arXiv subjects

Paul Fons

Publications and source records attributed to Paul Fons.

18 recordsLinked to original sources

arXiv2026

An ultrafast diamond nonlinear photonic sensor

The integration of light and materials technology is key to the creation of innovative sensing technologies. Sensing of electric and magnetic fields, and temperature with high spatio-temporal resolution is a critical task for the development of the next-generation of nanometer-scale quantum devices. Color centers in diamonds are attractive for potential applications owing to their characteristic quantum states, although they require metallic contacts for the introduction of external microwaves. Here, we build an ultrafast diamond nonlinear photonic sensor to assess the surface electric field; an electro-optic sensor based on nitrogen-vacancy centers in a diamond nanotip breaks the spatial-limit of conventional pump-probe techniques. The 10-fs near-infrared optical pulse modulates the surface electric field of a 2D transition metal dichalcogenide and we monitor the dynamics of the local electric field at nanometer-femtosecond spatio-temporal resolutions. Our nanoscopic technique will provide new horizons to the sensing of advanced nano materials.

physics.optics↗

arXiv2024

Cooperative dynamic polaronic picture of diamond color centers

Polarons can control carrier mobility and can also be used in the design of quantum devices. Although much effort has been directed into investigating the nature of polarons, observation of defect-related polarons is challenging due to electron-defect scattering. Here we explore the polaronic behavior of nitrogen-vacancy (NV) centers in a diamond crystal using an ultrafast pump-probe technique. A 10-fs optical pulse acts as a source of high electric field exceeding the dielectric breakdown threshold, in turn exerting a force on the NV charge distribution and polar optical phonons. The electronic and phononic responses are enhanced by an order of magnitude for a low density of NV centers, which we attribute to a combination of cooperative polaronic effects and scattering by defects. First-principles calculations support the presence of dipolar Fr\"ohlich interaction via non-zero Born effective charges. Our findings provide insights into the physics of color centers in diamonds.

cond-mat.mtrl-sci↗

arXiv2024

Spin dependent bandgap renormalization and state filling effect in Bi$_2$Se$_3$ observed by ultrafast Kerr rotation

We investigate the ultrafast spin dynamics of the prototypical topological insulator $\mathrm{Bi_{2}Se_{3}}$ using time-resolved Kerr-rotation (polarization-change) measurements across near-infrared wavelengths. The Kerr-rotation angle $\Delta \theta_{K}$ of $\mathrm{Bi_{2}Se_{3}}$ was found to significantly depend on photon energy around a resonance transition ($\sim 1.0\ \mathrm{eV}$) of bulk states, as well as the ellipticity of the pump light, in the presence of spin excitation. The observed photon-energy dependence of $\Delta \theta_{K}$ can be well simulated by assuming spin-dependent refractive-index changes in the presence of band-gap renormalization and state-filling effect upon photoexcitation. Our study delivers comprehensive insights into the opto-spintronic properties of bulk $\mathrm{Bi_{2}Se_{3}}$ and the fundamental physical processes underlying polarization changes. These findings are expected to be crucial in developing ultrafast magneto-optical memory devices, which can perform read-and-write operations in the Terahertz regime.

cond-mat.mtrl-sci↗

arXiv2022

Photo-induced Tellurium segregation in $\mathrm{MoTe_2}$

We report on the coherent phonon spectroscopy of polymorphic $\mathrm{MoTe_2}$ single crystals using a femtosecond-pulsed laser to investigate the relationship between structural phase transitions and photo-thermal effects induced by high-density laser excitation. Even when a femtosecond pulsed laser was used, which generally induces fewer heat accumulation effects than the case for a CW laser, tellurium segregation was observed in coherent phonon spectra with increasing excitation density, while no structural phase transition among polymorphs of $\mathrm{MoTe_2}$ was observed. The use of higher photon-energy excitation, however, was found to suppress tellurium segregation.

cond-mat.mtrl-sci↗

arXiv2021

Ultrafast scattering dynamics of coherent phonons in Bi$_{1-x}$Sb$_{x}$ in the Weyl semimetal phase

