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Zhanybek Alpichshev

Publications and source records attributed to Zhanybek Alpichshev.

At least 19 recordsLinked to original sources

Second-order Raman and anharmonic lattice dynamics in lead-halide perovskites

We explore the microscopic origin of THz-driven lattice dynamics in methylammonium lead bromide CH$_3$NH$_3$PbBr$_3$ using two-dimensional THz Kerr-effect spectroscopy. The analysis of the experiment enables discrimination between competing nonlinear excitation mechanisms and reveals that the dominant pathway is phonon-mediated rather than purely photonic. In particular, we argue that the commonly observed 1.15~THz Raman-active $A_g$ mode is not excited directly by the THz electric field. Instead, it emerges through cubic anharmonic coupling to an infrared-active phonon at 0.68~THz. Furthermore, a satellite feature at 1.36~THz is identified as a two-phonon Raman response of the same infrared-active mode. The observation of strong quadratic coupling involving the infrared-active phonon suggests an unconventional form of electron-phonon dressing present in lead-halide perovskites.

cond-mat.mtrl-sci↗

Alignment-free ultra-broadband parametric frequency conversion in lead-halide perovskites

Lead-halide perovskites were demonstrated to exhibit some of the largest known optical nonlinearities, yet their potential for frequency conversion remains largely untapped. Here we demonstrate ultra-broadband four-wave mixing of near- and mid-infrared femtosecond pulses in thick single-crystal LHPs, generating bright, coherent, and highly collimated emission across an exceptionally wide continuous tuning range without phase-matching engineering, angular alignment, or dispersion optimization. Time resolved measurements reveal that the emission originates near the crystal surfaces, where phase-matching constraints are relaxed, while the unusually large intrinsic $χ^{(3)}$ response preserves efficient and directional frequency conversion despite the strongly localized interaction volume. These results position LHPs as a powerful bulk platform for ultra-broadband nonlinear photonics, opening a pathway toward compact, alignment-free architectures for ultrafast frequency conversion.

cond-mat.mtrl-sci↗

Observation of Analogue Dynamic Schwinger Effect and Non-Perturbative Light Sensing in Lead Halide Perovskites

Dielectric breakdown of physical vacuum (Schwinger effect) is the textbook demonstration of compatibility of Relativity and Quantum theory. Although observing this effect is still practically unachievable, its analogue generalizations have been shown to be more readily attainable. This paper demonstrates that a gapped Dirac semiconductor, methylammonium lead-bromide perovskite (MAPbBr$_3$), exhibits analogue dynamical Schwinger effect. Tunneling ionization under deep sub-gap mid-infrared irradiation leads to intense photoluminescence in the visible range, in full agreement with quasi-adiabatic theory. In addition to revealing a gapped extended system suitable for studying the analogue Schwinger effect, this observation holds great potential for non-perturbative field sensing, i.e., sensing electric fields through non-perturbative light-matter interactions. First, this paper illustrates this by measuring the local deviation from the nominally cubic phase of a perovskite single crystal, which can be interpreted in terms of frozen-in fields. Next, it is shown that analogue dynamic Schwinger effect can be used for nonperturbative amplification of non-parametric upconversion process in perovskites driven simultaneously by multiple optical fields. This discovery demonstrates the potential for material response beyond perturbation theory in the Schwinger regime, offering extremely sensitive light detection and amplification across an ultrabroad spectral range not accessible by conventional devices.

cond-mat.mes-hall↗

Nonlinear Terahertz Polaritonics in a Quantum Paraelectric

Terahertz (THz) frequency range holds immense potential for high-speed data processing and signal manipulation. However, a fundamental challenge remains: the efficient and tunable control of THz electromagnetic fields. One promising approach is polaritonic engineering, which leverages hybrid light-matter excitations to manipulate THz fields at sub-wavelength scales. Here, we introduce quantum paraelectric materials as a powerful new platform for THz phonon-polaritonics, leveraging the pronounced nonlinearities of incipient ferroelectrics. These nonlinearities enable strong self- and cross-coupling between polaritons, facilitating all-optical, reconfigurable THz signal control. Using a novel space- and time-resolved imaging technique, we directly observe the ballistic propagation of bulk phonon-polaritons in SrTiO$_3$, and uncover soliton-like, dispersion-free transport in its low-temperature, quantum-fluctuation-dominated phase. Our results establish quantum paraelectric solids as a versatile and highly tunable medium for next-generation THz photonics and ultrafast information processing.

