arXiv subjects

Hrvoje Petek

Publications and source records attributed to Hrvoje Petek.

At least 19 recordsLinked to original sources

arXiv2025

Observation of non-adiabatic Landau-Zener tunneling among Floquet states

Electromagnetic fields not only induce electronic transitions but also fundamentally modify the quantum states of matter through strong light-matter interactions. As one established route, Floquet engineering provides a powerful framework to dress electronic states with time-periodic fields, giving rise to quasi-stationary Floquet states. With increasing field strength, non-perturbative responses of the dressed states emerge, yet their nonlinear dynamics remain challenging to interpret. In this work we explore the emergence of non-adiabatic Landau-Zener transitions among Floquet states in Cu(111) under intense optical fields. At increasing field strength, we observe a transition from perturbative dressing to a regime where Floquet states undergo non-adiabatic tunneling, revealing a breakdown of adiabatic Floquet evolution. These insights are obtained through interferometrically time-resolved multi-photon photoemission spectroscopy, which serves as a sensitive probe of transient Floquet state dynamics. Numerical simulations and the theory of instantaneous Floquet states allow us to directly examine real-time excitation pathways in this non-perturbative photoemission regime. Our results establish a direct connection the onset of light-dressing of matter, non-perturbative ultrafast lightwave electronics, and high-optical-harmonic generation in the solids.

cond-mat.mes-hall↗

arXiv2024

Plasmonic Vortices Host Magnetoelectric Interactions

The vector cross product and pseudoscalar dot products of electric (E) and magnetic (H) fields are separately finite in vacuum transverse electric and magnetic (TEM) plane waves, and angular momentum structured light. Current theories of interactions beyond the standard model of particle physics invoke non-zero dot(E,H) as the source term in the axion law that describes interactions with the cosmological dark matter axion particles outside of the quartet of Maxwells equations. The non-zero dot(E,H) also drives relativistic spin-charge magnetoelectric excitations of axion quasiparticles at a distinctively higher condensed matter scale in magnetic and topological materials. Yet, how to drive coherent dot(E,H) responses is unknown, and provides motivation to examine the field polarizations in structured light on a deep sub-diffraction limited spatial scale and sub-optical cycle temporal scale by ultrafast nonlinear photoemission electron microscopy. By analytical theory and ultrafast coherent photoemission electron microscopy, we image dot(E,H) fields in surface plasmon polariton vortex cores at subwavelength scales, where we find that the magnetoelectric relative to the dipole density is intensified on a ~10 nm diameter scale as a universal property of plasmonic vortex fields. The generation and nanoscale localization of dot(E,H) fields introduces the magnetoelectric symmetry class, having the parity and time reversal broken, but the joint parity-time reversal symmetry preserved. The ability to image the optical fields of plasmonic vortex cores opens the research of ultrafast microscopy of magnetoelectric responses and interactions with axion quasiparticles in solid state materials.

cond-mat.mes-hall↗

arXiv2023

Selective coupling of coherent optical phonons in YBa$_2$Cu$_3$O$_{7-δ}$ with electronic transitions

We investigate coherent lattice dynamics in optimally doped YBa$_2$Cu$_3$O$_{7-δ}$ driven by ultrashort ($\sim$ 12 fs) near infrared (NIR) and near ultraviolet (NUV) pulses. Transient reflectivity experiments, performed at room temperature and under moderate ($<$0.1 mJ/cm$^2$) excitation fluence, reveal $A_g$-symmetry phonon modes related to the O(2,3) bending in the CuO$_2$ planes and to the apical O(4) stretching at frequencies between 10 and 15 THz, in addition to the previously reported Ba and Cu(2) vibrations at 3.5 and 4.5 THz. The relative coherent phonon amplitudes are in stark contrast to the relative phonon intensities in the spontaneous Raman scattering spectrum excited at the same wavelength. This contrast indicates mode-dependent contributions of the Raman and non-Raman mechanisms to the coherent phonon generation. We show that the particularly intense coherent Cu(2) phonon, together with its initial phase, supports its generation predominately via a displacive mechanism, possibly involving the charge transfer within the CuO$_2$ planes. The small amplitude of the coherent out-of-phase O(2,3) bending mode at 10 THz also suggests the involvement of non-Raman generation mechanism. The generation of the other coherent phonons can in principle be explained within the framework of Raman mechanism. When the pump light has the polarization component perpendicular to the CuO$_2$ plane, the coherent O(4) mode at 15 THz is strongly enhanced compared to the in-plane excitation, corresponding to the large polarizability component associated with the hopping between the apical and the chain oxygens, O(4) and O(1).

