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High Harmonic Spectroscopy from Lower-Order to Higher-Order Topological Insulators
Authors:
Bryan Lorenzo,
Carlos Batista,
Milad Jangjan,
Dasol Kim,
Jean Menotti,
Feng Liu,
Wenlong Gao,
Shambhu Ghimire,
Camilo Granados,
Alexis Chacon
Abstract:
Over the past decades, high-harmonic spectroscopy (HHS) has emerged as a powerful tool for all-optical probing of topological properties of solids. There are outstanding questions regarding universal nature of the spectral features of harmonics in their relationship to the non-trivial topological properties. Here, we present a systematic theoretical study of HHS in topological materials, including…
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Over the past decades, high-harmonic spectroscopy (HHS) has emerged as a powerful tool for all-optical probing of topological properties of solids. There are outstanding questions regarding universal nature of the spectral features of harmonics in their relationship to the non-trivial topological properties. Here, we present a systematic theoretical study of HHS in topological materials, including lower-order and higher-order topological insulators (LOTIs and HOTIs), focusing on observables such as helicity, circular dichroism, ellipticity dependence, and channel-resolved intensity yields. Using the Haldane, Kane-Mele, and breathing Kagome lattice models, we theoretically extend all-optical approaches from the LOTI to the HOTI regime by explicitly incorporating contributions from bulk, edge, and it corner states. Depending on the crystalline system, our calculations suggest that these observables can encode topological information through distinct modifications of the HHG spectra in topological phases. In particular, we identify significant enhancements of the harmonic intensity yields, reaching up to two orders of magnitude relative to trivial phases, together with distinct spectral signatures associated with edge and corner contributions revealed through channel-resolved intensity yields. These results show that channel-resolved HHS provides a promising route for probing topological states in both LOTIs and HOTIs.
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Submitted 24 May, 2026; v1 submitted 21 August, 2025;
originally announced August 2025.
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Quantum interference and occupation control in high harmonic generation from monolayer $WS_2$
Authors:
Minjeong Kim,
Taeho Kim,
Anna Galler,
Dasol Kim,
Alexis Chacon,
Xiangxin Gong,
Yuhui Yang,
Rouli Fang,
Kenji Watanabe,
Takashi Taniguchi,
B. J. Kim,
Sang Hoon Chae,
Moon-Ho Jo,
Angel Rubio,
Ofer Neufeld,
Jonghwan Kim
Abstract:
Two-dimensional hexagonal materials such as transition metal dichalcogenides exhibit valley degrees of freedom, offering fascinating potential for valley-based quantum computing and optoelectronics. In nonlinear optics, the K and K' valleys provide excitation resonances that can be used for ultrafast control of excitons, Bloch oscillations, and Floquet physics. Under intense laser fields, however,…
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Two-dimensional hexagonal materials such as transition metal dichalcogenides exhibit valley degrees of freedom, offering fascinating potential for valley-based quantum computing and optoelectronics. In nonlinear optics, the K and K' valleys provide excitation resonances that can be used for ultrafast control of excitons, Bloch oscillations, and Floquet physics. Under intense laser fields, however, the role of coherent carrier dynamics away from the K/K' valleys is largely unexplored. In this study, we observe quantum interferences in high harmonic generation from monolayer $WS_2$ as laser fields drive electrons from the valleys across the full Brillouin zone. In the perturbative regime, interband resonances at the valleys enhance high harmonic generation through multi-photon excitations. In the strong-field regime, the high harmonic spectrum is sensitively controlled by light-driven quantum interferences between the interband valley resonances and intraband currents originating from electrons occupying various points in the Brillouin zone, also away from K/K' valleys such as $Γ$ and M. Our experimental observations are in strong agreement with quantum simulations, validating their interpretation. This work proposes new routes for harnessing laser-driven quantum interference in two-dimensional hexagonal systems and all-optical techniques to occupy and read-out electronic structures in the full Brillouin zone via strong-field nonlinear optics, advancing quantum technologies.
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Submitted 9 March, 2025; v1 submitted 6 March, 2025;
originally announced March 2025.
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Optimization strategies and artefacts of time-involved small angle neutron scattering experiments
Authors:
Denis Mettus,
Alfonso Chacon,
Andreas Bauer,
Sebastian Mühlbauer,
Christian Pfleiderer
Abstract:
Kinetic small-angle neutron scattering provides access to the microscopic properties of mesoscale systems under slow, periodic perturbations. By interlocking the phases of neutron pulse, sample modulation, and detector signal, so-called Time-Involved Small Angle Neutron scattering Experiments (TISANE) allow to exploit the neutron velocity spread and record data without major sacrifice in intensity…
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Kinetic small-angle neutron scattering provides access to the microscopic properties of mesoscale systems under slow, periodic perturbations. By interlocking the phases of neutron pulse, sample modulation, and detector signal, so-called Time-Involved Small Angle Neutron scattering Experiments (TISANE) allow to exploit the neutron velocity spread and record data without major sacrifice in intensity at time-scales down to micro-seconds. We review the optimization strategies of TISANE that arise from specific aspects of the process of data acquisition and data analysis starting from the basic principles of operation. Typical artefacts of data recorded in TISANE due to the choice of time-binning and neutron chopper pulse width are illustrated by virtue of the response of the skyrmion lattice in MnSi under periodic changes of the direction of the magnetic field stabilizing the skyrmion lattice.
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Submitted 13 December, 2022;
originally announced December 2022.
