arXiv subjects

A. Pashkin

Publications and source records attributed to A. Pashkin.

At least 19 recordsLinked to original sources

arXiv2023

Coherent phonon and unconventional carriers in the magnetic kagome metal Fe$_3$Sn$_2$

Temperature- and fluence-dependent carrier dynamics of the magnetic Kagome metal Fe$_3$Sn$_2$ were studied using the ultrafast optical pump-probe technique. Two carrier relaxation processes ($\tau_1$ and $\tau_2$) and a laser induced coherent optical phonon were observed. By using the two-temperature model for metals, we ascribe the shorter relaxation $\tau_1$ (~1 ps) to hot electrons transferring their energy to the crystal lattice via electron-phonon scattering. $\tau_2$ (~25 ps), on the other hand, cannot be explained as a conventional process and is attributed to the unconventional (localized) carriers in the material. The observed coherent oscillation is assigned to be a totally symmetric A$_{1g}$ optical phonon dominated by Sn displacements out of the Kagome planes, and possesses a prominently large amplitude, on the order of 10$^{-3}$, comparable to the maximum of the reflectivity change ($\Delta$R/R). This amplitude is equivalent to charge-density-wave (CDW) systems, although no signs of such an instability were hitherto reported in Fe$_3$Sn$_2$. Our results set an unexpected connection between Fe$_3$Sn$_2$ and kagome metals with CDW instabilities, and suggest a unique interplay between phonon and electron dynamics in this compound.

cond-mat.str-el↗

arXiv2018

Slow noncollinear Coulomb scattering in the vicinity of the Dirac point in graphene

The Coulomb scattering dynamics in graphene in energetic proximity to the Dirac point is investigated by polarization resolved pump-probe spectroscopy and microscopic theory. Collinear Coulomb scattering rapidly thermalizes the carrier distribution in k-directions pointing radially away from the Dirac point. Our study reveals, however, that in almost intrinsic graphene full thermalization in all directions relying on noncollinear scattering is much slower. For low photon energies, carrier-optical-phonon processes are strongly suppressed and Coulomb mediated noncollinear scattering is remarkably slow, namely on a ps timescale. This effect is very promising for infrared and THz devices based on hot carrier effects.

cond-mat.mes-hall↗

arXiv2017

Doubly dressed bosons - exciton-polaritons in a strong terahertz field

We demonstrate the existence of a novel quasiparticle: an exciton in a semiconductor doubly dressed with two photons of different wavelengths: near infrared cavity photon and terahertz (THz) photon, with the THz coupling strength approaching the ultra-strong coupling regime. This quasiparticle is composed of three different bosons, being a mixture of a matter-light quasiparticle. Our observations are confirmed by a detailed theoretical analysis, treating quantum mechanically all three bosonic fields. The doubly dressed quasiparticles retain the bosonic nature of their constituents, but their internal quantum structure strongly depends on the intensity of the applied terahertz field.

cond-mat.quant-gas↗

arXiv2015

Tunneling Breakdown of a Strongly Correlated Insulating State in VO$_2$ Induced by Intense Multi-Terahertz Excitation

We directly trace the near- and mid-infrared transmission change of a VO$_2$ thin film during an ultrafast insulator-to-metal transition triggered by high-field multi-terahertz transients. Non-thermal switching into a metastable metallic state is governed solely by the amplitude of the applied terahertz field. In contrast to resonant excitation below the threshold fluence, no signatures of excitonic self-trapping are observed. Our findings are consistent with the generation of spatially separated charge pairs and a cooperative transition into a delocalized metallic state by THz field-induced tunneling. The tunneling process is a condensed-matter analogue of the Schwinger effect in nonlinear quantum electrodynamics. We find good agreement with the pair production formula by replacing the Compton wavelength with an electronic correlation length of 2.1 $Å$.

cond-mat.str-el↗

arXiv2012

Non-perturbative Interband Response of InSb Driven Off-resonantly by Few-cycle Electromagnetic Transients

