arXiv subjects

M. Mootz

Publications and source records attributed to M. Mootz.

15 recordsLinked to original sources

arXiv2025

Observation of Superconducting Solitons by Terahertz-Light-Driven Persistent Pseudo-Spin Coherence

Overcoming the decoherence bottleneck remains a central challenge for advancing coherent superconducting quantum device and information technologies. Solitons -- non-dispersive wave packets stabilized by the collective synchronization of quantum excitations -- offer a robust pathway to mitigating dephasing, yet their realization in superconductors has remained experimentally elusive. Here, we report the observation of a driven soliton state in epitaxial thin films of an iron-based superconductor (Co-doped BaFe$_2$As$_2$), induced by intense, multi-cycle terahertz (THz) periodic driving. The dynamical transition to this soliton state is marked by the emergence of Floquet-like spectral sidebands that exhibit a strongly nonlinear dependence on THz laser field strength and a resonant enhancement with temperature. Quantum kinetic simulations corroborate these observations, allowing us to underpin the emergence of synchronized Anderson pseudo-spin oscillations -- analogous to Dicke superradiance -- mediated by persistent order parameter oscillations. In this coherently driven state, the observed sidebands result from difference-frequency mixing between the THz drive and persistent soliton dynamics. These findings establish a robust framework for coherently driving and controlling superconducting soliton time-crystal-like phases using low dissipation, time-periodic THz fields, enabling prospects for THz-speed quantum gate operations, long-lived quantum memory, and robust quantum sensing based on enhanced macroscopic pseudo-spin coherence.

cond-mat.supr-con↗

arXiv2024

Coherent Transfer of Lattice Entropy via Extreme Nonlinear Phononics in Metal Halide Perovskites

Entropy transfer in metal halide perovskites, characterized by significant lattice anharmonicity and low stiffness, underlies the remarkable properties observed in their optoelectronic applications, ranging from solar cells to lasers. The conventional view of this transfer involves stochastic processes occurring within a thermal bath of phonons, where lattice arrangement and energy flow from higher to lower frequency modes. Here we unveil a comprehensive chronological sequence detailing a conceptually distinct, coherent transfer of entropy in a prototypical perovskite CH$_3$NH$_3$Pbl$_3$. The terahertz periodic modulation imposes vibrational coherence into electronic states, leading to the emergence of mixed (vibronic) quantum beat between approximately 3 THz and 0.3 THz. We highlight a well-structured, bi-directional time-frequency transfer of these diverse phonon modes, each developing at different times and transitioning from high to low frequencies from 3 to 0.3 THz, before reversing direction and ascending to around 0.8 THz. First-principles molecular dynamics simulations disentangle a complex web of coherent phononic coupling pathways and identify the salient roles of the initial modes in shaping entropy evolution at later stages. Capitalizing on coherent entropy transfer and dynamic anharmonicity presents a compelling opportunity to exceed the fundamental thermodynamic (Shockley-Queisser) limit of photoconversion efficiency and to pioneer novel optoelectronic functionalities.

cond-mat.mtrl-sci↗

arXiv2024

Extreme Terahertz Magnon Multiplication Induced by Resonant Magnetic Pulse Pairs

Nonlinear interactions of spin-waves and their quanta, magnons, have emerged as prominent candidates for interference-based technology, ranging from quantum transduction to antiferromagnetic spintronics. Yet magnon multiplication in the terahertz (THz) spectral region represents a major challenge. Intense, resonant magnetic fields from THz pulse-pairs with controllable phases and amplitudes enable high order THz magnon multiplication, distinct from non-resonant nonlinearities such as the high harmonic generation by below-band gap electric fields. Here, we demonstrate exceptionally high-order THz nonlinear magnonics. It manifests as 7$^\text{th}$-order spin-wave-mixing and 6$^\text{th}$ harmonic magnon generation in an antiferromagnetic orthoferrite. We use THz multi-dimensional coherent spectroscopy to achieve high-sensitivity detection of nonlinear magnon interactions up to six-magnon quanta in strongly-driven many-magnon correlated states. The high-order magnon multiplication, supported by classical and quantum spin simulations, elucidates the significance of four-fold magnetic anisotropy and Dzyaloshinskii-Moriya symmetry breaking. Moreover, our results shed light on the potential quantum fluctuation properties inherent in nonlinear magnons.