We investigate ultrafast phonon dynamics in the Bi$_{1-x}$Sb$_{x}$ alloy system for various compositions $x$ using a reflective femtosecond pump-probe technique. The coherent optical phonons corresponding to the A$_{1g}$ local vibrational modes of Bi-Bi, Bi-Sb, and Sb-Sb are generated and observed in the time domain with a few picoseconds dephasing time. The frequencies of the coherent optical phonons were found to change as the Sb composition $x$ was varied, and more importantly, the relaxation time of those phonon modes was dramatically reduced for $x$ values in the range 0.5--0.8. We argue that the phonon relaxation dynamics are not simply governed by alloy scattering, but are significantly modified by anharmonic phonon-phonon scattering with implied minor contributions from electron-phonon scattering in a Weyl-semimetal phase.

cond-mat.mtrl-sci↗

arXiv2019

All-optical detection of periodic structure of chalcogenide superlattice using coherent folded acoustic phonons

Chalcogenide superlattices (SL) consist of alternate stacking of GeTe and Sb$_{2}$Te$_{3}$ layers. The structure can become a 3D topological insulator depending on the constituent layer thicknesses, making the design of the SL period a central issue for advancing chalcogenide SL as potential candidates for spin devices as well as for optimization of the current generation of phase-change memory devices. Here we explore the periodic structure of chalcogenide SL by observing coherent folded longitudinal acoustic (FLA) phonons excited by femtosecond laser pulse irradiation. The peak frequency of the FLA modes was observed to change upon variation of the thickness of the GeTe layer, which was well reproduced by means of an elastic continuum model. In addition, a new SL structure is unveiled for a sample consisting of thin GeTe and Sb$_{2}$Te$_{3}$ layers, which suggests intermixing of Ge atoms. This all-optical technique based on observation of coherent FLA modes offers a non-destructive characterization of superlattice structures at atomic resolution.

cond-mat.mtrl-sci↗

arXiv2019

A topological phase buried in a chalcogenide superlattice monitored by a helicity dependent Kerr measurement

Chalcogenide superlattices (SL), formed by the alternate stacking of GeTe and Sb$_{2}$Te$_{3}$ layers, also referred to as interfacial phase change memory (iPCM), are a leading candidate for spin based memory device applications. Theoretically, the iPCM structure it has been predicted to form a 3D topological insulator or Dirac semimetal depending on the constituent layer thicknesses. Here, we experimentally investigate the topological insulating nature of chalcogenide SLs using a helicity dependent time-resolved Kerr measurement. The helicity dependent Kerr signal is observed to exhibit a four cycle oscillation with $\pi$/2 periodicity suggesting the existence of a Dirac-like cone in some chalcogenide SLs. Furthermore, we found that increasing the thickness of the GeTe layer dramatically changes the periodicity, indicating a phase transition from a Dirac semimetal into a trivial insulator. Our results demonstrate that thickness-tuned chalcogenide SLs can play an important role in the manipulation of topological states, which may open up new possibilities for spintronic devices based on chalcogenide SLs.

cond-mat.mes-hall↗

arXiv2019

Photon Energy Dependence of Kerr Rotation in Chalcogenide Superlattices

We report on pump-probe based helicity dependent time-resolved Kerr measurements of chalcogenide superlattices, consisting of alternately stacked GeTe and Sb$_{2}$Te$_{3}$ layers under infrared excitation. The Kerr rotation signal consists of the specular Inverse Faraday effect (SIFE) and the specular optical Kerr effect (SOKE), both of which are found to monotonically increase with decreasing photon energy over a sub-eV energy range. Although the dependence of the SIFE can be attributed to a response function of direct third-order nonlinear susceptibility, the magnitude of the SOKE reflects cascading second-order nonlinear susceptibility resulting from electronic transitions from bulk valence band to interface-originating Dirac states of the superlattice.

cond-mat.mtrl-sci↗

arXiv2018

Zener Tunneling Breakdown in Phase-Change Materials Revealed by Intense Terahertz Pulses

We have systematically investigated the spatial and temporal dynamics of crystallization that occurs in the phase-change material Ge2Sb2Te5 upon irradiation with an intense THz pulse. THz pump and optical probe spectroscopy revealed that Zener tunneling induces a nonlinear increase in the conductivity of the crystalline phase. This result indicates that the large electric field associated with the THz pulses causes a nonlinear increase only at the edge of the crystallized area. The electric field concentrating in this area causes a temperature increase via Joule heating, which in turn leads to nanometer scale crystal growth parallel to the field and the formation of filamentary conductive domains across the sample.

cond-mat.mtrl-sci↗

arXiv2018

Ultrafast Dynamics of Electron-phonon Coupling in Transition-metal Dichalcogenides