cond-mat.mtrl-sci↗

arXiv2022

Realization of one-dimensional electronic flat bands in an untwisted moire superlattice

Two-dimensional electronic flat bands and their induced correlated electronic interactions have been discovered, probed, and tuned in interlayer regions of hexagonally shaped van der Waals moire superlattices. Fabrication of anisotropic one-dimensional correlated bands by moire interference of 2D, however, remains a challenge. Here, we report an experimental discovery of 1D electronic flat bands near the Fermi level in an anisotropic rectangular moire superlattice composed of in situ grown, vdW stacked two-atomic-layer thick Bi(110) well-aligned on a SnSe(001) substrate. The epitaxial lattice mismatch between the aligned Bi and SnSe zigzag atomic chains causes strong three-dimensional anisotropic atomic relaxations with associated one-dimensional out-of- and in-plane strain distributions that are expressed in electronic bands of the Bi(110) layer, which are characterized jointly by scanning probe microscopy and density functional theory. At the regions of the strongest out-of-plane shear strain, a series of 1D flat bands near the Fermi level are experimentally observed and defined in our calculations. We establish that 1D flat bands can arise in moiré superlattices in absence of the relative layer twist, but solely through the lattice strain. We generalize the strategy of utilizing strain in lattice mismatched rectangular hetero-bilayers for engineering correlated anisotropic electronic bands.

cond-mat.mes-hall↗

arXiv2022

Electron emission from plasmonically induced Floquet bands at metal surfaces

We explore the possibility of existence of plasmonically generated electronic Floquet bands at metal surfaces by studying the gauge transformed electron-surface plasmon interaction in the prepumped plasmonic coherent state environment. These bands may promote non-Einsteinian electron emission from metal surfaces exposed to primary interactions with strong electromagnetic fields. Resonant behaviour and scaling of emission yield with the parent electronic structure and plasmonic state parameters are estimated for Ag(111) surface. Relative yield intensities from non-Einsteinian emission channels in photoelectron spectra offer the means to calibrate the mediating plasmonic fields and therefrom ensuing surface Floquet bands.

cond-mat.mtrl-sci↗

arXiv2021

Plasmonically assisted channels of photoemission from metals

We analyse recently measured nonlinear photoemission spectra from Ag surfaces that reveal resonances whose energies do not scale with the applied photon energy but stay pinned to multiples of bulk plasmon energy $\hbarω_p$ above the Fermi level. To elucidate these unexpected and peculiar features we investigate the spectra of plasmons generated in a solid by the optically pumped electronic polarization and their effect on photoemission. By combining quadratic response formalism for calculations of photoemission yield, a nonperturbative approach to inelastic electron scattering, and first-principles calculations for the electronic structure, we demonstrate the dependence of probability amplitude for single- and multiplasmon excitations on the basic parameters characterizing the photon pulse and the system. The resulting multiexcitation spectrum evolves towards a truncated plasmonic coherent state. Analogous concept is extrapolated to interpret plasmon generation by multiphoton excited electronic polarization. Based on this we elaborate a scenario that the thus created real plasmons act as supplementary frequency-locked pump field for non-Einsteinian plasmonically assisted channels of photoemission from metals. The established paradigm enables assignment and assessment of the observed linear $\hbarω_p$- and nonlinear $2\hbarω_p$-electron yields from Ag. Such effects may be exploited for selective filtering of optical energy conversion in electronic systems.

cond-mat.mtrl-sci↗

arXiv2021

Two-dimensional Dirac nodal-line semimetal protected by symmetry

Dirac nodal line semimetals (DNLSs) host relativistic quasiparticles in their one-dimensional (1D) Dirac nodal line (DNL) bands that are protected by certain crystalline symmetries. Their novel low-energy fermion quasiparticle excitations and transport properties invite studies of relativistic physics in the solid state where their linearly dispersing Dirac bands cross at continuous lines with four-fold degeneracy. In materials studied up to now, the four-fold degeneracy, however, has been vulnerable to suppression by the ubiquitous spin-orbit coupling (SOC). Despite the current effort to discover 3D DNLSs that are robust to SOC by theory, positive experimental evidence is yet to emerge. In 2D DNLSs, because of the decreased total density of states as compared with their 3D counterparts, it is anticipated that their physical properties would be dominated by the electronic states defined by the DNL. It has been even more challenging, however, to discover robust 2D DNLSs against SOC because of their lowered symmetry; no such materials have yet been predicted by theory. By combining molecular beam epitaxy growth, STM, nc-AFM characterisation, with DFT calculations and space group theory analysis, here we reveal a novel class of 2D crystalline DNLSs that host the exact symmetry that protects them against SOC. The discovered quantum material is a brick phase 3-AL Bi(110), whose symmetry protection and thermal stability are imparted by the compressive vdW epitaxial growth on black phosphorus substrates. The BP substrate templates the growth of 3-AL Bi(110) nano-islands in a non-symmorphic space group structure. This crystalline symmetry protects the DNL electronic phase against SOC independent of any orbital or elemental factors. We theoretically establish that this intrinsic symmetry imparts a general, robust protection of DNL in a series of isostructural 2D quantum materials.

