Knowledge of the refractive index of water in the deeply supercooled metastable liquid state is important, for example, for an accurate description of optical reflection and refraction processes occurring in clouds. However, a measurement of both the temperature and wavelength dependence of the refractive index under such extreme conditions is challenging. Here, we employ Raman spectroscopy in combination with microscopic water jets in vacuum to obtain the refractive index of supercooled water to a lowest temperature of 230.3 K. While our approach is based on the analysis of Mie resonances in Raman spectra measured by using a single excitation wavelength at 532 nm, it allows us to obtain the refractive index in a wide visible wavelength range from 534 to 675 nm. Because of a direct link between the refractive index and density of water, our results provide a promising approach to help improve our understanding of water's anomalous behavior.
Crystallization is a fundamental process in materials science, providing the primary route for the realization of a wide range of new materials. Crystallization rates are also considered to be useful probes of glass-forming ability1-3. At the microscopic level, crystallization is described by the classical crystal nucleation and growth theories4,5, yet in general solid formation is a far more complex process. In particular, the observation of apparently different crystal growth regimes in many binary liquid mixtures greatly challenges our understanding of crystallization1,6-12. Here, we study by experiments, theory and computer simulations the crystallization of supercooled mixtures of argon and krypton, showing that crystal growth rates in these systems can be reconciled with existing crystal growth models only by explicitly accounting for the non-ideality of the mixtures. Our results highlight the importance of thermodynamic aspects in describing the crystal growth kinetics, providing a substantial step towards a more sophisticated theory of crystal growth.
Wave-particle duality is an inherent peculiarity of the quantum world. The double-slit experiment has been frequently used for understanding different aspects of this fundamental concept. The occurrence of interference rests on the lack of which-way information and on the absence of decoherence mechanisms, which could scramble the wave fronts. Here, we report on the observation of two-center interference in the molecular-frame photoelectron momentum distribution upon ionization of the neon dimer by a strong laser field. Postselection of ions, which are measured in coincidence with electrons, allows choosing the symmetry of the residual ion, leading to observation of both, gerade and ungerade, types of interference.
X-ray spectroscopy is a method, ideally suited for investigating the electronic structure of matter, which has been enabled by the rapid developments in light sources and instruments. The x-ray fluorescence lines of life-relevant elements such as carbon, nitrogen, and oxygen are located in the soft x-ray regime and call for suitable spectrometer devices. In this Letter, we present a high-resolution spectrum of liquid water, recorded with a soft x-ray spectrometer based on a reflection zone plate (RZP) design. The RZP-based spectrometer with meridional variation of line space density from 2953 to 3757 l/mm offers extremely high detection efficiency and, at the same time, medium energy resolution. We can reproduce the well-known splitting of liquid water in the lone pair regime with 10 s acquisition time.
This corrects the article DOI: 10.1103/PhysRevLett.120.015501.
The fast evaporative cooling of micrometer-sized water droplets in a vacuum offers the appealing possibility to investigate supercooled water-below the melting point but still a liquid-at temperatures far beyond the state of the art. However, it is challenging to obtain a reliable value of the droplet temperature under such extreme experimental conditions. Here, the observation of morphology-dependent resonances in the Raman scattering from a train of perfectly uniform water droplets allows us to measure the variation in droplet size resulting from evaporative mass losses with an absolute precision of better than 0.2%. This finding proves crucial to an unambiguous determination of the droplet temperature. In particular, we find that a fraction of water droplets with an initial diameter of 6379±12 nm remain liquid down to 230.6±0.6 K. Our results question temperature estimates reported recently for larger supercooled water droplets and provide valuable information on the hydrogen-bond network in liquid water in the hard-to-access deeply supercooled regime.
Quantum tunneling is a ubiquitous phenomenon in nature and crucial for many technological applications. It allows quantum particles to reach regions in space which are energetically not accessible according to classical mechanics. In this "tunneling region," the particle density is known to decay exponentially. This behavior is universal across all energy scales from nuclear physics to chemistry and solid state systems. Although typically only a small fraction of a particle wavefunction extends into the tunneling region, we present here an extreme quantum system: a gigantic molecule consisting of two helium atoms, with an 80% probability that its two nuclei will be found in this classical forbidden region. This circumstance allows us to directly image the exponentially decaying density of a tunneling particle, which we achieved for over two orders of magnitude. Imaging a tunneling particle shows one of the few features of our world that is truly universal: the probability to find one of the constituents of bound matter far away is never zero but decreases exponentially. The results were obtained by Coulomb explosion imaging using a free electron laser and furthermore yielded He2's binding energy of [Formula: see text] neV, which is in agreement with most recent calculations.