Time-domain femtosecond laser spectroscopic measurements of the ultrafast lattice dynamics in 2H-MoTe2 bulk crystals were carried out to understand the carrier-phonon interactions that govern electronic transport properties. An unusually long lifetime coherent A1g phonon mode was observed even in the presence of very large density of photo-excited carriers at room temperature. The decay rate was observed to decrease with increasing excitation laser fluence. Based on the laser fluence dependence including the inducement of significant phonon softening and a peculiar decrease in phonon decay rate, we attribute the long lifetime lattice dynamics to weak anharmonic phonon-phonon coupling and a carrier-density-dependent deformation potential electron-phonon coupling.

cond-mat.mtrl-sci↗

arXiv2018

Coherent Dirac plasmons in topological insulators

We explore the ultrafast reflectivity response from photo-generated coupled phonon-surface Dirac plasmons in Sb$_2$Te$_3$ topological insulators several quintuple layers thick. The transient coherent phonon spectra obtained at different time frames exhibit a Fano-like asymmetric line shape of the $A^2_{1g}$ mode, which is attributed to quantum interference between continuum-like coherent Dirac-plasmons and phonons. By analyzing the time-dependent asymmetric line shape using the two-temperature model (TTM), it was determined that a Fano-like resonance persisted up to $\approx$1 ps after photo-excitation with a relaxation profile dominated by Gaussian decay at $\leq$200 fs. The asymmetry parameter could be well described by the TTM for $\geq$200 fs, therefore suggesting the coherence time of the Dirac plasmon is $\approx$200 fs.

cond-mat.str-el↗

arXiv2018

A cascading nonlinear magneto-optical effect in topological insulators

Topological insulators (TIs) are characterized by possessing metallic (gapless) surface states and a finite band-gap state in the bulk. As the thickness of a TI layer decreases down to a few nanometer, hybridization between the top and bottom surfaces takes place due to quantum tunneling, consequently at a critical thickness a crossover from a 3D-TI to a 2D insulator occurs. Although such a crossover is generally accessible by scanning tunneling microscopy, or by angle-resolved photoemission spectroscopy, such measurements require clean surfaces. Here, we demonstrate that a cascading nonlinear magneto-optical effect induced via strong spin-orbit coupling can examine such crossovers. The helicity dependence of the time-resolved Kerr rotation exhibits a robust change in periodicity at a critical thickness, from which it is possible to predict the formation of a Dirac cone in a film several quintuple layers thick. This method enables prediction of a Dirac cone using a fundamental nonlinear optical effect that can be applied to a wide range of TIs and related 2D materials.

cond-mat.mtrl-sci↗

arXiv2017

Sub-nanometre resolution of atomic motion during electronic excitation in phase-change materials

Phase-change materials based on Ge-Sb-Te alloys are widely used in industrial applications such as nonvolatile memories, but reaction pathways for crystalline-to-amorphous phase-change on picosecond timescales remain unknown. Femtosecond laser excitation and an ultrashort x-ray probe is used to show the temporal separation of electronic and thermal effects in a long-lived ($>$100 ps) transient metastable state of Ge$_{2}$Sb$_{2}$Te$_{5}$ with muted interatomic interaction induced by a weakening of resonant bonding. Due to a specific electronic state, the lattice undergoes a reversible nondestructive modification over a nanoscale region, remaining cold for 4 ps. An independent time-resolved x-ray absorption fine structure experiment confirms the existence of an intermediate state with disordered bonds. This newly unveiled effect allows the utilization of non-thermal ultra-fast pathways enabling artificial manipulation of the switching process, ultimately leading to a redefined speed limit, and improved energy efficiency and reliability of phase-change memory technologies.

cond-mat.mtrl-sci↗

arXiv2015

Coherent gigahertz phonons in Ge$_{2}$Sb$_{2}$Te$_{5}$ phase-change materials

Using $\approx$40 fs ultrashort laser pulses, we investigate the picosecond acoustic response from a prototypical phase change material, thin Ge$_{2}$Sb$_{2}$Te$_{5}$ (GST) films with various thicknesses. After excitation with a 1.53 eV-energy pulse with a fluence of $\approx$ 5 mJ/cm$^{2}$, the time-resolved reflectivity change exhibits transient electronic response, followed by a combination of exponential-like strain and coherent acoustic phonons in the gigahertz (GHz) frequency range. The time-domain shape of the coherent acoustic pulse is well reproduced by the use of the strain model by Thomsen et al. (Phys. Rev. B 34, 4129, 1986). We found that the decay rate (the inverse of the relaxation time) of the acoustic phonon both in the amorphous and in the crystalline phases decreases as the film thickness increases. The thickness dependence of the acoustic phonon decay is well modeled based on both phonon-defect scattering and acoustic phonon attenuation at the GST/Si interface, and it is revealed that those scattering and attenuation are larger in crystalline GST films than those in amorphous GST films.

