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1.
We report a theoretical study of phase transition kinetics in confined two-dimensional systems, motivated by recent experimental results on the amorphous-to-crystalline transition in supported, thin amorphous water films [E.H.G. Backus, M.L. Grecea, A.W. Kleyn, and M. Bonn, Phys. Rev. Lett. (to be published)]. We generalize and extend existing theories to simultaneously describe the converted (crystalline) fractions in the bulk, at the sample-vacuum surface, and at the sample-support interface as a function of time. The general approach presented here results in expressions for the time-dependent converted bulk, surface, and interface fractions, for arbitrary desorption rate from the thin film, nucleation and growth rates and also includes finite nucleation grain size. The converted bulk, surface, and interface fractions are calculated for nucleation of the new phase occurring (i) in the bulk, (ii) at the support-sample interface, and (iii) at the sample surface (sample-vacuum interface), resulting in nine expressions. The results demonstrate the advantage of monitoring bulk, surface and interface fractions simultaneously to make definite statements regarding the location of the nucleation, and to reliably determine the values of the relevant crystallization parameters. 相似文献
2.
Pulse compression by use of deformable mirrors 总被引:7,自引:0,他引:7
Zeek E Maginnis K Backus S Russek U Murnane M Mourou G Kapteyn H Vdovin G 《Optics letters》1999,24(7):493-495
An electrostatically deformable, gold-coated, silicon nitride membrane mirror was used as a phase modulator to compress pulses from 92 to 15 fs. Both an iterative genetic algorithm and single-step dispersion compensation based on frequency-resolved optical gating calibration of the mirror were used to compress pulses to within 10% of the transform limit. Frequency-resolved optical gating was used to characterize the pulses and to test the range of the deformable-mirror-based compressor. 相似文献
3.
We demonstrate that the crystallization of thin, supported amorphous solid water layers is initiated at the water surface. This is concluded from the observation of sequential crystallization of amorphous water at the surface, in the bulk, and at the water-support interface. A surface nucleation model quantitatively reproduces the observed transformation kinetics at the three sites. 相似文献
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We demonstrate the use of a deformable-mirror pulse shaper, combined with an evolutionary optimization algorithm, to correct high-order residual phase aberrations in a 1-mJ, 1-kHz, 15-fs laser amplifier. Frequency-resolved optical gating measurements reveal that the output pulse duration of 15.2 fs is within our measurement error of the theoretical transform limit. This technique significantly reduces the pulse duration and the temporal prepulse energy of the pulse while increasing the peak intensity by 26%. It is demonstrated, for what is believed to be the first time, that the problem of pedestals in laser amplifiers can be addressed by spectral-domain correction. 相似文献
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Barry CS Backus KM Barry CE Davis BG 《Journal of the American Chemical Society》2011,133(34):13232-13235
Mycobacterium tuberculosis Antigen 85 enzymes are vital to the integrity of the highly impermeable cell envelope and are potential therapeutic targets. Kinetic analysis using a label-free assay revealed both mechanistic details and a substrate profile that allowed the design and construction of a selective in vitro mechanism-based inhibitor. 相似文献
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9.
Jene D. Cyran Ellen H. G. Backus Marc‐Jan vanZadel Mischa Bonn 《Angewandte Chemie (International ed. in English)》2019,58(11):3620-3624
Small organic molecules on ice and water surfaces are ubiquitous in nature and play a crucial role in many environmentally relevant processes. Herein, we combine surface‐specific vibrational spectroscopy and a controllable flow cell apparatus to investigate the molecular adsorption of acetone onto the basal plane of single‐crystalline hexagonal ice with a large surface area. By comparing the adsorption of acetone on the ice/air and the water/air interface, we observed two different types of acetone adsorption, as apparent from the different responses of both the free O?H and the hydrogen‐bonded network vibrations for ice and liquid water. Adsorption on ice occurs preferentially through interactions with the free OH group, while the interaction of acetone with the surface of liquid water appears less specific. 相似文献
10.
Sudipta Das Mischa Bonn Ellen H. G. Backus 《Angewandte Chemie (International ed. in English)》2019,58(44):15636-15639
The behavior of hydroxide and hydrated protons, the auto‐ionization products of water, at surfaces is important for a wide range of applications and disciplines. However, it is unknown at which bulk concentration these ions start to become surface active at the water–air interface. Here, we report changes in the D2O–air interface in the presence of excess D+hyd/OD?hyd determined using surface‐sensitive vibrational sum‐frequency generation (SFG) spectroscopy. The onset of the perturbation of the D2O surface occurs at a bulk concentration as low as 2.7±0.2 mm D+hyd. In contrast, a concentration of several hundred mm OD?hyd is required to change the D2O surface. The hydrated proton is thus orders of magnitude more surface‐active than hydroxide at the water–air interface. 相似文献