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Small-angle neutron scattering of long-wavelength magnetic modulations in reduced sample dimensions
Authors:
Grace L. Causer,
Alfonso Chacon,
André Heinemann,
Christian Pfleiderer
Abstract:
Magnetic small-angle neutron scattering (SANS) is ideally suited to provide direct, reciprocal-space information of long-wavelength magnetic modulations, such as helicoids, solitons, merons, or skyrmions. SANS of such structures in thin films or micro-structured bulk materials is strongly limited by the tiny scattering volume vis a vis the prohibitively large background scattering by the substrate…
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Magnetic small-angle neutron scattering (SANS) is ideally suited to provide direct, reciprocal-space information of long-wavelength magnetic modulations, such as helicoids, solitons, merons, or skyrmions. SANS of such structures in thin films or micro-structured bulk materials is strongly limited by the tiny scattering volume vis a vis the prohibitively large background scattering by the substrate and support structures. Considering near-surface scattering closely above the critical angle of reflection, where unwanted signal contributions due to substrate or support structures becomes very small, we establish equivalent scattering patterns of the helical, conical, skyrmion lattice, and fluctuation-disordered phases in a polished bulk sample of MnSi between conventional transmission and near-surface SANS geometries. This motivates the prediction of a complete repository of scattering patterns expected for thin films in the near-surface SANS geometry for each orientation of the magnetic order with respect to the scattering plane.
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Submitted 11 November, 2022;
originally announced November 2022.
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Ultrafast Nonequilibrium Dynamics in Two-dimensional Quantum Spin-Hall Materials
Authors:
Rajesh K. Malla,
Dasol Kim,
Dong Eon Kim,
Alexis Chacón,
Wilton J. M. Kort-Kamp
Abstract:
We develop the theoretical framework of nonequilibrium ultrafast photonics in monolayer quantum spin-Hall insulators supporting a multitude of topological states. In these materials, ubiquitous strong light-matter interactions in the femtosecond scale lead to non-adiabatic quantum dynamics, resulting in topology-dependent nonlinear optoelectronic transport phenomena. We investigate the mechanism d…
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We develop the theoretical framework of nonequilibrium ultrafast photonics in monolayer quantum spin-Hall insulators supporting a multitude of topological states. In these materials, ubiquitous strong light-matter interactions in the femtosecond scale lead to non-adiabatic quantum dynamics, resulting in topology-dependent nonlinear optoelectronic transport phenomena. We investigate the mechanism driving topological Dirac fermions interacting with strong ultrashort light pulses and uncover various experimentally accessible physical quantities that encode fingerprints of the quantum material's topological electronic state from the high harmonic generated spectrum. Our work sets the theoretical cornerstones to realize the full potential of time-resolved harmonic spectroscopy for identifying topological invariants in two-dimensional quantum spin-Hall solid state systems.
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Submitted 27 July, 2022; v1 submitted 26 July, 2022;
originally announced July 2022.
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Understanding Brownian yet non-Gaussian diffusion via long-range molecular interactions
Authors:
Francisco E. Alban Chacón,
Erick A. Lamilla Rubio,
Manuel S. Alvarez Alvarado
Abstract:
In the last years, a few experiments in the fields of biological and soft matter physics in colloidal suspensions have reported normal diffusion with a Laplacian probability distribution in the particles displacements (i.e., Brownian yet non Gaussian diffusion). To model this behavior different stochastic models had been proposed, with all of them introducing new random elements that incorporate o…
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In the last years, a few experiments in the fields of biological and soft matter physics in colloidal suspensions have reported normal diffusion with a Laplacian probability distribution in the particles displacements (i.e., Brownian yet non Gaussian diffusion). To model this behavior different stochastic models had been proposed, with all of them introducing new random elements that incorporate our lack of information about the media. Although these models work in practice, due to their own nature a thorough understanding of how the media interacts with itself and with the Brownian particle in Brownian yet non Gaussian diffusion is outside of their aim and scope. For this reason, a comprehensive mathematical model to explain Brownian yet non Gaussian diffusion that includes molecular interactions is proposed in this paper. Based on the theory of interfaces by Gennes and Langevin dynamics, it is shown that long-range interactions in a weakly interacting fluid and in a microscopic regime of zero viscosity leads to a Laplacian probability distribution in the particles displacements. Further, it is shown that a phase transition can explain a high diffusivity and causes this Laplacian distribution to evolve towards a Gaussian via a transition probability in the interval of time as it was observed in experiments. To validate these model predictions, the experimental data of the Brownian motion of colloidal beads on phospholipid bilayer by Wang et al. is used and compared with the results of the theory. This comparison suggests that the proposed model not only is able to explain qualitatively the Brownian yet non-Gaussian diffusion, but also quantitatively.
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Submitted 28 February, 2022;
originally announced March 2022.
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Effect of interlayer coupling and symmetry on high-order harmonic generation from monolayer and bilayer hexagonal boron nitride
Authors:
Dasol Kim,
Yeon Lee,
Alexis Chacón,
Dong Eon Kim
Abstract:
High-order harmonic generation (HHG) is a fundamental process which can be simplified as the production of high energetic photons from a material subjected to a strong driving laser field. This highly nonlinear optical process contains rich information concerning the electron structure and dynamics of matter, for instance, gases, solids and liquids. Moreover, the HHG from solids has recently attra…
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High-order harmonic generation (HHG) is a fundamental process which can be simplified as the production of high energetic photons from a material subjected to a strong driving laser field. This highly nonlinear optical process contains rich information concerning the electron structure and dynamics of matter, for instance, gases, solids and liquids. Moreover, the HHG from solids has recently attracted the attention of both attosecond science and condensed matter physicist, since the HHG spectra can carry information of electron-hole dynamics in bands and inter- and intra-band current dynamics. In this paper, we study the effect of interlayer coupling and symmetry in two-dimensional (2D) material by analyzing high-order harmonic generation from monolayer and two differently stacked bilayer hexagonal boron nitrides (hBNs). These simulations reveal that high-order harmonic emission patterns strongly depend on crystal inversion symmetry (IS), rotation symmetry and interlayer coupling.
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Submitted 19 December, 2021;
originally announced December 2021.
