Field-induced Quantum Critical Point Research Articles

Significant inverse magnetocaloric effect induced by quantum criticality

The criticality-enhanced magnetocaloric effect (MCE) near a field-induced quantum critical point (QCP) in the spin systems constitutes a very promising and highly tunable alternative to conventional adiabatic demagnetization refrigeration. Strong fluctuations in the low-$T$ quantum critical regime can give rise to a large thermal entropy change and thus significant cooling effect when approaching the QCP. In this work, through efficient and accurate many-body calculations, we show there exists a significant inverse MCE (iMCE) in the spin-1 quantum chain materials (${\mathrm{CH}}_{3}{)}_{4}\mathrm{NNi}{({\mathrm{NO}}_{2})}_{3}$ (TMNIN) and ${\mathrm{NiCl}}_{2}\text{\ensuremath{-}}4\mathrm{SC}{({\mathrm{NH}}_{2})}_{2}$ (DTN), where DTN has substantial low-$T$ refrigeration capacity while requiring only moderate magnetic fields. The iMCE characteristics, including the adiabatic temperature change $\mathrm{\ensuremath{\Delta}}{T}_{\mathrm{ad}}$, isothermal entropy change $\mathrm{\ensuremath{\Delta}}S$, differential Gr\"uneisen parameter, and the entropy change rate, are obtained with quantum many-body calculations at finite temperature. The cooling performance, i.e., the efficiency factor and hold time, of the two compounds is also discussed. Based on the many-body calculations on realistic models for the spin-chain materials, we conclude that the compound DTN constitutes a very promising and highly efficient quantum magnetic coolant with pronounced iMCE properties. We advocate that such quantum magnets can be used in cryofree refrigeration for space applications and quantum computing environments.

Magnetic ground state of the one-dimensional ferromagnetic chain compoundsM(NCS)2(thiourea)2(M=Ni,Co)

The magnetic properties of the two isostructural molecule-based magnets, Ni(NCS)$_{2}$(thiourea)$_{2}$, $S$ = 1, [thiourea = SC(NH$_2$)$_2$] and Co(NCS)$_{2}$(thiourea)$_{2}$, $S$ = 3/2, are characterised using several techniques in order to rationalise their relationship with structural parameters and ascertain magnetic changes caused by substitution of the spin. Zero-field heat capacity and muon-spin relaxation measurements reveal low-temperature long-range ordering in both compounds, in addition to Ising-like ($D < 0$) single-ion anisotropy ($D_{\rm{Co}} \sim$ -100 K, $D_{\rm{Ni}} \sim$ -10 K). Crystal and electronic structure, combined with DC-field magnetometry, affirm highly quasi-one-dimensional behaviour, with ferromagnetic intrachain exchange interactions $J_{\rm{Co}}\approx+4$ K and $J_{\rm{Ni}}\sim+100$ K and weak antiferromagnetic interchain exchange, on the order of $J'$ $\sim-0.1$ K. Electron charge and spin-density mapping reveals through-space exchange as a mechanism to explain the large discrepancy in $J$-values despite, from a structural perspective, the highly similar exchange pathways in both materials. Both species can be compared to the similar compounds $M$Cl$_2$(thiourea)$_4$, $M$ = Ni(II) (DTN) and Co(II) (DTC), where DTN is know to harbour two magnetic field-induced quantum critical points. Direct comparison of DTN and DTC with the compounds studied here shows that substituting the halide Cl$^-$ ion, for the NCS$^-$ ion, results in a dramatic change in both the structural and magnetic properties.

Robust Fermi-Surface Morphology of CeRhIn_{5} across the Putative Field-Induced Quantum Critical Point.