physics.optics↗

Using optical tweezers to simultaneously trap, charge and measure the charge of a microparticle in air

Optical tweezers are widely used as a highly sensitive tool to measure forces on micron-scale particles. One such application is the measurement of the electric charge of a particle, which can be done with high precision in liquids, air, or vacuum. We experimentally investigate how the trapping laser itself can electrically charge such a particle, in our case a $\sim 1\,\mathrm{μm\;SiO_2}$ sphere in air. We model the charging mechanism as a two-photon process which reproduces the experimental data with high fidelity.

cond-mat.soft↗

Disentangling Electronic and Ionic Nonlinear Polarization Effects in the THz Kerr Response of LaAlO$_{3}$

Nonlinear responses to intense terahertz (THz) fields provide unique insights into complex dynamics of contemporary material systems. However, the interpretation of the obtained data, in particular, distinguishing genuine ionic oscillations from the instantaneous electronic responses in THz Kerr effect remains challenging. Here, we combine two-dimensional Terahertz Kerr effect (2D-TKE) spectroscopy experiments and their modeling to unravel complex THz-induced temporal oscillations in twinned LaAlO$_3$ crystals at low temperatures. We identify the 1.1 THz mode as $E_g$ Raman phonon, while 0.86 THz and 0.36 THz signals are due to spurious effects resulting from the co- and counter-propagation of THz and optical probe pulses in birefringent twin domains. Furthermore, we determine that the $E_g$ mode is excited via a two-photon process, whereas THz pulse reflections at the sample surface produce a temporal response that can mimic anharmonic phonon coupling. Our findings highlight the importance of propagation effects in nonlinear THz experiments and provide a refined framework for interpreting THz polarization dynamics in birefringent crystals.

cond-mat.mtrl-sci↗

Massive Dirac-Pauli physics in lead-halide perovskites

In standard quantum electrodynamics (QED), the so-called non-minimal (Pauli) coupling is suppressed for elementary particles and has no physical implications. Here, we show that the Pauli term naturally appears in a known family of Dirac materials -- the lead-halide perovskites, suggesting a novel playground for the study of analogue QED effects. We outline measurable manifestations of the Pauli term in the phenomena pertaining to (i) relativistic corrections to bound states (ii) the Klein paradox, and (iii) spin effects in scattering. In particular, we demonstrate that (a) the binding energy of an electron in the vicinity of a positively charged defect is noticeably decreased due to the polarizability of lead ions and the appearance of a Darwin-like term, (b) strong spin-orbit coupling due to the Pauli term affects the exciton states, and (c) scattering of an electron off an energy barrier with broken mirror symmetry produces spin polarization in the outgoing current. Our study adds to understanding of quantum phenomena in lead-halide perovskites, and paves the way for tabletop simulations of analogue Dirac-Pauli equations.

cond-mat.mes-hall↗

Spontaneous flexoelectricity in cubic lead-halide perovskite MAPbBr$_3$

Lead-halide perovskites exhibit remarkable efficiency in photovoltaics, driven by exceptionally long carrier diffusion lengths and recombination times. Paradoxically, this performance persists even in defect-rich, solution-grown samples. Here, we use a suite of optical and charge transport measurements to reveal that key optoelectronic properties of perovskites arise from localized flexoelectric polarization confined to the interfaces between domains of spontaneous strain, present even in nominally cubic single crystals. This insight provides a microscopic link between structural composition and charge transport in these materials, reconciling conflicting prior observations and offering new design principles for perovskite-based solar cells.

cond-mat.mtrl-sci↗

Interferometric determination of intrinsic nonlinear Kerr index in lead-halide perovskites

Lead halide perovskites have recently been reported to demonstrate an exceptionally high nonlinear (Kerr) refractive index n$_2$ of up to 10$^{-8}$ cm$^2$/W in CH$_3$NH$_3$PbBr$_3$. Other researchers however observe different, substantially more conservative numbers. In order to resolve this disagreement the nonlinear Kerr index of a bulk sample of lead halide perovskite was measured directly by means of an interferometer. This approach has many advantages as compared to the more standard z-scan technique. In particular this method allows studying the induced changes to the refractive index in a time-resolved manner, thus enabling to separate the different contributions to $n_2$. The extracted n$_2$ values for CsPbBr$_3$ and MAPbBr$_3$ at $λ\approx 1μm$ are $n_2=+2.1\times$ 10$^{-14}$ cm$^2$/W and $n_2=+6\times$ 10$^{-15}$ cm$^2$/W respectively hence substantially lower than what has been indicated in most of the previous reports implying the latter should be regarded with a great care.

