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1.
Phys Chem Chem Phys ; 25(21): 14836-14847, 2023 May 31.
Artigo em Inglês | MEDLINE | ID: mdl-37198941

RESUMO

To understand the mechanism underlying the high radio-sensitisation of living cells possessing brominated genomic DNA, X-ray photoelectron spectroscopy (XPS) using synchrotron X-rays with energies of 2000 or 2500 eV was used to study brominated and nonbrominated nucleobases, nucleosides and nucleotides. The bromine atom significantly reduced the energy gap between the valence and conduction states, although the core level states were not greatly affected. This finding was supported by quantum chemical calculation for the nucleobases and nucleosides. Our findings strongly indicate that the energy gaps between the valence and conduction levels of the molecules are significantly reduced by bromination. Furthermore, the brominated molecules are more likely to produce inelastic scattering low energy electrons upon exposure to 2000 or 3000 eV X-rays. This modification of electronic properties around the brominated group may both facilitate electron transfer to the brominated site in DNA and increase the probability of reaction with low energy electrons. These processes can induce DNA damage, presumably resulting in debromination of the uracil moiety and a subsequent cytotoxic effect.


Assuntos
Bromo , DNA , DNA/química , Uracila/química , Dano ao DNA
2.
Phys Rev Lett ; 121(23): 237001, 2018 Dec 07.
Artigo em Inglês | MEDLINE | ID: mdl-30576177

RESUMO

We have measured magnetization at high pressure in the uranium ferromagnetic superconductor UGe_{2} and analyzed the magnetic data using Takahashi's spin fluctuation theory. There is a peak in the pressure dependence of the width of the spin fluctuation spectrum in the energy space T_{0} at P_{x}, the phase boundary of FM1 and FM2 where the superconducting transition temperature T_{sc} is highest. This suggests a clear correlation between the superconductivity and pressure-enhanced magnetic fluctuations developed at P_{x}. The pressure effect on T_{Curie}/T_{0}, where T_{Curie} is the Curie temperature, suggests that the less itinerant ferromagnetic state FM2 is changed to a more itinerant one FM1 across P_{x}. Peculiar features in relations between T_{0} and T_{sc} in uranium ferromagnetic superconductors UGe_{2}, URhGe, and UCoGe are discussed in comparison with those in high-T_{c} cuprate and heavy fermion superconductors.

3.
Phys Rev Lett ; 114(14): 147002, 2015 Apr 10.
Artigo em Inglês | MEDLINE | ID: mdl-25910153

RESUMO

Low-energy quasiparticle excitations in the superconducting (SC) state of UBe_{13} were studied by means of specific-heat (C) measurements in a rotating field. Quite unexpectedly, the magnetic-field dependence of C(H) is linear in H with no angular dependence at low fields in the SC state, implying that the gap is fully open over the Fermi surfaces, in stark contrast to previous expectations. In addition, a characteristic cubic anisotropy of C(H) was observed above 2 T with a maximum (minimum) for H∥[001] ([111]) within the (11[over ¯]0) plane, in the normal as well as in the SC states. This oscillation possibly originates from the anisotropic response of the heavy quasiparticle bands, and might be a key to understand the unusual properties of UBe_{13}.

4.
Sci Adv ; 10(6): eadk3772, 2024 Feb 09.
Artigo em Inglês | MEDLINE | ID: mdl-38324692

RESUMO

The recently discovered superconductor UTe2 is a promising candidate for spin-triplet superconductors, but the symmetry of the superconducting order parameter remains highly controversial. Here, we determine the superconducting gap structure by the thermal conductivity of ultraclean UTe2 single crystals. We find that the a-axis thermal conductivity divided by temperature κ/T in zero-temperature limit is vanishingly small for both magnetic field H‖a and H‖c axes up to H/Hc2 ∼ 0.2, demonstrating the absence of nodes around the a axis contrary to the previous belief. The present results, combined with the reduction of nuclear magnetic resonance Knight shift, indicate that the superconducting order parameter belongs to the isotropic Au representation with a fully gapped pairing state, analogous to the B phase of superfluid 3He. These findings reveal that UTe2 is likely to be a long-sought three-dimensional strong topological superconductor, hosting helical Majorana surface states on any crystal plane.