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High harmonic generation in monolayer and bilayer of transition metal dichalcogenide
Authors:
Yeon Lee,
Dasol Kim,
Dong Eon Kim,
Alexis Chacón
Abstract:
In transition metal dichalcogenides (TMDCs), charge carriers have spin, pseudospin, and valley degrees of freedom associated with magnetic moments. The monolayers and bilayers of the TMDCs, in particular, MoS$_2$, lead strong couplings between the spin and pseudospin effects. This feature have drawn attention to TMDCs for their potential use in advanced tech devices. Meanwhile, high-order harmonic…
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In transition metal dichalcogenides (TMDCs), charge carriers have spin, pseudospin, and valley degrees of freedom associated with magnetic moments. The monolayers and bilayers of the TMDCs, in particular, MoS$_2$, lead strong couplings between the spin and pseudospin effects. This feature have drawn attention to TMDCs for their potential use in advanced tech devices. Meanwhile, high-order harmonic generation (HHG) has recently been applied to the characterization of the electronic structure of solids, such as energy dispersion, Berry-curvature, and topological properties. Here, we show theoretical results obtained with the `philosophy' of using HHG to investigate the structural effects of the monolayer and bilayers of MoS$_2$ on nonlinear optical emission. We use a simple model for MoS$_2$ in the 3R AB staking. We find that the pseudospin and valley indexes (the Berry curvature and the dipole transition matrix element) in TMDC driven by circularly polarized laser (CPL) can encode in the high energy photon emissions. This theoretical investigation is expected to pave the way for the ultrafast manipulation of valleytronics and lead to new questions concerning the spin-obit-coupling (SOC) effects on TMDC materials, Weyl Semimetals, and topological phases and transitions in topological insulators.
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Submitted 24 November, 2021; v1 submitted 22 November, 2021;
originally announced November 2021.
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Compositional Studies of Metals with Complex Order by means of the Optical Floating-Zone Technique
Authors:
Andreas Bauer,
Georg Benka,
Andreas Neubauer,
Alexander Regnat,
Alexander Engelhardt,
Christoph Resch,
Sabine Wurmehl,
Christian G. F. Blum,
Tim Adams,
Alfonso Chacon,
Rainer Jungwirth,
Robert Georgii,
Anatoliy Senyshyn,
Björn Pedersen,
Martin Meven,
Christian Pfleiderer
Abstract:
The availability of large high-quality single crystals is an important prerequisite for many studies in solid-state research. The optical floating-zone technique is an elegant method to grow such crystals, offering potential to prepare samples that may be hardly accessible with other techniques. As elaborated in this report, examples include single crystals with intentional compositional gradients…
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The availability of large high-quality single crystals is an important prerequisite for many studies in solid-state research. The optical floating-zone technique is an elegant method to grow such crystals, offering potential to prepare samples that may be hardly accessible with other techniques. As elaborated in this report, examples include single crystals with intentional compositional gradients, deliberate off-stoichiometry, or complex metallurgy. For the cubic chiral magnets Mn$_{1-x}$Fe$_{x}$Si and Fe$_{1-x}$Co$_{x}$Si, we prepared single crystals in which the composition was varied during growth from $x = 0 - 0.15$ and from $x = 0.1 - 0.3$, respectively. Such samples allowed us to efficiently study the evolution of the magnetic properties as a function of composition, as demonstrated by means of neutron scattering. For the archetypical chiral magnet MnSi and the itinerant antiferromagnet CrB$_{2}$, we grew single crystals with varying initial manganese (0.99 to 1.04) and boron (1.95 to 2.1) content. Measurements of the low-temperature properties addressed the correlation between magnetic transition temperature and sample quality. Furthermore, we prepared single crystals of the diborides ErB$_{2}$, MnB$_{2}$, and VB$_{2}$. In addition to high vapor pressures, these materials suffer from peritectic formation, potential decomposition, and high melting temperature, respectively.
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Submitted 18 November, 2021;
originally announced November 2021.
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All-optical probe of three-dimensional topological insulators based on high-harmonic generation by circularly-polarized laser fields
Authors:
Denitsa Baykusheva,
Alexis Chacón,
Jian Lu,
Trevor P. Bailey,
Jonathan A. Sobota,
Hadas Soifer,
Patrick S. Kirchmann,
Costel R. Rotundu,
Ctirad Uher,
Tony F. Heinz,
David A. Reis,
Shambhu Ghimire
Abstract:
We report the observation of a novel nonlinear optical response from the prototypical three-dimensional topological insulator Bi$_2$Se$_3$ through the process of high-order harmonic generation. We find that the generation efficiency increases as the laser polarization is changed from linear to elliptical, and it becomes maximum for circular polarization. With the aid of a microscopic theory and a…
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We report the observation of a novel nonlinear optical response from the prototypical three-dimensional topological insulator Bi$_2$Se$_3$ through the process of high-order harmonic generation. We find that the generation efficiency increases as the laser polarization is changed from linear to elliptical, and it becomes maximum for circular polarization. With the aid of a microscopic theory and a detailed analysis of the measured spectra, we reveal that such anomalous enhancement encodes the characteristic topology of the band structure that originates from the interplay of strong spin-orbit coupling and time-reversal symmetry protection. Our study reveals a new platform for chiral strong-field physics and presents a novel, contact-free, all-optical approach for the spectroscopy of topological insulators. The implications are in ultrafast probing of topological phase transitions, light-field driven dissipationless electronics, and quantum computation.
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Submitted 30 September, 2021;
originally announced September 2021.
