecular-level insight on the effects
of crowding and host–guest interactions on azobenzene isomerization. The detailed
picture elucidated by this study may enable the rational design of photoswitchable
systems whose reactivity can be controlled via host–guest interactions.
article_processing_charge: No
article_type: original
author:
- first_name: Luca
full_name: Pesce, Luca
last_name: Pesce
- first_name: Claudio
full_name: Perego, Claudio
last_name: Perego
- first_name: Angela B.
full_name: Grommet, Angela B.
last_name: Grommet
- first_name: Rafal
full_name: Klajn, Rafal
id: 8e84690e-1e48-11ed-a02b-a1e6fb8bb53b
last_name: Klajn
- first_name: Giovanni M.
full_name: Pavan, Giovanni M.
last_name: Pavan
citation:
ama: Pesce L, Perego C, Grommet AB, Klajn R, Pavan GM. Molecular factors controlling
the isomerization of Azobenzenes in the cavity of a flexible coordination cage.
Journal of the American Chemical Society. 2020;142(21):9792-9802. doi:10.1021/jacs.0c03444
apa: Pesce, L., Perego, C., Grommet, A. B., Klajn, R., & Pavan, G. M. (2020).
Molecular factors controlling the isomerization of Azobenzenes in the cavity of
a flexible coordination cage. Journal of the American Chemical Society.
American Chemical Society. https://doi.org/10.1021/jacs.0c03444
chicago: Pesce, Luca, Claudio Perego, Angela B. Grommet, Rafal Klajn, and Giovanni
M. Pavan. “Molecular Factors Controlling the Isomerization of Azobenzenes in the
Cavity of a Flexible Coordination Cage.” Journal of the American Chemical Society.
American Chemical Society, 2020. https://doi.org/10.1021/jacs.0c03444.
ieee: L. Pesce, C. Perego, A. B. Grommet, R. Klajn, and G. M. Pavan, “Molecular
factors controlling the isomerization of Azobenzenes in the cavity of a flexible
coordination cage,” Journal of the American Chemical Society, vol. 142,
no. 21. American Chemical Society, pp. 9792–9802, 2020.
ista: Pesce L, Perego C, Grommet AB, Klajn R, Pavan GM. 2020. Molecular factors
controlling the isomerization of Azobenzenes in the cavity of a flexible coordination
cage. Journal of the American Chemical Society. 142(21), 9792–9802.
mla: Pesce, Luca, et al. “Molecular Factors Controlling the Isomerization of Azobenzenes
in the Cavity of a Flexible Coordination Cage.” Journal of the American Chemical
Society, vol. 142, no. 21, American Chemical Society, 2020, pp. 9792–802,
doi:10.1021/jacs.0c03444.
short: L. Pesce, C. Perego, A.B. Grommet, R. Klajn, G.M. Pavan, Journal of the American
Chemical Society 142 (2020) 9792–9802.
date_created: 2023-08-01T09:37:12Z
date_published: 2020-04-30T00:00:00Z
date_updated: 2023-08-07T10:18:53Z
day: '30'
doi: 10.1021/jacs.0c03444
extern: '1'
external_id:
pmid:
- '32353237'
intvolume: ' 142'
issue: '21'
keyword:
- Colloid and Surface Chemistry
- Biochemistry
- General Chemistry
- Catalysis
language:
- iso: eng
main_file_link:
- open_access: '1'
url: https://doi.org/10.1021/jacs.0c03444
month: '04'
oa: 1
oa_version: Published Version
page: 9792-9802
pmid: 1
publication: Journal of the American Chemical Society
publication_identifier:
eissn:
- 1520-5126
issn:
- 0002-7863
publication_status: published
publisher: American Chemical Society
quality_controlled: '1'
scopus_import: '1'
status: public
title: Molecular factors controlling the isomerization of Azobenzenes in the cavity
of a flexible coordination cage
type: journal_article
user_id: 2DF688A6-F248-11E8-B48F-1D18A9856A87
volume: 142
year: '2020'
...
---
_id: '8408'
abstract:
- lang: eng
text: Aromatic residues are located at structurally important sites of many proteins.
Probing their interactions and dynamics can provide important functional insight
but is challenging in large proteins. Here, we introduce approaches to characterize
dynamics of phenylalanine residues using 1H-detected fast magic-angle spinning
(MAS) NMR combined with a tailored isotope-labeling scheme. Our approach yields
isolated two-spin systems that are ideally suited for artefact-free dynamics measurements,
and allows probing motions effectively without molecular-weight limitations. The
application to the TET2 enzyme assembly of ~0.5 MDa size, the currently largest
protein assigned by MAS NMR, provides insights into motions occurring on a wide
range of time scales (ps-ms). We quantitatively probe ring flip motions, and show
the temperature dependence by MAS NMR measurements down to 100 K. Interestingly,
favorable line widths are observed down to 100 K, with potential implications
for DNP NMR. Furthermore, we report the first 13C R1ρ MAS NMR relaxation-dispersion
measurements and detect structural excursions occurring on a microsecond time
scale in the entry pore to the catalytic chamber and at a trimer interface that
was proposed as exit pore. We show that the labeling scheme with deuteration at
ca. 50 kHz MAS provides superior resolution compared to 100 kHz MAS experiments
with protonated, uniformly 13C-labeled samples.
article_processing_charge: No
article_type: original
author:
- first_name: Diego F.
full_name: Gauto, Diego F.
last_name: Gauto
- first_name: Pavel
full_name: Macek, Pavel
last_name: Macek
- first_name: Alessandro
full_name: Barducci, Alessandro
last_name: Barducci
- first_name: Hugo
full_name: Fraga, Hugo
last_name: Fraga
- first_name: Audrey
full_name: Hessel, Audrey
last_name: Hessel
- first_name: Tsutomu
full_name: Terauchi, Tsutomu
last_name: Terauchi
- first_name: David
full_name: Gajan, David
last_name: Gajan
- first_name: Yohei
full_name: Miyanoiri, Yohei
last_name: Miyanoiri
- first_name: Jerome
full_name: Boisbouvier, Jerome
last_name: Boisbouvier
- first_name: Roman
full_name: Lichtenecker, Roman
last_name: Lichtenecker
- first_name: Masatsune
full_name: Kainosho, Masatsune
last_name: Kainosho
- first_name: Paul
full_name: Schanda, Paul
id: 7B541462-FAF6-11E9-A490-E8DFE5697425
last_name: Schanda
orcid: 0000-0002-9350-7606
citation:
ama: Gauto DF, Macek P, Barducci A, et al. Aromatic ring dynamics, thermal activation,
and transient conformations of a 468 kDa enzyme by specific 1H–13C labeling and
fast magic-angle spinning NMR. Journal of the American Chemical Society.
2019;141(28):11183-11195. doi:10.1021/jacs.9b04219
apa: Gauto, D. F., Macek, P., Barducci, A., Fraga, H., Hessel, A., Terauchi, T.,
… Schanda, P. (2019). Aromatic ring dynamics, thermal activation, and transient
conformations of a 468 kDa enzyme by specific 1H–13C labeling and fast magic-angle
spinning NMR. Journal of the American Chemical Society. American Chemical
Society. https://doi.org/10.1021/jacs.9b04219
chicago: Gauto, Diego F., Pavel Macek, Alessandro Barducci, Hugo Fraga, Audrey Hessel,
Tsutomu Terauchi, David Gajan, et al. “Aromatic Ring Dynamics, Thermal Activation,
and Transient Conformations of a 468 KDa Enzyme by Specific 1H–13C Labeling and
Fast Magic-Angle Spinning NMR.” Journal of the American Chemical Society.
American Chemical Society, 2019. https://doi.org/10.1021/jacs.9b04219.
ieee: D. F. Gauto et al., “Aromatic ring dynamics, thermal activation, and
transient conformations of a 468 kDa enzyme by specific 1H–13C labeling and fast
magic-angle spinning NMR,” Journal of the American Chemical Society, vol.