5.
Int J Radiat Biol ; 99(1): 82-88, 2023.
Artigo em Inglês | MEDLINE | ID: mdl-32720858

RESUMO

PURPOSE: To clarify the radiosensitization mechanism masking the Auger effect of the cells possessing brominated DNA, the electronic properties of DNA-related molecules containing Br were investigated by X-ray spectroscopy and specific heat measurement. MATERIALS AND METHODS: X-ray absorption near-edge structure (XANES) and X-ray photoemission spectroscopy (XPS) were used to measure the electronic properties of the nucleotides with and without Br. We determined the specific heat of 5-bromouracil crystals with thymine as a reference molecule at low temperatures of 3-48 K to calculate the microscopic state numbers. RESULTS: Obtained XANES and XPS spectra indicated that both the lowest unoccupied molecular orbital (LUMO) and the core-levels were not affected by the Br incorporation. The state numbers of 5-bromouracil calculated from the specific heats obtained around 25 K was about 1.5 times larger than that for thymine below 20 K, although the numbers were almost the same below 5 K. DISCUSSION: Our results suggest that the Br atom may not contribute substantially to the LUMO and core-level electronic states of the molecule, but rather to the microscopic states related to the excitation of lattice vibrations, which may be involved in valence electronic states.


Assuntos
Bromo , Timina , Bromouracila , DNA
6.
Nat Commun ; 14(1): 2966, 2023 May 23.
Artigo em Inglês | MEDLINE | ID: mdl-37221184

RESUMO

Chiral spin-triplet superconductivity is a topologically nontrivial pairing state with broken time-reversal symmetry, which can host Majorana quasiparticles. The heavy-fermion superconductor UTe2 exhibits peculiar properties of spin-triplet pairing, and the possible chiral state has been actively discussed. However, the symmetry and nodal structure of its order parameter in the bulk, which determine the Majorana surface states, remains controversial. Here we focus on the number and positions of superconducting gap nodes in the ground state of UTe2. Our magnetic penetration depth measurements for three field orientations in three crystals all show the power-law temperature dependence with exponents close to 2, which excludes single-component spin-triplet states. The anisotropy of low-energy quasiparticle excitations indicates multiple point nodes near the ky- and kz-axes in momentum space. These results can be consistently explained by a chiral B3u + iAu non-unitary state, providing fundamentals of the topological properties in UTe2.

7.
Phys Rev Lett ; 109(21): 217001, 2012 Nov 21.
Artigo em Inglês | MEDLINE | ID: mdl-23215607

RESUMO

We have performed precise dc magnetization measurements for a single crystal of UBe(13) down to 0.14 K, up to 80 kOe. We observed a magnetic anomaly in the superconducting (SC) mixed state at a field, named H(Mag)(*) (~ 26 kOe, at 0.14 K), implying that UBe(13) has a magnetically unusual SC state. We studied the magnetization curves of UBe(13), assuming that the H(Mag)(*) anomaly originates from (1) and unusual SC diamagnetic response, or (2) a peculiarity of the normal-state magnetization due to vortices in the SC mixed state. The origin of the H(Mag)(*) anomaly is discussed.

8.
Sci Adv ; 3(9): eaao0362, 2017 09.
Artigo em Inglês | MEDLINE | ID: mdl-28948229

RESUMO

Orbital-related physics attracts growing interest in condensed matter research, but direct real-space access of the orbital degree of freedom is challenging. We report a first, real-space, imaging of a surface-assisted orbital ordered structure on a cobalt-terminated surface of the well-studied heavy fermion compound CeCoIn5. Within small tip-sample distances, the cobalt atoms on a cleaved (001) surface take on dumbbell shapes alternatingly aligned in the [100] and [010] directions in scanning tunneling microscopy topographies. First-principles calculations reveal that this structure is a consequence of the staggered d xz -d yz orbital order triggered by enhanced on-site Coulomb interaction at the surface. This so far overlooked surface-assisted orbital ordering may prevail in transition metal oxides, heavy fermion superconductors, and other materials.

