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Experimental investigation of heavy fermion quantum criticality
Stockholm University, Faculty of Science, Department of Physics.ORCID iD: 0000-0002-7645-2922
2025 (English)Doctoral thesis, comprehensive summary (Other academic)
Abstract [en]

Advancements in technology are increasingly driven by the development of new functional materials. One such family is the heavy fermions, obtained by combining rare-earth elements with metallic host material. These heavy fermions display exotic quantum mechanical properties at low temperatures. Key techniques that measures properties such as specific heat, magnetic susceptibility, and nuclear spin-lattice relaxation provide valuable insights of the interactions within these systems, enabling the exploration of their unique characteristics  and guiding the discovery of new related materials.

In this thesis, AC calorimetry is used to measure specific heat as a primary tool to characterize these materials. Specific heat contains all the contributions associated with different subsystems in the material. Accurate measurement and careful interpretation of the measurements are essential, as these materials comprise of multiple subsystems such as electronic, nuclear, and magnetic, having different time scales. Due to multiple time scales involved, traditional calorimetry methods become challenging. To solve this issue we here develop a new experimental technique based on AC calorimetry that can disentangle different contributions to specific heat at low temperatures. The technique, that we call Thermal Impedance Spectroscopy (TISP), allows independent measurement of the electronic and nuclear specific heat at low temperatures. This is because the relaxation time of the nuclear subsystem to equilibrate with the lattice (electrons and phonons) is slow and can be captured by the frequency response of the calorimeter-sample assembly. This relaxation time, known as the nuclear spin-lattice relaxation time T1, provides an additional probe for the electronic subsystem. The method's effectiveness is demonstrated using indium, a known metallic system, with results aligning well with expectations and prior Nuclear Magnetic Resonance (NMR) studies.

TISP was applied to investigate several quantum materials, including heavy fermions close to or at a quantum critical point. The role of the magnetic field on the quantum criticality of these systems was investigated using TISP, and complementary techniques such as magnetic susceptibility and X-ray measurements were employed to further investigate these materials.

Place, publisher, year, edition, pages
Stockholm: Department of Physics, Stockholm University , 2025. , p. 124
Keywords [en]
heavy fermions, quantum criticality, strongly correlated electron systems, specific heat
National Category
Condensed Matter Physics
Research subject
Physics
Identifiers
URN: urn:nbn:se:su:diva-240744ISBN: 978-91-8107-158-0 (print)ISBN: 978-91-8107-159-7 (electronic)OAI: oai:DiVA.org:su-240744DiVA, id: diva2:1944163
Public defence
2025-04-25, Hörsal 4, hus 2, Albano, Albanovägen 20, Stockholm, 13:00 (English)
Opponent
Supervisors
Available from: 2025-04-02 Created: 2025-03-12 Last updated: 2025-03-28Bibliographically approved
List of papers
1. Calorimetric measurement of nuclear spin-lattice relaxation rate in metals
Open this publication in new window or tab >>Calorimetric measurement of nuclear spin-lattice relaxation rate in metals
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2023 (English)In: Physical Review B, ISSN 2469-9950, E-ISSN 2469-9969, Vol. 107, no 19, article id 195145Article in journal (Refereed) Published
Abstract [en]

The quasiparticle density of states in correlated and quantum-critical metals directly probes the effect of electronic correlations on the Fermi surface. Measurements of the nuclear spin-lattice relaxation rate provide one such experimental probe of quasiparticle mass through the electronic density of states. By far the most common way of accessing the spin-lattice relaxation rate is via nuclear magnetic resonance and nuclear quadrupole resonance experiments, which require resonant excitation of nuclear spin transitions. Here we report nonresonant access to spin-lattice relaxation dynamics in AC-calorimetric measurements. The nuclear spin-lattice relaxation rate is inferred in our measurements from its effect on the frequency dispersion of the thermal response of the calorimeter-sample assembly. We use fast, lithographically defined nanocalorimeters to access the nuclear spin-lattice relaxation times in metallic indium from 0.3 to 7 K and in magnetic fields up to 35 T.

