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1.
Phys Rev Lett ; 119(7): 078002, 2017 Aug 18.
Artigo em Inglês | MEDLINE | ID: mdl-28949673

RESUMO

Transient molecular networks, a class of adaptive soft materials with remarkable application potential, display complex, and intriguing dynamic behavior. By performing dynamic light scattering on a wide angular range, we study the relaxation dynamics of a reversible network formed by DNA tetravalent nanoparticles, finding a slow relaxation mode that is wave vector independent at large q and crosses over to a standard q^{-2} viscoelastic relaxation at low q. Exploiting the controlled properties of our DNA network, we attribute this mode to fluctuations in local elasticity induced by connectivity rearrangement. We propose a simple beads and springs model that captures the basic features of this q^{0} behavior.

2.
Proc Natl Acad Sci U S A ; 110(39): 15633-7, 2013 Sep 24.
Artigo em Inglês | MEDLINE | ID: mdl-24019470

RESUMO

Colloidal particles with directional interactions are key in the realization of new colloidal materials with possibly unconventional phase behaviors. Here we exploit DNA self-assembly to produce bulk quantities of "DNA stars" with three or four sticky terminals, mimicking molecules with controlled limited valence. Solutions of such molecules exhibit a consolution curve with an upper critical point, whose temperature and concentration decrease with the valence. Upon approaching the critical point from high temperature, the intensity of the scattered light diverges with a power law, whereas the intensity time autocorrelation functions show a surprising two-step relaxation, somehow reminiscent of glassy materials. The slow relaxation time exhibits an Arrhenius behavior with no signs of criticality, demonstrating a unique scenario where the critical slowing down of the concentration fluctuations is subordinate to the large lifetime of the DNA bonds, with relevant analogies to critical dynamics in polymer solutions. The combination of equilibrium and dynamic behavior of DNA nanostars demonstrates the potential of DNA molecules in diversifying the pathways toward collective properties and self-assembled materials, beyond the range of phenomena accessible with ordinary molecular fluids.


Assuntos
DNA/química , Nanopartículas/química , Transição de Fase , Isocoros
3.
Soft Matter ; 11(16): 3132-8, 2015 Apr 28.
Artigo em Inglês | MEDLINE | ID: mdl-25747102

RESUMO

Kinetic arrest in colloidal dispersions with isotropic attractive interactions usually occurs through the destabilization of the homogeneous phase and the formation of a non-equilibrium network of jammed particles. Theory and simulations predict that a different route to gelation should become available when the valence of each colloidal particle is suitably reduced. Under these conditions, gelation should be achievable through a reversible sequence of equilibrium states. Here we report the reversible dynamic arrest of a dispersion of DNA-based nanoparticles with anisotropic interactions and a coordination number equal to four. As the temperature is decreased, the relaxation time for density fluctuations slows down by about five orders of magnitude, following an Arrhenius scaling in the entire experimentally accessible temperature window. The system is in thermodynamic equilibrium at all temperatures. Gelation in our system mimics the dynamic arrest of networking atomic strong glass formers such as silica, for which it could thus provide a suitable colloidal model.


Assuntos
DNA/química , Géis/química , Vidro/química , Nanopartículas/química , Coloides/química , Luz , Modelos Teóricos , Espalhamento de Radiação , Propriedades de Superfície , Temperatura , Termodinâmica
4.
Eur Phys J E Soft Matter ; 38(6): 64, 2015 Jun.
Artigo em Inglês | MEDLINE | ID: mdl-26123767

RESUMO

Self-assembling DNA-nanostars are ideal candidates to explore equilibrium gelation in systems composed of limited-valence particles. We present here a light scattering study of the dynamics in a trivalent DNA-nanostars equilibrium gel and of its dependence on ionic strength and concentration. Reversible bonds between different nanostars, whose formation is sensitively dependent on temperature, concentration and ionic strength, are provided by complementary DNA sticky ends. We find that the decay of the density correlations is described by a two-step relaxation process characterised by: i) a slow time scale that varies over nearly four orders of magnitude in a temperature window of less than 30 degrees; ii) an increase of the amplitude (the so-called non-ergodicity factor) of the slow relaxation. The slow process follows an Arrhenius law with temperature. We observe that the activation enthalpy does not depend on the ionic strength and that the dependence of the relaxation time on the ionic strength can be rationalized in terms of the free-energy cost of forming a sticky-end duplex. Finally, we observe that dynamics is insensitive to nanostar concentration, in full agreement with the predicted behaviour in equilibrium gels.


Assuntos
DNA/química , Nanopartículas/química , Sequência de Bases , Géis/química , Simulação de Dinâmica Molecular , Dados de Sequência Molecular , Concentração Osmolar
5.
Photochem Photobiol ; 99(1): 101-105, 2023 01.
Artigo em Inglês | MEDLINE | ID: mdl-35578782

RESUMO

The ongoing emergency provoked by the SARS-CoV-2 pandemic demands the development of technologies to mitigate the spread of infection, and UV irradiation is a technique that can efficiently address this issue. However, proper use of UV equipment for disinfection requires an understanding of how the effects on SARS-CoV-2 are dependent on certain parameters. In this work, we determined the UV-C inactivation constant k for SARS-CoV-2 using an LED source at λ = 280 nm. Specifically, a Log3 reduction was measured after irradiation for 24 min with a delivered UV-C dose of 23 J m-2 . By multitarget model fitting, n = 2 and k = 0.32 ± 0.02 m2 J-1 were obtained. A lag time for the inactivation effect was also observed, which was attributed to the low irradiation levels used to perform the study. The combination of k and delay time allows for reliable estimation of disinfection times in small, closed environments.


Assuntos
COVID-19 , SARS-CoV-2 , Humanos , COVID-19/prevenção & controle , Raios Ultravioleta , Desinfecção/métodos , Pandemias/prevenção & controle , Inativação de Vírus/efeitos da radiação
7.
Phys Rev E ; 93(1): 012704, 2016 Jan.
Artigo em Inglês | MEDLINE | ID: mdl-26871132

RESUMO

We study phases and structures of mixtures of two representative chromonic liquid crystal materials, sunset yellow FCF (SSY) and disodium cromoglycate (DSCG), in water. A variety of combinations of isotropic, nematic (N), and columnar (also called M) phases are observed depending on their concentrations, and a phase diagram is made. We find a tendency for DSCG-rich regions to show higher-order phases while SSY-rich regions show lower-order ones. We observe uniform mesophases only when one of the materials is sparse in the N phases. Their miscibility in M phases is so low that essentially complete phase separation occurs. X-ray scattering and spectroscopy studies confirm that SSY and DSCG molecules do not mix when they form chromonic aggregates and neither do their aggregates when they form M phases.


Assuntos
Compostos Azo/química , Cromolina Sódica/química , Cristais Líquidos/química , Água/química , Microscopia , Estrutura Molecular , Transição de Fase , Análise Espectral , Difração de Raios X
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