9.
J Phys Condens Matter ; 28(42): 425601, 2016 10 26.
Artigo em Inglês | MEDLINE | ID: mdl-27541709

RESUMO

We succeeded in growing a new high quality single crystal of a ternary uranium compound UPd2Cd20. From the electrical resistivity, magnetization, magnetic susceptibility, and specific heat experiments, UPd2Cd20 is found to be an antiferromagnetic heavy-fermion compound with the Néel temperature [Formula: see text] = 5 K and exhibits the large electronic specific heat coefficient γ exceeding 500 mJ (K(2)· mol)(-1). This compound is the first one that exhibits the magnetic ordering with the magnetic moments of the U atom in a series of UT2X20 (T: transition metal, X = Al, Zn, Cd). UPd2Cd20 shows typical characteristic features in heavy-fermion systems such as a broad maximum in the magnetic susceptibility at [Formula: see text] and a large coefficient A of T (2) term in the resistivity.

10.
Rev Sci Instrum ; 84(4): 046105, 2013 Apr.
Artigo em Inglês | MEDLINE | ID: mdl-23635239

RESUMO

Two modifications have been made to a miniature ceramic anvil high pressure cell (mCAC) designed for magnetic measurements at pressures up to 12.6 GPa in a commercial superconducting quantum interference (SQUID) magnetometer [N. Tateiwa et al., Rev. Sci. Instrum. 82, 053906 (2011); ibid. 83, 053906 (2012)]. Replacing the Cu-Be piston in the former mCAC with a composite piston composed of the Cu-Be and ceramic cylinders reduces the background magnetization significantly smaller at low temperatures, enabling more precise magnetic measurements at low temperatures. A second modification to the mCAC is the utilization of a ceramic anvil with a hollow in the center of the culet surface. High pressures up to 5 GPa were generated with the "cupped ceramic anvil" with the culet size of 1.0 mm.

11.
J Phys Condens Matter ; 25(29): 296002, 2013 Jul 24.
Artigo em Inglês | MEDLINE | ID: mdl-23803419

RESUMO

We have investigated quadrupole effects in tetragonal crystals of PrCu2Si2 and DyCu2Si2 by means of low-temperature ultrasonic measurements. The elastic constant C44 of PrCu2Si2 exhibits pronounced softening below 70 K down to a Néel temperature TN = 20 K, which is described in terms of a quadrupole susceptibility for a Γ5 doublet ground state and a Γ3 singlet first excited state located at 15.6 K in the crystalline electric field scheme. The C44 and C66 of DyCu2Si2 also show softening below 70 K down to TN1 = 9.7 K. A low-lying pseudo-sextet state consisting of three Kramers doublets of Γ6⊕2Γ7 brings about softening of C44 and C66 in DyCu2Si2.


Assuntos
Complexos de Coordenação/química , Cobre/química , Disprósio/química , Modelos Químicos , Praseodímio/química , Teoria Quântica , Silício/química , Cristalização
12.
Rev Sci Instrum ; 83(5): 053906, 2012 May.
Artigo em Inglês | MEDLINE | ID: mdl-22667632

