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1.
Proc Natl Acad Sci U S A ; 118(34)2021 Aug 24.
Article in English | MEDLINE | ID: mdl-34413195

ABSTRACT

During the last decade, translational and rotational symmetry-breaking phases-density wave order and electronic nematicity-have been established as generic and distinct features of many correlated electron systems, including pnictide and cuprate superconductors. However, in cuprates, the relationship between these electronic symmetry-breaking phases and the enigmatic pseudogap phase remains unclear. Here, we employ resonant X-ray scattering in a cuprate high-temperature superconductor [Formula: see text] (Nd-LSCO) to navigate the cuprate phase diagram, probing the relationship between electronic nematicity of the Cu 3d orbitals, charge order, and the pseudogap phase as a function of doping. We find evidence for a considerable decrease in electronic nematicity beyond the pseudogap phase, either by raising the temperature through the pseudogap onset temperature T* or increasing doping through the pseudogap critical point, p*. These results establish a clear link between electronic nematicity, the pseudogap, and its associated quantum criticality in overdoped cuprates. Our findings anticipate that electronic nematicity may play a larger role in understanding the cuprate phase diagram than previously recognized, possibly having a crucial role in the phenomenology of the pseudogap phase.

2.
Inorg Chem ; 55(24): 12897-12903, 2016 Dec 19.
Article in English | MEDLINE | ID: mdl-27989196

ABSTRACT

The crystal structure of KRuO4 is refined at both 280 and 3.5 K from neutron powder data, and magnetic properties are reported for the first time. The scheelite structure, I41/a, is confirmed at both temperatures. Atomic positions of greater accuracy than the original 1954 X-ray study are reported. The rare Ru7+ ion resides in a site of distorted tetrahedral symmetry with nominal electronic configuration 4d1(e1). Curie-Weiss parameters are near free ion values for the effective moment and θ = -77 K, indicating dominant antiferromagnetic (AF) correlations. A broad susceptibility maximum occurs near 34 K, but long-range AF order sets in only below 22.4 K as determined by magnetization and heat capacity data. The entropy loss below 50 K is only 44% of the expected R ln 2, indicating the presence of short-range spin correlations over a wide temperature range. The Ru sublattice consists of centered, corner-sharing tetrahedra which can lead to geometric frustration if both the nearest-neighbor, J1, and the next-nearest-neighbor, J2, exchange constants are AF and of similar magnitude. A spin dimer analysis finds J1/J2 ≈ 25, indicating weak frustration, and a (dz2)1 ground state. A single, weak magnetic reflection was indexed as (110). The absence of the (002) magnetic reflection places the Ru moments parallel to the c axis. The Ru7+ moment is estimated to be 0.57(7) µB, reduced from an expected value near 1 µB. A recent computational study of isostructural, isoelectronic KOsO4 predicts a surprisingly large orbital moment due to spin-orbit coupling (SOC). However, the free ion SOC constant for Ru7+ is only ∼30% that of Os7+, so it is unclear that this effect can be implicated in the low ordered moment for KRuO4. The origin of the short-range spin correlations is also not understood.

