We probe the local and global structure of spin-coated colloidal crystals via laser diffraction measurements and scanning electron and atomic force microscopies, and find that they are unique three-dimensional orientationally correlated polycrystals, exhibiting short-range positional order but long-range radial orientational correlations, reminiscent of-but distinct from-two-dimensional colloidal hexatic phases. Thickness and symmetries are controllable by solvent choice and spin speed. While the polycrystallinity of these colloidal films limits their applicability to photonics, we demonstrate their feasibility as templates to make crack-free magnetic patterns.
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http://dx.doi.org/10.1103/PhysRevE.77.050402 | DOI Listing |
ACS Appl Mater Interfaces
January 2025
Group of Characterization of Materials, Departament de Física, Universitat Politècnica de Catalunya, Campus Diagonal-Besòs, Av. Eduard Maristany 10-14, Barcelona 08019, Spain.
Hybrid organic-inorganic perovskites (HOIP) have emerged in recent years as highly promising semiconducting materials for a wide range of optoelectronic and energy applications. Nevertheless, the rotational dynamics of the organic components and many-molecule interdependencies, which may strongly impact the functional properties of HOIP, are not yet fully understood. In this study, we quantitatively analyze the orientational disorder and molecular correlations in archetypal perovskite CHNHPbI (MAPI) by performing comprehensive molecular dynamics simulations and entropy calculations.
View Article and Find Full Text PDFJ Am Chem Soc
July 2024
Department of Chemistry and Biochemistry, Utah State University, Logan, Utah 84322, United States.
Conical intersections (CIs) hold significant stake in manipulating and controlling photochemical reaction pathways of molecules at interfaces and surfaces by affecting molecular dynamics therein. Currently, there is no tool for characterizing CIs at interfaces and surfaces. To this end, we have developed phase-cycling interface-specific two-dimensional electronic spectroscopy (i2D-ES) and combined it with advanced computational modeling to explore nonadiabatic CI dynamics of molecules at the air/water interface.
View Article and Find Full Text PDFJ Am Soc Mass Spectrom
April 2024
Department of Chemistry, University of Michigan, 930 North University Avenue, Ann Arbor, Michigan 48109-1055, United States.
We previously discovered that electron attachment to gaseous peptide anions can occur within a relatively narrow electron energy range. The resulting charge-increased radical ions undergo dissociation analogous to conventional cation electron capture/transfer dissociation (ECD/ETD), thus enabling a novel tandem mass spectrometry (MS/MS) technique that we termed negative ion electron capture dissociation (niECD). We proposed that gaseous zwitterionic structures are required for niECD with electron capture either occurring at or being directed by a positively charged site.
View Article and Find Full Text PDFJ Chem Theory Comput
February 2024
Institute for Applied Physics, University of Tübingen, Auf der Morgenstelle 10, 72076 Tübingen, Germany.
Anisotropic patchy particles have become an archetypical statistical model system for associating fluids. Here, we formulate an approach to the Kern-Frenkel model via the classical density functional theory to describe the positionally and orientationally resolved equilibrium density distributions in flat wall geometries. The density functional is split into a reference part for the orientationally averaged density and an orientational part in mean-field approximation.
View Article and Find Full Text PDFJ Chem Phys
October 2023
Laboratory for Soft Matter and Biophysics, Department of Physics and Astronomy, KU Leuven, Leuven 3001, Belgium.
Highly acidic protic ionic liquids (PILs) are promising materials for potential electrochemical applications due to their high proton conductivity and excellent thermal stability. Still, little is known about the correlation between charge transport and structural dynamics as well as the proton transport mechanism despite the large body of literature on this topic. Here, we have examined the charge transport and structural dynamics by employing broadband dielectric spectroscopy in two highly acidic PILs in their supercooled liquid and glassy states, which included the same anion [TfO]- and different cations, [Tau]+ vs [Ahs]+.
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