National Category
Materials Chemistry
Identifiers
urn:nbn:se:su:diva-229906 (URN)10.1103/PhysRevB.107.195145 (DOI)001003873700003 ()2-s2.0-85161289837 (Scopus ID)
Available from: 2024-05-30 Created: 2024-05-30 Last updated: 2025-03-12Bibliographically approved
2. Multi-flavor quantum criticality
Open this publication in new window or tab >>Multi-flavor quantum criticality
(English)Manuscript (preprint) (Other academic)
Abstract [en]

The electronic density of states, and, hence, the quasiparticle mass on the Fermi surface, is strongly enhanced through electronic correlations in quantum-critical metals. The nature of electronic correlations in such systems can be constrained by comparing different probes of the electronic density of states. Comparative studies in high-Tc superconductors present a significant challenge because of the masking effect of the superconducting phase. In contrast, the normal state can be readily accessed in the unconventional superconductor CeCoIn5 because the energy scale associated with superconductivity is small. Here, we use thermal impedance spectroscopy to simultaneously access the electronic density of states in CeCoIn5 in two independent ways; via the nuclear spin-lattice relaxation rate and via the electronic specific heat. We establish that the temperature and magnetic field dependence of the nuclear spin-lattice relaxation rate is determined entirely by the electronic density of states on the Fermi surface, where mass enhancement is cut off at high magnetic fields. Surprisingly, the specific heat reveals excess entropy in addition to that associated with the density of states on the Fermi surface. The electronic nature of this excess entropy is evidenced by its suppression in the superconducting state. We postulate that a second 'flavor' of boson generates the observed quantum critical physics beyond the mass renormalization on the Fermi surface in CeCoIn5 and suggest such a multi-flavor character for a broader range of quantum critical metals.

Keywords
heavy fermions, quantum criticality, strongly correlated electron systems, specific heat.
National Category
Condensed Matter Physics
Research subject
Physics
Identifiers
urn:nbn:se:su:diva-240738 (URN)
Available from: 2025-03-12 Created: 2025-03-12 Last updated: 2025-03-12
3. Element-specific probe of quantum criticality in CeCoIn5
Open this publication in new window or tab >>Element-specific probe of quantum criticality in CeCoIn5
(English)Manuscript (preprint) (Other academic)
Abstract [en]

Employing the elemental sensitivity of x-ray absorption spectroscopy (XAS) and x-ray magnetic circular dichroism (XMCD), we study the valence and magnetic order in the heavy fermion superconductor CeCoIn5. We probe spin population of the f-electrons in Ce and d-electrons in Co as a function of temperature (down to 0.1 K) and magnetic field (up to 6 T). From the XAS we find a pronounced contribution of Ce4+ component at low temperature and a clear temperature dependence of the Ce valence below 5 K, suggesting enhanced valence fluctuations, an indication for the presence of a nearby quantum critical point (QCP). We observe no significant corresponding change with magnetic field. The XMCD displays a weak signal for Ce becoming clear only at 6 T. This splitting of the Kramers doublet ground state of Ce3+ is significantly smaller than expected for independent but screened ions, indicating strong antiferromagnetic pair interactions. The unconventional character of superconductivity in CeCoIn5 is evident in the extremely large specific heat step at the superconducting transition.

Keywords
heavy fermions, quantum criticality, strongly correlated electron systems, x-ray spectroscopy.
National Category
Condensed Matter Physics
Research subject
Physics
Identifiers
urn:nbn:se:su:diva-240739 (URN)
Available from: 2025-03-12 Created: 2025-03-12 Last updated: 2025-03-12
4. Precursor to quantum criticality in Ce-Au-Al quasicrystal approximants
Open this publication in new window or tab >>Precursor to quantum criticality in Ce-Au-Al quasicrystal approximants
(English)Manuscript (preprint) (Other academic)
Abstract [en]