We report a comprehensive de Haas-van Alphen (dHvA) study of the heavy-fermion material CeRhIn_{5} in magnetic fields up to 70T. Several dHvA frequencies gradually emerge at high fields as a result of magnetic breakdown. Among them is the thermodynamically important β_{1} branch, which has not been observed so far. Comparison of our angle-dependent dHvA spectra with those of the non-4f compound LaRhIn_{5} and with band-structure calculations evidences that the Ce 4f electrons in CeRhIn_{5} remain localized over the whole field range. This rules out any significant Fermi-surface reconstruction, either at the suggested nematic phase transition at B^{*}≈30 T or at the putative quantum critical point at B_{c}≃50 T. Our results rather demonstrate the robustness of the Fermi surface and the localized nature of the 4f electrons inside and outside of the antiferromagnetic phase.

Non-monotonic pressure dependence of high-field nematicity and magnetism in CeRhIn5

CeRhIn5 provides a textbook example of quantum criticality in a heavy fermion system: Pressure suppresses local-moment antiferromagnetic (AFM) order and induces superconductivity in a dome around the associated quantum critical point (QCP) near pc ≈ 23 kbar. Strong magnetic fields also suppress the AFM order at a field-induced QCP at Bc ≈ 50 T. In its vicinity, a nematic phase at B* ≈ 28 T characterized by a large in-plane resistivity anisotropy emerges. Here, we directly investigate the interrelation between these phenomena via magnetoresistivity measurements under high pressure. As pressure increases, the nematic transition shifts to higher fields, until it vanishes just below pc. While pressure suppresses magnetic order in zero field as pc is approached, we find magnetism to strengthen under strong magnetic fields due to suppression of the Kondo effect. We reveal a strongly non-mean-field-like phase diagram, much richer than the common local-moment description of CeRhIn5 would suggest.

Low temperature magnetism in the rare-earth perovskite GdScO3**The work at SUSTech was supported by the National Natural Science Foundation of China (Grant No. 11974157). Part of this work was also supported by the National Natural Science Foundation of China (Grant No. 11875265), the Scientific Instrument Developing Project of the Chinese Academy of Sciences (3He-based neutron polarization devices), and the Institute

The magnetic phase diagram of rare-earth perovskite compound, GdScO3, has been investigated by magnetization and heat capacity. The system undergoes an antiferromagnetic phase transition at TN = 2.6 K, with an easy axis of magnetization along the a axis. The magnetization measurements show that it exists a spin-flop transition around 0.3 T for the applied field along the a axis. The critical magnetic field for the antiferromagnetic-to-paramagnetic transition is near 3.2 T when temperature approaches zero. By scaling susceptibilities, we presume this point (B = 3.2 T, T = 0 K) might be a field-induced quantum critical point and the magnetic critical fluctuations can even be felt above TN.

Tuning low-energy scales in YbRh2Si2 by non-isoelectronic substitution and pressure

The heavy-fermion metal YbRh$_2$Si$_2$ realizes a field-induced quantum critical point with multiple vanishing energy scales $T_{\rm N}(B)$ and $T^\ast(B)$. We investigate their change with partial non-isoelectronic substitutions, chemical and hydrostatic pressure. Low-temperature electrical resistivity, specific heat and magnetic susceptibility of Yb(Rh$_{1-x}$T$_x$)$_2$Si$_2$ with T=Fe or Ni for $x\leq 0.1$, magnetic fields $B\leq 0.3$~T (applied perpendicular to the c-axis) and hydrostatic pressure $p\leq 1.5$~GPa are reported. The data allow to disentangle the combined influences of hydrostatic and chemical pressure, as well as non-isoelectronic substitution. In contrast to Ni- and Co-substitution, which enhance magnetic order, Fe-substitution acts oppositely. For $x=0.1$ it also completely suppresses the $T^\ast$ crossover and eliminates ferromagnetic fluctuations. The pressure, magnetic field and temperature dependences of $T^\ast$ are incompatible with its interpretation as Kondo breakdown signature.

Z=2 Quantum Critical Dynamics in a Spin Ladder.