Intense multi-THz pulses are used to study the coherent nonlinear response of bulk InSb by means of field-resolved four-wave mixing spectroscopy. At amplitudes above 5 MV/cm the signals show a clear temporal substructure which is unexpected in perturbative nonlinear optics. Simulations based on a two-level quantum system demonstrate that in spite of the strongly off-resonant character of the excitation the high-field pulses drive the interband resonances into a non-perturbative regime of Rabi flopping.

physics.optics↗

arXiv2012

Ultrafast transient generation of spin-densitywave order in the normal state of BaFe2As2 driven by coherent lattice vibrations

The interplay among charge, spin and lattice degrees of freedom in solids gives rise to intriguing macroscopic quantum phenomena such as colossal magnetoresistance, multiferroicity and high-temperature superconductivity. Strong coupling or competition between various orders in these systems presents the key to manipulate their functional properties by means of external perturbations such as electric and magnetic fields or pressure. Ultrashort and intense optical pulses have emerged as an interesting tool to investigate elementary dynamics and control material properties by melting an existing order. Here, we employ few-cycle multi-terahertz pulses to resonantly probe the evolution of the spin-density-wave (SDW) gap of the pnictide compound BaFe2As2 following excitation with a femtosecond optical pulse. When starting in the low-temperature ground state, optical excitation results in a melting of the SDW order, followed by ultrafast recovery. In contrast, the SDW gap is induced when we excite the normal state above the transition temperature. Very surprisingly, the transient ordering quasi-adiabatically follows a coherent lattice oscillation at a frequency as high as 5.5 THz. Our results attest to a pronounced spin-phonon coupling in pnictides that supports rapid development of a macroscopic order on small vibrational displacement even without breaking the symmetry of the crystal.

cond-mat.supr-con↗

arXiv2011

Ultrafast Insulator-Metal Phase Transition in VO2 Studied by Multiterahertz Spectroscopy

The ultrafast photoinduced insulator-metal transition in VO2 is studied at different temperatures and excitation fluences using multi-THz probe pulses. The spectrally resolved mid-infrared response allows us to trace separately the dynamics of lattice and electronic degrees of freedom with a time resolution of 40 fs. The critical fluence of the optical pump pulse which drives the system into a long-lived metallic state is found to increase with decreasing temperature. Under all measurement conditions we observe a modulation of the eigenfrequencies of the optical phonon modes induced by their anharmonic coupling to the coherent wave packet motion of V-V dimers at 6.1 THz. Furthermore, we find a weak quadratic coupling of the electronic response to the coherent dimer oscillation resulting in a modulation of the electronic conductivity at twice the frequency of the wave packet motion. The findings are discussed in the framework of a qualitative model based on an approximation of local photoexcitation of the vanadium dimers from the insulating state.

cond-mat.str-el↗

arXiv2010

Femtosecond Quasiparticle and Phonon Dynamics in Superconducting YBa2Cu3O7 Studied by Wideband Terahertz Spectroscopy

We measure the anisotropic mid-infrared response of electrons and phonons in bulk YBa2Cu3O7 after femtosecond photoexcitation. A line shape analysis of specific lattice modes reveals their transient occupation and coupling to the superconducting condensate. The apex oxygen vibration is strongly excited within 150 fs demonstrating that the lattice absorbs a major portion of the pump energy before the quasiparticles are thermalized. Our results attest to substantial electron-phonon scattering and introduce a powerful concept probing electron-lattice interactions in a variety of complex materials.

cond-mat.supr-con↗

arXiv2009

Deconfinement transition and dimensional crossover in the Bechgaard-Fabre salts: pressure- and temperature-dependent optical investigations