cond-mat.mtrl-sci↗

arXiv2020

Electron-phonon coupling in d-electron solids: A temperature dependent study of rutile TiO2 by first-principles theory and two-photon photoemission

Rutile TiO2 is a paradigmatic transition metal oxide with applications in optics, electronics, photocatalysis, etc., that are subject to pervasive electron-phonon interaction. To understand how energies of its electronic bands, and in general semiconductors or metals where the frontier orbitals have a strong d-band character, depend on temperature, we perform a comprehensive theoretical and experimental study of the effects of electron-phonon (e-p) interactions. In a two-photon photoemission (2PP) spectroscopy study we observe an unusual temperature dependence of electronic band energies within the conduction band of reduced rutile TiO2, which is contrary to the well understood sp-band semiconductors and points to a so far unexplained dichotomy in how the e-p interactions affect differently the materials where the frontier orbitals are derived from the sp- and d-orbitals. To develop a broadly applicable model, we employ state-of-the-art first-principles calculations that explain how phonons promote interactions between the Ti-3d orbitals of the conduction band within the octahedral crystal field. The characteristics differences in e-p interactions experienced by the Ti 3d-orbitals of rutile TiO2 crystal lattice are contrasted with the more familiar behavior of the Si 2s-orbitals of stishovite SiO2 polymorph, in which the frontier 2s-orbital experience a similar crystal field with the opposite effect...

cond-mat.mtrl-sci↗

arXiv2020

Towards full surface Brillouin zone mapping by coherent multi-photon photoemission

We report a novel approach for coherent multi-photon photoemission band mapping of the entire Brillouin zone with infrared light that is readily implemented in a laboratory setting. We excite a solid state material, Ag(110), with intense femtosecond laser pulses to excite higher-order multi-photon photoemission; angle-resolved electron spectroscopic acquisition records photoemission at large in-plane momenta involving optical transitions from the occupied to unoccupied bands of the sample that otherwise might remain hidden by the photoemission horizon. We propose this as a complementary ultrafast method to time- and angle-resolved two-color, e.g. infrared pump and extreme ultraviolet probe, photoemission spectroscopy, with the advantage of being able to measure and control the coherent electron dynamics.

cond-mat.other↗

arXiv2019

The Birth of a Plasmonic Topological Quasiparticle on the Nanofemto Scale

At interface of the classical and quantum physics Maxwell and Schrödinger equations describe how optical fields drive and control electronic phenomena at THz or PHz frequencies and on ultra-small scales to enable lightwave electronics. Light striking a metal surface triggers electric field-electron particle/wave interactions to coherently imprint and transfer its attributes on the attosecond time scale. Here we create and image by ultrafast photoemission electron microscopy a new quasiparticle of optical field-collective electron interaction where the design of geometrical phase creates a plasmonic topological spin angular momentum texture. The spin texture resembles that of magnetic meron quasiparticle, is localized within 1/2 wavelength of light, and exists on ~20 fs (2^10-14 s) time scale of the plasmonic field. The quasiparticle is created in a nanostructured silver film, which converts coherent linearly polarized light pulse into an evanescent surface plasmon polariton light-electron wave with a tailored geometric phase to form a plasmonic vortex. Ultrafast coherent microscopy imaging of electromagnetic waves propagating at the local speed of light of 255 nm/fs, electromagnetic simulations, and analytic theory find a new quasiparticle within the vortex core, with topological spin properties of a meron that are defined by the optical field and sample geometry. The new quasiparticle is an ultrafast topological defect whose chiral field breaks the time-inversion symmetry on the nanoscale; its creation, symmetry breaking topology, and dynamics pertain to contexts ranging from the cosmological structure creation to topological phase transitions in quantum liquids and gases, and may act as a transducer for quantum information on the nanofemto scale.