By means of inelastic neutron scattering we investigate finite temperature dynamics in the quantum spin ladder compound (C_{5}H_{12}N)_{2}CuBr_{4} (BPCB) near the magnetic field induced quantum critical point with dynamical exponent z=2. We observe universal finite-temperature scaling of the transverse local dynamic structure factor in spectacular quantitative agreement with long-standing theoretical predictions. At the same time, already at rather low temperatures, we observe strong nonuniversal longitudinal fluctuations. To separate the two, we make use of an intrinsic leg-exchange symmetry of the spin ladder. Complementary measurements of specific heat also reveal striking scaling behavior near the quantum critical point.

Magnetic field induced quantum criticality and the Luttinger sum rule

We show that when there is a sudden transition from a small to a large Fermi surface at a field-induced quantum critical point, similar to what may have been observed in some heavy-fermion compounds, an additional term has to be taken into account in the Luttinger-Friedel sum rule.We calculate this additional term for a local model which has a field-induced quantum critical point (QCP) and show that it changes abruptly at the transition, such that it satisfies a generalized Luttinger-Friedel sum rule on each side of the transition, and characterizes the two Fermi-liquid phases separated by the QCP as a discrete (topological) index.

Evolution of the Kondo lattice and non-Fermi liquid excitations in a heavy-fermion metal

Strong electron correlations can give rise to extraordinary properties of metals with renormalized Landau quasiparticles. Near a quantum critical point, these quasiparticles can be destroyed and non-Fermi liquid behavior ensues. YbRh2Si2 is a prototypical correlated metal exhibiting the formation of quasiparticle and Kondo lattice coherence, as well as quasiparticle destruction at a field-induced quantum critical point. Here we show how, upon lowering the temperature, Kondo lattice coherence develops at zero field and finally gives way to non-Fermi liquid electronic excitations. By measuring the single-particle excitations through scanning tunneling spectroscopy, we find the Kondo lattice peak displays a non-trivial temperature dependence with a strong increase around 3.3 K. At 0.3 K and with applied magnetic field, the width of this peak is minimized in the quantum critical regime. Our results demonstrate that the lattice Kondo correlations have to be sufficiently developed before quantum criticality can set in.

Magnetization, resistivity, specific heat and ab initio calculations of Gd5Sb3

We report on the combined results of the structural, magnetic, transport and calorimetric properties of Mn5Si3-type hexagonal Gd5Sb3, together with ab initio calculations. It exhibits a ferromagnetic (FM)-like transition at 265 K, antiferromagnetic (AFM) Néel transition at 95.5 K followed by a spin-orientation transition at 62 K. The system is found to be in AFM state down to 2 K in a field of 70 kOe. The FM-AFM phase coexistence is not noticeable despite large positive Curie–Weiss temperature ( K). Instead, low-temperature AFM and high-temperature FM-like phases are separated in large temperatures. Temperature-magnetic field (H-T) phase diagram reveals field-driven complex magnetic phases. Within the AFM phase, the system is observed to undergo field-driven spin-orientation transitions. Field-induced tricritical and quantum critical points appear to be absent due to the strong AFM nature and by the intervention of FM-like state between paramagnetic and AFM states, respectively. The metallic behavior of the compound is inferred from resistivity along with large Sommerfeld parameter. However, no sign of strong electron-correlations is reasoned from the Kadowaki–Wood’s ratio cm · (mol · K)2(mJ)−2, despite heavy γ. Essentially, ab initio calculations accounting for electronic correlations confirm AFM nature of low-temperature magnetic state in Gd5Sb3 and attainable FM ordering in agreement with experimental data.

Anomalous Change in the de Haas-van Alphen Oscillations of CeCoIn_{5} at Ultralow Temperatures.

