arXiv subjects

D. Hüvonen

Publications and source records attributed to D. Hüvonen.

At least 19 recordsLinked to original sources

arXiv2017

Magnetic Excitations and Continuum of a Field-Induced Quantum Spin Liquid in $α$-RuCl$_3$

We report on terahertz spectroscopy of quantum spin dynamics in $α$-RuCl$_3$, a system proximate to the Kitaev honeycomb model, as a function of temperature and magnetic field. An extended magnetic continuum develops below the structural phase transition at $T_{s2}=62$K. With the onset of a long-range magnetic order at $T_N=6.5$K, spectral weight is transferred to a well-defined magnetic excitation at $\hbar ω_1 = 2.48$meV, which is accompanied by a higher-energy band at $\hbar ω_2 = 6.48$meV. Both excitations soften in magnetic field, signaling a quantum phase transition at $B_c=7$T where we find a broad continuum dominating the dynamical response. Above $B_c$, the long-range order is suppressed, and on top of the continuum, various emergent magnetic excitations evolve. These excitations follow clear selection rules and exhibit distinct field dependencies, characterizing the dynamical properties of the field-induced quantum spin liquid.

cond-mat.str-el↗

arXiv2017

Effect of disorder on a pressure-induced $z=1$ magnetic quantum phase transition

Pressure-induced ordering close to a $z=1$ quantum critical point is studied in the presence of bond disorder in the quantum spin system (C$_4$H$_{12}$N$_2$)Cu$_2$(Cl$_{1-x}$Br$_{x}$)$_6$ (PHCX) by means of muon-spin rotation and relaxation. As for the pure system (C$_4$H$_{12}$N$_2$)Cu$_2$Cl$_6$, pressure allows PHCX with small levels of disorder ($x\leq 7.5\%$) to be driven through a quantum critical point separating a low-pressure quantum paramagnetic phase from magnetic order at high pressures. However, the pressure-induced ordered state is highly inhomogeneous for disorder concentrations $x>1\%$. This behavior might be related to the formation of a quantum Griffiths phase above a critical disorder concentration $7.5\%<x_{\rm c}<15\%$. Br-substitution increases the critical pressure and suppresses critical temperatures and ordered moment sizes.

cond-mat.str-el↗

arXiv2015

Finite-temperature scaling of spin correlations in a partially magnetized Heisenberg $S=1/2$ chain

Inelastic neutron scattering is employed to study transverse spin correlations of a Heisenberg $S=1/2$ chain compound in a magnetic field of 7.5 T. The target compound is the antiferromagnetic Heisenberg $S=1/2$ chain material 2(1,4-Dioxane)$\cdot$2(H$_2$O)$\cdot$CuCl$_2$, or CuDCl for short. The validity and the limitations of the scaling relation for the transverse dynamic structure factor are tested, discussed and compared to the Tomonaga-Luttinger spin liquid theory and to Bethe-ansatz results for the Heisenberg model.

cond-mat.str-el↗

arXiv2015

Dynamics of a bond-disordered $S=1$ quantum magnet near $z=1$ criticality

Neutron scattering is used to study NiCl$_{2-2x}$Br$_{2x}\cdot$4SC(NH$_2$)$_2$, $x=0.06$, a bond-disordered modification of the well-known gapped $S=1$ antiferromagnetic quantum spin system NiCl$_{2}\cdot$4SC(NH$_2$)$_2$. The magnetic excitation spectrum throughout Brillouin zone is mapped out at $T=60$ mK using high-resolution time-of-flight spectroscopy. It is found that the dispersion of spin excitation is renormalized, as compared to that in the parent compound. The lifetime of excitations near the bottom of the band is substantially decreased. No localized states are found below the gap energy $Δ\simeq0.2$ meV. At the same time, localized zero wave vector states are detected above the top of the band. The results are consistent with a more or less continuous random distribution of bond strengths, and a discrete, possibly bimodal, distribution of single-ion anisotropies in the disordered material.

cond-mat.str-el↗

arXiv2015

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 ($\text{Ni(N,N'-bis(3-aminopropyl)propane-1,3-diamine)(}μ\text{-NO}_2\text{)ClO}_4$), at its field-induced Ising quantum critical point. The validity and the limitations of the theoretically predicted scaling relations are tested.