Rare-earth element containing aperiodic quasicrystals and their related periodic approximant crystals can exhibit non-trivial physical properties at low temperatures. Here, we investigate the 1/1 and 2/1 approximant crystal phases of the Ce-Au-Al system by studying the ac-susceptibility and specific heat at low temperatures and in magnetic fields up to 12 T. We find that these systems display signs of quantum criticality similar to the observations in other claimed quantum critical systems, including the related Yb-Au-Al quasicrystal. In particular, the ac-susceptibility at low temperatures shows a diverging behavior χ ∝1/T as the temperature decreases as well as cutoff behavior in magnetic field. Notably, the field dependence of χ closely resembles that of quantum critical systems. However, the ac-susceptibility both in zero and nonzero magnetic fields can be understood from the splitting of a ground state Kramers doublet of Ce3+. The high-temperature Curie-Weiss fit yields an effective magnetic moment of approximately 2.54µB per Ce for both approximant systems, which is reduced to∼2.0µB at temperatures below 10 K. The low-temperature specific heat is dominated by the Schottky anomaly originating from the splitting of the Ce3+ Kramers doublet, resulting in an entropy of Rln2 at around 10 K.

Keywords
quasicrystals, approximants, specific heat, heavy fermions, quantum criticality..
National Category
Condensed Matter Physics
Research subject
Physics
Identifiers
urn:nbn:se:su:diva-240740 (URN)
Available from: 2025-03-12 Created: 2025-03-12 Last updated: 2025-03-12
5. Quantum critical scaling of specific heat in a quasicrystal
Open this publication in new window or tab >>Quantum critical scaling of specific heat in a quasicrystal
(English)Manuscript (preprint) (Other academic)
Abstract [en]

In strongly correlated systems, interactions give rise to critical fluctuations surrounding the quantum critical point (QCP) of a quantum phase transition. Quasicrystals allow the study of quantum critical phenomena in aperiodic systems with frustrated magnetic interactions. Here, we study the magnetic field and temperature scaling of the low-temperature specific heat for the quantum critical Yb-Au-Al quasicrystal. We devise a scaling function that encapsulates the limiting behaviors as well as the area where the system goes from a temperature-limited to a field-limited quantum critical region, where magnetic field acts as a cutoff for critical fluctuations. The zero-field electronic specific heat is described by a power-law divergence, Cel/T ∝T−0.54, aligning with previously observed ac-susceptibility and specific heat measurements. The field dependence of the electronic specific heat at high magnetic fields shows a similar power-law Cel/T ∝B−0.50. In the zero-field and low-field region, we observe two small but distinct anomalies in the specific heat, located at 0.7 K and 2.1 K.

Keywords
heavy fermions, quantum criticality, strongly correlated electron systems, specific heat.
National Category
Condensed Matter Physics
Research subject
Physics
Identifiers
urn:nbn:se:su:diva-240742 (URN)
Available from: 2025-03-12 Created: 2025-03-12 Last updated: 2025-03-12
6. Magnetic monopole relaxation effects in spin ice Dy2Ti2O7
Open this publication in new window or tab >>Magnetic monopole relaxation effects in spin ice Dy2Ti2O7
(English)Manuscript (preprint) (Other academic)
Abstract [en]

Spin ice compounds enable the exploration of the dynamics of magnetic monopoles in condensed matter systems. In this study, we use modulation calorimetry to probe the dynamical response of the heat capacity of the classical spin-ice compounds Dy2Ti2O7 at low temperatures (0.5− 5 K). Using modulation frequencies of 0.01-500 Hz we find a strong frequency dependence in the measured heat capacity and are able to study thermal relaxation effects on the corresponding timescales. From the frequency dependence of the heat capacity, the relaxation time τ is extracted from the frequency below which the probed heat capacity is independent of the frequency. The relaxation time shows a divergent behavior below 1 K reaching∼6 s at 0.65 K, similar to the spin relaxation time seen in previous studies. Corresponding specific heat shows a maximum around this temperature. Performing dynamic Monte Carlo simulations we verify that the specific heat frequency response has its origin in the slow magnetic monopole dynamics indigenous to spin ice. We find a timescale of 20 ms per Monte Carlo step at 4 K in contrast to 2.5 ms mentioned in previous studies by other techniques.

Keywords
spin ice, spin freezing, specific heat.
National Category
Condensed Matter Physics
Research subject
Physics
Identifiers
urn:nbn:se:su:diva-240743 (URN)
Available from: 2025-03-12 Created: 2025-03-12 Last updated: 2025-03-12

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