141, no. 28. American Chemical Society, pp. 11183–11195, 2019.
ista: Gauto DF, Macek P, Barducci A, Fraga H, Hessel A, Terauchi T, Gajan D, Miyanoiri
Y, Boisbouvier J, Lichtenecker R, Kainosho M, Schanda P. 2019. Aromatic ring dynamics,
thermal activation, and transient conformations of a 468 kDa enzyme by specific
1H–13C labeling and fast magic-angle spinning NMR. Journal of the American Chemical
Society. 141(28), 11183–11195.
mla: Gauto, Diego F., et al. “Aromatic Ring Dynamics, Thermal Activation, and Transient
Conformations of a 468 KDa Enzyme by Specific 1H–13C Labeling and Fast Magic-Angle
Spinning NMR.” Journal of the American Chemical Society, vol. 141, no.
28, American Chemical Society, 2019, pp. 11183–95, doi:10.1021/jacs.9b04219.
short: D.F. Gauto, P. Macek, A. Barducci, H. Fraga, A. Hessel, T. Terauchi, D. Gajan,
Y. Miyanoiri, J. Boisbouvier, R. Lichtenecker, M. Kainosho, P. Schanda, Journal
of the American Chemical Society 141 (2019) 11183–11195.
date_created: 2020-09-17T10:29:00Z
date_published: 2019-06-14T00:00:00Z
date_updated: 2021-01-12T08:19:04Z
day: '14'
doi: 10.1021/jacs.9b04219
extern: '1'
external_id:
pmid:
- '31199882'
intvolume: ' 141'
issue: '28'
keyword:
- Colloid and Surface Chemistry
- Biochemistry
- General Chemistry
- Catalysis
language:
- iso: eng
month: '06'
oa_version: Submitted Version
page: 11183-11195
pmid: 1
publication: Journal of the American Chemical Society
publication_identifier:
issn:
- 0002-7863
- 1520-5126
publication_status: published
publisher: American Chemical Society
quality_controlled: '1'
status: public
title: Aromatic ring dynamics, thermal activation, and transient conformations of
a 468 kDa enzyme by specific 1H–13C labeling and fast magic-angle spinning NMR
type: journal_article
user_id: 2DF688A6-F248-11E8-B48F-1D18A9856A87
volume: 141
year: '2019'
...
---
_id: '8413'
abstract:
- lang: eng
text: NMR relaxation dispersion methods provide a holistic way to observe microsecond
time-scale protein backbone motion both in solution and in the solid state. Different
nuclei (1H and 15N) and different relaxation dispersion techniques (Bloch–McConnell
and near-rotary-resonance) give complementary information about the amplitudes
and time scales of the conformational dynamics and provide comprehensive insights
into the mechanistic details of the structural rearrangements. In this paper,
we exemplify the benefits of the combination of various solution- and solid-state
relaxation dispersion methods on a microcrystalline protein (α-spectrin SH3 domain),
for which we are able to identify and model the functionally relevant conformational
rearrangements around the ligand recognition loop occurring on multiple microsecond
time scales. The observed loop motions suggest that the SH3 domain exists in a
binding-competent conformation in dynamic equilibrium with a sterically impaired
ground-state conformation both in solution and in crystalline form. This inherent
plasticity between the interconverting macrostates is compatible with a conformational-preselection
model and provides new insights into the recognition mechanisms of SH3 domains.
article_processing_charge: No
article_type: original
author:
- first_name: Petra
full_name: Rovó, Petra
last_name: Rovó
- first_name: Colin A.
full_name: Smith, Colin A.
last_name: Smith
- first_name: Diego
full_name: Gauto, Diego
last_name: Gauto
- first_name: Bert L.
full_name: de Groot, Bert L.
last_name: de Groot
- first_name: Paul
full_name: Schanda, Paul
id: 7B541462-FAF6-11E9-A490-E8DFE5697425
last_name: Schanda
orcid: 0000-0002-9350-7606
- first_name: Rasmus
full_name: Linser, Rasmus
last_name: Linser
citation:
ama: Rovó P, Smith CA, Gauto D, de Groot BL, Schanda P, Linser R. Mechanistic insights
into microsecond time-scale motion of solid proteins using complementary 15N and
1H relaxation dispersion techniques. Journal of the American Chemical Society.
2019;141(2):858-869. doi:10.1021/jacs.8b09258
apa: Rovó, P., Smith, C. A., Gauto, D., de Groot, B. L., Schanda, P., & Linser,
R. (2019). Mechanistic insights into microsecond time-scale motion of solid proteins
using complementary 15N and 1H relaxation dispersion techniques. Journal of
the American Chemical Society. American Chemical Society. https://doi.org/10.1021/jacs.8b09258
chicago: Rovó, Petra, Colin A. Smith, Diego Gauto, Bert L. de Groot, Paul Schanda,
and Rasmus Linser. “Mechanistic Insights into Microsecond Time-Scale Motion of
Solid Proteins Using Complementary 15N and 1H Relaxation Dispersion Techniques.”
Journal of the American Chemical Society. American Chemical Society, 2019.
https://doi.org/10.1021/jacs.8b09258.
ieee: P. Rovó, C. A. Smith, D. Gauto, B. L. de Groot, P. Schanda, and R. Linser,
“Mechanistic insights into microsecond time-scale motion of solid proteins using
complementary 15N and 1H relaxation dispersion techniques,” Journal of the
American Chemical Society, vol. 141, no. 2. American Chemical Society, pp.
858–869, 2019.
ista: Rovó P, Smith CA, Gauto D, de Groot BL, Schanda P, Linser R. 2019. Mechanistic
insights into microsecond time-scale motion of solid proteins using complementary
15N and 1H relaxation dispersion techniques. Journal of the American Chemical
Society. 141(2), 858–869.
mla: Rovó, Petra, et al. “Mechanistic Insights into Microsecond Time-Scale Motion
of Solid Proteins Using Complementary 15N and 1H Relaxation Dispersion Techniques.”
Journal of the American Chemical Society, vol. 141, no. 2, American Chemical
Society, 2019, pp. 858–69, doi:10.1021/jacs.8b09258.
short: P. Rovó, C.A. Smith, D. Gauto, B.L. de Groot, P. Schanda, R. Linser, Journal
of the American Chemical Society 141 (2019) 858–869.
date_created: 2020-09-17T10:29:50Z
date_published: 2019-01-08T00:00:00Z
date_updated: 2021-01-12T08:19:07Z
day: '08'
doi: 10.1021/jacs.8b09258
extern: '1'
external_id:
pmid:
- '30620186'
intvolume: ' 141'
issue: '2'
keyword:
- Colloid and Surface Chemistry
- Biochemistry
- General Chemistry
- Catalysis
language:
- iso: eng
month: '01'
oa_version: Submitted Version
page: 858-869
pmid: 1
publication: Journal of the American Chemical Society
publication_identifier:
issn:
- 0002-7863
- 1520-5126
publication_status: published
publisher: American Chemical Society
quality_controlled: '1'
status: public
title: Mechanistic insights into microsecond time-scale motion of solid proteins using
complementary 15N and 1H relaxation dispersion techniques
type: journal_article
user_id: 2DF688A6-F248-11E8-B48F-1D18A9856A87
volume: 141
year: '2019'
...
---
_id: '13373'
abstract:
- lang: eng
text: The reversible photoisomerization of azobenzene has been utilized to construct
a plethora of systems in which optical, electronic, catalytic, and other properties
can be controlled by light. However, owing to azobenzene’s hydrophobic nature,
most of these examples have been realized only in organic solvents, and systems
operating in water are relatively scarce. Here, we show that by coadsorbing the
inherently hydrophobic azobenzenes with water-solubilizing ligands on the same
nanoparticulate platforms, it is possible to render them essentially water-soluble.
