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Vitaly V. Kresin

Publications and source records attributed to Vitaly V. Kresin.

At least 19 recordsLinked to original sources

Isotope effect in the work function of lithium

The work functions of 7Li and 6Li metals have been measured as a function of temperature, by using photoionization of pure isolated metal nanoparticles in a beam. These data reveal a marked isotope effect in the temperature variation of these work functions. Furthermore, for both isotopes the curvature of this temperature variation is found to be significantly larger than may be ascribed purely to a change in the electron gas density. These findings enhance the characterization of lithium as a quantum material in which the interplay between electronic and ionic degrees of freedom is nontrivial, and call for a microscopic understanding beyond simple models. Additionally, the slope of the work function curves was observed to vanish in the low temperature limit, as had been predicted on the basis of the Third Law of thermodynamics.

cond-mat.mes-hall↗

Photoionization of temperature-controlled nanoparticles in a beam: Accurate and efficient determination of ionization energies and work functions

A beam of free alkali metal nanoparticles is produced by a condensation source, passed through a thermalizing tube adjustable over a broad temperature range, and ionized by tunable light. High stability of the particle flux and an automated data acquisition routine allow efficient collection of photoionization yield curves. A careful fit of the data to the universal Fowler function makes it possible to obtain nanoparticle ionization energies, and from those, the metal work functions, with $\sim$0.2% precision. The experimental arrangement, nanoparticle thermalization rates, and ionization threshold analysis are described in detail. The use of ultrapure and temperature-controlled gas-phase nanoparticles facilitates the analysis of electronic properties, such as work functions, and of their interplay with thermal lattice dynamics.

cond-mat.mes-hall↗

Temperature-dependent photoionization thresholds of alkali-metal nanoparticles reveal thermal expansion and the melting transition

A precision measurement of the photoionization of pure sodium and potassium nanoparticles isolated in a beam enabled an accurate determination of their work functions as a function of temperature. In addition to resolving and quantifying the initial gradual decrease of the work function with temperature, which is associated with thermal expansion, the experiment revealed that the work function then undergoes a distinct drop both in magnitude and in slope that signifies the onset of nanoparticle melting. This establishes that a structural phase transition can be detected via a high-resolution measurement of the photoemission threshold. The melting temperature of nanoparticles with diameters of 7-9 nm is reduced by nearly 100 K relative to the bulk value. This suppression aligns with predictions from the Gibbs-Thomson equation which describes finite-size phase transitions.

cond-mat.mes-hall↗

Stern-Gerlach deflection of cryogenically cold polyatomic molecules in superfluid nanodroplets

Beam deflection is capable of providing valuable information about the magnetic moments of molecules and clusters as well as the relaxation dynamics of their spins. However, observations have been hampered by magnetic couplings to excited vibrational and rotational states of polyatomic systems, which are challenging to control, characterize, and systematize. In this work, we carried out deflection measurements on superfluid helium nanodroplets doped with high-spin FeCl2 and CoCl2 molecules and their complexes. This enabled quantitative determination of the magnetic moments of molecules and clusters at extremely low, and fully defined, temperature of all of their degrees of freedom. The spin magnetic moments become thermalized and oriented along the applied field. Dimers and trimers are found to be antiferromagnetically ordered. The issue of rates and mechanisms of molecular spin relaxation within the cryogenic helium matrix is highlighted.

physics.atm-clus↗

Magnetic deflection of high-spin sodium dimers formed on helium nanodroplets

Spectroscopic data on alkali-atom dimers residing on the surface of liquid helium nanodroplets have revealed that they are detected primarily in the weakly bound, metastable, spin-triplet state. Here, by measuring the magnetic Stern-Gerlach deflection of a sodium-doped nanodroplet beam, we transparently demonstrate the abundance of high-magnetic-moment dimers. Their electron spins thermalize with the cryogenic superfluid droplets and become fully oriented by the external magnetic field.

physics.atm-clus↗

Shift of nanodroplet and nanocluster size distributions induced by dopant pick-up statistics

In pick-up experiments using nanodroplet and nanocluster beams, the size distribution of hosts carrying a specified number of dopants changes when the vapor density in the pick-up region is altered. This change, analyzed here, has quantitative consequences for the interpretation of data that are sensitive to host size, such as mass spectrometric, spectroscopic, and deflection measurements.

