We probe the mechanical response of two supercooled liquids, glycerol and ortho-terphenyl, by conducting rheological experiments at very weak stresses. We find a complex fluid behavior suggesting the gradual emergence of an extended, delicate solidlike network in both materials in the supercooled state-i.e., above the glass transition. This network stiffens as it ages, and very early in this process it already extends over macroscopic distances, conferring all well known features of soft glassy rheology (yieldstress, shear thinning, aging) to the supercooled liquids. Such viscoelastic behavior of supercooled molecular glass formers is difficult to observe because the large stresses in conventional rheology can easily shear-melt the solid-like structure. glass transition ͉ glycerol ͉ ortho-terphenyl ͉ yield-stress
We demonstrate a novel technique to achieve fast thermal cycles of a small sample (a few femtoliters). Modulating a continuous near-infrared laser focused on a metal film, we can drive the local temperature from 130 to 300 K and back, within a few microseconds. By fluorescence microscopy of dyes in a thin glycerol film, we record images of the hot spot, calibrate its temperature, and follow its variations in real time. The temperature dependence of fluorescence anisotropy, due to photophysics and rotational diffusion, gives a steady-state temperature calibration between 200 and 350 K. From 200 to 220 K, we monitor temperature more accurately by fluorescence autocorrelation, a probe for rotational diffusion. Time-resolved measurements of fluorescence anisotropy give heating and cooling times of a few microseconds, short enough to supercool pure water. We designed our method to repeatedly cycle a single (bio)molecule between ambient and cryostat temperatures with microsecond time resolution. Successive measurements of a structurally relevant variable will decompose a dynamical process into structural snapshots. Such temperature-cycle experiments, which combine a high time resolution with long observation times, can thus be expected to yield new insights into complex processes such as protein folding.
Photothermal absorption microscopy of single Au nanoparticles was conducted at temperatures and pressures near the critical point of Xenon (Tc = 16.583 °C, Pc = 5.842 MPa). The divergence of the thermal expansion coefficient at the critical point makes the refractive index highly sensitive to changes in temperature, which directly translates to a large enhancement of the photothermal signal. We find that measurements taken near the critical point of Xe give a signal enhancement factor of up to 440 ± 130 over those taken in glycerol. The highest sensitivity recorded here corresponds to power dissipation of 64 pW, achieving a signal-to-noise ratio of 9.4 for 5 nm Au nanoparticles with an integration time of 50 ms, making this the most sensitive of any absorption microscopy technique reported to date. Enhancing the sensitivity of absorption microscopy lowers the operating heating power, allowing the technique to be more compatible with absorbers with absorption coefficient and photochemical stability lower than that of Au.
We present the design and implementation of a mechanical low-pass filter vibration isolation used to reduce the vibrational noise in a cryogen-free dilution refrigerator operated at 10 mK, intended for scanning probe techniques. We discuss the design guidelines necessary to meet the competing requirements of having a low mechanical stiffness in combination with a high thermal conductance. We demonstrate the effectiveness of our approach by measuring the vibrational noise levels of an ultrasoft mechanical resonator positioned above a SQUID. Starting from a cryostat base temperature of 8 mK, the vibration isolation can be cooled to 10.5 mK, with a cooling power of 113 µW at 100 mK. We use the low vibrations and low temperature to demonstrate an effective cantilever temperature of less than 20 mK. This results in a force sensitivity of less than 500 zN/ √ Hz, and an integrated frequency noise as low as 0.4 mHz in a 1 Hz measurement bandwidth.
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