RESUMO

A miniature ceramic anvil high pressure cell (mCAC) was earlier designed by us for magnetic measurements at pressures up to 7.6 GPa in a commercial superconducting quantum interference magnetometer [N. Tateiwa et al., Rev. Sci. Instrum. 82, 053906 (2011)]. Here, we describe methods to generate pressures above 10 GPa in the mCAC. The efficiency of the pressure generation is sharply improved when the Cu-Be gasket is sufficiently preindented. The maximum pressure for the 0.6 mm culet anvils is 12.6 GPa when the Cu-Be gasket is preindented from the initial thickness of 300-60 µm. The 0.5 mm culet anvils were also tested with a rhenium gasket. The maximum pressure attainable in the mCAC is about 13 GPa. The present cell was used to study YbCu(2)Si(2) which shows a pressure induced transition from the non-magnetic to magnetic phases at 8 GPa. We confirm a ferromagnetic transition from the dc magnetization measurement at high pressure. The mCAC can detect the ferromagnetic ordered state whose spontaneous magnetic moment is smaller than 1 µ(B) per unit cell. The high sensitivity for magnetic measurements in the mCAC may result from the simplicity of cell structure. The present study shows the availability of the mCAC for precise magnetic measurements at pressures above 10 GPa.

13.
Rev Sci Instrum ; 82(5): 053906, 2011 May.
Artigo em Inglês | MEDLINE | ID: mdl-21639517

RESUMO

A miniature opposed-anvil high-pressure cell has been developed for magnetic measurement in a commercial superconducting quantum interference device magnetometer. Non-magnetic anvils made of composite ceramic material were used to generate high-pressure with a Cu-Be gasket. We have examined anvils with different culet sizes (1.8, 1.6, 1.4, 1.2, 1.0, 0.8, and 0.6 mm). The pressure generated at low temperature was determined by the pressure dependence of the superconducting transition of lead (Pb). The maximum pressure P(max) depends on the culet size of the anvil: the values of P(max) are 2.4 and 7.6 GPa for 1.8 and 0.6 mm culet anvils, respectively. We revealed that the composite ceramic anvil has potential to generate high-pressure above 5 GPa. The background magnetization of the Cu-Be gasket is generally two orders of magnitude smaller than the Ni-Cr-Al gasket for the indenter cell. The present cell can be used not only with ferromagnetic and superconducting materials with large magnetization but also with antiferromagnetic compounds with smaller magnetization. The production cost of the present pressure cell is about one tenth of that of a diamond anvil cell. The anvil alignment mechanism is not necessary in the present pressure cell because of the strong fracture toughness (6.5 MPa m(1∕2)) of the composite ceramic anvil. The simplified pressure cell is easy-to-use for researchers who are not familiar with high-pressure technology. Representative results on the magnetization of superconducting MgB(2) and antiferromagnet CePd(5)Al(2) are reported.

14.
Rev Sci Instrum ; 80(12): 123901, 2009 Dec.
Artigo em Inglês | MEDLINE | ID: mdl-20059148

RESUMO

The fourteen kinds of pressure-transmitting media were evaluated by the ruby fluorescence method at room temperature, 77 K using the diamond anvil cell (DAC) up to 10 GPa in order to find appropriate media for use in low temperature physics. The investigated media are a 1:1 mixture by volume of Fluorinert FC-70 and FC-77, Daphne 7373 and 7474, NaCl, silicon oil (polydimethylsiloxane), Vaseline, 2-propanol, glycerin, a 1:1 mixture by volume of n-pentane and isopentane, a 4:1 mixture by volume of methanol and ethanol, petroleum ether, nitrogen, argon, and helium. The nonhydrostaticity of the pressure is discussed from the viewpoint of the broadening effect of the ruby R(1) fluorescence line. The R(1) line basically broadens above the liquid-solid transition pressure at room temperature. However, the nonhydrostatic effects do constantly develop in all the media from the low-pressure region at low temperature. The relative strength of the nonhydrostatic effects in the media at the low temperature region is discussed. The broadening effect of the ruby R(1) line in the nitrogen, argon, and helium media are significantly small at 77 K, suggesting that the media are more appropriate for cryogenic experiments under high pressure up to 10 GPa with the DAC. The availability of the three media was also confirmed at 4.2 K.

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