physics.atm-clus↗

Substrate-Selective Adhesion of Metal Nanoparticles to Graphene Devices

Nanostructured electronic devices, such as those based on graphene, are typically grown on top of the insulator SiO2. Their exposure to a flux of small size-selected silver nanoparticles has revealed remarkably selective adhesion: the graphene channel can be made fully metallized while the insulating substrate remains coverage-free. This conspicuous contrast derives from the low binding energy between the metal nanoparticles and a contaminant-free passivated silica surface. In addition to providing physical insight into nanoparticle adhesion, this effect may be of value in applications involving deposition of metallic layers on device working surfaces: it eliminates the need for masking the insulating region and the associated extensive and potentially deleterious pre- and postprocessing.

physics.atm-clus↗

Shells in CO$_2$ Clusters

Abundance spectra of (CO$_2$)$_N$ clusters (up to $N \approx$ 500) acquired under a wide range of adiabatic expansion conditions are analyzed within the evaporative ensemble framework. Analysis reveals that cluster stability functions display strikingly universal patterns for all expansion conditions. These patterns reflect the inherent properties of individual clusters. From this analysis the size-dependent cluster binding energies are determined, shell and subshell closing sizes identified, and cuboctahedral packing ordering for sizes above $N \approx 130$ is confirmed. It is demonstrated that a few percent variation in the dissociation energies translates into significant abundance variations, especially for the larger clusters.

physics.atm-clus↗

Probing the presence and absence of metal-fullerene electron transfer reactions in helium nanodroplets by deflection measurements

Metal-fullerene compounds are characterized by significant electron transfer to the fullerene cage, giving rise to an electric dipole moment. We use the method of electrostatic beam deflection to verify whether such reactions take place within superfluid helium nanodroplets between an embedded C$_{60}$ molecule and either alkali (heliophobic) or rare-earth (heliophilic) atoms. The two cases lead to distinctly different outcomes: C$_{60}$Na$_n$ ($n$=1-4) display no discernible dipole moment, while C$_{60}$Yb is strongly polar. This suggests that the fullerene and small alkali clusters fail to form a charge-transfer bond in the helium matrix despite their strong van der Waals attraction. The C$_{60}$Yb dipole moment, on the other hand, is in agreement with the value expected for an ionic complex.

physics.atm-clus↗

Kinetic energy deposited into a nanodroplet, cluster, or molecule in a sticking collision with background gas

In processes when particles such as nanodroplets, clusters, or molecules move through a dilute background gas and undergo capture collisions, it is often important to know how much translational kinetic energy is deposited into the particles by these pick-up events. For sticking collisions with a Maxwell-Boltzmann gas, an exact expression is derived which is valid for arbitrary relative magnitudes of the particle and thermal gas speeds.

physics.atm-clus↗

Electric deflection of imidazole dimers and trimers in helium nanodroplets: Dipole moments, structure, and fragmentation

Deuterated imidazole (IM) molecules, dimers and trimers formed in liquid helium nanodroplets are studied by the electrostatic beam deflection method. Monitoring the deflection profile of (IM)D+ provides a direct way to establish that it is the primary product of the ionization-induced fragmentation both of (IM)2 and (IM)3. The magnitude of the deflection determines the electric dipole moments of the parent clusters: nearly 9 D for the dimer and 14.5 D for the trimer. These very large dipole values confirm theoretical predictions and derive from a polar chain bonding arrangement of the heterocyclic imidazole molecules.

physics.atm-clus↗

Strong permanent magnet gradient deflector for Stern-Gerlach-type experiments on molecular beams

We describe the design, assembly, and testing of a magnet intended to deflect beams of paramagnetic nanoclusters, molecules, and atoms. It is energized by high-grade permanent neodymium magnets. This offers a convenient option in terms of cost, portability, and scalability of the construction, while providing field and gradient values (1.1 T, 330 T/m) which are fully comparable with commonly used electromagnet deflectors.

physics.ins-det↗

Direct detection of polar structure formation in helium nanodroplets by beam deflection measurements

Long-range intermolecular forces are able to steer polar molecules submerged in superfluid helium nanodroplets into highly polar metastable configurations. We demonstrate that the presence of such special structures can be identified, in a direct and determinative way, by electrostatic deflection of the doped nanodroplet beam. The measurement also establishes the structures' electric dipole moments. In consequence, the introduced approach is complementary to spectroscopic studies of low-temperature molecular assembly reactions. It is enabled by the fact that within the cold superfluid matrix the molecular dipoles become nearly completely oriented by the applied electric field. As a result, the massive (tens of thousands of helium atoms) nanodroplets undergo significant deflections. The method is illustrated here by an application to dimers and trimers of dimethyl sulfoxide (DMSO) molecules. We interpret the experimental results with ab initio theory, mapping the potential energy surface of DMSO complexes and simulating their low temperature aggregation dynamics.

physics.atm-clus↗

Oriented polar molecules trapped in cold helium nanodroplets: Electrostatic deflection, size separation, and charge migration