The infrared response of the organic conductor (TMTSF)$_2$PF$_6$ and the Mott insulator (TMTTF)$_2$PF$_6$ are investigated as a function of temperature and pressure and for the polarization parallel and perpendicular to the molecular stacks. By applying external pressure on (TMTTF)$_2$PF$_6$, the Mott gap rapidly diminishes until the deconfinement transition occurs when the gap energy is approximately twice the interchain transfer integral. In its deconfined state (TMTTF)$_2$PF$_6$ exhibits a crossover from a quasi-one-dimensional to a higher-dimensional metal upon reducing the temperature. For (TMTSF)$_2$PF$_6$ this dimensional crossover is observed either with increase in external pressure or with decrease in temperature. We quantitatively determine the dimensional crossover line in the pressure-temperature diagram based on the degree of coherence in the optical response perpendicular to the molecular stacks.

cond-mat.str-el↗

arXiv2009

Pressure-induced structural phase transition in the Bechgaard-Fabre salts

The crystal structures of the quasi-one-dimensional organic salts (TMTTF)$_2$PF$_6$ and (TMTSF)$_2$PF$_6$ were studied by pressure-dependent x-ray diffraction up to 10 GPa at room temperature. The unit-cell parameters exhibit a clear anomaly due to a structural phase transition at 8.5 and 5.5 GPa for (TMTTF)$_2$PF$_6$ and (TMTSF)$_2$PF$_6$, respectively.

cond-mat.str-el↗

arXiv2009

Effect of high pressure on multiferroic BiFeO3

We report experimental evidence for pressure instabilities in the model multiferroic BiFeO3 and namely reveal two structural phase transitions around 3 GPa and 10 GPa by using diffraction and far-infrared spectroscopy at a synchrotron source. The intermediate phase from 3 to 9 GPa crystallizes in a monoclinic space group, with octahedra tilts and small cation displacements. When the pressure is further increased the cation displacements (and thus the polar character) of BiFeO3 is suppressed above 10 GPa. The above 10 GPa observed non-polar orthorhombic Pnma structure is in agreement with recent theoretical ab-initio prediction, while the intermediate monoclinic phase was not predicted theoretically.

cond-mat.mtrl-sci↗

arXiv2008

Mott-Hubbard gap closure and structural phase transition in the oxyhalides TiOBr and TiOCl under pressure

Pressure-dependent transmittance and reflectance spectra of TiOBr and TiOCl single crystals at room temperature suggest the closure of the Mott-Hubbard gap, i.e., the gap is filled with additional electronic states extending down to the far-infrared range. According to pressure-dependent x-ray powder diffraction data the gap closure coincides with a structural phase transition. The transition in TiOBr occurs at slightly lower pressure ($p$=14 GPa) compared to TiOCl ($p$=16 GPa) under hydrostatic conditions, which is discussed in terms of the chemical pressure effect. The results of pressure-dependent transmittance measurements on TiOBr at low temperatures reveal similar effects at 23 K, where the compound is in the spin-Peierls phase at ambient pressure.

cond-mat.str-el↗

arXiv2007

Pressure-induced phase transitions in the multiferroic perovskite BiFeO3 studied by far-infrared micro-spectroscopy

We present the results of pressure-dependent far-infrared reflectivity measurements on the multiferroic perovskite BiFeO3 at room temperature. The observed behavior of the infrared-active phonon modes as a funtion of pressure clearly reveals two structural phase transitions around 3.0 and 7.5 GPa, supporting the results of recent Raman and x-ray diffraction studies under pressure. Based on the pressure-dependent frequency shifts of the infrared-active phonon modes we discuss the possible character of the phase transitions.

cond-mat.other↗

arXiv2007

Pressure-induced metallization and structural phase transition of the Mott-Hubbard insulator TiOBr

We investigated the pressure-dependent optical response of the low-dimensional Mott-Hubbard insulator TiOBr by transmittance and reflectance measurements in the infrared and visible frequency range. A suppression of the transmittance above a critical pressure and a concomitant increase of the reflectance are observed, suggesting a pressure-induced metallization of TiOBr. The metallic phase of TiOBr at high pressure is confirmed by the presence of additional excitations extending down to the far-infrared range. The pressure-induced metallization coincides with a structural phase transition, according to the results of x-ray powder diffraction experiments under pressure.

