Raman scattering under extreme conditions

Raman scattering is a versatile and powerful technique and has been widely used in modern scientific research and vast industrial applications. It is one of the fundamental experimental techniques in condensed matter physics, since it can sensitively probe the basic elementary excitations in solids like electron, phonon, magnon, etc. The application of extreme conditions(low temperature, high magnetic field, high pressure, etc.) to Raman scattering, will push its capability up to an unprecedented level, because this enables us to look into new quantum phases driven by extreme conditions, trace the evolution of the excitations and their coupling, and hence uncover the underlying physics. This review contains two topics.In the first part, we will introduce the Raman facility under extreme conditions, belonging to the optical spectroscopy station of Synergetic Extreme Condition User Facilities(SECUF), with emphasis on the system design and the capability the facility can provide. Then in the second part we will focus on the applications of Raman scattering under extreme conditions to a variety of condensed matter systems such as superconductors, correlated electron systems, charge density waves(CDW) materials, etc. Finally, as a rapidly developing technique, time-resolved Raman scattering will be highlighted here.     

Space plasma under extreme conditions

Attributes of extreme conditions in space and the new properties which plasma acquires in this case are discussed. The discussion is focussed on the features of interaction between plasma and radiation in strong magnetic fields of degenerate stars—white dwarfs or neutron stars. The specific role of cyclotron scattering, radiation pressure at cyclotron frequencies, and vacuum birefringence in the formation of plasma envelopes and the observed spectra of these objects is pointed out. The contents of this paper provided the basis for the report at the scientific session of the General Physics and Astronomy Division of the Russian Academy of Sciences devoted to the eightieth anniversary of Vitaly L. Ginzburg. Institute of Applied Physics, Russian Academy of Sciences, Nizhny Novgorod; Max Plank Institut für Extraterrestrische Physik, Garching, Germany. Translated from Izvestiya Vysshikh Uchebnykh Zavedenii, Radiofizika, Vol. 40, Nos. 1–2, pp. 17–36, January–February, 1997.     

Radiation-induced decomposition of explosives under extreme conditions

We present high-pressure and high temperature studies of the synchrotron radiation-induced decomposition of powder secondary high explosives pentaerythritol tetranitrate (PETN) and 1,3,5-triamino-2,4,6-trinitrobenzene (TATB) using white beam synchrotron radiation at the 16 BM-B and 16 BM-D sectors of the HP-CAT beamline at the Advanced Photon Source. The radiation-induced decomposition rate TATB showed dramatic slowing with pressure up to 26.6 GPa (the highest pressure studied), implying a positive activation volume of the activated complex. The decomposition rate of PETN varied little with pressure up to 15.7 GPa (the highest pressure studied). Diffraction line intensities were measured as a function of time using energy-dispersive methods. By measuring the decomposition rate as a function of pressure and temperature, kinetic and other constants associated with the decomposition reactions were extracted.     

Biomolecular self-assembly under extreme Martian mimetic conditions

The recent discovery of subsurface water on Mars has challenged our understanding of the natural limits of life. The presence of magnesium perchlorate (Mg(ClO₄)₂) on the Martian surface raises the possibility that it may also be present in this subsurface lake. Given that the subsurface lakes on Earth, such as Lake Vostok and Lake Whillans, are capable of harbouring surprising amounts of life, these new findings raise interesting possibilities for how biomolecules might self-assemble in this environment on Mars. Here we investigate the self-association and hydration of the amino acid glycine in aqueous Mg(ClO₄)₂ at 25°C and ?20°C using neutron diffraction with hydrogen isotope substitution and subsequent analysis with empirical potential structure refinement to yield a simulated box of atoms consistent with the scattering data. We find that although the highly chaotropic properties of Mg(ClO₄)₂ disrupt the hydration and hydrogen bonding ability of the amino acid, as well as the bulk water structure, glycine molecules are nonetheless still able to self-associate. This occurs more readily at lower temperature, where clusters of up to three molecules are observed, allowing us to speculate that the formation of biological molecules is possible in the Martian environment.     

Measurement-based entanglement under conditions of extreme photon loss

The act of measuring optical emissions from two remote qubits can entangle them. By demanding that a photon from each qubit reaches the detectors, one can ensure that no photon was lost. But retaining both photons is rare when loss rates are high, as in Moehring et al. where 30 successes occurred per 10(9) attempts. We describe a means to exploit the low grade entanglement heralded by the detection of a lone photon: A subsequent perfect operation is quickly achieved by consuming this noisy resource. We require only two qubits per node, and can tolerate both path length variation and loss asymmetry. The impact of photon loss upon the failure rate is then linear; realistic high-loss devices can gain orders of magnitude in performance and thus support quantum computing.     

