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An optical photobleaching technique has been used to measure the reorientation of dilute probes in freestanding polystyrene films as thin as 14 nm. Temperature-ramping and isothermal anisotropy measurements reveal the existence of two subsets of probe molecules with different dynamics. While the slow subset shows bulk-like dynamics, the more mobile subset reorients within a few hundred seconds even at T(g,DSC) - 25 K (T(g,DSC) is the glass transition temperature of bulk polystyrene). At T(g,DSC)

Temperature-ramping anisotropy measurements were used to probe the molecular mobility of fluorescent probes in polystyrene, poly(methyl methacrylate), and poly(2-vinyl pyridine) films supported upon silicon wafers with native oxide coatings. All polymer films showed evidence of high mobility at the free surface. The fraction of a film with high mobility was characterized as a mobile surface layer thickness, which increased with temperature. The mobile surface layer thickness for supported films

A photobleaching technique has been used to measure the reorientation of dilute fluorescent probes in free-standing polymer films from 7 nm to 20 μm thick. Similar to our previous report on free-standing polystyrene films, two subsets of probes with distinct dynamics were observed in free-standing poly(methyl methacrylate) films. The more mobile subset of probes is consistently interpreted in terms of a surface layer, and the thickness of the mobile surface layer is shown to increase with temper

The concept of dynamic heterogeneity and the picture of the supercooled liquid as a mosaic of environments with distinct dynamics that interchange in time have been invoked to explain the nonexponential relaxations measured in these systems. The spatial extent and temporal persistence of these regions of distinct dynamics have remained challenging to identify. Here, single-molecule fluorescence measurements using a probe similar in size and mobility to the host o-terphenyl unambiguously reveal e

In a polymeric material near its glass transition temperature, segmental dynamics of a given spatial region may differ considerably from that of neighboring regions without apparent structural origin, analogous to the supercooled liquid state of low molecular weight glass formers. Given that the supercooled liquid state is a (metastable) equilibrium state, spatial variations in dynamics are expected to average out in time, consistent with ergodicity of the system. By probing the rotations of flu

Much of the interesting behavior that has been observed in supercooled liquids appears to be related to dynamic heterogeneity, the presence of distinct dynamic environments - with no apparent underlying structural basis - in these systems. To most directly interrogate these environments, proposed to span regions just a few nanometers across, molecular length scale probes are required. Single molecule fluorescent microscopy was introduced to the field a decade ago and has provided strong evidence

A temperature-ramping anisotropy measurement is introduced as an efficient way to study molecular motion in polymer glasses. For these experiments, fluorescent molecules were dispersed in the polymer glass and the reorientation of these dyes was used as a probe of segmental dynamics. For thick samples of polystyrene, poly (4-tert-butyl styrene), and poly(2-vinyl pyridine), temperature-ramping anisotropy measurements have a shape similar to differential scanning calorimetry measurements and nearl

Since the chemical and thermal stability of organic thin film layers in organic light-emitting diodes (OLEDs) highly influences the operational device lifetime, a rational advanced design of materials and device structures is quite necessary. Here, we report a significant improvement in the device thermal stability and operational lifetime of blue-fluorescent OLEDs by adopting a mixed electron transporting layer (mETL) of 4,7-diphenyl-1,10-phenanthroline (BPhen) and hydroxyquinolinolato-lithium

Metal-organic frameworks (MOFs) based on Cu-benzene tricarboxylate (CuBTC) are widely used for gas storage and removal applications. However, they readily lose their crystal structures under humid conditions, limiting their practical applications. This structural decomposition reduces the specific surface area, gas adsorption capability, and recyclability of CuBTC considerably. In this study, a stable MOF against water exposure was designed based on FeBTC nanoparticle-covered CuBTC (FeCuBTC). A

Abstract Rotational-translational decoupling, in which translational motion is apparently enhanced over rotational motion in violation of Stokes-Einstein (SE) and Debye-Stokes-Einstein (DSE) predictions, has been observed in materials near their glass transition temperatures (T g ). This has been posited to result from ensemble averaging in the context of dynamic heterogeneity. In this work, ensemble and single molecule experiments are performed in parallel on a fluorescent probe in high molecul

How tethered probes report dynamics of host polymers near the glass transition was investigated by changing the length of the flexible linkers and the number of tethering points via imaging rotational fluorescence correlation microscopy and compared with free probes of different sizes. The results show that tethering did not alter the temperature-dependence of polymer dynamics and the shape of the correlation decay reported by the probe; however, the rotation slowed down up to ≈1 decade when bot

A photobleaching method was used to measure the reorientation of dilute probes in liquid o-terphenyl near a crystal growth front. Near the glass-transition temperature Tg, mobility in the supercooled liquid was enhanced within ∼10 μm of the crystal growth front, by as much as a factor of 4. This enhanced mobility appears to be caused by tension created in the sample as a result of the density difference between the supercooled liquid and crystal. The maximum observed mobility enhancement corresp

Using extrinsic probes to study a host system relies on the probes’ ability to accurately report the host properties under study. Probes have long been used to characterize dynamic heterogeneity, the phenomenon in which a liquid near its glass transition exhibits distinct dynamics as a function of time and position, with molecules within nanometers of each other exhibiting dynamics that may vary by orders of magnitude. The spatial and temporal characteristics of dynamic heterogeneity demand the