To this end, we developed a modified nanoparticle functionalization procedure
allowing us to precisely fine-tune the amount of azobenzene on the functionalized
nanoparticles. Molecular dynamics simulations helped us to identify two distinct
supramolecular architectures (depending on the length of the background ligand)
on these nanoparticles, which can explain their excellent aqueous solubilities.
Azobenzenes adsorbed on these water-soluble nanoparticles exhibit highly reversible
photoisomerization upon exposure to UV and visible light. Importantly, the mixed-monolayer
approach allowed us to systematically investigate how the background ligand affects
the switching properties of azobenzene. We found that the nature of the background
ligand has a profound effect on the kinetics of azobenzene switching. For example,
a hydroxy-terminated background ligand is capable of accelerating the back-isomerization
reaction by more than 6000-fold. These results pave the way toward the development
of novel light-responsive nanomaterials operating in aqueous media and, in the
long run, in biological environments.
article_processing_charge: No
article_type: original
author:
- first_name: Zonglin
full_name: Chu, Zonglin
last_name: Chu
- first_name: Yanxiao
full_name: Han, Yanxiao
last_name: Han
- first_name: Tong
full_name: Bian, Tong
last_name: Bian
- first_name: Soumen
full_name: De, Soumen
last_name: De
- first_name: Petr
full_name: Král, Petr
last_name: Král
- first_name: Rafal
full_name: Klajn, Rafal
id: 8e84690e-1e48-11ed-a02b-a1e6fb8bb53b
last_name: Klajn
citation:
ama: Chu Z, Han Y, Bian T, De S, Král P, Klajn R. Supramolecular control of azobenzene
switching on nanoparticles. Journal of the American Chemical Society. 2019;141(5):1949-1960.
doi:10.1021/jacs.8b09638
apa: Chu, Z., Han, Y., Bian, T., De, S., Král, P., & Klajn, R. (2019). Supramolecular
control of azobenzene switching on nanoparticles. Journal of the American Chemical
Society. American Chemical Society. https://doi.org/10.1021/jacs.8b09638
chicago: Chu, Zonglin, Yanxiao Han, Tong Bian, Soumen De, Petr Král, and Rafal Klajn.
“Supramolecular Control of Azobenzene Switching on Nanoparticles.” Journal
of the American Chemical Society. American Chemical Society, 2019. https://doi.org/10.1021/jacs.8b09638.
ieee: Z. Chu, Y. Han, T. Bian, S. De, P. Král, and R. Klajn, “Supramolecular control
of azobenzene switching on nanoparticles,” Journal of the American Chemical
Society, vol. 141, no. 5. American Chemical Society, pp. 1949–1960, 2019.
ista: Chu Z, Han Y, Bian T, De S, Král P, Klajn R. 2019. Supramolecular control
of azobenzene switching on nanoparticles. Journal of the American Chemical Society.
141(5), 1949–1960.
mla: Chu, Zonglin, et al. “Supramolecular Control of Azobenzene Switching on Nanoparticles.”
Journal of the American Chemical Society, vol. 141, no. 5, American Chemical
Society, 2019, pp. 1949–60, doi:10.1021/jacs.8b09638.
short: Z. Chu, Y. Han, T. Bian, S. De, P. Král, R. Klajn, Journal of the American
Chemical Society 141 (2019) 1949–1960.
date_created: 2023-08-01T09:39:19Z
date_published: 2019-02-06T00:00:00Z
date_updated: 2023-08-07T10:51:12Z
day: '06'
doi: 10.1021/jacs.8b09638
extern: '1'
external_id:
pmid:
- '30595017'
intvolume: ' 141'
issue: '5'
keyword:
- Colloid and Surface Chemistry
- Biochemistry
- General Chemistry
- Catalysis
language:
- iso: eng
month: '02'
oa_version: Published Version
page: 1949-1960
pmid: 1
publication: Journal of the American Chemical Society
publication_identifier:
eissn:
- 1520-5126
issn:
- 0002-7863
publication_status: published
publisher: American Chemical Society
quality_controlled: '1'
scopus_import: '1'
status: public
title: Supramolecular control of azobenzene switching on nanoparticles
type: journal_article
user_id: 2DF688A6-F248-11E8-B48F-1D18A9856A87
volume: 141
year: '2019'
...
---
_id: '13380'
abstract:
- lang: eng
text: Although dissipative self-assembly is ubiquitous in nature, where it gives
rise to structures and functions critical to life, examples of artificial systems
featuring this mode of self-assembly are rare. Here, we identify the presence
of ephemeral assemblies during seeded growth of gold nanoparticles. In this process,
hydrazine reduces Au(III) ions, which attach to the existing nanoparticles “seeds”.
The attachment is accompanied by a local increase in the concentration of a surfactant,
which therefore forms a bilayer on nanoparticle surfaces, inducing their assembly.
The resulting aggregates gradually disassemble as the surfactant concentration
throughout the solution equilibrates. The lifetimes of the out-of-equilibrium
aggregates depend on and can be controlled by the size of the constituent nanoparticles.
We demonstrate the utility of our out-of-equilibrium aggregates to form transient
reflective coatings on polar surfaces.
article_processing_charge: No
article_type: original
author:
- first_name: Michał
full_name: Sawczyk, Michał
last_name: Sawczyk
- first_name: Rafal
full_name: Klajn, Rafal
id: 8e84690e-1e48-11ed-a02b-a1e6fb8bb53b
last_name: Klajn
citation:
ama: Sawczyk M, Klajn R. Out-of-equilibrium aggregates and coatings during seeded
growth of metallic nanoparticles. Journal of the American Chemical Society.
2017;139(49):17973-17978. doi:10.1021/jacs.7b09111
apa: Sawczyk, M., & Klajn, R. (2017). Out-of-equilibrium aggregates and coatings
during seeded growth of metallic nanoparticles. Journal of the American Chemical
Society. American Chemical Society. https://doi.org/10.1021/jacs.7b09111
chicago: Sawczyk, Michał, and Rafal Klajn. “Out-of-Equilibrium Aggregates and Coatings
during Seeded Growth of Metallic Nanoparticles.” Journal of the American Chemical
Society. American Chemical Society, 2017. https://doi.org/10.1021/jacs.7b09111.
ieee: M. Sawczyk and R. Klajn, “Out-of-equilibrium aggregates and coatings during
seeded growth of metallic nanoparticles,” Journal of the American Chemical
Society, vol. 139, no. 49. American Chemical Society, pp. 17973–17978, 2017.
ista: Sawczyk M, Klajn R. 2017. Out-of-equilibrium aggregates and coatings during
seeded growth of metallic nanoparticles. Journal of the American Chemical Society.
139(49), 17973–17978.
mla: Sawczyk, Michał, and Rafal Klajn. “Out-of-Equilibrium Aggregates and Coatings
during Seeded Growth of Metallic Nanoparticles.” Journal of the American Chemical
Society, vol. 139, no. 49, American Chemical Society, 2017, pp. 17973–78,
doi:10.1021/jacs.7b09111.
short: M. Sawczyk, R. Klajn, Journal of the American Chemical Society 139 (2017)
17973–17978.
date_created: 2023-08-01T09:41:01Z
date_published: 2017-12-01T00:00:00Z
date_updated: 2023-08-07T11:19:30Z
day: '01'
doi: 10.1021/jacs.7b09111
extern: '1'
external_id:
pmid:
- '29193964'
intvolume: ' 139'
issue: '49'
keyword:
- Colloid and Surface Chemistry
- Biochemistry
- General Chemistry
- Catalysis
language:
- iso: eng
month: '12'
oa_version: None
page: 17973-17978
pmid: 1
publication: Journal of the American Chemical Society
publication_identifier:
eissn:
- 1520-5126
issn:
- 0002-7863
publication_status: published
publisher: American Chemical Society
quality_controlled: '1'
scopus_import: '1'
status: public
title: Out-of-equilibrium aggregates and coatings during seeded growth of metallic
nanoparticles
type: journal_article
user_id: 2DF688A6-F248-11E8-B48F-1D18A9856A87
volume: 139
year: '2017'
...