cond-mat.str-el↗

arXiv2023

Discovery of an Unconventional Quantum Echo by Interference of Higgs Coherence

Nonlinearities in quantum systems are fundamentally characterized by the interplay of phase coherences, their interference, and state transition amplitudes. Yet the question of how quantum coherence and interference manifest in transient, massive Higgs excitations, prevalent within both the quantum vacuum and superconductors, remains elusive. One hallmark example is photon echo, enabled by the generation, preservation, and retrieval of phase coherences amid multiple excitations. Here we reveal an unconventional quantum echo arising from the Higgs coherence in superconductors, and identify distinctive signatures attributed to Higgs anharmonicity. A terahertz pulse-pair modulation of the superconducting gap generates a "time grating" of coherent Higgs population, which scatters echo signals distinct from conventional spin- and photon-echoes in atoms and semiconductors. These manifestations appear as Higgs echo spectral peaks occurring at frequencies forbidden by equilibrium particle-hole symmetry, an asymmetric delay in the echo formation from the dynamics of the "reactive" superconducting state, and negative time signals arising from Higgs-quasiparticle anharmonic coupling. The Higgs interference and anharmonicity control the decoherence of driven superconductivity and may enable applications in quantum memory and entanglement.

cond-mat.str-el↗

arXiv2022

Quantum Coherence Tomography of Lightwave Controlled Superconductivity

Lightwave periodic driving of nearly dissipation-less currents has recently emerged as a universal control concept for both superconducting (SC) and topological electronics applications. While exciting progress has been made towards THz-driven superconductivity, our understanding of the interactions able to drive non-equilibrium pairing is still limited, partially due to the lack of direct measurements of high-order correlation functions. Such measurements would exceed conventional single-particle spectroscopies and perturbative responses to fully characterize quantum states far-from-equilibrium. Particularly, sensing of the exotic collective modes that would uniquely characterize lightwave-driven SC coherence, in a way analogous to the Meissner effect, is very challenging but much needed. Here we report the discovery of lightwave-controlled superconductivity via parametric time-periodic driving of the strongly-coupled bands in iron-based superconductors by a unique phase-amplitude collective mode assisted by broken-symmetry THz supercurrents. We are able to measure non-perturbative, high-order correlations in this strongly-driven superconductivity by separating the THz multi-dimensional coherent spectra into conventional pump-probe, Higgs collective mode, and pronounced bi--Higgs frequency sideband peaks with highly nonlinear field dependence. We attribute the drastic transition in the coherent spectra to parametric excitation of time-dependent pseudo--spin canting states modulated by a phase-amplitude collective mode that manifests as a strongly nonlinear shift from $ω_\mathrm{Higgs}$ to 2$ω_\mathrm{Higgs}$. Remarkably, the latter higher--order sidebands dominate over the lower-order pump-probe and Higgs mode peaks above critical field, which indicates the breakdown of the susceptibility perturbative expansion in the parametrically-driven SC state.

cond-mat.supr-con↗

arXiv2021

Ultrafast generation and detection of propagating coherent acoustic phonon wave packets in ultra-thin iron pnictide films

We observe pronounced oscillations in differential reflectivity of 9 nm and 60 nm BaFe\textsubscript{2}As\textsubscript{2} (Ba-122) thin films using ultrafast optical spectroscopy. Our studies show that the oscillations result from propagating longitudinal acoustic (LA) phonon wave packets with strong thickness and temperature dependence. Particularly, the experimentally measured oscillation frequency approaches to 50 GHz for the ultra-thin film. Our calculations show that Young's modulus of 9 nm thin film is nearly four times as large as that of 60 nm thin film, consistent with the experiment. The increase in Young's modulus as thickness decrease was attributed to the decrease in parent Ba-122 tetragonality $c/a$ near the film-substrate interface due to material-substrate mismatch effect. %Temperature dependence of LA phonon mode frequency for 9 nm Ba-122 thin film is reported. The temperature-dependent change in LA phonon frequency was attributed to the change in parent Ba-122 othorhombicity $(a-b)/(a+b)$.

cond-mat.mtrl-sci↗

arXiv2020

Light Quantum Control of Persisting Higgs Modes in Iron-Based Superconductors

The Higgs mechanism, i.e., spontaneous symmetry breaking of the quantum vacuum, is a cross-disciplinary principle, universal for understanding dark energy, antimatter and quantum materials, from superconductivity to magnetism. Yet, Higgs modes in one-band superconductors (SCs) are currently under debate due to their competition with charge-density fluctuations. A distinct Higgs mode, controllable by terahertz (THz) laser pulses, can arise in multi-band, unconventional SCs via strong {\em interband} Coulomb interaction, but is yet to be accessed. Here we both discover and demonstrate quantum control of such collective mode in iron-based high-temperature superconductors. Using two-pulse, phase coherent THz spectroscopy, we observe a tunable and coherent 2$Δ_{\mathrm{SC}}$ amplitude oscillation of the complex order parameter in such SC with coupled lower and upper bands. The nonlinear dependence of the amplitude mode oscillations on the THz driving fields is distinct from any one-band and conventional SC results: we observe a large nonlinear change of resonance strength, yet with a persisting mode frequency. We argue that this result provides compelling evidence for a transient coupling between the electron and hole amplitude modes via strong interband coherent interaction. To support this scenario, we perform quantum kinetic modeling of a hybrid Higgs mechanism without invoking extra disorder or phonons. In addition to distinguishing between collective modes and charge fluctuations, the light quantum control of multiband SCs can be extended to probe and manipulate many-body entanglement and hidden symmetries in different quantum materials.