We perform de Haas-van Alphen (dHvA) measurements of the heavy-fermion superconductor CeCoIn_{5} down to 2mK above the upper critical field. We find that the dHvA amplitudes show an anomalous suppression, concomitantly with a shift of the dHvA frequency, below the transition temperature T_{n}=20 mK. We suggest that the change is owing to magnetic breakdown caused by a field-induced antiferromagnetic (AFM) state emerging below T_{n}, revealing the origin of the field-induced quantum critical point (QCP) in CeCoIn_{5}. The field dependence of T_{n} is found to be very weak for 7-10T, implying that an enhancement of AFM order by suppressing the critical spin fluctuations near the AFM QCP competes with the field suppression effect on the AFM phase. We suggest that the appearance of a field-induced AFM phase is a generic feature of unconventional superconductors, which emerge near an AFM QCP, including CeCoIn_{5}, CeRhIn_{5}, and high-T_{c} cuprates.

Magnetic Properties of 4f Localized Ferromagnet CeAgSb2 under Transverse Magnetic Fields

We performed dc-magnetization and ac-susceptibility measurements to clarify how the magnetic properties of CeAgSb2, which shows ferromagnetic order along the c-axis below 9.6 K, evolve with the application of a transverse magnetic field (Hab). The Curie temperature (TC) is suppressed to zero by the application of Hab, and the ac-susceptibility measured along the c-axis \(\chi '_{c}\) under Hab continuously shows a critical-divergence-like anomaly at TC, indicating the presence of a field-induced ferromagnetic quantum critical point in this compound. On the other hand, the magnitude of \(\chi '_{c}\) at TC rapidly decreases with increasing Hab up to around 0.5 T. This result suggests that the magnetic properties around TC rapidly change with Hab in the relatively lower Hab range.

Reentrant behaviors in the phase diagram of spin-1 planar ferromagnet with single-ion anisotropy

We used the two-time Green function framework to investigate the role played by the easy-axis single-ion anisotropy on the phase diagram of (d>2)-dimensional spin-1planar ferromagnets, which exhibit a magnetic field induced quantum phase transition. We tackled the problem using two different kind of approximations: the Anderson-Callen decoupling scheme and the Devlin approach. In the latter scheme, the exchange anisotropy terms in the equations of motion are treated at the Tyablikov decoupling level while the crystal field anisotropy contribution is handled exactly. The emerging key result is a reentrant structure of the phase diagram close to the quantum critical point, for certain values of the single-ion anisotropy parameter. We compare the results obtained within the two approximation schemes. In particular, we recover the same qualitative behavior. We show the phase diagram, close to the field-induced quantum critical point and the behavior of the susceptibility for different values of the single-ion anisotropy parameter, enhancing the differences between the two different scenarios (i.e. with and without reentrant behavior).

Field-induced quantum criticality in the Kitaev system α−RuCl3

$\alpha$-RuCl$_3$ has attracted enormous attention since it has been proposed as a prime candidate to study fractionalized magnetic excitations akin to Kitaev's honeycomb-lattice spin liquid. We have performed a detailed specific-heat investigation at temperatures down to $0.4$ K in applied magnetic fields up to $9$ T for fields parallel to the $ab$ plane. We find a suppression of the zero-field antiferromagnetic order, together with an increase of the low-temperature specific heat, with increasing field up to $\mu_0H_c\approx 6.9$ T. Above $H_c$, the magnetic contribution to the low-temperature specific heat is strongly suppressed, implying the opening of a spin-excitation gap. Our data point toward a field-induced quantum critical point (QCP) at $H_c$; this is supported by universal scaling behavior near $H_c$. Remarkably, the data also reveal the existence of a small characteristic energy scale well below $1$~meV above which the excitation spectrum changes qualitatively. We relate the data to theoretical calculations based on a $J_1$--$K_1$--$\Gamma_1$--$J_3$ honeycomb model.

Magnetic field-induced Fermi surface reconstruction and quantum criticality in

We present detailed results of the field evolution of the de Haas–van Alphen (dHvA) effect in . A magnetic field-induced reconstruction of the Fermi surface is clearly shown to occur inside the antiferromagnetic state, in an applied field of around T, which is evidenced by the appearance of several new dHvA branches. The angular dependence of the dHvA frequencies reveals that the Fermi surfaces of at and are similar. The results suggest that the Ce-4f electrons in become itinerant at due to the Kondo effect, prior to the field-induced quantum critical point (QCP) at T. The electronic states at the field-induced QCP are therefore different from that of the pressure-induced QCP where a dramatic Fermi surface reconstruction occurs exactly at the critical pressure, indicating that multiple types of QCP may exist in .