RIXS in correlated electron systems under extreme conditions

ABSTRACT

We report here on the application of Resonant Inelastic X-ray Scattering (RIXS) in correlated electrons systems under pressure. Thanks to its bulk sensitivity and superior resolving power, RIXS appears as a powerful spectroscopic technique to unravel the local electronic and magnetic properties of materials at extreme conditions. The method is illustrated in vanadium-oxides- and Fe-based superconductors at high pressure.     

Behavior of nuclear matter under extreme conditions in fission

The spontaneous fission of ²⁵²Cf has been studied via γ-γ-γ coincidence and γ-γ light charged particle coincidence with Gammasphere. The binary fission yields of correlated Mo?Ba pairs with 0–10 neutron emission have been remeasured. The existence of “hot” fission mode with 8–10 neutron emission seen previously in the Mo?Ba split is confirmed but with lower intensities. By gating on the light charged particles detected in ΔE-E detectors and a γ ray in one partner, the relative yields of correlated pairs in alpha ternary SF with zero to 6n emission are observed for the first time with the distribution peaked at 2.5n. New correlated pairs are identified in ¹⁰Be ternary SF. We observed essentially only cold, On ¹⁰Be and little, if any, hot, xn ¹⁰Be. New γ-γ-γ data with 2.3 times the total events show weak non-Doppler broadened high energy peaks in coincidence with transitions in correlated pairs in ¹⁰Be SF shifted by the same 6,1 to 26 keV from the 2-0 energy in ¹⁰Be as seen earlier.     

Thresholds and hysteresis of surface ionization under nonuniform conditions

The influence of nonuniformity of the atom arrival rate, of the emitter temperature and of the adsorption properties of its surface on characteristics of thresholds and hysteresis of the surface ionization is analyzed. It is shown that, unlike the uniform conditions, in the threshold zone the ion current changes with the emitter temperature monotonically and not in a form of a jump ; the width of hysteresis is substantially diminished ; the slope of the first threshold curve is not obligatory equal to the heat of ion adsorption; for a polycrystalline surface the critical temperature for hysteresis to vanish is related to the minimum work function and not to the effective work function.     

Experimental system for X-ray magnetic diffraction under extreme conditions

An experimental system for X-ray magnetic diffraction (XMD) under extreme conditions was constructed on the beamline BL39XU at SPring-8. This system aims at studying magnetic properties of ferromagnets through the measurements of magnetic form factors under the conditions of low temperature (5 K), high magnetic field (6 T) and high pressure (10 GPa). This system consists of a superconducting magnet (SCM), a diamond anvil cell (DAC), a two-axis manipulator for the DAC, a five-axis goniometer for the SCM, and an X-ray polarizer with a phase plate. Details of this system are presented. Experimental results on uranium telluride are shown as a performance test with this instrumentation.     

Thermo-physical properties of body-centered cubic iron-magnesium alloys under extreme conditions

Using density functional theory formulated within the framework of the exact muffin-tin orbitals method, we investigate the thermo-physical properties of body-centered cubic (bcc) iron-magnesium alloys, containing 5 and 10 atomic % Mg, under extreme conditions, at high pressure and high temperature. The temperature effect is taken into account via the Fermi-Dirac distribution of the electrons. We find that at high pressures pure bcc iron is dynamically unstable at any temperature, having a negative tetragonal shear modulus (C^′). Magnesium alloying significantly increases C^′ of Fe, and bcc Fe-Mg alloys become dynamically stable at high temperature. The electronic structure origin of the stabilization effect of Mg is discussed in detail. We show that the thermo-physical properties of a bcc Fe-Mg alloy with 5% Mg agree well with those of the Earth’s inner core as provided by seismic observations.     

Theoretical prediction of the elastic properties of body-centered cubic Fe-Ni-Mg alloys under extreme conditions

Using density functional theory formulated within the framework of the exact muffin-tin orbital method, we investigate the elastic properties of the body-centered cubic Fe_0.85Ni_0.1Mg_0.05 alloy in the conditions at the Earth's inner core. We demonstrate that in this system, the chemical stabilization effect of Mg is significantly larger than that of Ni. We show that the elastic properties of Fe_0.85Ni_0.1Mg_0.05 are in good agreement with those of the Earth's inner core, as given by seismic observations. We find that the excellent mechanical properties of Fe_0.85Ni_0.1Mg_0.05 are primarily due to Mg.     