cond-mat.mtrl-sci↗

arXiv2015

Femtosecond structural transformation of phase-change materials far from equilibrium monitored by coherent phonons

Multi-component chalcogenides, such as quasi-binary GeTe-Sb$_{2}$Te$_{3}$ alloys, are widely used in optical data storage media in the form of rewritable optical discs. Ge$_{2}$Sb$_{2}$Te$_{5}$ (GST) in particular has proven to be one of the best-performing materials, whose reliability allows more than 10$^{6}$ write-erase cycles. Despite these industrial applications, the fundamental kinetics of rapid phase-change in GST remain controversial and active debate continues over the ultimate speed limit. Here we explore ultrafast structural transformation in a photo-excited GST superlattice, where GeTe and Sb$_{2}$Te$_{3}$ are spatially separated, using coherent phonon spectroscopy with pump-pump-probe sequences. By analysing the coherent phonon spectra in different time regions, complex structural dynamics upon excitation are observed in GST superlattice (but not in GST alloys), which can be described as the mixing of Ge sites from two different coordination environments. Our results suggest possible applicability of GST superlattice for ultrafast switching devices.

cond-mat.mtrl-sci↗

arXiv2014

Coherent phonon study of (GeTe)$_{l}$(Sb$_{2}$Te$_{3}$)$_{m}$ interfacial phase change memory materials

The time-resolved reflectivity measurements were carried out on the interfacial phase change memory (iPCM) materials ([(GeTe)$_{2}$(Sb$_{2}$Te$_{3}$)$_{4}$]$_{8}$ and [(GeTe)$_{2}$(Sb$_{2}$Te$_{3}$)$_{1}$]$_{20}$) as well as conventional Ge$_{2}$Sb$_{2}$Te$_{5}$ alloy at room temperature and above the RESET-SET phase transition temperature. In the high-temperature phase, coherent phonons were clearly observed in the iPCM samples while drastic attenuation of coherent phonons was induced in the alloy. This difference strongly suggests the atomic rearrangement during the phase transition in iPCMs is much smaller than that in the alloy. These results are consistent with the unique phase transition model in which a quasi-one-dimensional displacement of Ge atoms occurs for iPCMs and a conventional amorphous-crystalline phase transition takes place for the alloy.

cond-mat.mtrl-sci↗

arXiv2014

Picosecond strain dynamics in Ge$_{2}$Sb$_{2}$Te$_{5}$ monitored by time-resolved x-ray diffraction

Coherent phonons (CP) generated by laser pulses on the femtosecond scale have been proposed as a means to achieve ultrafast, non-thermal switching in phase-change materials such as Ge$_{2}$Sb$_{2}$Te$_{5}$(GST). Here we use ultrafast optical pump pulses to induce coherent acoustic phonons and stroboscopically measure the corresponding lattice distortions in GST using 100 ps x-ray pulses from the ESRF storage ring. A linear-chain model provides a good description of the observed changes in the diffraction signal, however, the magnitudes of the measured shifts are too large to be explained by thermal effects alone implying the presence of transient non-equilibrium electron heating in addition to temperature driven expansion. The information on the movement of atoms during the excitation process can lead to greater insight into the possibilities of using CP-induced phase-transitions in GST.

cond-mat.mtrl-sci↗

arXiv2012

Polarization Dependent Optical Control of Atomic Arrangement in Multilayer Ge-Sb-Te Phase Change Materials

We report the optical perturbation of atomic arrangement in the layered GeTe/Sb_{2}Te_{3} phase change memory material. To observe the structural change, the coherent A_{1} mode of GeTe_{4} local structure is investigated at various polarization angles of femtosecond pump pulses with the fluence at < 78 μJ/cm^{2}. p-polarization found to be more effective in inducing the A_{1} frequency shift that can be either reversible or irreversible, depending on the pump fluence. The predominant origin of this shift is attributed to rearrangement of Ge atoms driven by anisotropic dissociation of the Ge-Te bonds along the [111] axis after the p-polarized pulse irradiation.

cond-mat.mtrl-sci↗