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Wang, Q., Zhang, Q., Zhang, Q.-W. -., Li, X., Zhao, C.-X. -., Xu, T.-Y. -., . . . Tian, H. (2020). Color-tunable single-fluorophore supramolecular system with assembly-encoded emission. Nature Communications, 11(1), Article ID 158.
Open this publication in new window or tab >>Color-tunable single-fluorophore supramolecular system with assembly-encoded emission
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2020 (English)In: Nature Communications, ISSN 2041-1723, E-ISSN 2041-1723, Vol. 11, no 1, article id 158Article in journal (Refereed) Published
Abstract [en]

Regulating the fluorescent properties of organic small molecules in a controlled and dynamic manner has been a fundamental research goal. Although several strategies have been exploited, realizing multi-color molecular emission from a single fluorophore remains challenging. Herein, we demonstrate an emissive system by combining pyrene fluorophore and acylhydrazone units, which can generate multi-color switchable fluorescent emissions at different assembled states. Two kinds of supramolecular tools, amphiphilic self-assembly and γ-cyclodextrin mediated host-guest recognition, are used to manipulate the intermolecular aromatic stacking distances, resulting in the tunable fluorescent emission ranging from blue to yellow, including a pure white-light emission. Moreover, an external chemical signal, amylase, is introduced to control the assembly states of the system on a time scale, generating a distinct dynamic emission system. The dynamic properties of this multi-color fluorescent system can be also enabled in a hydrogel network, exhibiting a promising potential for intelligent fluorescent materials.

Place, publisher, year, edition, pages
Nature Research, 2020
National Category
Chemical Sciences
Identifiers
urn:nbn:se:kth:diva-267775 (URN)10.1038/s41467-019-13994-6 (DOI)000511898900009 ()31919416 (PubMedID)2-s2.0-85077733109 (Scopus ID)
Note

QC 20200304

Available from: 2020-03-04 Created: 2020-03-04 Last updated: 2020-05-11Bibliographically approved
Li, C., Zhang, K., Ishida, M., Li, Q., Shimomura, K., Baryshnikov, G. V., . . . Xie, Y. (2020). Tripyrrin-armed isosmaragdyrins: synthesis, heterodinuclear coordination, and protonation-triggered helical inversion. Chemical Science, 11(10), 2790-2795
Open this publication in new window or tab >>Tripyrrin-armed isosmaragdyrins: synthesis, heterodinuclear coordination, and protonation-triggered helical inversion
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2020 (English)In: Chemical Science, ISSN 2041-6520, E-ISSN 2041-6539, Vol. 11, no 10, p. 2790-2795Article in journal (Refereed) Published
Abstract [en]

Oxidative ring closure of linear oligopyrroles is one of the synthetic approaches to novel porphyrinoids with dinuclear coordination sites and helical chirality. The spatial arrangement of the pyrrolic groups of octapyrrole (P8) affected the position of the intramolecular oxidative coupling of the pyrrolic units; tripyrrin-armed isosmaragdyrin analogue (1) containing a beta,beta-linked bipyrrole moiety was synthesized regioselectively in a high yield by using FeCl3. Ni-II-coordination at the armed tripyrrin site of 1 allowed the formation of diastereomeric helical twisted complexes (2A and 2B) and succeeding Cu-II-coordination at the macrocyclic core afforded heterodinuclear Ni-II/Cu-II-complexes (3A and 3B). Each of them comprised a pair of separable enantiomers, exhibiting P- and M-helices, respectively. Notably, diastereomeric interconversion from 2A to 2B was quantitatively achieved as a consequence of helical transformation under acidic conditions.