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Theory for all-optical responses in topological materials: the velocity gauge picture
Authors:
Dasol Kim,
Dongbin Shin,
Alexandra S. Landsman,
Dong Eon Kim,
Alexis Chacón
Abstract:
High Harmonic Generation (HHG), which has been widely used in atomic gas, has recently expanded to solids as a means to study highly nonlinear electronic response in condensed matter and produce coherent high frequency radiation with new properties. Most recently, attention has turned to Topological Materials (TMs) and the use of HHG to characterize topological bands and invariants. Theoretical in…
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High Harmonic Generation (HHG), which has been widely used in atomic gas, has recently expanded to solids as a means to study highly nonlinear electronic response in condensed matter and produce coherent high frequency radiation with new properties. Most recently, attention has turned to Topological Materials (TMs) and the use of HHG to characterize topological bands and invariants. Theoretical interpretation of nonlinear electronic response in TMs, however, presents many challenges. In particular, the Bloch wavefunction phase of TMs has undefined points in the Brillouin Zone. This leads to singularities in calculating the inter-band and intra-band transition dipole matrix elements of Semiconductor Bloch Equations (SBEs). Here, we use the laser-electromagnetic velocity gauge ${\boldsymbol p}\cdot {\bf A}(t)$ to numerically integrate the SBEs and treat the singularity in the production of the electrical currents and HHG spectra. We use a prototype of Chern Insulators (CIs), the Haldane model, to demonstrate our approach. We find good qualitative agreement of the velocity gauge compared to the length gauge and the Time-Dependent Density Functional theory in the case of topologically trivial materials such as MoS$_2$. For velocity gauge and length gauge, our two-band Haldane model reproduces key HHG spectra features: ($\textit i$) The selection rules for linear and circular light drivers, ($\textit ii$) The linear cut-off law scaling and ($\textit iii$) The anomalous circular dichroism. We conclude that the velocity-gauge approach captures experimental observations and provides theoretical tools to investigate topological materials.
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Submitted 25 May, 2021;
originally announced May 2021.
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Observation of two independent skyrmion phases in a chiral magnetic material
Authors:
A. Chacon,
L. Heinen,
M. Halder,
A. Bauer,
W. Simeth,
S. Mühlbauer,
H. Berger,
M. Garst,
A. Rosch,
C. Pfleiderer
Abstract:
Magnetic materials can host skyrmions, which are topologically non-trivial spin textures. In chiral magnets with cubic lattice symmetry, all previously-observed skyrmion phases require thermal fluctuations to become thermodynamically stable in bulk materials, and therefore exist only at relatively high temperature, close to the helimagnetic transition temperature. Other stabilization mechanisms re…
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Magnetic materials can host skyrmions, which are topologically non-trivial spin textures. In chiral magnets with cubic lattice symmetry, all previously-observed skyrmion phases require thermal fluctuations to become thermodynamically stable in bulk materials, and therefore exist only at relatively high temperature, close to the helimagnetic transition temperature. Other stabilization mechanisms require a lowering of the cubic crystal symmetry. Here, we report the identification of a second skyrmion phase in Cu$_{2}$OSeO$_{3}$ at low temperature and in the presence of an applied magnetic field. The new skyrmion phase is thermodynamically disconnected from the well-known, nearly-isotropic, high-temperature phase, and exists, in contrast, when the external magnetic field is oriented along the $\langle100\rangle$ crystal axis only. Theoretical modelling provides evidence that the stabilization mechanism is given by well-known cubic anisotropy terms, and accounts for an additional observation of metastable helices tilted away from the applied field. The identification of two distinct skyrmion phases in the same material and the generic character of the underlying mechanism suggest a new avenue for the discovery, design, and manipulation of topological spin textures.
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Submitted 2 April, 2021;
originally announced April 2021.
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Thermodynamic evidence of a second skyrmion lattice phase and tilted conical phase in Cu$_2$0SeO$_3$
Authors:
M. Halder,
A. Chacon,
A. Bauer,
W. Simeth,
S. Mühlbauer,
H. Berger,
L. Heinen,
M. Garst,
A. Rosch,
C. Pfleiderer
Abstract:
Precision measurements of the magnetization and ac susceptibility of Cu$_2$0SeO$_3$ are reported for magnetic fields along different crystallographic directions, focussing on the border between the conical and the field-polarized state for a magnetic field along the $\langle 100 \rangle$ axis, complemented by selected specific heat data. Clear signatures of the emergence of a second skyrmion phase…
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Precision measurements of the magnetization and ac susceptibility of Cu$_2$0SeO$_3$ are reported for magnetic fields along different crystallographic directions, focussing on the border between the conical and the field-polarized state for a magnetic field along the $\langle 100 \rangle$ axis, complemented by selected specific heat data. Clear signatures of the emergence of a second skyrmion phase and a tilted conical phase are observed, as recently identified by means of small-angle neutron scattering. The low-temperature skyrmion phase displays strongly hysteretic phase boundaries, but no dissipative effects. In contrast, the tilted conical phase is accompanied by strong dissipation and higher-harmonic contributions, while the transition fields are essentially nonhysteretic. The formation of the second skyrmion phase and tilted conical phase are found to be insensitive to a vanishing demagnetization factor. A quantitative estimate of the temperature dependence of the magnetocrystalline anisotropy may be consistently inferred from the magnetization and the upper critical field and agrees well with a stabilization of the low-temperature skyrmion phase and tilted conical state by conventional cubic magnetic anisotropies.
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Submitted 31 March, 2021; v1 submitted 30 March, 2021;
originally announced March 2021.