cond-mat.mes-hall↗

arXiv2019

Ultrafast Microscopy of a Plasmonic Spin Skyrmion

We present an ultrafast microscopy imaging experiment and a general analytical description of a new quasiparticle composed of plasmonic Skyrmion-like spin texture at the core of a surface plasmon polariton (SPP) vortex. The illumination of a circular coupling structure milled in an Ag film by circularly polarized light (CPL) couples its spin angular momentum (SAM) into orbital angular momentum (OAM) of SPPs launching them to form a plasmonic vortex. The coupling of the cycloidal motion of the SPP polarization at the 2D interface, with their orbital swirl at the vortex core causes the plasmonic field to generate 3D SAM pseudovectors, whose topological texture has integer Skyrmion number and is homotopic to a twisted magnetic Skyrmion quasiparticle with the boundary defined by an optical L-line singularity contour. An analytical description finds that the dielectric discontinuity at the Ag/vacuum interface supports on each side entwined twisted Skyrmion pairs that are characterized by stable topological textures with opposite Skyrmion numbers. The SAM texture of the Skyrmion pair within the primary vortex ring corresponds to a monopole-hedgehog type SAM texture, with a SAM singularity at the vortex core. Interferometric time-resolved two-photon photoemission electron microscopy (ITR-2P-PEEM) imaging of the nanofemto spatiotemporal evolution of the SPP fields and simulation by an analytical model, establish the twisted topological plasmonic SAM Skyrmion quasiparticle at the vortex core. The SAM textures can probe and simulate topological responses in trivial and topological materials that can be coupled in the near-field of the SPP vortex. The theory anticipates different field structures and the accompanying topological spin textures that construct single Skyrmion and meron-like quasiparticles as well as their arrays.

cond-mat.mes-hall↗

arXiv2018

Coherent optical and acoustic phonons generated at lattice-matched GaP/Si(001) heterointerfaces

Thin GaP films can be grown on an exact Si(001) substrate with nearly perfect lattice match. We perform all-optical pump-probe measurements to investigate the ultrafast electron-phonon coupling at the buried interface of GaP/Si. Above-bandgap excitation with a femtosecond laser pulse can induce coherent longitudinal optical (LO) phonons both in the GaP opverlayer and in the Si substrate. The coupling of the GaP LO phonons with photoexcited plasma is reduced significantly with decreasing the GaP layer thickness from 56 to 16 nm due to the quasi-two-dimensional confinement of the plasma. The same laser pulse can also generate coherent longitudinal acoustic (LA) phonons in the form of a strain pulse. The strain induces not only a periodic modulation in the optical reflectivity as they propagate in the semiconductors, but also a sharp spike when it arrives at the GaP layer boundaries. The acoustic pulse induced at the GaP/Si interface is remarkably stronger than that at the Si surface, suggesting a possible application of the GaP/Si heterostructure as an opto-acoustic transducer. The amplitude and the phase of the reflectivity modulation varies with the GaP layer thickness, which can be understood in terms of the interference caused by the multiple acoustic pulses generated at the top surface and at the buried interface.

cond-mat.mtrl-sci↗

arXiv2018

Excitation of two-photon photoemission where epsilon is near zero on Ag(111)

Because silver has epsilon-near-zero (ENZ) in the near-UV spectral region, its optical response is expected to be dominantly plasmonic and nonperturbatively nonlinear. The ENZ properties of Ag have made it the material of choice for investigation of plasmonic optical effects in physics, chemistry, optics, and nanotechnology. We investigate the nonlinear angle-resolved two-photon photoemission (2PP) spectroscopy of Ag(111) surface in the ENZ region. In addition to the well-understood and documented spectroscopic features of Einsteinian photoemission involving dipole excitations of the single-particle occupied and unoccupied surface states, 2PP spectra possess other distinct features where the optical fields excite or are modified by the collective virtual and real plasmon excitations.

cond-mat.mes-hall↗

arXiv2018

Ultrafast asymmetric Rosen-Zener-like coherent phonon responses observed in silicon

We investigate the spectral profiles of time signals attributed to coherent phonon generation in an undoped Si crystal. Here, the retarded longitudinal-optical (LO) phonon Green function relevant to the temporal variance of induced charge density of ionic cores is calculated by employing the polaronic quasiparticle model developed by the authors [Y. Watanabe et al., Phys. Rev. B 95, 014301 (2017); ibid., 96, 125204 (2017)]. The spectral asymmetry is revealed in the frequency domain of the signals under the condition that an LO phonon mode stays almost energetically resonant with a plasmon mode in the early time region; this lasts for approximately 100 fs immediately after the irradiation of an ultrashort pump-laser pulse. It is understood that based on the adiabatic picture in time, this asymmetry is caused by the Rosen-Zener coupling between both modes. The associated experimental results are obtained by measuring time-dependent electro-optic reflectivity signals, and it is proved that these are in harmony with the calculated ones. The spectra become more symmetric, as the photoexcited carrier density further changes from that meeting the above condition to higher and lower sides of carrier densities. Moreover, the effect of optical nutation of carrier density on the CP signals is addressed, and the present results are compared with the asymmetry caused by transient Fano resonance, and the spectral profiles observed in a GaAs crystal in the text.