Place, publisher, year, edition, pages
ROYAL SOC CHEMISTRY, 2020
National Category
Theoretical Chemistry
Identifiers
urn:nbn:se:kth:diva-271757 (URN)10.1039/c9sc06197e (DOI)000519742300019 ()2-s2.0-85081982643 (Scopus ID)
Note

QC 20200407

Available from: 2020-04-07 Created: 2020-04-07 Last updated: 2020-04-07Bibliographically approved
Lu, Y., Song, H., Li, X., Ågren, H., Liu, Q., Zhang, J., . . . Xie, Y. (2019). Multiply Wrapped Porphyrin Dyes with a Phenothiazine Donor: A High Efficiency of 11.7% Achieved through a Synergetic Coadsorption and Cosensitization Approach. ACS Applied Materials and Interfaces, 11(5), 5046-5054
Open this publication in new window or tab >>Multiply Wrapped Porphyrin Dyes with a Phenothiazine Donor: A High Efficiency of 11.7% Achieved through a Synergetic Coadsorption and Cosensitization Approach
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2019 (English)In: ACS Applied Materials and Interfaces, ISSN 1944-8244, E-ISSN 1944-8252, Vol. 11, no 5, p. 5046-5054Article in journal (Refereed) Published
Abstract [en]

Photocurrent (J) and photovoltage (Vac) are two important parameters for dye-sensitized solar cells (DSSCs) to achieve high power conversion efficiencies (PCEs). Herein, we synthesize four novel porphyrin dyes, XW36 XW39, using an N-phenyl-substituted phenothiazine donor to pursue higher PCE. For XW36 and XW37, the N-phenyl group is wrapped with two ortho-alkoxy chains. In contrast, it is substituted with a para-alkoxy group in XW38 and XW39. The phenothiazine wrapping in XW36 and XW37 induces more serious distortion, which is beneficial for anti-aggregation but unfavorable for the electron transfer from donor to a porphyrin framework. Thus, individual porphyrin dyes XW36 and XW37 exhibit efficiencies of 9.05 and 9.58%, respectively, lower than those of 9.51 and 10.0% achieved for XW38 and XW39, respectively. Besides, the introduction of a methyl group into a benzoic acid acceptor unit is conducive to anti-aggregation and thus improves the V-oc and efficiencies. Therefore, higher efficiencies were achieved for XW37 and XW39, compared with XW36 and XW38, respectively. Interestingly, although the individual XW36 dye shows a lowest efficiency among the four dyes, a highest efficiency of 11.7% was obtained for XW36 on the basis of synergetic adsorption with chenodeoxycholic acid and PT-C6 because of simultaneously improved J and Voc, which may be ascribed to the lowest dye-loading amount of XW36 among all of these porphyrin dyes, with the largest vacancy area left on the TiO2 surface available for cosensitizer PT-C6, resulting in a highest J. The high efficiency of 11.7% is one of the highest efficiencies using I-/I-3(-) electrolytes in DSSCs. These results provide an effective strategy for developing efficient DSSCs by the targeted coadsorption and cosensitization of porphyrin sensitizers optimized through introducing a bis(ortho-alkoxy)-wrapped phenyl group into the phenothiazine donor and/or methyl groups into the benzoic acid acceptor unit.

Place, publisher, year, edition, pages
AMER CHEMICAL SOC, 2019
Keywords
phenothiazine, porphyrin, wrapped structure, coadsorption, cosensitization
National Category
Other Chemistry Topics
Identifiers
urn:nbn:se:kth:diva-245144 (URN)10.1021/acsami.8b19077 (DOI)000458347900036 ()30644719 (PubMedID)2-s2.0-85061138430 (Scopus ID)
Note

QC 20190313

Available from: 2019-03-13 Created: 2019-03-13 Last updated: 2020-03-09Bibliographically approved
Li, Q., Ishida, M., Kai, H., Gu, T., Li, C., Li, X., . . . Xie, Y. (2019). Skeletal Rearrangement of Twisted Thia-Norhexaphyrin: Multiply Annulated Polypyrrolic Aromatic Macrocycles. Angewandte Chemie International Edition, 58(18), 5925-5929
Open this publication in new window or tab >>Skeletal Rearrangement of Twisted Thia-Norhexaphyrin: Multiply Annulated Polypyrrolic Aromatic Macrocycles
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2019 (English)In: Angewandte Chemie International Edition, ISSN 1433-7851, E-ISSN 1521-3773, Vol. 58, no 18, p. 5925-5929Article in journal (Refereed) Published
Abstract [en]