---
_id: '13401'
abstract:
- lang: eng
text: A compound combining the features of a molecular rotor and a photoswitch was
synthesized and was shown to exist as three diastereomers, which interconvert
via a reversible cyclic reaction scheme. Each of the three diastereomers was isolated,
and by following the equilibration kinetics, activation barriers for all reactions
were calculated. The results indicate that the properties of molecular switches
depend heavily on their immediate chemical environment. The conclusions are important
in the context of designing new switchable molecules and materials.
article_processing_charge: No
article_type: original
author:
- first_name: Pintu K.
full_name: Kundu, Pintu K.
last_name: Kundu
- first_name: Avishai
full_name: Lerner, Avishai
last_name: Lerner
- first_name: Kristina
full_name: Kučanda, Kristina
last_name: Kučanda
- first_name: Gregory
full_name: Leitus, Gregory
last_name: Leitus
- first_name: Rafal
full_name: Klajn, Rafal
id: 8e84690e-1e48-11ed-a02b-a1e6fb8bb53b
last_name: Klajn
citation:
ama: Kundu PK, Lerner A, Kučanda K, Leitus G, Klajn R. Cyclic kinetics during thermal
equilibration of an axially chiral bis-spiropyran. Journal of the American
Chemical Society. 2014;136(32):11276-11279. doi:10.1021/ja505948q
apa: Kundu, P. K., Lerner, A., Kučanda, K., Leitus, G., & Klajn, R. (2014).
Cyclic kinetics during thermal equilibration of an axially chiral bis-spiropyran.
Journal of the American Chemical Society. American Chemical Society. https://doi.org/10.1021/ja505948q
chicago: Kundu, Pintu K., Avishai Lerner, Kristina Kučanda, Gregory Leitus, and
Rafal Klajn. “Cyclic Kinetics during Thermal Equilibration of an Axially Chiral
Bis-Spiropyran.” Journal of the American Chemical Society. American Chemical
Society, 2014. https://doi.org/10.1021/ja505948q.
ieee: P. K. Kundu, A. Lerner, K. Kučanda, G. Leitus, and R. Klajn, “Cyclic kinetics
during thermal equilibration of an axially chiral bis-spiropyran,” Journal
of the American Chemical Society, vol. 136, no. 32. American Chemical Society,
pp. 11276–11279, 2014.
ista: Kundu PK, Lerner A, Kučanda K, Leitus G, Klajn R. 2014. Cyclic kinetics during
thermal equilibration of an axially chiral bis-spiropyran. Journal of the American
Chemical Society. 136(32), 11276–11279.
mla: Kundu, Pintu K., et al. “Cyclic Kinetics during Thermal Equilibration of an
Axially Chiral Bis-Spiropyran.” Journal of the American Chemical Society,
vol. 136, no. 32, American Chemical Society, 2014, pp. 11276–79, doi:10.1021/ja505948q.
short: P.K. Kundu, A. Lerner, K. Kučanda, G. Leitus, R. Klajn, Journal of the American
Chemical Society 136 (2014) 11276–11279.
date_created: 2023-08-01T09:46:12Z
date_published: 2014-08-13T00:00:00Z
date_updated: 2023-08-08T07:25:37Z
day: '13'
doi: 10.1021/ja505948q
extern: '1'
external_id:
pmid:
- '25072292'
intvolume: ' 136'
issue: '32'
keyword:
- Colloid and Surface Chemistry
- Biochemistry
- General Chemistry
- Catalysis
language:
- iso: eng
month: '08'
oa_version: None
page: 11276-11279
pmid: 1
publication: Journal of the American Chemical Society
publication_identifier:
eissn:
- 1520-5126
issn:
- 0002-7863
publication_status: published
publisher: American Chemical Society
quality_controlled: '1'
scopus_import: '1'
status: public
title: Cyclic kinetics during thermal equilibration of an axially chiral bis-spiropyran
type: journal_article
user_id: 2DF688A6-F248-11E8-B48F-1D18A9856A87
volume: 136
year: '2014'
...
---
_id: '13403'
abstract:
- lang: eng
text: We show that bimolecular reactions between species confined to the surfaces
of nanoparticles can be manipulated by the nature of the linker, as well as by
the curvature of the underlying particles.
article_processing_charge: No
article_type: original
author:
- first_name: Tino
full_name: Zdobinsky, Tino
last_name: Zdobinsky
- first_name: Pradipta
full_name: Sankar Maiti, Pradipta
last_name: Sankar Maiti
- first_name: Rafal
full_name: Klajn, Rafal
id: 8e84690e-1e48-11ed-a02b-a1e6fb8bb53b
last_name: Klajn
citation:
ama: Zdobinsky T, Sankar Maiti P, Klajn R. Support curvature and conformational
freedom control chemical reactivity of immobilized species. Journal of the
American Chemical Society. 2014;136(7):2711-2714. doi:10.1021/ja411573a
apa: Zdobinsky, T., Sankar Maiti, P., & Klajn, R. (2014). Support curvature
and conformational freedom control chemical reactivity of immobilized species.
Journal of the American Chemical Society. American Chemical Society. https://doi.org/10.1021/ja411573a
chicago: Zdobinsky, Tino, Pradipta Sankar Maiti, and Rafal Klajn. “Support Curvature
and Conformational Freedom Control Chemical Reactivity of Immobilized Species.”
Journal of the American Chemical Society. American Chemical Society, 2014.
https://doi.org/10.1021/ja411573a.
ieee: T. Zdobinsky, P. Sankar Maiti, and R. Klajn, “Support curvature and conformational
freedom control chemical reactivity of immobilized species,” Journal of the
American Chemical Society, vol. 136, no. 7. American Chemical Society, pp.
2711–2714, 2014.
ista: Zdobinsky T, Sankar Maiti P, Klajn R. 2014. Support curvature and conformational
freedom control chemical reactivity of immobilized species. Journal of the American
Chemical Society. 136(7), 2711–2714.
mla: Zdobinsky, Tino, et al. “Support Curvature and Conformational Freedom Control
Chemical Reactivity of Immobilized Species.” Journal of the American Chemical
Society, vol. 136, no. 7, American Chemical Society, 2014, pp. 2711–14, doi:10.1021/ja411573a.
short: T. Zdobinsky, P. Sankar Maiti, R. Klajn, Journal of the American Chemical
Society 136 (2014) 2711–2714.
date_created: 2023-08-01T09:46:44Z
date_published: 2014-02-19T00:00:00Z
date_updated: 2023-08-08T07:32:11Z
day: '19'
doi: 10.1021/ja411573a
extern: '1'
external_id:
pmid:
- '24320557'
intvolume: ' 136'
issue: '7'
keyword:
- Colloid and Surface Chemistry
- Biochemistry
- General Chemistry
- Catalysis
language:
- iso: eng
month: '02'
oa_version: None
page: 2711-2714
pmid: 1
publication: Journal of the American Chemical Society
publication_identifier:
eissn:
- 1520-5126
issn:
- 0002-7863
publication_status: published
publisher: American Chemical Society
quality_controlled: '1'
scopus_import: '1'
status: public
title: Support curvature and conformational freedom control chemical reactivity of
immobilized species
type: journal_article
user_id: 2DF688A6-F248-11E8-B48F-1D18A9856A87
volume: 136
year: '2014'
...