3.
Inorg Chem ; 55(20): 10701-10713, 2016 Oct 17.
Article in English | MEDLINE | ID: mdl-27700052

ABSTRACT

Double perovskites (DP) of the general formula Ba2MReO6, where M = Mg, Zn, and Y2/3, all based on Re6+ (5d1, t2g1), were synthesized and studied using magnetization, heat capacity, muon spin relaxation, and neutron-scattering techniques. All are cubic, Fm3̅m, at ambient temperature to within the resolution of the X-ray and neutron diffraction data, although the muon data suggest the possibility of a local distortion for M = Mg. The M = Mg DP is a ferromagnet, Tc = 18 K, with a saturation moment ∼0.3 bohr magnetons at 3 K. There are two anomalies in the heat capacity: a sharp feature at 18 K and a broad maximum centered near 33 K. The total entropy loss below 45 K is 9.68 e.u., which approaches R ln 4 (11.52 e.u.) supporting a j = 3/2 ground state. The unit cell constants of Ba2MgReO6 and the isostructural, isoelectronic analogue, Ba2LiOsO6, differ by only 0.1%, yet the latter is an anti-ferromagnet. The M = Zn DP also appears to be a ferromagnet, Tc = 11 K, µsat(Re) = 0.1 µB. In this case the heat capacity shows a somewhat broad peak near 10 K and a broader maximum at ∼33 K, behavior that can be traced to a smaller particle size, ∼30 nm, for this sample. For both M = Mg and Zn, the low-temperature magnetic heat capacity follows a T3/2 behavior, consistent with a ferromagnetic spin wave. An attempt to attribute the broad 33 K heat capacity anomalies to a splitting of the j = 3/2 state by a crystal distortion is not supported by inelastic neutron scattering, which shows no transition at the expected energy of ∼7 meV nor any transition up to 100 meV. However, the results for the two ferromagnets are compared to the theory of Chen, Pereira, and Balents, and the computed heat capacity predicts the two maxima observed experimentally. The M = Y2/3 DP, with a significantly larger cell constant (3%) than the ferromagnets, shows predominantly anti-ferromagnetic correlations, and the ground state is complex with a spin frozen component Tg = 16 K from both direct current and alternating current susceptibility and µSR data but with a persistent dynamic component. The low-temperature heat capacity shows a T1 power law. The unit cell constant of B = Y2/3 is less than 1% larger than that of the ferromagnetic Os7+ (5d1) DP, Ba2NaOsO6.

5.
Proc Math Phys Eng Sci ; 470(2171): 20140387, 2014 Nov 08.
Article in English | MEDLINE | ID: mdl-25383026

ABSTRACT

We present the results of experimental determination of the heat capacity of the pyrochlore Er2Ti2O7 as a function of temperature (0.35-300 K) and magnetic field (up to 9 T), and for magnetically diluted solid solutions of the general formula (Er1-x Y x )2Ti2O7 (x≤0.471). On either doping or increase of magnetic field, or both, the Néel temperature first shifts to lower temperature until a critical point above which there is no well-defined transition but a Schottky-like anomaly associated with the splitting of the ground state Kramers doublet. By taking into account details of the lattice contribution to the heat capacity, we accurately isolate the magnetic contribution to the heat capacity and hence to the entropy. For pure Er2Ti2O7 and for (Er1-x Y x )2Ti2O7, the magnetic entropy as a function of temperature evolves with two plateaus: the first at [Formula: see text], and the other at [Formula: see text]. When a very high magnetic field is applied, the first plateau is washed out. The influence of dilution at low values is similar to the increase of magnetic field, as we show by examination of the critical temperature versus critical field curve in reduced terms.

6.
Nat Commun ; 5: 4970, 2014 Sep 18.
Article in English | MEDLINE | ID: mdl-25233136

ABSTRACT

In condensed matter systems, formation of long-range order (LRO) is often accompanied by new excitations. However, in many geometrically frustrated magnetic systems, conventional LRO is suppressed, while non-trivial spin correlations are still observed. A natural question to ask is then what is the nature of the excitations in this highly correlated state without broken symmetry? Frequently, applying a symmetry breaking field stabilizes excitations whose properties reflect certain aspects of the anomalous state without LRO. Here we report a THz spectroscopy study of novel excitations in quantum spin ice Yb2Ti2O7 under a <001> directed magnetic field. At large positive fields, both right- and left-handed magnon and two-magnon-like excitations are observed. The g-factors of these excitations are dramatically enhanced in the low-field limit, showing a crossover of these states into features consistent with the quantum string-like excitations proposed to exist in quantum spin ice in small <001> fields.