A hybrid thia-norhexaphyrin comprising a directly linked N-confused pyrrole and thiophene unit (1) revealed unique macrocycle transformations to afford multiply inner-annulated aromatic macrocycles. Oxidation with 2,3-dichloro-5,6-dicyano-1,4-benzoquinone triggered a cleavage of the C-S bond of the thiophene unit, accompanied with skeletal rearrangement to afford unique pi-conjugated products: a thiopyrrolo-pentaphyrin embedded with a pyrrolo[1,2]isothiazole (2), a sulfur-free pentaphyrin incorporating an indolizine moiety (3), and a thiopyranyltriphyrinoid containing a 2H-thiopyran unit (4). Furthermore, 2 underwent desulfurization reactions to afford a fused pentaphyrin containing a pyrrolizine moiety (5) under mild conditions. Using expanded porphyrin scaffolds, oxidative thiophene cleavage and desulfurization of the hitherto unknown N-confused core-modified macrocycles would be a practical approach for developing unique polypyrrolic aromatic macrocycles.

Place, publisher, year, edition, pages
WILEY-V C H VERLAG GMBH, 2019
Keywords
aromaticity, macrocycles, porphyrinoids, skeletal rearrangement
National Category
Organic Chemistry
Identifiers
urn:nbn:se:kth:diva-251277 (URN)10.1002/anie.201900010 (DOI)000465413400019 ()30843636 (PubMedID)2-s2.0-85063590252 (Scopus ID)
Note

QC 20190517

Available from: 2019-05-17 Created: 2019-05-17 Last updated: 2019-05-17Bibliographically approved
Rinkevicius, Z., Li, X., Vahtras, O., Ahmadzadeh, K., Brand, M., Ringholm, M., . . . Norman, P. (2019). VeloxChem: A Python-driven density-functional theory program for spectroscopy simulations in high-performance computing environments. Wiley Interdisciplinary Reviews. Computational Molecular Science, Article ID e1457.
Open this publication in new window or tab >>VeloxChem: A Python-driven density-functional theory program for spectroscopy simulations in high-performance computing environments
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2019 (English)In: Wiley Interdisciplinary Reviews. Computational Molecular Science, ISSN 1759-0876, E-ISSN 1759-0884, article id e1457Article in journal (Refereed) Published
Abstract [en]

An open-source program named VeloxChem has been developed for the calculation of electronic real and complex linear response functions at the levels of Hartree–Fock and Kohn–Sham density functional theories. With an object-oriented program structure written in a Python/C++ layered fashion, VeloxChem enables time-efficient prototyping of novel scientific approaches without sacrificing computational efficiency, so that molecular systems involving up to and beyond 500 second-row atoms (or some 10,000 contracted and in part diffuse Gaussian basis functions) can be routinely addressed. In addition, VeloxChem is equipped with a polarizable embedding scheme for the treatment of the classical electrostatic interactions with an environment that in turn is modeled by atomic site charges and polarizabilities. The underlying hybrid message passing interface (MPI)/open multiprocessing (OpenMP) parallelization scheme makes VeloxChem suitable for execution in high-performance computing cluster environments, showing even slightly beyond linear scaling for the Fock matrix construction with use of up to 16,384 central processing unit (CPU) cores. An efficient—with respect to convergence rate and overall computational cost—multifrequency/gradient complex linear response equation solver enables calculations not only of conventional spectra, such as visible/ultraviolet/X-ray electronic absorption and circular dichroism spectra, but also time-resolved linear response signals as due to ultra-short weak laser pulses. VeloxChem distributed under the GNU Lesser General Public License version 2.1 (LGPLv2.1) license and made available for download from the homepage https://veloxchem.org. This article is categorized under: Software > Quantum Chemistry Electronic Structure Theory > Density Functional Theory Theoretical and Physical Chemistry > Spectroscopy.