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Strong-field physics in three-dimensional topological insulators
Authors:
Denitsa Baykusheva,
Alexis Chacón,
Dasol Kim,
Dong Eon Kim,
David A. Reis,
Shambhu Ghimire
Abstract:
We investigate theoretically the strong-field regime of light-matter interactions in the topological-insulator class of quantum materials. In particular, we focus on the process of non-perturbative high-order harmonic generation from the paradigmatic three-dimensional topological insulator bismuth selenide (Bi$_2$Se$_3$) subjected to intense mid-infrared laser fields. We analyze the contributions…
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We investigate theoretically the strong-field regime of light-matter interactions in the topological-insulator class of quantum materials. In particular, we focus on the process of non-perturbative high-order harmonic generation from the paradigmatic three-dimensional topological insulator bismuth selenide (Bi$_2$Se$_3$) subjected to intense mid-infrared laser fields. We analyze the contributions from the spin-orbit-coupled bulk states and the topological surface bands separately and reveal a major difference in how their harmonic yields depend on the ellipticity of the laser field. Bulk harmonics show a monotonous decrease in their yield as the ellipticity increases, in a manner reminiscent of high harmonic generation in gaseous media. However, the surface contribution exhibits a highly non-trivial dependence, culminating with a maximum for circularly polarized fields. We attribute the observed anomalous behaviour to: (i) the enhanced amplitude and the circular pattern of the interband dipole and the Berry connections in the vicinity of the Dirac point; and (ii) the influence of the higher-order, "hexagonal warping" terms in the Hamiltonian, which are responsible for the hexagonal deformation of the energy surface at higher momenta. The latter are associated directly with spin-orbit-coupling parameters. Our results thus establish the sensitivity of strong-field driven high harmonic emission to the topology of the band structure as well as to the manifestations of spin-orbit interaction.
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Submitted 3 August, 2020;
originally announced August 2020.
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Weak crystallization of fluctuating skyrmion textures in MnSi
Authors:
J. Kindervater,
I. Stasinopoulos,
A. Bauer,
F. X. Haslbeck,
F. Rucker,
A. Chacon,
S. Mühlbauer,
C. Franz,
M. Garst,
D. Grundler,
C. Pfleiderer
Abstract:
We report an experimental study of the emergence of non-trivial topological winding and long-range order across the paramagnetic to skyrmion lattice transition in the transition metal helimagnet MnSi. Combining measurements of the susceptibility with small angle neutron scattering, neutron resonance spin echo spectroscopy and all-electrical microwave spectroscopy, we find evidence of skyrmion text…
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We report an experimental study of the emergence of non-trivial topological winding and long-range order across the paramagnetic to skyrmion lattice transition in the transition metal helimagnet MnSi. Combining measurements of the susceptibility with small angle neutron scattering, neutron resonance spin echo spectroscopy and all-electrical microwave spectroscopy, we find evidence of skyrmion textures in the paramagnetic state exceeding $10^3$Åwith lifetimes above several 10$^{-9}$s. Our experimental findings establish that the paramagnetic to skyrmion lattice transition in MnSi is well-described by the Landau soft-mode mechanism of weak crystallization, originally proposed in the context of the liquid to crystal transition. As a key aspect of this theoretical model, the modulation-vectors of periodic small amplitude components of the magnetization form triangles that add to zero. In excellent agreement with our experimental findings, these triangles of the modulation-vectors entail the presence of the non-trivial topological winding of skyrmions already in the paramagnetic state of MnSi when approaching the skyrmion lattice transition.
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Submitted 12 November, 2019;
originally announced November 2019.
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Evolution of magneto-crystalline anisotropies in Mn$_{1-x}$Fe$_x$Si and Mn$_{1-x}$Co$_x$Si as inferred from small-angle neutron scattering and bulk properties
Authors:
J. Kindervater,
T. Adams,
A. Bauer,
F. Haslbeck,
A. Chacon,
S. Mühlbauer,
F. Jonietz,
A. Neubauer,
U. Gasser,
G. Nagy,
N. Martin,
W. Häußler,
R. Georgii,
M. Garst,
C. Pfleiderer
Abstract:
We report a comprehensive small-angle neutron scattering~(SANS) study of Mn$_{1-x}$Fe$_{x}$Si at zero magnetic field. To delineate changes of magneto-crystalline anisotropies (MCAs) from effects due to defects and disorder, we recorded complementary susceptibility and specific heat data, and investigated selected compositions of Mn$_{1-x}$Co$_{x}$Si. For all systems studied the transition temperat…
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We report a comprehensive small-angle neutron scattering~(SANS) study of Mn$_{1-x}$Fe$_{x}$Si at zero magnetic field. To delineate changes of magneto-crystalline anisotropies (MCAs) from effects due to defects and disorder, we recorded complementary susceptibility and specific heat data, and investigated selected compositions of Mn$_{1-x}$Co$_{x}$Si. For all systems studied the transition temperature and magnetic phase diagrams evolve monotonically with composition consistent with literature. The SANS patterns of the magnetic order recorded under zero-field cooling display strong changes of the directions of the intensity maxima and smeared out intensity distributions as a function of composition. We show that cubic MCAs account for the complex evolution of the SANS patterns, where for increasing $x$ the character of the MCAs shifts from terms that are fourth-order to terms that are sixth order in spin--orbit coupling. The magnetic field dependence of the susceptibility and SANS establishes that the helix reorientation as a function of magnetic field for Fe- or Co-doped MnSi is dominated by pinning due to defects and disorder. The presence of thermodynamic anomalies of the specific heat at the phase boundaries of the skyrmion lattice phase in the doped samples and properties observed in Mn$_{1-x}$Co$_{x}$Si establishes that the pinning due to defects and disorder remains, however, weak and comparable to the field scale of the helix reorientation. The observation that MCAs, that are sixth order in spin-orbit coupling, play an important role for the spontaneous order in Mn$_{1-x}$Fe$_{x}$Si and Mn$_{1-x}$Co$_{x}$Si, offering a fresh perspective for a wide range of topics in cubic chiral magnets such as the generic magnetic phase diagram, the morphology of topological spin textures, the paramagnetic-to-helical transition, and quantum phase transitions.
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Submitted 5 March, 2020; v1 submitted 29 November, 2018;
originally announced November 2018.
