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Patrick Pilch

Publications and source records attributed to Patrick Pilch.

11 recordsLinked to original sources

Magnetization processes and spin dynamics across field-induced phase transitions in the quasi-two-dimensional quantum magnet Cu$_2$(OH)$_3$Br

We present magnetic-field-dependent evolution of magnetization and spin dynamics in the quasi-two-dimensional spin-$1/2$ magnet $\mathrm{Cu_2(OH)_3Br}$, consisting of alternately coupled ferromagnetic Cu1 and antiferromagnetic Cu2 spin chains. Terahertz spectroscopy reveals a pronounced field-direction dependence of the low-energy magnetic excitation spectrum. For magnetic fields applied perpendicular to the spin chains, $B\parallel a$ and $B\parallel c^*$, the spectra undergo abrupt reconstructions at the spin-flop transitions identified independently by high-field magnetization measurements. For $B\parallel b$, by contrast, no spin-flop occurs; instead, the excitation spectrum evolves continuously with field and exhibits a strong terahertz radiation polarization dependence as the ferromagnetic Cu1 subsystem becomes progressively polarized. At higher fields, the complex low-field spectrum is replaced by a reduced set of broad excitations, consistent with a weakening of the coupling between the ferromagnetic and antiferromagnetic chain subsystems. Complementary Raman spectroscopy resolves magnon and spinon excitations alongside several phonon modes and traces the characteristic temperature- and magnetic-field-dependent evolution of the magnetic excitations. The combined spectroscopic and magnetization results map out how a magnetic field reorganizes the coupled ferromagnetic and antiferromagnetic subsystems in $\mathrm{Cu_2(OH)_3Br}$ across field-induced phase transitions.

cond-mat.str-el

Giant enhancement of terahertz high-harmonic generation by cavity engineering of a three-dimensional Dirac semimetal

We report on time-resolved ultrafast terahertz high-harmonic generation of strong field driven-dynamics of many-body Dirac fermions. We demonstrate an experimental realization of near saturation regime of the high-order nonlinear responses with a giant enhancement of terahertz third- and fifth-order harmonic yields by cavity-engineering a three-dimensional Dirac semimetal Cd3As2. By fabricating a designed structure of metasurface microcavities on a nanometer Cd3As2 thin film, we significantly enhance the near-field intensity of a picosecond terahertz excitation pulse in resonance with the microcavity eigenmode. The strong terahertz field drives the far-from-equilibrium Dirac fermions deeply into a nonperturbative regime, leading to the observation of near-saturation high-harmonic emission. Our experimental results confirm the predictions by Boltzmann transport theory, and substantiate a field-driven kinetic description of the strong nonthermal nonlinearity at the terahertz frequencies.

cond-mat.mtrl-sci

Terahertz third-harmonic generation of lightwave driven Weyl fermions far from equilibrium

We report on time-resolved ultrafast terahertz third-harmonic generation spectroscopy of nonequilibrium dynamics of Weyl fermions in a nanometer thin film of the Weyl semimetal TaP. Terahertz third-harmonic generation is observed at room temperature under the drive of a multicycle narrowband terahertz pulse with a peak field strength of down to tens of kV/cm. The observed terahertz third-harmonic generation exhibits a perturbative cubic power-law dependence on the terahertz drive. By varying the polarization of the drive pulse from linear to elliptical, we realize a sensitive tuning of the third harmonic yield. By carrying out theoretical analysis based on the Boltzmann transport theory, we can properly describe the experimental results and ascribe the observed THz nonlinearity to field-driven kinetics of the Weyl fermions.

cond-mat.str-el

Quantum spin dynamics of the honeycomb magnet K$_2$Co$_2$TeO$_6$ in high magnetic fields

We present terahertz spectroscopic measurements of quantum spin dynamics in the honeycomb magnet K$_2$Co$_2$TeO$_6$ as a function of temperature, polarization and in an external magnetic field applied in the honeycomb plane. Magnetic excitations are resolved below the magnetic ordering temperature of $T_\text{N}$ = 12 K. In the applied magnetic field, we reveal characteristic field dependence not only for the magnetic excitations observed at zero field, but also a rich set of modes emerging in finite fields. The observed magnetic excitations exhibit clear dependence on the terahertz polarization, and characteristic features at field-induced phase transitions consistent with our high-field magnetization data. We cannot evidently resolve a continuumlike feature, even when the long-range magnetic order is presumably suppressed in the strong magnetic field, indicating that a Kitaev-type interaction, if existing, is subleading in this compound.

cond-mat.str-el

Distinct terahertz third-harmonic generation of many-body excitonic states

The dynamics of an electron-hole plasma governed by strong Coulomb interaction is a challenging many-body problem.We report on experimental realization of electron-hole many-body states in the picosecond time scale, with tunable densities in a representative semiconductor Cu$_2$O. By using time-resolved optical-pump terahertz third-harmonic-generation spectroscopy, we study the nonlinear terahertz dynamical characteristics of the many-body electron-hole states. We find not only efficient and nonperturbative terahertz third-harmonic yield associated with the excitonic formation, but also a nonmonotonic dependence of the excitonic nonlinear response on the electron-hole density, reflecting the exciton dissociation at high charge density. Our results provide an efficient excitonic sensing of the far-from-equilibrium electron-hole many-body states.