cond-mat.str-el↗

arXiv2015

Spin dynamics in pressure-induced magnetically-ordered phases in PHCC

We present inelastic neutron scattering experiments on the $S=1/2$ frustrated gapped quantum magnet piperazinium hexachlorodicuprate under applied hydrostatic pressure. These results show that at 9 kbar the magnetic triplet excitations in the system are gapless, contrary to what was previously reported. We show that the changes in the excitation spectrum can be primarily attributed to the change in a single exchange pathway.

cond-mat.str-el↗

arXiv2014

Critical exponents and intrinsic broadening of the field-induced transition in NiCl$_2$$\cdot$4SC(NH$_2$)$_2$

The field-induced ordering transition in the quantum spin system NiCl$_2$$\cdot$4SC(NH$_2$)$_2$ is studied by means of neutron diffraction, AC magnetometry and relaxation calorimetry. The interpretation of the data is strongly influenced by a finite distribution of transition fields in the samples, which was present but disregarded in previous studies. Taking this effect into account, we find that the order-parameter critical exponent is inconsistent with the BEC universality class even at temperatures below 100 mK. All results are discussed in comparison with previous measurements and with recent similar studies of disordered Ni(Cl$_{1-x}$Br$_x$)$_2$$\cdot$4SC(NH$_2$)$_2$.

cond-mat.str-el↗

arXiv2014

Formation of gapless triplets in the bond-doped spin-gap antiferromagnet (C$_4$H$_{12}$N$_2$)(Cu$_2$Cl$_6$)

We report results of an electron spin resonance (ESR) study of a spin-gap antiferromagnet (C$_4$H$_{12}$N$_2$)(Cu$_2$Cl$_6$) (nicknamed PHCC) with chlorine ions partially substituted by bromine. We found that up to 10% of nominal doping the contribution of the random defects to the absorption spectra remains at about 0.1% per copper ion, almost the same as in the pure system. Instead, a particular kind of ESR absorption corresponding to gapless S=1 triplets is observed at low temperatures in samples with high nominal bromine content x>5%. Increase of bromine concentration also leads to the systematic broadening of ESR absorption line indicating reduction of the quasi-particles lifetime.

cond-mat.str-el↗

arXiv2014

Pressure-induced quantum critical and multicritical points in a frustrated spin liquid

The quantum spin liquid compound (C$_4$H$_{12}$N$_2$)Cu$_2$Cl$_6$ (PHCC) is studied by $μ$SR under hydrostatic pressures up to 23.6 kbar. At low temperatures, pressure-induced incommensurate magnetic order is detected beyond a quantum critical point at $P_c\sim4.3$ kbar. An additional phase transition to a different ordered phase is observed at $P_1\sim 13.4$ kbar. The data indicate that the high-pressure phase may be a commensurate one. The established $(P-T)$ phase diagram reveals the corresponding pressure-induced multicritical point at $P_1$, $T_1=2.0$ K.

cond-mat.str-el↗

arXiv2013

Field-concentration phase diagram of a quantum spin liquid with bond defects

The magnetic susceptibility of the gapped quantum spin liquid compound (C$_4$H$_{12}$N$_2$)Cu$_2$Cl$_6$ and its chemically disordered derivatives (C$_4$H$_{12}$N$_2$)Cu$_2$(Cl$_{1-x}$Br$_{x}$)$_6$ are systematically studied in magnetic fields of up to 45 T, as a function of Br concentration. The corresponding field-temperature and field-concentration phase diagrams are determined. Measurements on the disorder-free parent compound are not fully consistent with previously published results by other authors [PRL{\bf 96}, 257203 (2006)]. The effect of Br/Cl substitution on the magnetic properties is superficially similar to that of finite temperature. However, important differences are identified and discussed with reference to the previously studied magnetic excitation spectra.