---
_id: '9167'
abstract:
- lang: eng
text: We introduce a self-propelled colloidal hematite docker that can be steered
to a small particle cargo many times its size, dock, transport the cargo to a
remote location, and then release it. The self-propulsion and docking are reversible
and activated by visible light. The docker can be steered either by a weak uniform
magnetic field or by nanoscale tracks in a textured substrate. The light-activated
motion and docking originate from osmotic/phoretic particle transport in a concentration
gradient of fuel, hydrogen peroxide, induced by the photocatalytic activity of
the hematite. The docking mechanism is versatile and can be applied to various
materials and shapes. The hematite dockers are simple single-component particles
and are synthesized in bulk quantities. This system opens up new possibilities
for designing complex micrometer-size factories as well as new biomimetic systems.
article_processing_charge: No
article_type: original
arxiv: 1
author:
- first_name: Jérémie A
full_name: Palacci, Jérémie A
id: 8fb92548-2b22-11eb-b7c1-a3f0d08d7c7d
last_name: Palacci
orcid: 0000-0002-7253-9465
- first_name: Stefano
full_name: Sacanna, Stefano
last_name: Sacanna
- first_name: Adrian
full_name: Vatchinsky, Adrian
last_name: Vatchinsky
- first_name: Paul M.
full_name: Chaikin, Paul M.
last_name: Chaikin
- first_name: David J.
full_name: Pine, David J.
last_name: Pine
citation:
ama: Palacci JA, Sacanna S, Vatchinsky A, Chaikin PM, Pine DJ. Photoactivated colloidal
dockers for cargo transportation. Journal of the American Chemical Society.
2013;135(43):15978-15981. doi:10.1021/ja406090s
apa: Palacci, J. A., Sacanna, S., Vatchinsky, A., Chaikin, P. M., & Pine, D.
J. (2013). Photoactivated colloidal dockers for cargo transportation. Journal
of the American Chemical Society. American Chemical Society. https://doi.org/10.1021/ja406090s
chicago: Palacci, Jérémie A, Stefano Sacanna, Adrian Vatchinsky, Paul M. Chaikin,
and David J. Pine. “Photoactivated Colloidal Dockers for Cargo Transportation.”
Journal of the American Chemical Society. American Chemical Society, 2013.
https://doi.org/10.1021/ja406090s.
ieee: J. A. Palacci, S. Sacanna, A. Vatchinsky, P. M. Chaikin, and D. J. Pine, “Photoactivated
colloidal dockers for cargo transportation,” Journal of the American Chemical
Society, vol. 135, no. 43. American Chemical Society, pp. 15978–15981, 2013.
ista: Palacci JA, Sacanna S, Vatchinsky A, Chaikin PM, Pine DJ. 2013. Photoactivated
colloidal dockers for cargo transportation. Journal of the American Chemical Society.
135(43), 15978–15981.
mla: Palacci, Jérémie A., et al. “Photoactivated Colloidal Dockers for Cargo Transportation.”
Journal of the American Chemical Society, vol. 135, no. 43, American Chemical
Society, 2013, pp. 15978–81, doi:10.1021/ja406090s.
short: J.A. Palacci, S. Sacanna, A. Vatchinsky, P.M. Chaikin, D.J. Pine, Journal
of the American Chemical Society 135 (2013) 15978–15981.
date_created: 2021-02-18T14:31:26Z
date_published: 2013-10-30T00:00:00Z
date_updated: 2021-02-22T10:10:41Z
day: '30'
doi: 10.1021/ja406090s
extern: '1'
external_id:
arxiv:
- '1310.5724'
pmid:
- '24131488'
intvolume: ' 135'
issue: '43'
keyword:
- Colloid and Surface Chemistry
- Biochemistry
- General Chemistry
- Catalysis
language:
- iso: eng
main_file_link:
- open_access: '1'
url: https://arxiv.org/abs/1310.5724
month: '10'
oa: 1
oa_version: Preprint
page: 15978-15981
pmid: 1
publication: Journal of the American Chemical Society
publication_identifier:
eissn:
- '15205126'
issn:
- '00027863'
publication_status: published
publisher: American Chemical Society
quality_controlled: '1'
scopus_import: '1'
status: public
title: Photoactivated colloidal dockers for cargo transportation
type: journal_article
user_id: D865714E-FA4E-11E9-B85B-F5C5E5697425
volume: 135
year: '2013'
...
---
_id: '13407'
abstract:
- lang: eng
text: We show that diamagnetic particles can be remotely manipulated by a magnet
by the reversible adsorption of dual-responsive, light-switchable/superparamagnetic
nanoparticles down to their surface. Adsorption occurs upon exposure to UV light,
and can be reversed thermally or by ambient light. The dynamic self-assembly of
thin films of the dual-responsive nanoparticles induces attractive interactions
between diamagnetic particles. We demonstrate that catalytic amounts of the dual-responsive
nanoparticles are sufficient to magnetically guide and deliver the diamagnetic
particles to desired locations, where they can then be released by disassembling
the dynamic layers of superparamagnetic nanoparticles with visible light.
article_processing_charge: No
article_type: original
author:
- first_name: Olga
full_name: Chovnik, Olga
last_name: Chovnik
- first_name: Renata
full_name: Balgley, Renata
last_name: Balgley
- first_name: Joel R.
full_name: Goldman, Joel R.
last_name: Goldman
- first_name: Rafal
full_name: Klajn, Rafal
id: 8e84690e-1e48-11ed-a02b-a1e6fb8bb53b
last_name: Klajn
citation:
ama: Chovnik O, Balgley R, Goldman JR, Klajn R. Dynamically self-assembling carriers
enable guiding of diamagnetic particles by weak magnets. Journal of the American
Chemical Society. 2012;134(48):19564-19567. doi:10.1021/ja309633v
apa: Chovnik, O., Balgley, R., Goldman, J. R., & Klajn, R. (2012). Dynamically
self-assembling carriers enable guiding of diamagnetic particles by weak magnets.
Journal of the American Chemical Society. American Chemical Society. https://doi.org/10.1021/ja309633v
chicago: Chovnik, Olga, Renata Balgley, Joel R. Goldman, and Rafal Klajn. “Dynamically
Self-Assembling Carriers Enable Guiding of Diamagnetic Particles by Weak Magnets.”
Journal of the American Chemical Society. American Chemical Society, 2012.
https://doi.org/10.1021/ja309633v.
ieee: O. Chovnik, R. Balgley, J. R. Goldman, and R. Klajn, “Dynamically self-assembling
carriers enable guiding of diamagnetic particles by weak magnets,” Journal
of the American Chemical Society, vol. 134, no. 48. American Chemical Society,
pp. 19564–19567, 2012.
ista: Chovnik O, Balgley R, Goldman JR, Klajn R. 2012. Dynamically self-assembling
carriers enable guiding of diamagnetic particles by weak magnets. Journal of the
American Chemical Society. 134(48), 19564–19567.
mla: Chovnik, Olga, et al. “Dynamically Self-Assembling Carriers Enable Guiding
of Diamagnetic Particles by Weak Magnets.” Journal of the American Chemical
Society, vol. 134, no. 48, American Chemical Society, 2012, pp. 19564–67,
doi:10.1021/ja309633v.
short: O. Chovnik, R. Balgley, J.R. Goldman, R. Klajn, Journal of the American Chemical
Society 134 (2012) 19564–19567.
date_created: 2023-08-01T09:47:42Z
date_published: 2012-11-26T00:00:00Z
date_updated: 2023-08-08T07:51:10Z
day: '26'
doi: 10.1021/ja309633v
extern: '1'
external_id:
pmid:
- '23181449'
intvolume: ' 134'
issue: '48'
keyword:
- Colloid and Surface Chemistry
- Biochemistry
- General Chemistry
- Catalysis
language:
- iso: eng
month: '11'
oa_version: Published Version
page: 19564-19567
pmid: 1
publication: Journal of the American Chemical Society
publication_identifier:
eissn:
- 1520-5126
issn:
- 0002-7863
publication_status: published
publisher: American Chemical Society
quality_controlled: '1'
scopus_import: '1'
status: public
title: Dynamically self-assembling carriers enable guiding of diamagnetic particles
by weak magnets
type: journal_article
user_id: 2DF688A6-F248-11E8-B48F-1D18A9856A87
volume: 134
year: '2012'
...