Place, publisher, year, edition, pages
Blackwell Publishing Inc., 2019
Keywords
circular dichroism, density functional theory (DFT), ECD, high-performance computing (HPC), MPI, OpenMP, response theory, UV/vis, Application programming interfaces (API), Cluster computing, Computation theory, Computational efficiency, Dichroism, Electronic structure, High level languages, Message passing, Object oriented programming, Open source software, Physical chemistry, Program processors, Quantum chemistry, Circular dichroism spectra, Electronic structure theory, High performance computing, High performance computing (HPC), High-performance computing clusters, Density functional theory
National Category
Theoretical Chemistry
Identifiers
urn:nbn:se:kth:diva-268434 (URN)10.1002/wcms.1457 (DOI)000502095100001 ()2-s2.0-85076863228 (Scopus ID)
Note

QC 20200429

Available from: 2020-04-29 Created: 2020-04-29 Last updated: 2020-04-29Bibliographically approved
Qian, Z., Li, X., Yuan, T., Huang, X., Wang, Q., Agren, H. & Tian, H. (2018). Divalent Pseudorotaxane with Polarized Plug-Socket and Padlock Functions. Organic Letters, 20(6), 1487-1490
Open this publication in new window or tab >>Divalent Pseudorotaxane with Polarized Plug-Socket and Padlock Functions
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2018 (English)In: Organic Letters, ISSN 1523-7060, E-ISSN 1523-7052, Vol. 20, no 6, p. 1487-1490Article in journal (Refereed) Published
Abstract [en]

A dual-pore structured host composed of one 24-crown-8 and one 34-crown-10, and a "U"-shaped guest consisting of two different recognition units, one dibenzylammonium and one viologen, were synthesized and bound 1:1 into a divalent pseudorotaxane P1. P1 can mimic the inserting and pulling out functions of a polarized plug-socket system under solvent driven stimulus and can also realize the locking and unlocking actions of a padlock under pH stimulus.

Place, publisher, year, edition, pages
AMER CHEMICAL SOC, 2018
National Category
Chemical Sciences
Identifiers
urn:nbn:se:kth:diva-225718 (URN)10.1021/acs.orglett.7b03867 (DOI)000428003600003 ()29488384 (PubMedID)2-s2.0-85044078009 (Scopus ID)
Note

QC 20180411

Available from: 2018-04-11 Created: 2018-04-11 Last updated: 2018-04-11Bibliographically approved
Wang, J., Li, X., Zhang, J. & Tian, H. (2018). Modulating a D-Π-A type diarylethene for on-demand Cu2+ check via photo-switchable detection range and sensitivity. Sensors and actuators. B, Chemical, 257, 77-86
Open this publication in new window or tab >>Modulating a D-Π-A type diarylethene for on-demand Cu2+ check via photo-switchable detection range and sensitivity
2018 (English)In: Sensors and actuators. B, Chemical, ISSN 0925-4005, E-ISSN 1873-3077, Vol. 257, p. 77-86Article in journal (Refereed) Published
Abstract [en]