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Ultrafast Laser Driven Many-Body Dynamics and Kondo Coherence Collapse
Authors:
W. Zhu,
Benedikt Fauseweh,
Alexis Chacon,
Jian-Xin Zhu
Abstract:
Ultrafast laser pulse has provided a systematic way to inspect the dynamics of electrons in condensed matter systems. In this paper, by means of time-dependent density matrix renormalization group, we study an ultrafast laser driven Kondo lattice model, in which conduction electrons are strongly coupled with magnetically local moments. The single-particle spectral function due to strong correlatio…
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Ultrafast laser pulse has provided a systematic way to inspect the dynamics of electrons in condensed matter systems. In this paper, by means of time-dependent density matrix renormalization group, we study an ultrafast laser driven Kondo lattice model, in which conduction electrons are strongly coupled with magnetically local moments. The single-particle spectral function due to strong correlation effects and photon emission in the non-equilibrium states under laser driving are calculated. We find laser field excited collective doublon-hole pairs and an associated transient melting of Kondo coherence phase, signifying the collapse of Kondo energy gap. Moreover, we show that the photon emission, induced by a strong laser field, exhibits a different intensity characteristics than in the equilibrium Kondo insulator, which could be explained by the Kondo collapse and related suppression of both intra-band and inter-band contribution in Kondo melting liquid. These theoretical insight is accessible with time- and angle-resolved photoemission spectroscopy and high-harmonic generation spectroscopy, and will stimulate the investigation of nonequilibrium dynamics and nonlinear phenomenon in heavy fermion systems.
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Submitted 1 March, 2021; v1 submitted 29 November, 2018;
originally announced November 2018.
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Search for pressure-induced tricriticality in Cr
Authors:
Alexander Schade,
Tim Adams,
Alfonso Chacon,
Christian Pfleiderer,
Peter B\''oni
Abstract:
The antiferromagnetic ordering of chromium has long been known for its peculiar physical properties. One of them is the observation of the weak first-order character of the N'eel transition that is explained by the lack of a stable fixed point by Bak and Mukamel. Barak et al. predicted that by lowering the symmetry of the order parameter by the application of uniaxial pressure along the [110] dire…
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The antiferromagnetic ordering of chromium has long been known for its peculiar physical properties. One of them is the observation of the weak first-order character of the N'eel transition that is explained by the lack of a stable fixed point by Bak and Mukamel. Barak et al. predicted that by lowering the symmetry of the order parameter by the application of uniaxial pressure along the [110] direction changes the N'eel transition to second-order. In a previous experiment by Fawcett et al., irreversible broadening of the Néel transition was already observed between 160 bar and 300 bar, which could, however, be caused by plastic deformation. Using an improved setup with reduced stress inhomogeneities we succeeded to increase the pressure range until irreversible broadening is observed above 450 bar. Despite the observed tripling of the intensity of the magnetic Bragg peak $[0, 0, 1-δ]$ at $p_{[110]}\geq450\,$bar, indicating a single $\bf{\text{Q}}_\pm$-domain state of the sample, no hints for a tricritical point were observed.
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Submitted 26 November, 2018;
originally announced November 2018.
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Circular dichroism in high-order harmonic generation: Heralding topological phases and transitions in Chern insulators
Authors:
Alexis Chacón,
Dasol Kim,
Wei Zhu,
Shane P. Kelly,
Alexandre Dauphin,
Emilio Pisanty,
Andrew S. Maxwell,
Antonio Picón,
Marcelo F. Ciappina,
Dong Eon Kim,
Christopher Ticknor,
Avadh Saxena,
Maciej Lewenstein
Abstract:
Topological materials are of interest to both fundamental science and advanced technologies, because topological states are robust with respect to perturbations and dissipation. Experimental detection of topological invariants is thus in great demand, but it remains extremely challenging. Ultrafast laser-matter interactions, and in particular high-harmonic generation (HHG), meanwhile, were propose…
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Topological materials are of interest to both fundamental science and advanced technologies, because topological states are robust with respect to perturbations and dissipation. Experimental detection of topological invariants is thus in great demand, but it remains extremely challenging. Ultrafast laser-matter interactions, and in particular high-harmonic generation (HHG), meanwhile, were proposed several years ago as tools to explore the structural and dynamical properties of various matter targets. Here we show that the high-harmonic emission signal produced by a circularly-polarized laser contains signatures of the topological phase transition in the paradigmatic Haldane model. In addition to clear shifts of the overall emissivity and harmonic cutoff, the high-harmonic emission shows a unique circular dichroism, which exhibits clear changes in behavior at the topological phase boundary. Our findings pave the way to understand fundamental questions about the ultrafast electron-hole pair dynamics in topological materials via non-linear high-harmonic generation spectroscopy.
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Submitted 15 July, 2020; v1 submitted 4 July, 2018;
originally announced July 2018.
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Reciprocal space mapping of magnetic order in thick epitaxial MnSi films
Authors:
B. Wiedemann,
A. Chacon,
S. L. Zhang,
Y. Khaydukov,
T. Hesjedal,
O. Soltwedel,
T. Keller,
S. Mühlbauer,
T. Adams,
M. Halder,
C. Pfleiderer,
P. Böni
Abstract:
We report grazing incidence small angle neutron scattering (GISANS) and complementary off-specular neutron reflectometry (OSR) of the magnetic order in a single-crystalline epitaxial MnSi film on Si(111) in the thick film limit. Providing a means of direct reciprocal space mapping, GISANS and OSR reveal a magnetic modulation perpendicular to the films under magnetic fields parallel and perpendicul…
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We report grazing incidence small angle neutron scattering (GISANS) and complementary off-specular neutron reflectometry (OSR) of the magnetic order in a single-crystalline epitaxial MnSi film on Si(111) in the thick film limit. Providing a means of direct reciprocal space mapping, GISANS and OSR reveal a magnetic modulation perpendicular to the films under magnetic fields parallel and perpendicular to the film, where additional polarized neutron reflectometry (PNR) and magnetization measurements are in excellent agreement with the literature. Regardless of field orientation, our data does not suggest the presence of more complex spin textures, notably the formation of skyrmions. This observation establishes a distinct difference with bulk samples of MnSi of similar thickness under perpendicular field, in which a skyrmion lattice dominates the phase diagram. Extended x-ray absorption fine structure measurements suggest that small shifts of the Si positions within the unstrained unit cell control the magnetic state, representing the main difference between the films and thin bulk samples.