---
_id: '13410'
abstract:
- lang: eng
text: A range (Au, Pt, Pd) of metal nanoparticles (MNPs) has been prepared and functionalized
with (a) redox-active stalks containing tetrathiafulvalene (TTF) units, (b) [2]pseudorotaxanes
formed between these stalks and cyclobis(paraquat-p-phenylene) (CBPQT4+) rings,
and (c) bistable [2]rotaxane molecules where the dumbbell component contains a
1,5-dioxynaphthalene (DNP) unit, as well as a TTF unit, encircled by a CBPQT4+
ring. It transpires that the molecules present in (a) and (c) and the supermolecules
described in (b) retain their switching characteristics, previously observed in
solution, when they are immobilized onto MNPs. Moreover, their oxidation potentials
depend on the fraction, χ, of the molecules or supermolecules on the surface of
the nanoparticles. A variation in χ affects the oxidation potentials of the TTF
units to the extent that switching can be subjected to fine tuning as a result.
Specifically, increasing χ results in positive shifts (i) in the oxidation potentials
of the TTF unit in (a)−(c) and (ii) the reduction potentials of the CBPQT4+ rings
in (c). These shifts can be attributed to an increase in the electrostatic potential
surrounding the MNPs. Both the magnitude and the direction of these shifts are
reproduced by a model, based on the Poisson−Boltzmann equation coupled with charge-regulating
boundary conditions. Furthermore, the kinetics of relaxation from the metastable
state coconformation (MSCC) to the ground-state coconformation (GSCC) of the bistable
[2]rotaxane molecules also depends on χ, as well as on the nanoparticle diameter.
Increasing either of these parameters accelerates the rate of relaxation from
the MSCC to the GSCC. This rate is a function of (i) the activation energy for
the relaxation process associated with the bistable [2]rotaxane molecules in solution
and (ii) the electrostatic potential surrounding the MNPs. The electrostatic potential
depends on (i) the diameter of the MNPs, (ii) the amount of the bistable [2]rotaxane
molecules on the surface of the MNPs, and (iii) the equilibrium distribution of
the CBPQT4+ rings between the DNP and TTF recognition sites in the GSCC. This
electrostatic potential has also been quantified using the Poisson−Boltzmann equation,
leading to faithful estimates of the rate constants.
article_processing_charge: No
article_type: original
author:
- first_name: Ali
full_name: Coskun, Ali
last_name: Coskun
- first_name: Paul J.
full_name: Wesson, Paul J.
last_name: Wesson
- first_name: Rafal
full_name: Klajn, Rafal
id: 8e84690e-1e48-11ed-a02b-a1e6fb8bb53b
last_name: Klajn
- first_name: Ali
full_name: Trabolsi, Ali
last_name: Trabolsi
- first_name: Lei
full_name: Fang, Lei
last_name: Fang
- first_name: Mark A.
full_name: Olson, Mark A.
last_name: Olson
- first_name: Sanjeev K.
full_name: Dey, Sanjeev K.
last_name: Dey
- first_name: Bartosz A.
full_name: Grzybowski, Bartosz A.
last_name: Grzybowski
- first_name: J. Fraser
full_name: Stoddart, J. Fraser
last_name: Stoddart
citation:
ama: 'Coskun A, Wesson PJ, Klajn R, et al. Molecular-mechanical switching at the
nanoparticle−solvent interface: Practice and theory. Journal of the American
Chemical Society. 2010;132(12):4310-4320. doi:10.1021/ja9102327'
apa: 'Coskun, A., Wesson, P. J., Klajn, R., Trabolsi, A., Fang, L., Olson, M. A.,
… Stoddart, J. F. (2010). Molecular-mechanical switching at the nanoparticle−solvent
interface: Practice and theory. Journal of the American Chemical Society.
American Chemical Society. https://doi.org/10.1021/ja9102327'
chicago: 'Coskun, Ali, Paul J. Wesson, Rafal Klajn, Ali Trabolsi, Lei Fang, Mark
A. Olson, Sanjeev K. Dey, Bartosz A. Grzybowski, and J. Fraser Stoddart. “Molecular-Mechanical
Switching at the Nanoparticle−solvent Interface: Practice and Theory.” Journal
of the American Chemical Society. American Chemical Society, 2010. https://doi.org/10.1021/ja9102327.'
ieee: 'A. Coskun et al., “Molecular-mechanical switching at the nanoparticle−solvent
interface: Practice and theory,” Journal of the American Chemical Society,
vol. 132, no. 12. American Chemical Society, pp. 4310–4320, 2010.'
ista: 'Coskun A, Wesson PJ, Klajn R, Trabolsi A, Fang L, Olson MA, Dey SK, Grzybowski
BA, Stoddart JF. 2010. Molecular-mechanical switching at the nanoparticle−solvent
interface: Practice and theory. Journal of the American Chemical Society. 132(12),
4310–4320.'
mla: 'Coskun, Ali, et al. “Molecular-Mechanical Switching at the Nanoparticle−solvent
Interface: Practice and Theory.” Journal of the American Chemical Society,
vol. 132, no. 12, American Chemical Society, 2010, pp. 4310–20, doi:10.1021/ja9102327.'
short: A. Coskun, P.J. Wesson, R. Klajn, A. Trabolsi, L. Fang, M.A. Olson, S.K.
Dey, B.A. Grzybowski, J.F. Stoddart, Journal of the American Chemical Society
132 (2010) 4310–4320.
date_created: 2023-08-01T09:48:27Z
date_published: 2010-03-31T00:00:00Z
date_updated: 2023-08-08T08:00:31Z
day: '31'
doi: 10.1021/ja9102327
extern: '1'
external_id:
pmid:
- '20218598'
intvolume: ' 132'
issue: '12'
keyword:
- Colloid and Surface Chemistry
- Biochemistry
- General Chemistry
- Catalysis
language:
- iso: eng
month: '03'
oa_version: None
page: 4310-4320
pmid: 1
publication: Journal of the American Chemical Society
publication_identifier:
eissn:
- 1520-5126
issn:
- 0002-7863
publication_status: published
publisher: American Chemical Society
quality_controlled: '1'
scopus_import: '1'
status: public
title: 'Molecular-mechanical switching at the nanoparticle−solvent interface: Practice
and theory'
type: journal_article
user_id: 2DF688A6-F248-11E8-B48F-1D18A9856A87
volume: 132
year: '2010'
...
---
_id: '13420'
abstract:
- lang: eng
text: 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.
article_processing_charge: No
article_type: original
author:
- first_name: Rafal
full_name: Klajn, Rafal
id: 8e84690e-1e48-11ed-a02b-a1e6fb8bb53b
last_name: Klajn
- first_name: Lei
full_name: Fang, Lei
last_name: Fang
- first_name: Ali
full_name: Coskun, Ali
last_name: Coskun
- first_name: Mark A.
full_name: Olson, Mark A.
last_name: Olson
- first_name: Paul J.
full_name: Wesson, Paul J.
last_name: Wesson
- first_name: J. Fraser
full_name: Stoddart, J. Fraser
last_name: Stoddart
- first_name: Bartosz A.
full_name: Grzybowski, Bartosz A.
last_name: Grzybowski
citation:
ama: Klajn R, Fang L, Coskun A, et al. Metal nanoparticles functionalized with molecular
and supramolecular switches. Journal of the American Chemical Society.
2009;131(12):4233-4235. doi:10.1021/ja9001585
apa: Klajn, R., Fang, L., Coskun, A., Olson, M. A., Wesson, P. J., Stoddart, J.
F., & Grzybowski, B. A. (2009). Metal nanoparticles functionalized with molecular
and supramolecular switches. Journal of the American Chemical Society.