cond-mat.str-el↗

arXiv2013

Infrared spectroscopy of small-molecule endofullerenes

Hydrogen is one of the few molecules which has been incarcerated in the molecular cage of C$_{60}$ and forms endohedral supramolecular complex H$_2$@C$_{60}$. In this confinement hydrogen acquires new properties. Its translational motion becomes quantized and is correlated with its rotations. We applied infrared spectroscopy to study the dynamics of hydrogen isotopologs H$_2$, D$_2$ and HD incarcerated in C$_{60}$. The translational and rotational modes appear as side bands to the hydrogen vibrational mode in the mid infrared part of the absorption spectrum. Because of the large mass difference of hydrogen and C$_{60}$ and the high symmetry of C$_{60}$ the problem is identical to a problem of a vibrating rotor moving in a three-dimensional spherical potential. The translational motion within the C$_{60}$ cavity breaks the inversion symmetry and induces optical activity of H$_2$. We derive potential, rotational, vibrational and dipole moment parameters from the analysis of the infrared absorption spectra. Our results were used to derive the parameters of a pairwise additive five-dimensional potential energy surface for H$_2$@C$_{60}$. The same parameters were used to predict H$_2$ energies inside C$_{70}$[Xu et al., J. Chem. Phys., {\bf 130}, 224306 (2009)]. We compare the predicted energies and the low temperature infrared absorption spectra of H$_2$@C$_{70}$.

physics.chem-ph↗

arXiv2012

Field-induced criticality in a gapped quantum magnet with bond disorder

Neutron diffraction and calorimetric measurements are used to study the field-induced quantum phase transition in piperazinium-Cu$_2$(Cl$_{1-x}$Br$_x$)$_6$ ($x=0$, x=3.5% and x=7.5%), a prototypical quantum antiferromagnet with random bonds. The critical indexes $ϕ$ and $β$ are determined. The findings contradict some original predictions for Bose Glass based on the assumption $z=d$, but are consistent with recent theoretical results implying $z<d$. Inelastic neutron experiments reveal that disorder has a profound effect on the lowest-energy magnetic gap excitation in the system.

cond-mat.str-el↗

arXiv2011

Electron spin resonance study of anisotropic interactions in a two-dimensional spin gap magnet PHCC

Fine details of the excitation spectrum of the two-dimensional spin-gap magnet PHCC are revealed by electron spin resonance investigations. The values of anisotropy parameters and the orientations of the anisotropy axes are determined by accurate measurements of the angular, frequency-field and temperature dependences of the resonance absorption. The properties of a spin-gap magnet in the vicinity of critical field are discussed in terms of sublevel splittings and g-factor anisotropy.

cond-mat.str-el↗

arXiv2011

Comment on "Transition from Bose glass to a condensate of triplons in Tl$_{1-x}$K$_x$CuCl$_3$"

We argue that the interpretation of the calorimetric data for disordered quantum antiferromagnets Tl$_{1-x}$K$_x$CuCl$_3$ in terms of Bose Glass physics by F. Yamada {\it et al.} in [Phys. Rev. B {\bf 83}, 020409(R) (2011)] is not unambiguous. A consistent analysis shows no difference in the crossover critical index for the disorder-free TlCuCl$_3$ and its disordered derivatives. Furthermore, we question the very existence of a proper field-induced thermodynamic phase transition in Tl$_{1-x}$K$_x$CuCl$_3$.

cond-mat.str-el↗

arXiv2009

Magnetic excitations and optical transitions in the multiferroic spin-1/2 system LiCu$_2$O$_2$

Magnetic excitations in cycloidal magnet LiCu$_2$O$_2$ are explored using THz absorption spectroscopy in magnetic fields up to 12 T. Below the spin ordering temperature we observe eight optically active transitions in the spin system of LiCu$_2$O$_2$ in the energy range from 4 to 30 cm$^{-1}$. In magnetic field the number of modes increases and the electric polarization flop is seen as a change in magnetic field dependence of mode energies. The polarization dependence of two of the modes in zero magnetic field fits the selection rules for the cycloid tilted by $θ=41\pm1^{\circ}$ from the bc plane. For the remaining six modes electric and magnetic dipole approximations cannot explain the observed polarization dependence. We do not see the electromagnon in the explored energy range although there is evidence that it could exist below 4 cm$^{-1}$.

cond-mat.str-el↗

arXiv2009

Rotor in a Cage: Infrared Spectroscopy of an Endohedral Hydrogen-Fullerene Complex