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Submitted 2 October, 2017;
originally announced October 2017.
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Entropy-limited topological protection of skyrmions
Authors:
J. Wild,
T. N. G. Meier,
S. Pöllath,
M. Kronseder,
A. Bauer,
A. Chacon,
M. Halder,
M. Schowalter,
A. Rosenauer,
J. Zweck,
J. Müller,
A. Rosch,
C. Pfleiderer,
C. H. Back
Abstract:
Magnetic skyrmions are topologically protected whirls that decay through singular magnetic configurations known as Bloch points. We have used Lorentz transmission electron microscopy to infer the energetics associated with the topological decay of magnetic skyrmions far from equilibrium in the chiral magnet Fe$_{1-x}$Co$_x$Si. We observed that the life time $τ$ of the skyrmions depends exponential…
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Magnetic skyrmions are topologically protected whirls that decay through singular magnetic configurations known as Bloch points. We have used Lorentz transmission electron microscopy to infer the energetics associated with the topological decay of magnetic skyrmions far from equilibrium in the chiral magnet Fe$_{1-x}$Co$_x$Si. We observed that the life time $τ$ of the skyrmions depends exponentially on temperature, $τ\sim τ_0 \, e^{ΔE/k_B T}$. The prefactor $τ_0$ of this Arrhenius law changes by more than 30 orders of magnitude for small changes of magnetic field reflecting a substantial reduction of the life time of skyrmions by entropic effects and thus an extreme case of enthalpy-entropy compensation. Such compensation effects, being well-known across many different scientific disciplines, affect topological transitions and thus topological protection on an unprecedented level.
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Submitted 9 May, 2017; v1 submitted 4 May, 2017;
originally announced May 2017.
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Symmetry breaking, slow relaxation dynamics, and topological defects at the field-induced helix reorientation in MnSi
Authors:
A. Bauer,
A. Chacon,
M. Wagner,
M. Halder. R. Georgii,
A. Rosch,
C. Pfleiderer,
M. Garst
Abstract:
We report a study of the reorientation of the helimagnetic order in the archetypal cubic chiral magnet MnSi as a function of magnetic field direction. The reorientation process as inferred from small-angle neutron scattering, the magnetization, and the ac susceptibility is in excellent agreement with an effective mean-field theory taking into account the precise symmetries of the crystallographic…
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We report a study of the reorientation of the helimagnetic order in the archetypal cubic chiral magnet MnSi as a function of magnetic field direction. The reorientation process as inferred from small-angle neutron scattering, the magnetization, and the ac susceptibility is in excellent agreement with an effective mean-field theory taking into account the precise symmetries of the crystallographic space group. Depending on the field and temperature history and the direction of the field with respect to the crystalline axes, the helix reorientation may exhibit a crossover, a first-order, or a second-order transition. The magnetization and ac susceptibility provide evidence that the reorientation of helimagnetic domains is associated with large relaxation times exceeding seconds. At the second-order transitions residual Ising symmetries are spontaneously broken at continuous elastic instabilities of the helimagnetic order. In addition, on the time scales explored in our experiments these transitions are hysteretic as a function of field suggesting, within the same theoretical framework, the formation of an abundance of plastic deformations of the helical spin order. These deformations comprise topologically non-trivial disclinations, promising novel routes to spintronics applications alongside skyrmions discovered recently in the same class of materials.
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Submitted 21 November, 2016;
originally announced November 2016.
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Spin-valley dynamics of electrically driven ambipolar carbon-nanotube quantum dots
Authors:
E. N. Osika,
A. Chacón,
M. Lewenstein,
B. Szafran
Abstract:
An ambipolar $n$-$p$ double quantum dot defined by potential variation along a semiconducting carbon-nanotube is considered. We focus on the (1e,1h) charge configuration with a single excess electron in the conduction band state confined in the $n$-type dot and a single missing electron in the valence band state of the $p$-dot for which lifting of the Pauli blockade of the current was observed in…
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An ambipolar $n$-$p$ double quantum dot defined by potential variation along a semiconducting carbon-nanotube is considered. We focus on the (1e,1h) charge configuration with a single excess electron in the conduction band state confined in the $n$-type dot and a single missing electron in the valence band state of the $p$-dot for which lifting of the Pauli blockade of the current was observed in the electric-dipole spin resonance [E. A. Laird et al. Nat. Nanotech. 8 , 565 (2013)]. The dynamics of the system driven by periodic electric field is studied with the Floquet theory and the time-dependent configuration interaction method with the single-electron spin-valley-orbitals determined for atomistic tight-binding Hamiltonian. We find that the transitions lifting the Pauli blockade are strongly influenced by coupling to a vacuum state with an empty $n$ dot and a fully filled $p$ dot. The coupling shifts the transition energies and strongly modifies the effective $g$ factors for axial magnetic field. The coupling is modulated by the bias between the dots but it appears effective for surprisingly large energy splitting between the (1e,1h) ground state and the vacuum (0e,0h) state. Multiphoton transitions and high harmonic generation effects are also discussed.
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Submitted 7 November, 2016;
originally announced November 2016.