American Chemical Society. https://doi.org/10.1021/ja9001585
chicago: Klajn, Rafal, Lei Fang, Ali Coskun, Mark A. Olson, Paul J. Wesson, J. Fraser
Stoddart, and Bartosz A. Grzybowski. “Metal Nanoparticles Functionalized with
Molecular and Supramolecular Switches.” Journal of the American Chemical Society.
American Chemical Society, 2009. https://doi.org/10.1021/ja9001585.
ieee: R. Klajn et al., “Metal nanoparticles functionalized with molecular
and supramolecular switches,” Journal of the American Chemical Society,
vol. 131, no. 12. American Chemical Society, pp. 4233–4235, 2009.
ista: Klajn R, Fang L, Coskun A, Olson MA, Wesson PJ, Stoddart JF, Grzybowski BA.
2009. Metal nanoparticles functionalized with molecular and supramolecular switches.
Journal of the American Chemical Society. 131(12), 4233–4235.
mla: Klajn, Rafal, et al. “Metal Nanoparticles Functionalized with Molecular and
Supramolecular Switches.” Journal of the American Chemical Society, vol.
131, no. 12, American Chemical Society, 2009, pp. 4233–35, doi:10.1021/ja9001585.
short: R. Klajn, L. Fang, A. Coskun, M.A. Olson, P.J. Wesson, J.F. Stoddart, B.A.
Grzybowski, Journal of the American Chemical Society 131 (2009) 4233–4235.
date_created: 2023-08-01T10:30:17Z
date_published: 2009-04-01T00:00:00Z
date_updated: 2023-08-08T09:06:00Z
day: '01'
doi: 10.1021/ja9001585
extern: '1'
external_id:
pmid:
- '19265400'
intvolume: ' 131'
issue: '12'
keyword:
- Colloid and Surface Chemistry
- Biochemistry
- General Chemistry
- Catalysis
language:
- iso: eng
month: '04'
oa_version: None
page: 4233-4235
pmid: 1
publication: Journal of the American Chemical Society
publication_identifier:
eissn:
- 1520-5126
issn:
- 0002-7863
publication_status: published
publisher: American Chemical Society
quality_controlled: '1'
scopus_import: '1'
status: public
title: Metal nanoparticles functionalized with molecular and supramolecular switches
type: journal_article
user_id: 2DF688A6-F248-11E8-B48F-1D18A9856A87
volume: 131
year: '2009'
...
---
_id: '8486'
abstract:
- lang: eng
text: 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.
article_processing_charge: No
article_type: original
author:
- first_name: Ewen
full_name: Lescop, Ewen
last_name: Lescop
- first_name: Paul
full_name: Schanda, Paul
id: 7B541462-FAF6-11E9-A490-E8DFE5697425
last_name: Schanda
orcid: 0000-0002-9350-7606
- first_name: Rodolfo
full_name: Rasia, Rodolfo
last_name: Rasia
- first_name: Bernhard
full_name: Brutscher, Bernhard
last_name: Brutscher
citation:
ama: Lescop E, Schanda P, Rasia R, Brutscher B. Automated spectral compression for
fast multidimensional NMR and increased time resolution in real-time NMR spectroscopy.
Journal of the American Chemical Society. 2007;129(10):2756-2757. doi:10.1021/ja068949u
apa: Lescop, E., Schanda, P., Rasia, R., & Brutscher, B. (2007). Automated spectral
compression for fast multidimensional NMR and increased time resolution in real-time
NMR spectroscopy. Journal of the American Chemical Society. American Chemical
Society. https://doi.org/10.1021/ja068949u
chicago: Lescop, Ewen, Paul Schanda, Rodolfo Rasia, and Bernhard Brutscher. “Automated
Spectral Compression for Fast Multidimensional NMR and Increased Time Resolution
in Real-Time NMR Spectroscopy.” Journal of the American Chemical Society.
American Chemical Society, 2007. https://doi.org/10.1021/ja068949u.
ieee: E. Lescop, P. Schanda, R. Rasia, and B. Brutscher, “Automated spectral compression
for fast multidimensional NMR and increased time resolution in real-time NMR spectroscopy,”
Journal of the American Chemical Society, vol. 129, no. 10. American Chemical
Society, pp. 2756–2757, 2007.
ista: Lescop E, Schanda P, Rasia R, Brutscher B. 2007. Automated spectral compression
for fast multidimensional NMR and increased time resolution in real-time NMR spectroscopy.
Journal of the American Chemical Society. 129(10), 2756–2757.
mla: Lescop, Ewen, et al. “Automated Spectral Compression for Fast Multidimensional
NMR and Increased Time Resolution in Real-Time NMR Spectroscopy.” Journal of
the American Chemical Society, vol. 129, no. 10, American Chemical Society,
2007, pp. 2756–57, doi:10.1021/ja068949u.
short: E. Lescop, P. Schanda, R. Rasia, B. Brutscher, Journal of the American Chemical
Society 129 (2007) 2756–2757.
date_created: 2020-09-18T10:13:21Z
date_published: 2007-02-17T00:00:00Z
date_updated: 2021-01-12T08:19:36Z
day: '17'
doi: 10.1021/ja068949u
extern: '1'
intvolume: ' 129'
issue: '10'
keyword:
- Colloid and Surface Chemistry
- Biochemistry
- General Chemistry
- Catalysis
language:
- iso: eng
month: '02'
oa_version: None
page: 2756-2757
publication: Journal of the American Chemical Society
publication_identifier:
issn:
- 0002-7863
- 1520-5126
publication_status: published
publisher: American Chemical Society
quality_controlled: '1'
status: public
title: Automated spectral compression for fast multidimensional NMR and increased
time resolution in real-time NMR spectroscopy
type: journal_article
user_id: 2DF688A6-F248-11E8-B48F-1D18A9856A87
volume: 129
year: '2007'
...
---
_id: '8487'
abstract:
- lang: eng
text: 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.
article_processing_charge: No
article_type: original
author:
- first_name: Maayan
full_name: Gal, Maayan
last_name: Gal
- first_name: Paul
full_name: Schanda, Paul
id: 7B541462-FAF6-11E9-A490-E8DFE5697425
last_name: Schanda
orcid: 0000-0002-9350-7606
- first_name: Bernhard
full_name: Brutscher, Bernhard
last_name: Brutscher
- first_name: Lucio
full_name: Frydman, Lucio
last_name: Frydman
citation:
ama: Gal M, Schanda P, Brutscher B, Frydman L. UltraSOFAST HMQC NMR and the repetitive
acquisition of 2D protein spectra at Hz rates. Journal of the American Chemical
Society. 2007;129(5):1372-1377. doi:10.1021/ja066915g
apa: Gal, M., Schanda, P., Brutscher, B., & Frydman, L. (2007). UltraSOFAST
HMQC NMR and the repetitive acquisition of 2D protein spectra at Hz rates. Journal
of the American Chemical Society. American Chemical Society. https://doi.org/10.1021/ja066915g
chicago: Gal, Maayan, Paul Schanda, Bernhard Brutscher, and Lucio Frydman. “UltraSOFAST
HMQC NMR and the Repetitive Acquisition of 2D Protein Spectra at Hz Rates.” Journal
of the American Chemical Society. American Chemical Society, 2007. https://doi.org/10.1021/ja066915g.
ieee: M. Gal, P. Schanda, B. Brutscher, and L. Frydman, “UltraSOFAST HMQC NMR and
the repetitive acquisition of 2D protein spectra at Hz rates,” Journal of the
American Chemical Society, vol. 129, no. 5. American Chemical Society, pp.