Helium nanodroplets doped with polar molecules are studied by electrostatic deflection. This broadly applicable method allows even polyatomic molecules to attain sub-Kelvin temperatures and nearly full orientation in the field. The resulting intense force from the field gradient strongly deflects even droplets with tens of thousands of atoms, the most massive neutral systems studied by beam "deflectometry." We use the deflections to extract droplet size distributions. Moreover, since each host droplet deflects according to its mass, spatial filtering of the deflected beam translates into size filtering of neutral fragile nanodroplets. As an example, we measure the dopant ionization probability as a function of droplet radius and determine the mean free path for charge hopping through the helium matrix. The technique will enable separation of doped and neat nanodroplets and size-dependent spectroscopic studies.

physics.atm-clus↗

The transparency of graphene and other direct-gap two dimensional materials

Graphene and other two-dimensional materials display remarkable optical properties, including a simple light transparency of $T \approx 1 - πα$ for light in the visible region. Most theoretical rationalizations of this "universal" opacity employ a model coupling light to the electron's crystal momentum and put emphasis on the linear dispersion of the graphene bands. However, such a formulation of interband absorption is not allowable within band structure theory, because it conflates the crystal momentum label with the canonical momentum operator. We show that the physical origin of the optical behavior of graphene can be explained within a straightforward picture with the correct use of canonical momentum coupling. Its essence lies in the two-dimensional character of the density of states rather than in the precise dispersion relation, and therefore the discussion is applicable to other systems such as semiconductor membranes. At higher energies the calculation predicts a peak corresponding to a van Hove singularity as well as a specific asymmetry in the absorption spectrum of graphene, in agreement with previous results.

cond-mat.mes-hall↗

Electrostatic deflection of a molecular beam of massive neutral particles: Fully field-oriented polar molecules within superfluid nanodroplets

Electric deflection measurements on liquid helium nanodroplets doped with individual polar molecules demonstrate that the cold superfluid matrix enables full orientation of the molecular dipole along the external field. This translates into a deflection force which is increased enormously by comparison with typical deflection experiments, and it becomes possible to measurably deflect neutral doped droplets with masses of tens to hundreds of thousands of Daltons. This approach permits preparation and study of continuous fluxes of fully oriented polar molecules and is broadly and generally applicable, including to complex and biological molecules. It is shown that the dipole moments of internally cryogenically cold molecules can be directly determined from a deflection measurement on the doped nanodroplet beam.

physics.atm-clus↗

Spectroscopy of metal "superatom" nanoclusters and high-$T_c$ superconducting pairing

A unique property of metal nanoclusters is the "superatom" shell structure of their delocalized electrons. The electronic shell levels are highly degenerate and therefore represent sharp peaks in the density of states. This can enable exceptionally strong electron pairing in certain clusters composed of tens to hundreds of atoms. In a finite system, such as a free nanocluster or a nucleus, pairing is observed most clearly via its effect on the energy spectrum of the constituent fermions. Accordingly, we performed a photoionization spectroscopy study of size-resolved aluminum nanoclusters and observed a rapid rise of the near-threshold density of states of several clusters ($Al_{37,44,66,68}$) with decreasing temperature. The characteristics of this behavior are consistent with compression of the density of states by a pairing transition into a high-temperature superconducting state with $T_c$>~100 K. This value exceeds that of bulk aluminum by two orders of magnitude. These results highlight the potential of novel pairing effects in size-quantized systems and the possibility to attain even higher critical temperatures by optimizing the particles' size and composition. As a new class of high-temperature superconductors, such metal nanocluster particles are promising building blocks for high-$T_c$ materials, devices, and networks.

cond-mat.supr-con↗

Nanocluster ionization energies and work function of aluminum, and their temperature dependence

Ionization threshold energies of Al$_n$ (n=32-95) nanoclusters are determined by laser ionization of free neutral metal clusters thermalized to several temperatures in the range from 65 K to 230 K. The photoion yield curves of cold clusters follow a quadratic energy dependence above threshold, in agreement with the Fowler law of surface photoemission. Accurate data collection and analysis procedures make it possible to resolve very small (few parts in a thousand) temperature-induced shifts in the ionization energies. Extrapolation of the data to the bulk limit enables a determination of the thermal shift of the polycrystalline metal work function, found to be in excellent agreement with theoretical prediction based on the influence of thermal expansion. Small clusters display somewhat larger thermal shifts, reflecting their greater susceptibility to thermal expansion. Ionization studies of free size-resolved nanoclusters facilitate understanding of the interplay of surface, electronic, and lattice properties under contamination-free conditions.

physics.atm-clus↗