Detection range and sensitivity are two important parameters in a sensing system. Unfortunately, in common sensory systems, wide detection range always suffers from low sensitivity and vice versa. Thus, it becomes more and more desirable to design sensors with both wide detection range and high sensitivity. Here, we report a sensory system based on a photo-switchable D-π-A type diarylethene (SDE), which presents both wide detection range and high sensitivity under alternate light modulation. The D-π-A structure endows the sensor with high energy level of HOMO, which enabled the oxidation of both photoisomer SDEo/SDEc by Cu2+. While the discrepancy in energy levels of oxidation potentials in SDE photoisomers leads to their different reactivity, or in another word, sensitivity towards Cu2+. The inherent oxidative cycloreversion of SDEc to SDEo, on the other hand, provides a possibility that two photoisomers would detect Cu2+ in different working concentrations. The open form was employed for the detection of Cu2+ in a wider concentration range (0–13.0 equivalent) with relatively lower sensitivity (6.4 × 10−7 M). While the closed form was able to probe Cu2+ in lower concentration (0–3.0 equivalent) with higher sensitivity (6.6 × 10−9 M). Based on this photo-switchable sensing activity, a molecular multimeter of variable detection range for Cu2+ was then constructed.

Place, publisher, year, edition, pages
Elsevier, 2018
Keywords
Copper sensors, D-π-A diarylethene, Molecular multimeter, Photo-switchable detection range and sensitivity, Radical cations
National Category
Analytical Chemistry
Identifiers
urn:nbn:se:kth:diva-218908 (URN)10.1016/j.snb.2017.10.099 (DOI)000418868700010 ()2-s2.0-85032899414 (Scopus ID)
Note

QC 20171201

Available from: 2017-12-01 Created: 2017-12-01 Last updated: 2018-01-29Bibliographically approved
Zhang, Q., Rao, S.-J., Xie, T., Li, X., Xu, T.-Y., Li, D.-W., . . . Tian, H. (2018). Muscle-like Artificial Molecular Actuators for Nanoparticles. CHEM, 4(11), 2670-2684
Open this publication in new window or tab >>Muscle-like Artificial Molecular Actuators for Nanoparticles
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2018 (English)In: CHEM, ISSN 2451-9294, Vol. 4, no 11, p. 2670-2684Article in journal (Refereed) Published
Abstract [en]

Muscle tissue performs crucial contraction/extension motions that generate mechanical force and work by consuming chemical energy. Inspired by this naturally created biomolecular machine, artificial molecular muscles are designed and synthesized to undertake linear actuation functions. However, most of these muscle-like actuators are performed at large ensembles, while to realize the nanoscale actuation at the single-to few-molecule level remains challenging. Herein, we developed an artificial muscle-like molecular actuator that can reversibly control the proximity of the attached nano-objects, gold nanoparticles, within the single-molecule length level by its stimuli-responsive muscle-like linear contraction/extension motion. The molecular actuation motion is accompanied by an optical signal output resulting from the plasmonic resonance properties of gold nanoparticles. Meanwhile, the thermal noise of the muscle-like molecular actuator can be overcome by integrating the optical signal over a sufficiently long period.

Place, publisher, year, edition, pages
Cell Press, 2018
National Category
Physiology
Identifiers
urn:nbn:se:kth:diva-239474 (URN)10.1016/j.chempr.2018.08.030 (DOI)000449667900016 ()2-s2.0-85057276876 (Scopus ID)
Note

QC 20181126

Available from: 2018-11-26 Created: 2018-11-26 Last updated: 2019-03-18Bibliographically approved
Liang, L. & Li, X. (2018). Theoretical insights into aggregation-induced helicity modulation of a perylene bisimide derivative. Journal of Molecular Modeling, 24(3), Article ID 51.
Open this publication in new window or tab >>Theoretical insights into aggregation-induced helicity modulation of a perylene bisimide derivative
2018 (English)In: Journal of Molecular Modeling, ISSN 1610-2940, E-ISSN 0948-5023, Vol. 24, no 3, article id 51Article in journal (Refereed) Published
Abstract [en]