1372–1377, 2007.
ista: Gal M, Schanda P, Brutscher B, Frydman L. 2007. UltraSOFAST HMQC NMR and the
repetitive acquisition of 2D protein spectra at Hz rates. Journal of the American
Chemical Society. 129(5), 1372–1377.
mla: Gal, Maayan, et al. “UltraSOFAST HMQC NMR and the Repetitive Acquisition of
2D Protein Spectra at Hz Rates.” Journal of the American Chemical Society,
vol. 129, no. 5, American Chemical Society, 2007, pp. 1372–77, doi:10.1021/ja066915g.
short: M. Gal, P. Schanda, B. Brutscher, L. Frydman, Journal of the American Chemical
Society 129 (2007) 1372–1377.
date_created: 2020-09-18T10:13:27Z
date_published: 2007-01-10T00:00:00Z
date_updated: 2021-01-12T08:19:37Z
day: '10'
doi: 10.1021/ja066915g
extern: '1'
intvolume: ' 129'
issue: '5'
keyword:
- Colloid and Surface Chemistry
- Biochemistry
- General Chemistry
- Catalysis
language:
- iso: eng
month: '01'
oa_version: None
page: 1372-1377
publication: Journal of the American Chemical Society
publication_identifier:
issn:
- 0002-7863
- 1520-5126
publication_status: published
publisher: American Chemical Society
quality_controlled: '1'
status: public
title: UltraSOFAST HMQC NMR and the repetitive acquisition of 2D protein spectra at
Hz rates
type: journal_article
user_id: 2DF688A6-F248-11E8-B48F-1D18A9856A87
volume: 129
year: '2007'
...
---
_id: '8488'
abstract:
- lang: eng
text: 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.
article_processing_charge: No
article_type: original
author:
- first_name: Paul
full_name: Schanda, Paul
id: 7B541462-FAF6-11E9-A490-E8DFE5697425
last_name: Schanda
orcid: 0000-0002-9350-7606
- first_name: Hélène
full_name: Van Melckebeke, Hélène
last_name: Van Melckebeke
- first_name: Bernhard
full_name: Brutscher, Bernhard
last_name: Brutscher
citation:
ama: Schanda P, Van Melckebeke H, Brutscher B. Speeding up three-dimensional protein
NMR experiments to a few minutes. Journal of the American Chemical Society.
2006;128(28):9042-9043. doi:10.1021/ja062025p
apa: Schanda, P., Van Melckebeke, H., & Brutscher, B. (2006). Speeding up three-dimensional
protein NMR experiments to a few minutes. Journal of the American Chemical
Society. American Chemical Society. https://doi.org/10.1021/ja062025p
chicago: Schanda, Paul, Hélène Van Melckebeke, and Bernhard Brutscher. “Speeding
up Three-Dimensional Protein NMR Experiments to a Few Minutes.” Journal of
the American Chemical Society. American Chemical Society, 2006. https://doi.org/10.1021/ja062025p.
ieee: P. Schanda, H. Van Melckebeke, and B. Brutscher, “Speeding up three-dimensional
protein NMR experiments to a few minutes,” Journal of the American Chemical
Society, vol. 128, no. 28. American Chemical Society, pp. 9042–9043, 2006.
ista: Schanda P, Van Melckebeke H, Brutscher B. 2006. Speeding up three-dimensional
protein NMR experiments to a few minutes. Journal of the American Chemical Society.
128(28), 9042–9043.
mla: Schanda, Paul, et al. “Speeding up Three-Dimensional Protein NMR Experiments
to a Few Minutes.” Journal of the American Chemical Society, vol. 128,
no. 28, American Chemical Society, 2006, pp. 9042–43, doi:10.1021/ja062025p.
short: P. Schanda, H. Van Melckebeke, B. Brutscher, Journal of the American Chemical
Society 128 (2006) 9042–9043.
date_created: 2020-09-18T10:13:36Z
date_published: 2006-06-21T00:00:00Z
date_updated: 2021-01-12T08:19:37Z
day: '21'
doi: 10.1021/ja062025p
extern: '1'
intvolume: ' 128'
issue: '28'
keyword:
- Colloid and Surface Chemistry
- Biochemistry
- General Chemistry
- Catalysis
language:
- iso: eng
month: '06'
oa_version: None
page: 9042-9043
publication: Journal of the American Chemical Society
publication_identifier:
issn:
- 0002-7863
- 1520-5126
publication_status: published
publisher: American Chemical Society
quality_controlled: '1'
status: public
title: Speeding up three-dimensional protein NMR experiments to a few minutes
type: journal_article
user_id: 2DF688A6-F248-11E8-B48F-1D18A9856A87
volume: 128
year: '2006'
...
---
_id: '13428'
abstract:
- lang: eng
text: 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.
article_processing_charge: No
article_type: original
author:
- first_name: Alexander M.
full_name: Kalsin, Alexander M.
last_name: Kalsin
- first_name: Bartlomiej
full_name: Kowalczyk, Bartlomiej
last_name: Kowalczyk
- first_name: Stoyan K.
full_name: Smoukov, Stoyan K.
last_name: Smoukov
- first_name: Rafal
full_name: Klajn, Rafal
id: 8e84690e-1e48-11ed-a02b-a1e6fb8bb53b
last_name: Klajn
- first_name: Bartosz A.
full_name: Grzybowski, Bartosz A.
last_name: Grzybowski
citation:
ama: Kalsin AM, Kowalczyk B, Smoukov SK, Klajn R, Grzybowski BA. Ionic-like behavior
of oppositely charged nanoparticles. Journal of the American Chemical Society.
2006;128(47):15046-15047. doi:10.1021/ja0642966
apa: Kalsin, A. M., Kowalczyk, B., Smoukov, S. K., Klajn, R., & Grzybowski,
B. A. (2006). Ionic-like behavior of oppositely charged nanoparticles. Journal
of the American Chemical Society. American Chemical Society. https://doi.org/10.1021/ja0642966
chicago: Kalsin, Alexander M., Bartlomiej Kowalczyk, Stoyan K. Smoukov, Rafal Klajn,
and Bartosz A. Grzybowski. “Ionic-like Behavior of Oppositely Charged Nanoparticles.”
Journal of the American Chemical Society. American Chemical Society, 2006.
https://doi.org/10.1021/ja0642966.
ieee: A. M. Kalsin, B. Kowalczyk, S. K. Smoukov, R. Klajn, and B. A. Grzybowski,
“Ionic-like behavior of oppositely charged nanoparticles,” Journal of the American
Chemical Society, vol. 128, no. 47. American Chemical Society, pp. 15046–15047,
2006.
ista: Kalsin AM, Kowalczyk B, Smoukov SK, Klajn R, Grzybowski BA. 2006. Ionic-like
behavior of oppositely charged nanoparticles. Journal of the American Chemical
Society. 128(47), 15046–15047.
mla: Kalsin, Alexander M., et al. “Ionic-like Behavior of Oppositely Charged Nanoparticles.”
Journal of the American Chemical Society, vol. 128, no. 47, American Chemical
Society, 2006, pp. 15046–47, doi:10.1021/ja0642966.
short: A.M. Kalsin, B. Kowalczyk, S.K. Smoukov, R. Klajn, B.A. Grzybowski, Journal
of the American Chemical Society 128 (2006) 15046–15047.
date_created: 2023-08-01T10:36:27Z
date_published: 2006-11-29T00:00:00Z
date_updated: 2023-08-08T11:30:06Z
day: '29'
doi: 10.1021/ja0642966
extern: '1'
external_id:
pmid:
- '17117829'
intvolume: ' 128'
issue: '47'
keyword:
- Colloid and Surface Chemistry
- Biochemistry
- General Chemistry
- Catalysis
language:
- iso: eng
month: '11'
oa_version: None
page: 15046-15047
pmid: 1
publication: Journal of the American Chemical Society
publication_identifier:
eissn:
- 1520-5126
issn:
- 0002-7863
publication_status: published
publisher: American Chemical Society
quality_controlled: '1'
scopus_import: '1'
status: public
title: Ionic-like behavior of oppositely charged nanoparticles
type: journal_article
user_id: 2DF688A6-F248-11E8-B48F-1D18A9856A87
volume: 128
year: '2006'
...