physics.optics↗

Bond polarizability as a probe of local crystal fields in hybrid lead-halide perovskites

A rotating organic cation and a dynamically disordered soft inorganic cage are the hallmark features of hybrid organic-inorganic lead-halide perovskites. Understanding the interplay between these two subsystems is a challenging problem but it is this coupling that is widely conjectured to be responsible for the unique behavior of photo-carriers in these materials. In this work, we use the fact that the polarizability of the organic cation strongly depends on the ambient electrostatic environment to put the molecule forward as a sensitive probe of local crystal fields inside the lattice cell. We measure the average polarizability of the C/N--H bond stretching mode by means of infrared spectroscopy, which allows us to deduce the character of the motion of the cation molecule, find the magnitude of the local crystal field and place an estimate on the strength of the hydrogen bond between the hydrogen and halide atoms. Our results pave the way for understanding electric fields in lead-halide perovskites using infrared bond spectroscopy.

cond-mat.mes-hall↗

Dispersive effects in ultrafast non-linear phenomena

It is a basic principle that an effect cannot come before the cause. Dispersive relations that follow from this fundamental fact have proven to be an indispensable tool in physics and engineering. They are most powerful in the domain of linear response where they are known as Kramers-Kronig relations. However when it comes to nonlinear phenomena the implications of causality are much less explored, apart from several notable exceptions. Here in this work we demonstrate how to apply the dispersive formalism to analyse the ultrafast nonlinear response in the context of the paradigmatic nonlinear Kerr effect. We find that the requirement of causality introduces a noticeable effect even under assumption that Kerr effect is mediated by quasi-instantaneous off-resonant electronic hyperpolarizability. We confirm this by experimentally measuring the time resolved Kerr dynamics in GaAs by means of a hybrid pump-probe Mach-Zehnder interferometer and demonstrate the presence of an intrinsic lagging between amplitude and phase responses as predicted by dispersive analysis. Our results describe a general property of the time-resolved nonlinear processes thereby highlighting the importance of accounting for dispersive effects in the nonlinear optical processes involving ultrashort pulses.

physics.optics↗

Mid-infrared Kerr index evaluation via cross-phase modulation with a near-infrared probe beam

We propose a simple method to measure nonlinear Kerr refractive index in mid-infrared frequency range that avoids using sophisticated infrared detectors. Our approach is based on using a near-infrared probe beam which interacts with a mid-IR beam via wavelength-non-degenerate cross-phase modulation (XPM). By carefully measuring XPM-induced spectral modifications in the probe beam and comparing the experimental data with simulation results we extract the value for the non-degenerate Kerr index. Finally, in order to obtain the value of degenerate mid-IR Kerr index we use the well-established two-band formalism of Sheik-Bahae et al., which is shown to become particularly simple in the limit of low frequencies. The proposed technique is complementary to the conventional techniques such as z-scan and has the advantage of not requiring any mid-infrared detectors.

physics.optics↗

Effective model for studying optical properties of lead-halide perovskites

We use general symmetry-based arguments to construct an effective model suitable for studying optical properties of lead-halide perovskites. To build the model, we identify an atomic-level interaction between electromagnetic fields and the spin degree of freedom that should be added to a minimally-coupled $\mathbf{k\cdot p}$ Hamiltonian. As a first application, we study two basic optical characteristics of the material: the Verdet constant and the refractive index. Beyond these linear characteristics of the material the model is suitable for calculating non-linear effects such as the third-order optical susceptibility. Analysis of this quantity shows that the geometrical properties of the spin-electric term imply isotropic optical response of the system, and that optical anisotropy of lead-halide perovskites is a manifestation of hopping of charge carriers. To illustrate this, we discuss third-harmonic generation.