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Wannier-Bloch approach to localization in high harmonics generation in solids
Authors:
Edyta N. Osika,
Alexis Chacón,
Lisa Ortmann,
Noslen Suárez,
Jose Antonio Pérez-Hernández,
Bartłomiej Szafran,
Marcelo F. Ciappina,
Fernando Sols,
Alexandra S. Landsman,
Maciej Lewenstein
Abstract:
Emission of high-order harmonics from solids provides a new avenue in attosecond science. On one hand, it allows to investigate fundamental processes of the non-linear response of electrons driven by a strong laser pulse in a periodic crystal lattice. On the other hand, it opens new paths toward efficient attosecond pulse generation, novel imaging of electronic wave functions, and enhancement of h…
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Emission of high-order harmonics from solids provides a new avenue in attosecond science. On one hand, it allows to investigate fundamental processes of the non-linear response of electrons driven by a strong laser pulse in a periodic crystal lattice. On the other hand, it opens new paths toward efficient attosecond pulse generation, novel imaging of electronic wave functions, and enhancement of high-order harmonic generation (HHG) intensity. A key feature of HHG in a solid (as compared to the well-understood phenomena of HHG in an atomic gas) is the delocalization of the process, whereby an electron ionized from one site in the periodic lattice may recombine with any other. Here, we develop an analytic model, based on the localized Wannier wave functions in the valence band and delocalized Bloch functions in the conduction band. This Wannier-Bloch approach assesses the contributions of individual lattice sites to the HHG process, and hence addresses precisely the question of localization of harmonic emission in solids. We apply this model to investigate HHG in a ZnO crystal for two different orientations, corresponding to wider and narrower valence and conduction bands, respectively. Interestingly, for narrower bands, the HHG process shows significant localization, similar to harmonic generation in atoms. For all cases, the delocalized contributions to HHG emission are highest near the band-gap energy. Our results pave the way to controlling localized contributions to HHG in a solid crystal, with hard to overestimate implications for the emerging area of atto-nanoscience.
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Submitted 26 July, 2016;
originally announced July 2016.
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Uniaxial pressure dependence of magnetic order in MnSi
Authors:
A. Chacon,
A. Bauer,
T. Adams,
F. Rucker,
G. Brandl,
R. Georgii,
M. Garst,
C. Pfleiderer
Abstract:
We report comprehensive small angle neutron scattering (SANS) measurements complemented by ac susceptibility data of the helical order, conical phase and skyrmion lattice phase (SLP) in MnSi under uniaxial pressures. For all crystallographic orientations uniaxial pressure favours the phase for which a spatial modulation of the magnetization is closest to the pressure axis. Uniaxial pressures as lo…
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We report comprehensive small angle neutron scattering (SANS) measurements complemented by ac susceptibility data of the helical order, conical phase and skyrmion lattice phase (SLP) in MnSi under uniaxial pressures. For all crystallographic orientations uniaxial pressure favours the phase for which a spatial modulation of the magnetization is closest to the pressure axis. Uniaxial pressures as low as 1kbar applied perpendicular to the magnetic field axis enhance the skyrmion lattice phase substantially, whereas the skyrmion lattice phase is suppressed for pressure parallel to the field. Taken together we present quantitative microscopic information how strain couples to magnetic order in the chiral magnet MnSi.
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Submitted 29 December, 2015;
originally announced December 2015.
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Versatile module for experiments with focussing neutron guides
Authors:
T. Adams,
G. Brandl,
A. Chacon,
J. N. Wagner,
M. Rahn,
S. Mühlbauer,
R. Georgii,
C. Pfleiderer,
P. Böni
Abstract:
We report the development of a versatile module that permits fast and reliable use of focussing neutron guides under varying scattering angles. A simple procedure for setting up the module and neutron guides is illustrated by typical intensity patterns to highlight operational aspects as well as typical parasitic artefacts. Combining a high-precision alignment table with separate housings for the…
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We report the development of a versatile module that permits fast and reliable use of focussing neutron guides under varying scattering angles. A simple procedure for setting up the module and neutron guides is illustrated by typical intensity patterns to highlight operational aspects as well as typical parasitic artefacts. Combining a high-precision alignment table with separate housings for the neutron guides on kinematic mounts, the change-over between neutron guides with different focussing characteristics requires no readjustments of the experimental set-up. Exploiting substantial gain factors, we demonstrate the performance of this versatile neutron scattering module in a study of the effects of uniaxial stress on the domain populations in the transverse spin density wave phase of single crystal Cr.
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Submitted 2 December, 2014;
originally announced December 2014.
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Long wavelength helimagnetic order and skyrmion lattice phase in Cu2OSeO3
Authors:
T. Adams,
A. Chacon,
M. Wagner,
A. Bauer,
G. Brandl,
B. Pedersen,
H. Berger,
P. Lemmens,
C. Pfleiderer
Abstract:
We report a long-wavelength helimagnetic superstructure in bulk samples of the ferrimagnetic insulator Cu2OSeO3. The magnetic phase diagram associated with the helimagnetic modulation inferred from small angle neutron scattering and magnetisation measurements includes a skyrmion lattice phase and is strongly reminiscent of MnSi, FeGe and Fe1-xCoxSi, i.e., binary isostructural siblings of Cu2OSeO3…
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We report a long-wavelength helimagnetic superstructure in bulk samples of the ferrimagnetic insulator Cu2OSeO3. The magnetic phase diagram associated with the helimagnetic modulation inferred from small angle neutron scattering and magnetisation measurements includes a skyrmion lattice phase and is strongly reminiscent of MnSi, FeGe and Fe1-xCoxSi, i.e., binary isostructural siblings of Cu2OSeO3 that order helimagnetically. The temperature dependence of the specific heat of Cu2OSeO3 is characteristic of nearly critical spin fluctuations at the helimagnetic transition. This provides putative evidence for effective spin currents as the origin of enhancements of the magneto-dielectric response instead of atomic displacements considered so far.
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Submitted 16 April, 2012;
originally announced April 2012.