High sensitivity heat capacity measurements on Sr2RuO4 under uniaxial pressure

Funding: Parts of this work were funded by the Deutsche Forschungsgemeinschaft (DFG, German Research Foundation) - TRR 288 -422213477 (projects A10 and B01). NK acknowledges the support from JSPS KAKENHI (nos. JP17H06136 and JP18K04715) and JST-Mirai Program (no. JPMJMI18A3) in Japan and YM from JSPS KAKENHI (nos. JP15H05852, JP15K21717) and JSPS core-to-core programme. YSL acknowledges the support of a St Leonard’s scholarship from the University of St Andrews, the Engineering and Physical Sciences Research Council via the Scottish Condensed Matter Centre for Doctoral Training under grant EP/G03673X/1, and the Max Planck Society.A key question regarding the unconventional superconductivity of Sr2RuO4 remains whether the order parameter is single- or two-component. Under a hypothesis of two-component superconductivity, uniaxial pressure is expected to lift their degeneracy, resulting in a split transition. The most direct and fundamental probe of a split transition is heat capacity. Here, we report development of new high-frequency methodology for measurement of heat capacity of samples subject to large and highly homogeneous uniaxial pressure. We place an upper limit on the heat capacity signature of any second transition of a few per cent of the primary superconducting transition. The normalized jump in heat capacity, Δ C/C, grows smoothly as a function of uniaxial pressure, but we find no qualitative evidence of a pressure-induced order parameter transition. Thanks to the high precision of our measurements, these findings place stringent constraints on theories of the superconductivity of Sr2RuO4.PostprintPeer reviewe

Strong peak in Tc of Sr2RuO4 under uniaxial pressure

Sr2RuO4 is an unconventional superconductor that has attracted widespread study because of its high purity and the possibility that its superconducting order parameter has odd parity. We study the dependence of its superconductivity on anisotropic strain. Applying uniaxial pressures of up to ~1 gigapascals along a 〈100〉 direction (a axis) of the crystal lattice results in the transition temperature (Tc) increasing from 1.5 kelvin in the unstrained material to 3.4 kelvin at compression by ≈0.6%, and then falling steeply. Calculations give evidence that the observed maximum Tc occurs at or near a Lifshitz transition when the Fermi level passes through a Van Hove singularity, and open the possibility that the highly strained, Tc = 3.4 K Sr2RuO4 has an even-parity, rather than an odd-parity, order parameter.PostprintPeer reviewe

Elastocaloric determination of the phase diagram of Sr2_2RuO4_4

One of the main developments in unconventional superconductivity in the past two decades has been the discovery that most unconventional superconductors form phase diagrams that also contain other strongly correlated states. Many systems of interest are therefore close to more than one instability, and tuning between the resultant ordered phases is the subject of intense research1. In recent years, uniaxial pressure applied using piezoelectric-based devices has been shown to be a particularly versatile new method of tuning, leading to experiments that have advanced our understanding of the fascinating unconventional superconductor Sr$_2$RuO$_4$. Here we map out its phase diagram using high-precision measurements of the elastocaloric effect in what we believe to be the first such study including both the normal and the superconducting states. We observe a strong entropy quench on entering the superconducting state, in excellent agreement with a model calculation for pairing at the Van Hove point, and obtain a quantitative estimate of the entropy change associated with entry to a magnetic state that is observed in proximity to the superconductivity. The phase diagram is intriguing both for its similarity to those seen in other families of unconventional superconductors and for extra features unique, so far, to Sr$_2$RuO$_4$

Kazalo

The superconducting state in the quasi-two-dimensional and strongly correlated Sr$_2$RuO$_4$ is uniquely held up as a solid state analog to superfluid $^3$He-$A$, with an odd-parity order parameter that also breaks time reversal symmetry, and for which the vector order parameter has the same direction in spin space for all electron momenta. The recent discovery that uniaxial pressure causes a steep rise and maximum in transition temperature ($T_c$) in strained samples motivated the study of $^{17}$O nuclear magnetic resonance (NMR) that we describe in this article. A reduction of Knight shifts $K$ was observed for all strain values and temperatures $T<T_c$, consistent with a drop in spin polarization in the superconducting state. In unstrained samples, our results are in contradiction with a body of previous NMR work, and with the most prominent previous proposals for the order parameter of Sr$_2$RuO$_4$. Possible alternative scenarios are discussed.Comment: Manuscript: 4 figures, 2 tables; Supplementary Information: 5 figure

