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DOE OSTI2019

Strong Spin–Charge Coupling and Its Manifestation in the Quasiparticle Structure, Cooper Instability, and Electromagnetic Properties of Cuprates

The Fermi excitation spectrum, the problem of Cooper instability, and the Londons magnetic field penetration depth in cuprate superconductors are considered using the unified conception based on accounting for the strong coupling between the spin of copper ions and holes at oxygen ions. This coupling leads to strong renormalization of the primary spectrum of oxygen holes with the formation of spin-polaron quasiparticles. Analysis of Cooper instability performed using the spin-polaron concept for different channels has shown that only the superconducting d-wave pairing occurs in the ensemble of spin-polaron quasiparticles, and there are no solutions corresponding to the s-wave pairing. It has been demonstrated that the superconducting d-wave pairing is not suppressed by the Coulomb repulsion of holes located at neighboring oxygen ions. This effect is due to peculiarities in the crystallographic structure of the CuO{sub 2} plane and the aforementioned strong spin–fermion coupling. As a result, such interaction of holes is omitted in the kernel of the integral equation for the superconducting order parameter with the d-wave symmetry. It has been shown the Hubbard repulsion of holes and their interaction for the second coordination sphere of the oxygen sublattice for actual intensities of the interaction do not suppress the d-wave type of superconductivity. For the spin-polaron ensemble, we have analyzed the dependence of the Londons magnetic field penetration depth on the temperature and hole concentration. It has been established that the peculiarities of this dependence are closely related to specific features of the spin-polaron spectrum.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

DOE OSTI2020

Excitons in two-dimensional metal-halide perovskites

Georgia Tech School of Chemistry and Biochemistry Special Summer Seminar Series, Prof Carlos Silva; While polarons --- charges bound to a lattice deformation induced by electron-phonon coupling --- are primary photoexcitations at room temperature in bulk metal-halide hybrid organic-inorganic perovskites (HOIP), excitons --- Coulomb-bound electron-hole pairs --- are the stable quasi-particles in their two-dimensional (2D) analogues. Here we address the fundamental question: are polaronic effects consequential for excitons in 2D-HIOPs? Based on our recent work, we argue that polaronic effects are manifested intrinsically in the exciton spectral structure, which is comprised of multiple non-degenerate resonances with constant inter-peak energy spacing. We highlight measurements of population and dephasing dynamics that point to the apparently deterministic role of polaronic effects in excitonic properties. We contend that an interplay of long-range and short-range exciton-lattice couplings give rise to exciton polarons, a character that fundamentally establishes their effective mass and radius, and consequently, their quantum dynamics. Given this complexity, a fundamentally far-reaching issue is how Coulomb-mediated many-body interactions---elastic scattering such as excitation-induced dephasing, inelastic exciton bimolecular scattering, and multi-exciton binding---depend upon the specific exciton-lattice coupling within the structured excitation lineshape. We measure the intrinsic and density-dependent exciton dephasing rates of the multiple excitons and their dependence on temperature by means of two-dimensional coherent excitation spectroscopy. We find that diverse excitons display distinct intrinsic dephasing rates mediated by phonon scattering involving different effective phonons, and contrasting rates of exciton-exciton elastic scattering. These findings establish specifically the consequence of distinct lattice dressing on exciton many-body quantum dynamics, which critically define fundamental optical properties that underpin photonics and quantum optoelectronics.

solar cells, metal-halide perovskites, excitons, p↗

DOE OSTI2017

Molecular dynamics and charge transport in organic semiconductors: a classical approach to modeling electron transfer

Organic photovoltaics (OPVs) are a promising carbon-neutral energy conversion technology, with recent improvements pushing power conversion efficiencies over 10%. A major factor limiting OPV performance is inefficiency of charge transport in organic semiconducting materials (OSCs). Due to strong coupling with lattice degrees of freedom, the charges form polarons, localized quasi-particles comprised of charges dressed with phonons. These polarons can be conceptualized as pseudo-atoms with a greater effective mass than a bare charge. Here we propose that due to this increased mass, polarons can be modeled with Langevin molecular dynamics (LMD), a classical approach with a computational cost much lower than most quantum mechanical methods. Here we present LMD simulations of charge transfer between a pair of fullerene molecules, which commonly serve as electron acceptors in OSCs. We find transfer rates consistent with experimental measurements of charge mobility, suggesting that this method may provide quantitative predictions of efficiency when used to simulate materials on the device scale. Our approach also offers information that is not captured in the overall transfer rate or mobility: in the simulation data, we observe exactly when and why intermolecular transfer events occur. In addition, we demonstrate that these simulations can shed light on the properties of polarons in OSCs. In conclusion, much remains to be learned about these quasi-particles, and there are no widely accepted methods for calculating properties such as effective mass and friction. Lastly, our model offers a promising approach to exploring mass and friction as well as providing insight into the details of polaron transport in OSCs.