cond-mat.mtrl-sci↗

arXiv2018

Coherent two-dimensional multiphoton photoelectron spectroscopy of metal surfaces

Light interacting with metals elicits an ultrafast coherent many-body screening response on sub- to few-femtosecond time-scales, which makes its experimental observation challenging. Here, we describe the coherent two-dimensional (2D) multi-photon photoemission study of the Shockley surface state (SS) of Ag(111) as a benchmark for spectroscopy of the coherent nonlinear response of metals to an optical field in the perturbative regime. Employing interferometrically time-resolved multi-photon photoemission spectroscopy (ITR-mPP), we correlate the coherent polarizations and populations excited in the sample with final photoelectron distributions where the interaction terminates. By measuring the non-resonant 3- and 4-photon photoemission of the SS state, as well as its replica structures in the above-threshold photoemission (ATP), we record the coherent response of the Ag(111) surface by 2D photoemission spectroscopy and relate it to its band structure. We interpret the mPP process by an optical Bloch equation (OBE) model, which reproduces the main features of the surface state coherent polarization dynamics recorded in ITR-mPP experiments: The spectroscopic components of the 2D photoelectron spectra are shown to depend on the nonlinear orders of the coherent photoemission process m as well as on the induced coherence n.

physics.optics↗

arXiv2017

Sub-picosecond acoustic pulses at buried GaP/Si interfaces

We report on the optical generation and detection of ultrashort acoustic pulses that propagate in three-dimensional semiconductor crystals. Photoexcitaiton of lattice-matched GaP layers grown on Si(001) gives rise to a sharp spike in transient reflectivity due to the acoustic pulse generated at the GaP/Si interface and detected at the GaP surface and vice versa. The extremely short width of the reflectivity spike, 0.5 ps, would translate to a spatial extent of 3 nm or 10 atomic bilayers, which is comparable with the width of the intermixing layer at the GaP/Si interface. The reflectivity signals are also modified by quasi-periodic Brillouin oscillations of GaP and Si arising from the acoustic pulses during the propagation in the crystals. The present results demonstrate the potential application of the simple optical pump-probe scheme in the nondestructive evaluation of the buried semiconductor interface quality.

cond-mat.mtrl-sci↗

arXiv2017

Intrinsic coherent acoustic phonons in indirect band gap semiconductors Si and GaP

We report on the intrinsic optical generation and detection of coherent acoustic phonons at (001)-oriented bulk Si and GaP without metallic phonon transducer structures. Photoexcitation by a 3.1-eV laser pulse generates a normal strain pulse within the $\sim$100-nm penetration depth in both semiconductors. The subsequent propagation of the strain pulse into the bulk is detected with a delayed optical probe as a periodic modulation of the optical reflectivity. Our theoretical model explains quantitatively the generation of the acoustic pulse via the deformation potential electron-phonon coupling and detection in terms of the spatially and temporally dependent photoelastic effect for both semiconductors. Comparison with our theoretical model reveals that the experimental strain pulses have finite build-up times of 1.2 and 0.4 ps for GaP and Si, which are comparable with the time required for the photoexcited electrons to transfer to the lowest X valley through intervalley scattering. The deformation potential coupling related to the acoustic pulse generation for GaP is estimated to be twice as strong as that for Si from our experiments, in agreement with a previous theoretical prediction.

cond-mat.mtrl-sci↗

arXiv2016

Direct Characterization of Band Bending in GaP/Si(001) Heterostructures with Hard X-ray Photoelectron Spectroscopy

We apply hard X-ray photoelectron spectroscopy (HAXPES) to investigate the electronic structures in ~50-nm thick epitaxial GaP layers grown on Si(001) under different conditions. Depth profiles of the local binding energies for the core levels are obtained by measuring the photoemission spectra at different incident photon energies between 3 and 7 keV and analyzing them with simple numerical models. The obtained depth profiles are in quantitative agreement with the band bending determinations for the same samples in a previous coherent phonon spectroscopic study. Our results demonstrate the applicability of the HAXPES with varying incident photon energy to characterize the electric potential profiles at buried semiconductor heterointerfaces.

cond-mat.mes-hall↗