Quantum theory dictates that upon weakening the two-body interaction in a three-body system, an infinite number of three-body bound states of a huge spatial extent emerge just before these three-body states become unbound. Three helium (He) atoms have been predicted to form a molecular system that manifests this peculiarity under natural conditions without artificial tuning of the attraction between particles by an external field. Here we report experimental observation of this long-predicted but experimentally elusive Efimov state of (4)He3 by means of Coulomb explosion imaging. We show spatial images of an Efimov state, confirming the predicted size and a typical structure where two atoms are close to each other while the third is far away.
We present real-time measurements of the crystallization process occurring in liquid para-hydrogen (para-H(2)) quenched to ≈0.65T(m) (T(m)=13.8 ââK is the melting point of bulk liquid para-H(2)). The combination of high spatial resolution Raman spectroscopy and liquid microjet generation allows, in situ, capturing structural changes with â¼10(-8) s time resolution. Our results provide a crystal growth rate that rules out a thermally activated freezing process and reveal that the quenched melt freezes into a metastable polymorph, which undergoes a structural transition. The achieved temporal control offers new opportunities for exploring the elementary processes of nonequilibrium phase transformations in supercooled liquids.
We present a laser driven soft x-ray source based on a novel solid argon filament. The continuously flowing micron-sized filament (diameter approximately 56 microm, flow speed approximately 5 mms) was used as a laser target in order to generate a plasma source of high brightness in the "water window" (2.2-4.4 nm) spectral range. The emission properties of the source were characterized in detail with respect to crucial parameters such as positional and energy stability using an extreme ultraviolet (XUV) sensitive pinhole camera and an XUV spectrometer. The results are compared with an argon plasma based on a gas puff target operated under the same experimental conditions showing an increase of the brilliance by a factor of 84. By changing the capillary geometry from a constant diameter to a convergent shape the flow speed of the filament was significantly increased up to 250 mms, facilitating the operation at higher repetition rates.
Argon/chemistry , Electrodes , Heating/instrumentation , Lasers , Spectrophotometry, Ultraviolet/instrumentation , Equipment Design , Equipment Failure Analysis , Heating/methods , Reproducibility of Results , Sensitivity and Specificity , Spectrophotometry, Ultraviolet/methods , X-Rays
Small weakly bound boson-fermion 4He(m) 3He(n) clusters formed in a free jet expansion are identified using nondestructive transmission grating diffraction. The observations confirm the existence of more than 11 very tenuous complexes including the three-body halo molecule 4He2 3He and the pseudo-Borromean complex 4He2 3He2. Effective cluster formation temperatures, extracted from a sudden freeze model for cluster growth using theoretical binding energies, increase smoothly with cluster size, thereby confirming the calculations with the possible exception of 4He2 3He2.
The total cross sections of the helium dimer, trimer, and tetramer for scattering from Kr atoms have been measured for cluster beam velocities between 250 and 820 m/s. The dimer cross section is twice that of the atom within 5% indicating that the Kr atoms scatter from the He atoms independently, which is consistent with the large dimer bond distance of about 50 A. The trimer and tetramer cross sections are somewhat larger and can be described by an impulse approximation with a multiple "eclipse" correction, extending ideas of Glauber for high energy collisions with the deuteron.
The HeH2 van der Waals complex has been identified in a molecular beam produced by a cryogenic (T0=24.7 K) free jet expansion of a 1% H2 mixture in 99% 4He gas. The weakly bound HeH2 complexes in the beam are identified via their first order diffraction angles after passing through a 100 nm period transmission grating. An electron impact mass spectrometer analysis of the diffraction patterns is used to discriminate against ion fragments of the constituent gas clusters.
The size distributions of neutral 4He clusters in cryogenic jet beams, analyzed by diffraction from a 100 nm period transmission grating, reveal magic numbers at N=10-11, 14, 22, 26-27, and 44 atoms. Whereas magic numbers in nuclei and clusters are attributed to enhanced stabilities, this is not expected for quantum fluid He clusters on the basis of numerous calculations. These magic numbers occur at threshold sizes for which the quantized excitations calculated with the diffusion Monte Carlo method are stabilized, thereby providing the first experimental confirmation for the energy levels of 4He clusters.