14 SOLAR ENERGY↗

DOE OSTI2017

Electronic and protonic conduction in LaFeO 3

Perovskite-type LaFeO3 has promising applications as a negative-electrode material for Ni/metal-hydride batteries. To further improve electrode performance, a thorough understanding of its charge-transport mechanisms is required. We use hybrid density functional theory to investigate the structural and electronic properties of bulk LaFeO3, as well as the effect of point defects and polarons on charge transport. Electronic charge localizes in the form of small hole and electron polarons; this self-trapping occurs in the bulk and also in the vicinity of point defects and impurities. We find that oxygen vacancies act as deep donors, while Fe and La vacancies are acceptors with the induced holes trapped as small polarons. Hydrogen interstitials and Ge and Ti impurities, on the other hand, act as donors that can trap small electron polarons. Hydrogen binds strongly to the La and Fe vacancies and hence these defects are detrimental to protonic conduction. We also elucidate how doping with Sr enhances the electrode performance of LaFeO3:Sr impurities substituting on La sites act as acceptors and enable electronic conductivity through hole polarons, with a hopping barrier of 0.39 eV. In addition, Sr impurities suppress the formation of cation vacancies, thereby enhancing proton conductivity.

Zhu, Zhen↗

DOE OSTI2014

The role of spin exchange in charge transfer in low-bandgap polymer: Fullerene bulk heterojunctions

Formation, relaxation and dynamics of polarons and methanofullerene anion radicals photoinitiated in poly[N-9″-hepta-decanyl-2,7-carbazole-alt-5,5-(4′,7′-di-2-thienyl-2′,1′, 3′-benzothiadiazole)]:-[6,6]-phenyl-C{sub 61}-butyric acid methyl ester (PCDTBT:PC{sub 61}BM) bulk heterojunctions were studied mainly by light-induced EPR (LEPR) spectroscopy in wide photon energy and temperature ranges. Some polarons are pinned by spin traps whose number and depth are governed by the composite morphology and photon energy. The proximity of the photon energy and the polymer bandgap reduces the number of such traps, inhibits recombination of mobile charge carriers, and facilitates their mobility in polymer network. Spin relaxation and charge carrier dynamics were studied by the steady-state saturation method at wide range of temperature and photon energy. These processes were shown to be governed by spin exchange as well as by the photon energy. Charge transfer in the composite is governed by the polaron scattering on the lattice phonons of crystalline domains embedded into amorphous polymer matrix and its activation hopping between polymer layers. The energy barrier required for polaron interchain hopping exceeds that of its intrachain diffusion. Anisotropy of polaron dynamics in the PCDTBT:PC61BM composite is less than that of poly(3-alkylthiophenes)-based systems that evidences for better ordering of the former. Lorentzian shape of LEPR lines of both charge carriers, lower concentration of spin traps as well as behaviours of the main magnetic resonance parameters were explained by layer ordered morphology of polymer matrix.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2018

Unraveling the Effect of Conformational and Electronic Disorder in the Charge Transport Processes of Semiconducting Polymers

Charge transport in semiconducting polymers is inextricably linked to their microstructure, making the characterization of polymer morphology at all length-scales essential for understanding the factors that limit mobility in these materials. Indeed, charge transport depends both on the ability of polarons to delocalize at the approximately nanometer length-scale and navigate a complex energetic and morphological mesoscale landscape. While characterization of the mesoscale morphology of polymers is well-established, studies of the local chain packing and nanoscale disorder, which affect delocalization, can be significantly more difficult to carry out. Additionally, through infrared charge modulation spectroscopy and theoretical modeling, the effect of the local chain environment on polaron delocalization is directly measured and quantified. Using a series of polymers based on the model system, poly(3-hexylthiophene), the link between disorder and polaron localization is systematically explored. Polaron delocalization is correlated with known trends in mobility, revealing that while charge delocalization is always beneficial, the formation of tie-chains is necessary to reach the highest mobilities in semicrystalline polymers. The results provide direct evidence for the importance of both nanoscale (charge carrier delocalization) and mesoscale (tie-chains) orders, demonstrating the need to distinguish the key length-scale limiting charge transport in the design of new, high mobility polymers.