Specific heat in high magnetic fields and magnetic phase diagram ofCePt2In7

We report specific heat measurements on a high quality single crystal of the heavy-fermion compound CePt$_2$In$_7$ in magnetic fields up to 27 T. The zero-field specific heat data above the N\'{e}el temperature, $T_N$, suggest a moderately enhanced value of the electronic specific heat coefficient $\gamma = 180 \; \rm{mJ/K^2mol}$. For $T<T_N$, the data at zero applied magnetic field are consistent with the existence of an anisotropic spin-density wave opening a gap on almost entire Fermi surface, suggesting extreme two-dimensional electronic and magnetic structures for CePt$_2$In$_7$. $T_N$ is monotonically suppressed by magnetic field applied along the $c$-axis. When field is applied parallel to the $a$-axis, $T_N$ first increases at low field up to about 10 T and then decreases monotonically at higher field. Magnetic phase diagram based on specific heat measurements suggests that a field-induced quantum critical point is likely to occur slightly below 60 T for both principal orientations of the magnetic field.

Quantum tricritical fluctuations driving mass enhancement and reentrant superconductivity in URhGe

The field-induced reentrant superconductivity (RSC) discovered near a quantum critical point (QCP) in a ferromagnetic superconductor URhGe highlights the close interplay between superconductivity and magnetism. While the origin of the RSC is broadly thought to be associated with quantum critical fluctuations, their exact nature had not been well identified. Here we review our recent 59Co NMR study in a single crystal of URh0.9Co0.1Ge. Our measurements of the NMR spin-spin relaxation reveal a divergence of electronic spin fluctuations in the vicinity of the field-induced QCP at HR ≈ 13 T. The fluctuations observed are characteristic of a tricritical point, followed by a phase bifurcation toward quantum wing-critical points. We show that these tricritical fluctuations enhance the effective mass of the conduction electrons and, further, drive the RSC near the HR.

Giant dielectric nonlinearities at a magnetic Bose-Einstein condensation

We experimentally investigate the dielectric response of the low-dimensional gapped quantum magnet Cu$_2$Cl$_{4}\cdot$H$_8$C$_4$SO$_2$ near a magnetic field-induced quantum critical point, which separates the quantum-disordered and helimagnetic ground states. The observed magnetocapacitive effect originates from an improper ferroelectric nature of the transition, which itself is perhaps one of the best known realizations of Bose--Einstein condensation of magnons. Despite that, we find that the magnetocapacitive effect associated with the transition exhibits huge and very unusual anharmonicities.

Thermal Conductivity through the Quantum Critical Point in YbRh_{2}Si_{2} at Very Low Temperature.

The thermal conductivity of YbRh_{2}Si_{2} has been measured down to very low temperatures under field in the basal plane. An additional channel for heat transport appears below 30 mK, both in the antiferromagnetic and paramagnetic states, respectively, below and above the critical field suppressing the magnetic order. This excludes antiferromagnetic magnons as the origin of this additional contribution to thermal conductivity. Moreover, this low temperature contribution prevails a definite conclusion on the validity or violation of the Wiedemann-Franz law at the field-induced quantum critical point.

Finite-temperature scaling of spin correlations in an experimental realization of the one-dimensional Ising quantum critical point

Inelastic neutron scattering is used to study the finite-temperature scaling behavior of the local dynamic structure factor in the quasi-one-dimensional quantum antiferromagnet NTENP ($\text{Ni(N,N'-bis(3-aminopropyl)propane-1,3-diamine)(}\mu\text{-NO}_2\text{)ClO}_4$), at its field-induced Ising quantum critical point. The validity and the limitations of the theoretically predicted scaling relations are tested.