cond-mat.str-el

Terahertz electro-optic Kerr effect in LaAlO3

In this letter, we investigate the terahertz (THz) electro-optic Kerr effect (KE) dynamics in LaAlO3 (LAO), a widely used substrate for thin film preparation. We show that the KE dynamics strongly depend on the material anisotropy due to interference between THz field-induced and strain-induced optical birefringence. Such interference leads to quasi-phase matching conditions of the KE, which becomes strongly frequency dependent. Depending on the THz frequency, the KE exhibits a uni- and bipolar shape of the quadratic response. The demonstrated effects will be present in a wide variety of materials used as substrates in different THz-pump laser-probe experiments and need to be considered in order to disentangle the different contributions to the measured ultrafast dynamic signals.

physics.optics

Low-energy spin excitations in field-induced phases of the spin-ladder antiferromagnet BiCu$_2$PO$_6$

We report on terahertz spectroscopic measurements of quantum spin dynamics on single crystals of a spin-1/2 frustrated spin-ladder antiferromagnet BiCu$_2$PO$_6$ as a function of temperature, polarization, and applied external magnetic fields. Spin triplon excitations are observed at zero field and split in applied magnetic fields. For magnetic fields applied along the crystallographic $a$ axis, a quantum phase transition at $B_{c1}=21.4 \mathrm{T}$ is featured by a low-energy excitation mode emerging above $B_{c1}$ which indicates a gap reopening. For fields along the $b$ axis and the $c$ axis, different field dependencies are observed for the spin triplon excitations, whereas no low-lying modes could be resolved at field-induced phase transitions. We perform a theoretical analysis of the magnetic field dependence of the spin triplon modes by using continuous unitary transformations to determine an effective low energy Hamiltonian. Through an exhaustive parameter search we find numerically optimized parameters to very well describe the experimentally observed modes, which corroborate the importance of significant magnetic anisotropy in the system.

cond-mat.str-el

Ultrafast unidirectional spin Hall magnetoresistance driven by terahertz light field

The ultrafast control of magnetisation states in magnetically ordered systems is a key technological challenge for developing memory devices operable at picosecond timescales or terahertz (THz) frequencies. Despite significant efforts in ultrafast magnetic switching, convenient ultrafast readout of magnetic states remains under investigation. Currently, many experiments exploit magneto-optical effects for detecting magnetisation states, necessitating laser sources and optical components. However, energy-efficient and cost-effective electrical detection is preferred for practical applications. Unidirectional spin-Hall magnetoresistance (USMR) was proposed as a simple two-terminal geometry for the electrical detection of the magnetisation state in magnetic heterostructures. Here, we demonstrate that USMR is active at THz frequencies for picosecond time readouts, and can be initiated with light fields. We detect ultrafast USMR in various types of ferromagnet/heavy metal thin film heterostructures through THz second harmonic generation. Our studies, combined with temperature-dependent measurements of USMR, reveal a significant contribution from electron-magnon spin-flip scattering. This suggests possibilities for all-electrical detection of THz magnon modes.

cond-mat.mes-hall

Population inversion and ultrafast terahertz nonlinearity of transient Dirac fermions in Cd$_3$As$_2$

Harmonic generation provides an efficient tool for the study of ultrafast nonlinear dynamics. We report on time-resolved optical-pump terahertz-harmonic-generation spectroscopic investigation of ultrafast nonlinearity in a prototypical three-dimensional Dirac semimetal Cd$_3$As$_2$. A transient population inversion characterized by excessive nonthermal Dirac electrons and holes is found to be very sensitive and responsive to a periodic terahertz drive, leading to very efficient terahertz third-harmonic generation. Based on the Boltzmann transport theory, we analyze the terahertz field-driven kinetics of the transient Dirac fermions that is responsible for the observed strong terahertz nonlinearity.

cond-mat.mtrl-sci

Field and Polarization Dependent Quantum Spin Dynamics in Honeycomb Magnet Na$_2$Co$_2$TeO$_6$: Magnetic Excitations and Continuum

We report terahertz spectroscopic measurements of quantum spin dynamics in the spin-1/2 honeycomb magnet Na$_2$Co$_2$TeO$_6$ as a function of applied magnetic field with different terahertz polarizations. Distinct field dependencies of the resolved spin dynamics are identified in three regimes, which are separated by two critical fields at $B_{c1}\approx 7$ and $B_{c2}\approx 10$ T. A polarization selective continuum is observed in the intermediate phase, featuring spin fluctuations of a proximate quantum spin liquid.

cond-mat.str-el

Ultrafast dynamics of optically excited charge carriers in the room-temperature antiferromagnetic semiconductor $\alpha $-MnTe

We report on time-resolved optical and terahertz ultrafast spectroscopy of charge-carrier dynamics in the room-temperature antiferromagnetic semiconductor $\alpha $-MnTe. By optically pumping the system with 1.55 eV photons at room temperature, we excite charge carriers in the conduction band through the indirect band gap and investigate the dynamical response of nonequilibrium states using optical as well as terahertz transmission probes. Three relaxation processes are revealed by their characteristic relaxation times of the order of 1, 10, and 100~ps, whose exact values are functions of the pump fluence. For high pump fluences nonlinear dependence on the pump fluence is observed both in the optical and terahertz probes.

cond-mat.mtrl-sci