7.
Phys Rev Lett ; 113(11): 117001, 2014 Sep 12.
Article in English | MEDLINE | ID: mdl-25259999

ABSTRACT

We take advantage of the site-selective nature of the ^{75}As and ^{63}Cu NMR techniques to probe the Cu substitution effects on the local magnetic properties of the FeAs planes in Ba(Fe_{1-x}Cu_{x})_{2}As_{2}. We show that the suppression of antiferromagnetic Fe spin fluctuations induced by Cu substitution is weaker than a naive expectation based on a simple rigid band picture, in which each Cu atom would donate three electrons to the FeAs planes. Comparison between ^{63}Cu and ^{75}As NMR data indicates that spin fluctuations are suppressed at the Cu and their neighboring Fe sites in the tetragonal phase, suggesting the strongly local nature of the Cu substitution effects. We attribute the absence of a large superconducting dome in the phase diagram of Ba(Fe_{1-x}Cu_{x})_{2}As_{2} to the emergence of a nearly magnetically ordered FeAs plane under the presence of orthorhombic distortion.

8.
Sci Rep ; 4: 4120, 2014 Feb 18.
Article in English | MEDLINE | ID: mdl-24844399

ABSTRACT

The interplay between magnetism and crystal structures in three CaFe2As2 samples is studied. For the nonmagnetic quenched crystals, different crystalline domains with varying lattice parameters are found, and three phases (orthorhombic, tetragonal, and collapsed tetragonal) coexist between TS=95 K and 45 K. Annealing of the quenched crystals at 350°C leads to a strain relief through a large (~1.3%) expansion of the c-parameter and a small (~0.2%) contraction of the a-parameter, and to local ~0.2 Šdisplacements at the atomic-level. This annealing procedure results in the most homogeneous crystals for which the antiferromagnetic and orthorhombic phase transitions occur at TN/TS=168(1) K. In the 700°C-annealed crystal, an intermediate strain regime takes place, with tetragonal and orthorhombic structural phases coexisting between 80 to 120 K. The origin of such strong shifts in the transition temperatures are tied to structural parameters. Importantly, with annealing, an increase in the Fe-As length leads to more localized Fe electrons and higher local magnetic moments on Fe ions. Synergistic contribution of other structural parameters, including a decrease in the Fe-Fe distance, and a dramatic increase of the c-parameter, which enhances the Fermi surface nesting in CaFe2As2, are also discussed.

9.
J Phys Condens Matter ; 25(43): 435902, 2013 Oct 30.
Article in English | MEDLINE | ID: mdl-24107620

ABSTRACT

Structural phase transitions in pyrochlore Cd2Nb2O7 were studied by means of single crystal x-ray scattering. On cooling below the ferroelastic transition at T1 = 204 K, the cubic Bragg peaks broaden in a manner consistent with weak orthorhombic distortion. The distortion evolves rather smoothly through the ferroelectric transition at T2 = 196 K, which explains the absence of sharp anomalies in the heat capacity and dielectric constant at this transition. At lower temperatures, the anomalous relaxor-like character of this compound is evident as a gradual reduction in the Bragg peak intensities, which continues down to the onset of another transition at T3 = 85 K. The studies of two Bragg peaks that are forbidden within the cubic phase reveal an interesting disparity: while the intensity for one of them increases in a classical mean-field manner below T1, the other shows unconventional behavior that is reminiscent of the pyrochlore superconductor Cd2Re2O7.

10.
Phys Rev Lett ; 109(16): 167201, 2012 Oct 19.
Article in English | MEDLINE | ID: mdl-23215118

ABSTRACT

Here we establish the systematic existence of a U(1) degeneracy of all symmetry-allowed Hamiltonians quadratic in the spins on the pyrochlore lattice, at the mean-field level. By extracting the Hamiltonian of Er(2)Ti(2)O(7) from inelastic neutron scattering measurements, we then show that the U(1)-degenerate states of Er(2)Ti(2)O(7) are its classical ground states, and unambiguously show that quantum fluctuations break the degeneracy in a way which is confirmed by experiment. The degree of symmetry protection of the classical U(1) degeneracy in Er(2)Ti(2)O(7) is unprecedented in other materials. As a consequence, our observation of order by disorder is unusually definitive. We provide further verifiable consequences of this phenomenon, and several additional comparisons between theory and experiment.