We report the observation of quantized translational and rotational motion of molecular hydrogen inside the cages of C60. Narrow infrared absorption lines at the temperature of 6K correspond to vibrational excitations in combination with translational and rotational excitations and show well resolved splittings due to the coupling between translational and rotational modes of the endohedral H2 molecule. A theoretical model shows that H2 inside C60 is a three-dimensional quantum rotor moving in a nearly spherical potential. The theory provides both the frequencies and the intensities of the observed infrared transitions. Good agreement with the experimental results is obtained by fitting a small number of empirical parameters to describe the confining potential, as well as the ortho to para ratio.

physics.chem-ph↗

arXiv2007

Magneto-optic far-infrared study of Sr$_{14}$Cu$_{24}$O$_{41}$: triplet excitations in chains

Using far-infrared spectroscopy we have studied the magnetic field and temperature dependence of the spin gap modes in the chains of Sr$_{14}$Cu$_{24}$O$_{41}$. Two triplet modes T$_1$ and T$_2$ were found in the center of the Brillouin zone at $Δ_1=9.65$ meV and $Δ_2=10.86$ meV in zero magnetic field. The T$_1$ mode was excited when the electric field vector ${\bf E}$ of the light was polarized along the b axis (perpendicular to the planes of chains and ladders) and T$_2$ was excited for ${\bf E}\parallel {\bf a}$ (perpendicular to the chains and along the rungs). Up to the maximum magnetic field of 18 T, applied along the chains, the electron $g$ factors of these two modes were similar, $g_{1c}=2.049$ and $g_{2c}=2.044$. Full linewidth at half maximum for both modes was 1 cm$^{-1}$ (0.12 meV) at 4K and increased with $T$. The temperature dependence of mode energies and line intensities was in agreement with the inelastic neutron scattering results from two groups [Matsuda {\it et al.}, Phys. Rev. B {\bf 59}, 1060 (1999) and Regnault {\it et al.}, Phys. Rev. B {\bf 59}, 1055 (1999)]. The T$_1$ mode has not been observed by inelastic neutron scattering in the points of the $k$-space equivalent to the center of the Brillouin zone. Our study indicates that the zone structure model of magnetic excitations of Sr$_{14}$Cu$_{24}$O$_{41}$ must be modified to include a triplet mode at 9.65 meV in the center of the magnetic Brillouin zone.

cond-mat.other↗

arXiv2004

Far-infrared spectroscopy of spin excitations and Dzyaloshinskii-Moriya interactions in a Shastry-Sutherland compound SrCu$_2$(BO$_3$)$_2

We have studied spin excitation spectra in the Shastry-Sutherland model compound SrCu$_2$(BO$_3$)$_2$ in magnetic fields using far-infrared Fourier spectroscopy. The transitions from the ground singlet state to the triplet state at 24 cm$^{-1}$ and to several bound triplet states are induced by the electric field component of the far-infrared light. To explain the light absorption in the spin system we invoke a dynamic Dzyaloshinskii-Moriya (DM) mechanism where light couples to a phonon mode, allowing the DM interaction. Two optical phonons couple light to the singlet to triplet transition in SrCu$_2$(BO$_3$)$_2$. One is $a$-polarized and creates an intra-dimer dynamic DM along the c axis. The other is $c$-polarized and creates an intra-dimer dynamic DM interaction, it is in the $(ab)$ plane and perpendicular to the dimer axis. Singlet levels at 21.5 and 28.6 cm$^{-1}$ anti-cross with the first triplet as is seen in far-infrared spectra. We used a cluster of two dimers with a periodic boundary condition to perform a model calculation with scaled intra- and inter-dimer exchange interactions. Two static DM interactions are sufficient to describe the observed triplet state spectra. The static inter-dimer DM in the c-direction $d_1=0.7$ cm$^{-1}$ splits the triplet state sub-levels in zero field [Cépas et al., Phys. Rev. Lett. \textbf{87}, 167205 (2001)]. The static intra-dimer DM in the $(ab)$ plane (perpendicular to the dimer axis) $d_2=1.8$ cm$^{-1}$, allowed by the buckling of CuBO$_3$ planes, couples the triplet state to the 28.6 cm$^{-1}$ singlet as is seen from the avoided crossing.

cond-mat.other↗