cond-mat.supr-con↗

arXiv2020

Discovery of Light-induced Metastable Martensitic Anomaly Controlled by Single-Cycle Terahertz Pulses

We report on an ultrafast photoinduced phase transition with a strikingly long-lived Martensitic anomaly driven by above-threshold single-cycle terahertz (THz) pulses in Nb$_3$Sn. A non-thermal, THz-induced depletion of low frequency conductivity indicates increased gap splitting of high energy $Γ_{12}$ bands by removal of their degeneracies which enhances the Martensitic phase. In contrast, optical pumping leads to a $Γ_{12}$ gap melting. Such light-induced non-equilibrium Martensitic instability persists up to a critical temperature $\sim$100 K, i.e., more than twice the equilibrium temperature, and can be stabilized beyond technologically-relevant, nanosecond timescales. Together with first-principle simulations, we identify a compelling THz tuning of structural fluctuations via E$_u$ phonons to achieve a non-equilibrium ordering at high temperatures far exceeding those for equilibrium states.

cond-mat.str-el↗

arXiv2019

Light-Driven Raman Coherence as a Non-Thermal Route to Ultrafast Topology Switching

A grand challenge underlies the entire field of topology-enabled quantum logic and information science: how to establish topological control principles driven by quantum coherence and understand the time-dependence of such periodic driving? Here we demonstrate a THz pulse-induced phase transition in Dirac materials that is periodically driven by vibrational coherence due to excitation of the lowest Raman-active mode. Above a critical field threshold, there emerges a long-lived metastable phase with unique Raman coherent phonon-assisted switching dynamics, absent for optical pumping. The switching also manifest itself by non-thermal spectral shape, relaxation slowing down near the Lifshitz transition where the critical Dirac point (DP) occurs, and diminishing signals at the same temperature that the Berry curvature induced Anomalous Hall Effect varnishes. These results, together with first-principles modeling, identify a mode-selective Raman coupling that drives the system from strong to weak topological insulators, STI to WTI, with a Dirac semimetal phase established at a critical atomic displacement controlled by the phonon pumping. Harnessing of vibrational coherence can be extended to steer symmetry-breaking transitions, i.e., Dirac to Weyl ones, with implications on THz topological quantum gate and error correction applications.

cond-mat.str-el↗

arXiv2019

Discovery of Terahertz Second Harmonic Generation from Lightwave Acceleration of Symmetry--Breaking Nonlinear Supercurrents

We report terahertz (THz) second harmonic generation (SHG) in superconductors (SC) with inversion symmetric equilibrium states that forbid even-order nonlinearities. Such SHG signal is observed in single-pulse emission by periodic driving with a multi-cycle THz electric field tuned below the SC energy gap and vanishes above the SC critical temperature. We explain the microscopic physics by a dynamical symmetry breaking principle at sub-THz-cycle by using quantum kinetic modeling of the interplay between strong THz-lightwave nonlinearity and pulse propagation. The resulting non-zero integrated pulse area inside the SC drives lightwave nonlinear supercurrents due to sub--cycle Cooper pair acceleration, in contrast to d.c.-biased superconductors, which can be controlled by the bandstructure and the THz pump field.

cond-mat.supr-con↗

arXiv2018

Competing Orders and Ultrafast Energy Transfer at the Quantum Limit in a Nb$_3$Sn Superconductor Probed by Terahertz Electrodynamics

We report the low-energy electrodynamics of a moderately clean A15 superconductor (SC) following ultrafast excitation to understand and manipulate terahertz (THz) quasi--particle (QP) transport by tuning pump photoexcitation of from competing orders. Using 35-fs optical pulses, we observe a non-thermal enhancement in the low frequency conductivity, opposite to that observed for THz pump, which persists up to an additional critical temperature, above the SC one, from an electronic order in the Martensitic normal state. In the SC state, the fluence dependence of pair breaking kinetics together with an analytic model provides evidence for a `one photon-to-one pair' non-resonant energy transfer during the laser pulse. Such initial transfer of photon energy $\hbarω$ to QPs at the {\em quantum} limit, set by $2Δ_{SC}/\hbarω$=0.33$\%$, is more than one order of magnitude smaller than in previously studied BCS SCs, which we attribute to strong electron--phonon coupling and possible influence of phonon condensation in A15 SCs.