cond-mat.mes-hall↗

Spin-Electric Coupling in Lead Halide Perovskites

Lead-halide perovskites enjoy a number of remarkable optoelectronic properties. To explain their origin, it is necessary to study how electromagnetic fields interact with these systems. We address this problem here by studying two classical quantities: Faraday rotation and the complex refractive index in a paradigmatic perovskite CH$_3$NH$_3$PbBr$_3$ in a broad wavelength range. We find that the minimal coupling of electromagnetic fields to the k$\cdot$p Hamiltonian is insufficient to describe the observed data even on the qualitative level. To amend this, we demonstrate that there exists a relevant atomic-level coupling between electromagnetic fields and the spin degree of freedom. This spin-electric coupling allows for quantitative description of a number of previous as well as present experimental data. In particular, we use it here to show that the Faraday effect in lead-halide perovskites is dominated by the Zeeman splitting of the energy levels, and has a substantial beyond-Becquerel contribution. Finally, we present general symmetry-based phenomenological arguments that in the low-energy limit our effective model includes all basis coupling terms to the electromagnetic field in the linear order.

cond-mat.other↗

The origin of exciton mass in a frustrated Mott insulator Na$_2$IrO$_3$

We use a three-pulse ultrafast optical spectroscopy to study the relaxation processes in a frustrated Mott insulator Na$_2$IrO$_3$. By being able to independently produce the out-of-equilibrium bound states (excitons) of doublons and holons with the first pulse and suppress the underlying antiferromagnetic order with the second one, we were able to elucidate the relaxation mechanism of quasiparticles in this system. By observing the difference in the exciton dynamics in the magnetically ordered and disordered phases we found that the mass of this quasiparticle is mostly determined by its interaction with the surrounding spins.

cond-mat.str-el↗

Observation of exciton-exciton interaction mediated valley depolarization in monolayer MoSe$_2$

The valley pseudospin in monolayer transition metal dichalcogenides (TMDs) has been proposed as a new way to manipulate information in various optoelectronic devices. This relies on a large valley polarization that remains stable over long timescales (hundreds of ns). However, time resolved measurements report valley lifetimes of only a few ps. This has been attributed to mechanisms such as phonon-mediated inter-valley scattering and a precession of the valley psedospin through electron-hole exchange. Here we use transient spin grating to directly measure the valley depolarization lifetime in monolayer MoSe$_{2}$. We find a fast valley decay rate that scales linearly with the excitation density at different temperatures. This establishes the presence of strong exciton-exciton Coulomb exchange interactions enhancing the valley depolarization. Our work highlights the microscopic processes inhibiting the efficient use of the exciton valley pseudospin in monolayer TMDs.

cond-mat.mes-hall↗

Disorder enabled band structure engineering of a topological insulator surface

Three dimensional topological insulators are bulk insulators with $\mathbf{Z}_2$ topological electronic order that gives rise to conducting light-like surface states. These surface electrons are exceptionally resistant to localization by non-magnetic disorder, and have been adopted as the basis for a wide range of proposals to achieve new quasiparticle species and device functionality. Recent studies have yielded a surprise by showing that in spite of resisting localization, topological insulator surface electrons can be reshaped by defects into distinctive resonance states. Here we use numerical simulations and scanning tunneling microscopy data to show that these resonance states have significance well beyond the localized regime usually associated with impurity bands. At native densities in the model Bi$_2$X$_3$ (X=Bi, Te) compounds, defect resonance states are predicted to generate a new quantum basis for an emergent electron gas that supports diffusive electrical transport.

cond-mat.mes-hall↗

Selective scattering between Floquet-Bloch and Volkov states in a topological insulator

The coherent optical manipulation of solids is emerging as a promising way to engineer novel quantum states of matter. The strong time periodic potential of intense laser light can be used to generate hybrid photon-electron states. Interaction of light with Bloch states leads to Floquet-Bloch states which are essential in realizing new photo-induced quantum phases. Similarly, dressing of free electron states near the surface of a solid generates Volkov states which are used to study non-linear optics in atoms and semiconductors. The interaction of these two dynamic states with each other remains an open experimental problem. Here we use Time and Angle Resolved Photoemission Spectroscopy (Tr-ARPES) to selectively study the transition between these two states on the surface of the topological insulator Bi2Se3. We find that the coupling between the two strongly depends on the electron momentum, providing a route to enhance or inhibit it. Moreover, by controlling the light polarization we can negate Volkov states in order to generate pure Floquet-Bloch states. This work establishes a systematic path for the coherent manipulation of solids via light-matter interaction.

cond-mat.mes-hall↗