Cotunneling signatures of Spin-Electric coupling in frustrated triangular molecular magnets

The ground state of frustrated (antiferromagnetic) triangular molecular magnets is characterized by two total-spin $S =1/2$ doublets with opposite chirality. According to a group theory analysis [M. Trif \textit{et al.}, Phys. Rev. Lett. \textbf{101}, 217201 (2008)] an external electric field can efficiently couple these two chiral spin states, even when the spin-orbit interaction (SOI) is absent. The strength of this coupling, $d$, is determined by an off-diagonal matrix element of the dipole operator, which can be calculated by \textit{ab-initio} methods [M. F. Islam \textit{et al.}, Phys. Rev. B \textbf{82}, 155446 (2010)]. In this work we propose that Coulomb-blockade transport experiments in the cotunneling regime can provide a direct way to determine the spin-electric coupling strength. Indeed, an electric field generates a $d$-dependent splitting of the ground state manifold, which can be detected in the inelastic cotunneling conductance. Our theoretical analysis is supported by master-equation calculations of quantum transport in the cotunneling regime. We employ a Hubbard-model approach to elucidate the relationship between the Hubbard parameters $t$ and $U$, and the spin-electric coupling constant $d$. This allows us to predict the regime in which the coupling constant $d$ can be extracted from experiment

Elementary Excitations of Ferromagnetic Metal Nanoparticles

We present a theory of the elementary spin excitations in transition metal ferromagnet nanoparticles which achieves a unified and consistent quantum description of both collective and quasiparticle physics. The theory starts by recognizing the essential role played by spin-orbit interactions in determining the energies of ferromagnetic resonances in the collective excitation spectrum and the strength of their coupling to low-energy particle-hole excitations. We argue that a crossover between Landau-damped ferromagnetic resonance and pure-state collective magnetic excitations occurs as the number of atoms in typical transition metal ferromagnet nanoparticles drops below approximately $10^4$, approximately where the single-particle level spacing, $\delta$, becomes larger than, $\sqrt{\alpha} E_{\rm res}$, where $E_{\rm res}$ is the ferromagnetic resonance frequency and $\alpha$ is the Gilbert damping parameter. We illustrate our ideas by studying the properties of semi-realistic model Hamiltonians, which we solve numerically for nanoparticles containing several hundred atoms. For small nanoparticles, we find one isolated ferromagnetic resonance collective mode below the lowest particle-hole excitation energy, at $E_{\rm res} \approx 0.1$ meV. The spectral weight of this pure excitation nearly exhausts the transverse dynamical susceptibility spectral weight. As $\delta$ approaches $\sqrt{\alpha} E_{\rm res}$, the ferromagnetic collective excitation is more likely to couple strongly with discrete particle-hole excitations. In this regime the distinction between the two types of excitations blurs. We discuss the significance of this picture for the interpretation of recent single-electron tunneling experiments.Comment: 19 pages, 13 figure

Magnetization orientation dependence of the quasiparticle spectrum and hysteresis in ferromagnetic metal nanoparticles

We use a microscopic Slater-Koster tight-binding model with short-range exchange and atomic spin-orbit interactions that realistically captures generic features of ferromagnetic metal nanoparticles to address the mesoscopic physics of magnetocrystalline anisotropy and hysteresis in nanoparticle quasiparticle excitation spectra. Our analysis is based on qualitative arguments supported by self-consistent Hartree-Fock calculations for nanoparticles containing up to 260 atoms. Calculations of the total energy as a function of magnetization direction demonstrate that the magnetic anisotropy per atom fluctuates by several percents when the number of electrons in the particle changes by one, even for the largest particles we consider. Contributions of individual orbitals to the magnetic anisotropy are characterized by a broad distribution with a mean more than two orders of magnitude smaller than its variance and with no detectable correlations between anisotropy contribution and quasiparticle energy. We find that the discrete quasiparticle excitation spectrum of a nanoparticle displays a complex non-monotonic dependence on an external magnetic field, with abrupt jumps when the magnetization direction is reversed by the field, explaining recent spectroscopic studies of magnetic nanoparticles. Our results suggests the existence of a broad cross-over from a weak spin-orbit coupling to a strong spin-orbit coupling regime, occurring over the range from approximately 200- to 1000-atom nanoparticles.Comment: 39 pages, 18 figures, to be published in Physical Review

Landau-Zener quantum tunneling in disordered nanomagnets

We study Landau-Zener macroscopic quantum transitions in ferromagnetic metal nanoparticles containing on the order of 100 atoms. The model that we consider is described by an effective giant-spin Hamiltonian, with a coupling to a random transverse magnetic field mimicking the effect of quasiparticle excitations and structural disorder on the gap structure of the spin collective modes. We find different types of time evolutions depending on the interplay between the disorder in the transverse field and the initial conditions of the system. In the absence of disorder, if the system starts from a low-energy state, there is one main coherent quantum tunneling event where the initial-state amplitude is completely depleted in favor of a few discrete states, with nearby spin quantum numbers; when starting from the highest excited state, we observe complete inversion of the magnetization through a peculiar ``backward cascade evolution''. In the random case, the disorder-averaged transition probability for a low-energy initial state becomes a smooth distribution, which is nevertheless still sharply peaked around one of the transitions present in the disorder-free case. On the other hand, the coherent backward cascade phenomenon turns into a damped cascade with frustrated magnetic inversion.Comment: 21 pages, 7 figures, to be published in Phys.Rev.

Thin films of a three-dimensional topological insulator in a strong magnetic field: a microscopic study

The response of thin films of Bi$_2$Se$_3$ to a strong perpendicular magnetic field is investigated by performing magnetic bandstructure calculations for a realistic multi-band tight-binding model. Several crucial features of Landau quantization in a realistic three-dimensional topological insulator are revealed. The $n=0$ Landau level is absent in ultra-thin films, in agreement with experiment. In films with a crossover thickness of five quintuple layers, there is a signature of the $n=0$ level, whose overall trend as a function of magnetic field matches the established low-energy effective-model result. Importantly, we find a field-dependent splitting and a strong spin-polarization of the $n=0$ level which can be measured experimentally at reasonable field strengths. Our calculations show mixing between the surface and bulk Landau levels which causes the character of levels to evolve with magnetic field.Comment: 5 pages, 4 figure