11.
Rev Sci Instrum ; 83(1): 013113, 2012 Jan.
Article in English | MEDLINE | ID: mdl-22299935

ABSTRACT

We have developed an application of a one-dimensional micro-strip detector for capturing x-ray diffraction data in pulsed magnetic fields. This detector consists of a large array of 50 µm-wide Si strips with a full-frame read out at 20 kHz. Its use substantially improves data-collection efficiency and quality as compared to point detectors, because diffraction signals are recorded along an arc in reciprocal space in a time-resolved manner. By synchronizing with pulsed fields, the entire field dependence of a two-dimensional swath of reciprocal space may be determined using a small number of field pulses.

12.
Rev Sci Instrum ; 80(11): 113902, 2009 Nov.
Article in English | MEDLINE | ID: mdl-19947737

ABSTRACT

We present a portable pulsed-magnet system for x-ray studies of materials in high magnetic fields (up to 30 T). The apparatus consists of a split-pair of minicoils cooled on a closed-cycle cryostat, which is used for x-ray diffraction studies with applied field normal to the scattering plane. A second independent closed-cycle cryostat is used for cooling the sample to near liquid helium temperatures. Pulsed magnetic fields (approximately 1 ms in total duration) are generated by discharging a configurable capacitor bank into the magnet coils. Time-resolved scattering data are collected using a combination of a fast single-photon counting detector, a multichannel scaler, and a high-resolution digital storage oscilloscope. The capabilities of this instrument are used to study a geometrically frustrated system revealing strong magnetostrictive effects in the spin-liquid state.

13.
J Clin Psychiatry ; 68(9): 1377-83, 2007 Sep.
Article in English | MEDLINE | ID: mdl-17915976

ABSTRACT

OBJECTIVE: To examine the antimanic efficacy of the relatively nonsedating antipsychotic aripiprazole in patients with bipolar I disorder and high or low baseline levels of agitation. METHOD: Data were pooled for this post hoc analysis from two 3-week, placebo-controlled trials of aripiprazole in acute mania (DSM-IV). Patients randomly assigned to aripiprazole 30 mg/day (N = 259) or placebo (N = 254) were classified as having either high (Positive and Negative Syndrome Scale [PANSS] Excited Component [PEC] score of >or=14 and a score of >or= 4 on at least one PEC item) or low (PEC < 14) levels of agitation at baseline. Efficacy measures were changes in Young Mania Rating Scale (YMRS) scores, Clinical Global Impressions-Bipolar (CGI-BP) scores, and PEC scores. Efficacy and agitation measurements were assessed by analysis of covariance. RESULTS: From the first week of therapy onward, aripiprazole-treated subjects had significantly greater reduction from baseline in YMRS total scores than placebo-treated subjects in both the high- and low-agitation groups (p < .05 for both groups) and significantly improved CGI-BP scores vs. placebo at end point (p < .05 for both). In highly agitated patients receiving aripiprazole, PEC scores were significantly decreased versus placebo at end point (p < .05). In patients with low agitation receiving aripiprazole, no increases in PEC scores were seen, and a significant reduction in agitation symptoms was apparent after adjustment for baseline PEC scores. CONCLUSIONS: Aripiprazole was superior to placebo in reducing the severity of both mania and agitation in highly agitated patients with bipolar I disorder and showed significant antimanic activity in patients with low levels of agitation without increasing agitation. These findings suggest that aripiprazole's antimanic effect is specific and not limited to control of agitation through sedation.


Subject(s)
Antimanic Agents/therapeutic use , Antipsychotic Agents/therapeutic use , Bipolar Disorder/drug therapy , Bipolar Disorder/epidemiology , Piperazines/therapeutic use , Psychomotor Agitation/drug therapy , Psychomotor Agitation/epidemiology , Quinolones/therapeutic use , Aripiprazole , Bipolar Disorder/diagnosis , Data Interpretation, Statistical , Diagnostic and Statistical Manual of Mental Disorders , Drug Administration Schedule , Female , Humans , Male , Middle Aged , Psychomotor Agitation/diagnosis , Severity of Illness Index , Surveys and Questionnaires
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