cond-mat.str-el↗

arXiv2007

Metal-insulator transition in the low-dimensional organic conductor (TMTSF)2FSO3 probed by infrared microspectroscopy

We present measurements of the infrared response of the quasi-one-dimensional organic conductor (TMTSF)2$SO3 along (E||a) and perpendicular (E||b') to the stacking axis as a function of temperature. Above the metal-insulator transition related to the anion ordering the optical conductivity spectra show a Drude-like response. Below the transition an energy gap of about 1500 cm-1 (185 meV) opens, leading to the corresponding charge transfer band in the optical conductivity spectra. The analysis of the infrared-active vibrations gives evidence for the long-range crystal structure modulation below the transition temperature and for the short-range order fluctuations of the lattice modulation above the transition temperature. Also we report about a new infrared mode at around 710 cm-1 with a peculiar temperature behavior, which has so far not been observed in any other (TMTSF)2X salt showing a metal-insulator transition. A qualitative model based on the coupling between the TMTSF molecule vibration and the reorientation of electrical dipole moment of the FSO3 anion is proposed, in order to explain the anomalous behavior of the new mode.

cond-mat.str-el↗

arXiv2006

Electronic properties of correlated metals in the vicinity of a charge order transition: optical spectroscopy of $α$-(BEDT-TTF)$_2M$Hg(SCN)$_4$ ($M$ = NH$_4$, Rb, Tl)

The infrared spectra of the quasi-two-dimensional organic conductors $α$-(BEDT-TTF)$_2$$M$Hg(SCN)$_4$ ($M$ = NH$_4$, Rb, Tl) were measured in the range from 50 to 7000 \cm down to low temperatures in order to explore the influence of electronic correlations in quarter-filled metals. The interpretation of electronic spectra was confirmed by measurements of pressure dependant reflectance of $α$-(BEDT-TTF)$_2$KHg(SCN)$_4$ at T=300 K. The signatures of charge order fluctuations become more pronounced when going from the NH$_4$ salt to Rb and further to Tl compounds. On reducing the temperature, the metallic character of the optical response in the NH$_4$ and Rb salts increases, and the effective mass diminishes. For the Tl compound, clear signatures of charge order are found albeit the metallic properties still dominate. From the temperature dependence of the electronic scattering rate the crossover temperature is estimated below which the coherent charge-carriers response sets in. The observations are in excellent agreement with recent theoretical predictions for a quarter-filled metallic system close to charge order.

cond-mat.str-el↗

arXiv2006

Pressure-induced deconfinement of the charge transport in the quasi-one-dimensional Mott insulator (TMTTF)_2AsF_6

We studied the pressure dependence of the room-temperature infrared reflectivity of (TMTTF)_2AsF_6 along all three optical axes. This anisotropic organic compound consists of molecular stacks with orbital overlap along the a direction; due to electronic correlations the system is a quasi-one-dimensional Mott insulator with a charge gap Δ_ρ= 70 meV. The gap is gradually reduced with increasing external pressure, accompanied by the onset of a Drude contribution along the stacking direction. In the perpendicular b' direction a Drude-like optical response is observed for pressures above 2 GPa. This behavior is interpreted in terms of a deconfinement of the electrons in a one-dimensional Mott insulator, i.e. an insulator-to-metal transition which occurs when the interchain transfer integral t_b is approximately equal to half of the charge gap energy. We estimate the values of t_b and the Luttinger liquid parameter K_ρas a function of pressure.

cond-mat.str-el↗

arXiv2006

Pressure-induced insulator-to-metal transition in low-dimensional TiOCl

We studied the transmittance and reflectance of the low-dimensional Mott-Hubbard insulator TiOCl in the infrared and visible frequency range as a function of pressure. The strong suppression of the transmittance and the abrupt increase of the near-infrared reflectance above 12 GPa suggest a pressure-induced insulator-to-metal transition. The pressure-dependent frequency shifts of the orbital excitations, as well as the pressure dependences of the charge gap and the spectral weight of the optical conductivity above the phase transition are presented.

cond-mat.str-el↗