Formation of helical chiroptical self-assemblies via noncovalent interaction is a widely observed phenomenon in nature, the mechanism of which remains insufficiently understood. Employing an amphiphilic perylene-sugar dyad molecule (PBI-HAG) as an example, we report that the modulatable supramolecular helicity may emerge from an aggregating process that is dominated by competition between two types of noncovalent interaction: hydrogen bonding and pi-pi stacking. The interplay between these two driving forces, which is greatly affected by the solvent environment, determines the morphology the supramolecular assembly of PBI-HAGs. In particular, a non-layered supramolecular structure was formed in octane owing to stabilization effects of intermolecular hydrogen bonds, whereas a layered supramolecular structure was formed in water because of energetically favorable pi-pi stacking of aromatic rings. The formation of distinct supramolecular architectures in different solvents was reinforced by simulated circular dichroism spectra, which show opposite signals consistent with experimental observations. The results of this study could help us understand aggregation-induced supramolecular chirality of noncovalent self-assemblies.

Place, publisher, year, edition, pages
Springer, 2018
Keywords
Supramolecular helicity, Aggregation-induced chirality, Self-assembly, Circular dichroism, Exciton model
National Category
Biochemistry and Molecular Biology
Identifiers
urn:nbn:se:kth:diva-224685 (URN)10.1007/s00894-018-3591-1 (DOI)000426730900007 ()29435668 (PubMedID)2-s2.0-85042265877 (Scopus ID)
Note

QC 20180326

Available from: 2018-03-26 Created: 2018-03-26 Last updated: 2018-03-26Bibliographically approved
Chen, S., Li, W., Li, X. & Zhu, W.-H. -. (2017). Aggregation-controlled photochromism based on a dithienylethene derivative with aggregation-induced emission. Journal of Materials Chemistry C, 5(10), 2717-2722
Open this publication in new window or tab >>Aggregation-controlled photochromism based on a dithienylethene derivative with aggregation-induced emission
2017 (English)In: Journal of Materials Chemistry C, ISSN 2050-7526, E-ISSN 2050-7534, Vol. 5, no 10, p. 2717-2722Article in journal (Refereed) Published
Abstract [en]

We report novel aggregation-induced emission (AIE) characteristics involving aggregation-controlled photochromism properties of a dithienylethene derivative, BTE-EQ, where two quinolinemalononitrile (EQ) units are covalently attached to a dithienylethene core. The typical AIE effect of BTE-EQ has been found to originate from the AIE character of the EQ units with respect to the reference compound BTE, which does not contain an EQ unit. The photochromism study, together with density functional theory calculations, reveals that the photochromic activity of BTE-EQ can be reversibly switched off and on by controlling the aggregation state during the AIE process, which provides a novel route to controlling the photochromism of diarylethenes.

Place, publisher, year, edition, pages
Royal Society of Chemistry, 2017
Keywords
Density functional theory, Photochromism, Aggregation state, Aggregation-induced emissions, Diarylethenes, Dithienylethene, Novel route, Reference compounds, Agglomeration
National Category
Chemical Engineering
Identifiers
urn:nbn:se:kth:diva-207440 (URN)10.1039/C7TC00023E (DOI)000396293400028 ()2-s2.0-85014897544 (Scopus ID)
Note

Funding details: PCSIRT_IRT_16R49, MOE, Ministry of Education; Funding details: NSFC, National Natural Science Foundation of China; Funding text: This work was supported by the National key Research and Development Program (No. 2016YFA0200300), NSFC for Creative Research Groups (21421004) and Distinguished Young Scholars (21325625), NSFC/China, Ministry of Education of China (PCSIRT_IRT_16R49), Shanghai Sci. & Tech. and Edu. Committee (14YF1409200 and 15XD1501400), the Oriental Scholarship, Programme of Introducing Talents of Discipline to Universities (B16017), and the Fundamental Research Funds for the Central Universities (WJ1416005). We also thank the Swedish National Infrastructure for Computing (SNIC) for providing computational resources for project SNIC 2015-16/10.

QC 20170523

Available from: 2017-05-23 Created: 2017-05-23 Last updated: 2017-05-23Bibliographically approved
Organisations
Identifiers
ORCID iD: ORCID iD iconorcid.org/0000-0001-6508-8355

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