Normal state 17O NMR studies of Sr2RuO4 under uniaxial stress

This work was supported in part by the Laboratory Directed Research and Development (LDRD) program of Los Alamos National Laboratory under Project No. 20170204ER. Y. L. acknowledges partial support through the LDRD and 1000 Youth Talents Plan of China. N. K. acknowledges the support from JSPS KAKNHI (Grant No. 18K04715). I. I.M. is supported by ONR through the NRL basic research program. This work is supported in part by the National Science Foundation (Grants No. DMR-1410343 and No. DMR-1709304).The effects of uniaxial compressive stress on the normal state 17O nuclear-magnetic-resonance properties of the unconventional superconductor Sr2RuO4 are reported. The paramagnetic shifts of both planar and apical oxygen sites show pronounced anomalies near the nominal a-axis strain ϵaa≡ϵv that maximizes the superconducting transition temperature Tc. The spin susceptibility weakly increases on lowering the temperature below T≃10  K, consistent with an enhanced density of states associated with passing the Fermi energy through a van Hove singularity. Although such a Lifshitz transition occurs in the γ band formed by the Ru dxy states hybridized with in-plane O pπ orbitals, the large Hund’s coupling renormalizes the uniform spin susceptibility, which, in turn, affects the hyperfine fields of all nuclei. We estimate this “Stoner” renormalization S by combining the data with first-principles calculations and conclude that this is an important part of the strain effect, with implications for superconductivity.Publisher PDFPeer reviewe

The ground state spectroscopic parameters and equilibrium structure of PD3

Infrared spectra of PD3 have been measured in the 20-320 cm-1 range and in the region of the ν2/ν4 and ν1/ν3 fundamental bands near 750 and 1690 cm-1, respectively, with a resolution of ca. 0.0025 cm-1. Furthermore, submillimeter-wave spectra covering the J = 4-3, 13-12, and 14-13 clusters in the vibrational ground state were recorded. The observed ΔJ = +1 rotational lines were augmented by about 5500 ground state combination differences formed from transitions belonging to the fundamental bands. Of these, 1300 involved perturbation-allowed lines with ΔK ≠ 0. These data and observations taken from the literature were appropriately weighted and fitted to 14 ground state molecular constants. The A and B reductions of the rotational Hamiltonian were found to be equivalent. Improved effective ground state and equilibrium structures were determined for both PH3 and PD3; the equilibrium structures, re (PH) = 141.1607(83) pm and αe (HPH) = 93.4184(95)° and re (PD) = 141.1785(57) pm and αe (DPD) = 93.4252(68)°, are in good agreement. © 2002 Elsevier Science (USA)

The superconductivity of Sr2RuO4 under c-axis uniaxial stress

Funding: F.J., A.P.M., and C.W.H. acknowledge the financial support of the Deutsche Forschungsgemeinschaft (DFG, German Research Foundation) - TRR 288 - 422213477 (project A10). H.S.R. and S.H.S. acknowledge the financial support of the Engineering and Physical Sciences Research Council (UK). H.S.R. acknowledges support from the Aker Scholarship. T.S. acknowledges the support of the Natural Sciences and Engineering Research Council of Canada (NSERC), in particular the Discovery Grant [RGPIN-2020-05842], the Accelerator Supplement [RGPAS-2020-00060], and the Discovery Launch Supplement [DGECR-2020-00222]. N.K. is supported by a KAKENHI Grants-in-Aids for Scientific Research (Grant Nos.17H06136, 18K04715, and 21H01033), and Core-to-Core Program (No. JPJSCCA20170002) from the Japan Society for the Promotion of Science (JSPS) and by a JST-Mirai Program (Grant No. JPMJMI18A3).Applying in-plane uniaxial pressure to strongly correlated low-dimensional systems has been shown to tune the electronic structure dramatically. For example, the unconventional superconductor Sr2RuO4 can be tuned through a single Van Hove point, resulting in strong enhancement of both Tc and Hc2. Out-of-plane (c axis) uniaxial pressure is expected to tune the quasi-two-dimensional structure even more strongly, by pushing it towards two Van Hove points simultaneously. Here, we achieve a record uniaxial stress of 3.2 GPa along the c axis of Sr2RuO4. Hc2 increases, as expected for increasing density of states, but unexpectedly Tc falls. As a first attempt to explain this result, we present three-dimensional calculations in the weak interaction limit. We find that within the weak-coupling framework there is no single order parameter that can account for the contrasting effects of in-plane versus c-axis uniaxial stress, which makes this new result a strong constraint on theories of the superconductivity of Sr2RuO4.Publisher PDFPeer reviewe

High resolution study of AsHD2: Ground state and the three bending fundamental bands v(3), v(4), and v(6)

International audienceFor the first time the infrared spectrum of the AsHD2 molecule has been measured in the region of the bending fundamental bands v(3), v(4), and v(6) on a Fourier transform spectrometer with a resolution of 0.0024 cm(-1) and analyzed. More than 5500 transitions with J(max) = 26 have been assigned and used both to obtain "ground state combination differences" and for the determination of upper state ro-vibrational energies of the triad (001000), (000100), and (000001). Rotational parameters including centrifugal distortion coefficients up to octic terms of the ground vibrational state were calculated by fitting more than 500 "ground state combination differences" with J(max) and K-a(max) = 21. The obtained set of 24 parameters provides a rms-deviation of 0.00011 cm(-1). The upper energies were fitted with 52 parameters of an effective Hamiltonian which takes into account strong resonance interactions between all vibrational states of the triad (001000), (000100), and (000001). The rms-deviation for the energy levels considered in the fit is 0.00014 cm(-1)