PRESS-MAG-O: A new facility to probe materials and phenomena under extreme conditions

In the recent years, several experiments performed under high magnetic fields (HMFs), at high pressure (HP) and/or at low temperature (LT) have led to spectacular discoveries in condensed matter. In many new systems, although challenging, it is strategic to perform a magneto-optical analysis, to investigate the phonon behavior in the far infrared (IR) domain. By combining HMF and HP in a wide temperature (T) range to perform concurrently IR magneto-optics and ac-magneto-dynamic experiments, it will be possible to achieve unique information on systems and/or new phenomena, almost impossible to obtain with standard spectroscopic methods. Here we present PRESS-MAG-O, a new facility under construction that will perform HP experiments under HMF in a wide T range. The system is expected to be operational by the end of 2008 and will be tested at SINBAD, the IR synchrotron radiation beamline operational since 2001 at DAΦNE (Double Annular Φ-factory for Nice Experiments), the storage ring of the INFN Frascati National Laboratory (LNF). While for IR experiments an interferometer will be used, for the magneto-dynamic experiments a SQUID magnetometer in the 10 Hz-2 KHz frequency range will be utilized. HP will be applied to samples by a Cu-Be diamond anvil cell (DAC), so that the device will be able to collect FTIR spectra and high harmonic ac susceptibility data in a dc magnetic field up to 8 T and to about 20 GPa in a wide temperature range (4.2-200 K).     

Cavitation intensity of water under practical ultrasonic cleaning conditions

When measuring cavitation during cooling of thermally degassed water cavitation maxima are frequently observed at various temperatures. Relations between this phenomenon and frequency and power of ultrasounds as well as air content in water have been examined. It was found out that the secondary water regassing with air is the reason.     

Multiphoton ionization of molecules under the conditions of strong field-induced perturbation of Rydberg states

Multiphonon ionization of the H₂ molecule under the action of a weak (probe) field, which provides the initial population of the low-lying (working) level, and intense monochromatic linearly polarized radiation is studied. The multiphoton ionization process occurs under the conditions of strong field perturbation of two intermediate Rydberg series, np0(¹Σ _u ⁺ and np2(¹Π_u), of the optical R(0)branch which have different ionization potentials. The series are occupied simultaneously as a result of single-photon absorption by an excited H ₂ ^* molecule in the working state 4s σH′¹Σ _g ⁺ (v=0). As a result of the irregularity in the arrangement of the intermediate levels from a large group of states that are combined in the multiphoton ionization process a sharp and irregular change occurs in the dependence of the shifts and widths Γ_n of the levels on the intensity f of the strong field in a transition from one level to another. It is shown that for field intensities f such that the level widths remain much less than the splitting between the levels (Γ_n≪/n ³) the stabilizing effect (i.e., the field-induced narrowing of the levels as f→∞) in the form Γ_n ∝ 1/f ² (as happens in atoms with a structureless core) is not observed in molecular systems. Zh. éksp. Teor. Fiz. 115, 1987–2000 (June 1999)     

Metal-semiconductor interface in extreme temperature conditions

We present an investigation of electrons’ and phonons’ temperatures in the volume of a semiconductor (or metal) sample and at the interface between metal and semiconductor. Two types of mismatch between electrons’ and phonons’ temperatures take place: at metal-semiconductor interfaces and in the volume of the sample. The temperature mismatch leads to nonlinear terms in expressions for heat and electricity transport. The nonlinear effects should be taken into consideration in the study of electrical and heat transport in composites and in electronic chips.     

Phase transition and chemical decomposition of liquid carbon dioxide and nitrogen mixture under extreme conditions

Thermodynamic and chemical properties of liquid carbon dioxide and nitrogen(CO_(2~–)N_2) mixture under the conditions of extremely high densities and temperatures are studied by using quantum molecular dynamic(QMD) simulations based on density functional theory including dispersion corrections(DFT-D). We present equilibrium properties of liquid mixture for 112 separate density and temperature points, by selecting densities ranging from ρ = 1.80 g/cm~3 to 3.40 g/cm~3 and temperatures from T = 500 K to 8000 K. In the range of our study, the liquid CO_(2~–)N_2 mixture undergoes a continuous transition from molecular to atomic fluid state and liquid polymerization inferred from pair correlation functions(PCFs)and the distribution of various molecular components. The insulator–metal transition is demonstrated by means of the electronic density of states(DOS).     

Local plasma parameters and integral characteristics of a magnetogasdynamic channel under conditions of ionization instability

Results are presented from an experimental investigation of the onset of ionization instability in a disk-shaped Faraday magnetogasdynamic channel attached to a shock tube. The experiments were carried out in a pure inert gas (xenon) without alkaline additives. A relation is found between the integral plasma characteristics of a nonequilibrium magnetogasdynamic channel and the local parameters of a plasma that is unstable against the ionization instability. Mechanisms for amplifying perturbations and increasing the effective conductivity are revealed. It is concluded that these effects stem mainly from the features of three-body recombination in rare gases.