cond-mat.str-el↗

arXiv2018

Ultrafast Terahertz Conductivity Probes of Topologically Enhanced Surface Transport Driven by Mid-Infrared Laser Pulses in Bi$_2$Se$_3$

The recent discovery of topology-protected charge transport of ultimate thinness on surfaces of three-dimensional topological insulators (TIs) are breaking new ground in fundamental quantum science and transformative technology. Yet a challenge remains on how to isolate and disentangle helical spin transport on the surface from bulk conduction. Here we show that selective midinfrared femtosecond photoexcitation of exclusive intraband electronic transitions at low temperature underpins topological enhancement of terahertz (THz) surface transport in doped Bi2Se3, with no complication from interband excitations or need for controlled doping. The unique, hot electron state is characterized by conserved populations of surface/bulk bands and by frequency-dependent hot carrier cooling times that directly distinguish the faster surface channel than the bulk. We determine the topological enhancement ratio between bulk and surface scattering rates, i.e., $γ_\text{BS}/γ_\text{SS}\sim$3.80 in equilibrium. These behaviors are absent at elevated lattice temperatures and for high pumpphoton frequencies and uences. The selective, mid-infrared-induced THz conductivity provides a new paradigm to characterize TIs and may apply to emerging topological semimetals in order to separate the transport connected with the Weyl nodes from other bulk bands.

cond-mat.mtrl-sci↗

arXiv2018

Theory of Ultrafast Spin--Charge Quantum Dynamics in Strongly Correlated Systems Controlled by Femtosecond Photoexcitation: an Application to Insulating Antiferromagnetic Manganites

We use a non-equilibrium many-body theory that engages the elements of transient coherence, correlation, and nonlinearity to describe changes in the magnetic and electronic phases of strongly correlated systems induced by femtosecond nonlinear photoexcitation. Using a generalized tight--binding mean field approach based on Hubbard operators and including the coupling of the laser field, we describe a mechanism for simultaneous insulator--to--metal and anti-- to ferro--magnetic transition to a transient state triggered by non-thermal ultrafast spin and charge coupled excitations. We demontrate, in particular, that photoexcitation of composite fermion quasiparticles induces quasi-instantaneous spin canting that quenches the energy gap of the antiferromagnetic insulator and acts as a nonadiabatic "initial condition" that triggers non-thermal lattice dynamics leading to an insulator to metal and antiferromagnetic (AFM) to ferromagnetic (FM) transitions. Our theoretical predictions are consistent with recent ultrafast pump-probe spectroscopy experiments that revealed a magnetic phase transition during 100fs laser pulse photoexcitation of the CE--type AFM insulating phase of colossal magnetoresistive manganites. In particular, experiment observes two distinct charge relaxation components, fs and ps, with nonlinear threshold dependence at a pump fluence threshold that coincides with that for femtosecond magnetization photo excitation. Our theory attributes the correlation between femtosecond spin and charge nonlinearity leading to transition in the magnetic and electronic state to spin/charge/lattice coupling and laser-induced quantum spin canting that accompanies the driven population inversion between two quasi--particle bands with different properties: a mostly occupied polaronic band and a mostly empty metallic band, whose dispersion is determined by quantum spin canting.

cond-mat.str-el↗

arXiv2018

Non-equilibrium Pair Breaking in Ba(Fe1-xCox)2As2 Superconductors: Evidence for Formation of Photo-Induced Excitonic Spin-Density-Wave State

Ultrafast terahertz (THz) pump{probe spectroscopy reveals unusual out-of-equilibrium Cooper pair dynamics driven by femtosecond (fs) optical quench of superconductivity (SC) in iron pnictides. We observe a two{step quench of the SC gap, where an abnormally slow (many 100's of ps) quench process is clearly distinguished from the usual fast (sub-ps) hot{phonon{mediated scattering channel. This pair breaking dynamics depends strongly on doping, pump uence, and temperature. The above observations, together with quantum kinetic modeling of non-equilibrium SC and magnetic correlations, provide evidence for photogeneration of a transient state where SC competes with build{up of spin-density-wave (SDW) excitonic correlation between quasi-particles (QP).

cond-mat.supr-con↗

arXiv2013

Pair-excitation energetics of highly correlated many-body states

A microscopic approach is developed to determine the excitation energetics of highly correlated quasi-particles in optically excited semiconductors based entirely on a pair-correlation function input. For this purpose, the Wannier equation is generalized to compute the energy per excited electron-hole pair of a many-body state probed by a weak pair excitation. The scheme is verified for the degenerate Fermi gas and incoherent excitons. In a certain range of experimentally accessible parameters, a new stable quasi-particle state is predicted which consists of four to six electron-hole pairs forming a liquid droplet of fixed radius. The energetics and pair-correlation features of these "quantum droplets" are analyzed.

cond-mat.mes-hall↗