36 MATERIALS SCIENCE↗

DOE OSTI2020

Combined Experimental and Theoretical Investigations of n-Type BiFeO 3 for Use as a Photoanode in a Photoelectrochemical Cell

Combined experimental and theoretical investigations were performed to evaluate the potential of n-type BiFeO 3 as a photoanode. While previous experimental and theoretical studies on BiFeO 3 mainly focused on its ferroelectric properties, several studies have reported the advantages of BiFeO 3 as a photoelectrode for solar water splitting (e.g. bandgap energy and band edge positions relative to water reduction and oxidation potentials). However, the photoelectrochemical properties of n-type BiFeO 3 have not yet been thoroughly investigated. In our experimental investigation, we developed an electrodeposition-based synthesis to prepare uniform n-type BiFeO 3 thin-film electrodes. Furthermore, using a heat treatment under a N 2 environment, we intentionally introduced additional oxygen vacancies into the pristine n-type BiFeO 3 electrodes to increase the majority carrier density. The bandgaps, flatband potentials, photocurrent onset potentials, photocurrent generation, and photoelectrochemical stabilities of the pristine and N 2 -treated BiFeO 3 photoanodes were investigated comparatively to improve our understanding of BiFeO 3 photoanodes and to examine the effect of oxygen vacancies on the photoelectrochemical properties of BiFeO 3 . In our theoretical investigation, we performed first-principles calculations and demonstrated the formation of a small polaron when an extra electron was introduced into the BiFeO 3 lattice. Changes in electronic states cause by the small polaron formation were carefully investigated. We also examined the effects of oxygen vacancies on electron polaron formation and carrier concentration in BiFeO 3 . Using charge formation energy calculations and referencing charge transition levels to the free electron polaron level instead of to the conduction band minimum, we showed that the oxygen vacancy is capable of serving as a donor to enhance the carrier concentration of BiFeO 3 . Furthermore, our theoretical results agree well with our experimental findings. Together, the new experimental and theoretical results and discussion provided in this study have considerably improved our understanding of n-type BiFeO 3 as a photoanode.

25 ENERGY STORAGE↗

DOE OSTI2025

Driving Force Dependent Photoinduced Charge Transfer Dynamics in Polymer-Wrapped Semiconducting Single-Walled Carbon Nanotubes

Here, we investigate the thermodynamic driving-force dependences of photoinduced charge separation (CS) and subsequent charge transfer dynamics in single-walled carbon nanotube (SWNT)–perylenediimide (PDI) donor–acceptor (D–A) superstructures. Pump–probe spectroscopy reveals that [SWNT (•+)n ]-(PDI –• ) n CS states form on an ∼100 fs time scale following photoexcitation; these dynamics are invariant across an ∼400 mV driving force range, indicating that SWNT hole polaron formation time scales are determined by nanotube lattice and solvent relaxation. These CS states feature SWNT hole polarons adjacent to (geminate) and nearby (nongeminate) PDI radical anions. Analysis of the free energy dependence for charge recombination (CR) of [SWNT •+ ] geminate -(PDI –• ) CS states highlights an ∼2 meV value for D–A electronic coupling (HAB) and ∼0.93 eV for the total reorganization energy (λ T ). A corresponding driving force dependence of the CR dynamics for [SWNT •+ ] nongeminate -(PDI –• ) CS states indicates a diminished H AB value (∼0.6 meV) and a larger λ T (∼1.1 eV), consistent with larger transfer distances. SWNT excitons that persist following photoinduced CS drive photooxidation of PDI –• components of [SWNT (•+)n ]-(PDI –• ) n CS states ( 1 SWNT* + PDI •– → PDI + SWNT •– ); this reaction manifests a significantly reduced λ T value (∼0.67 eV) as the initially prepared SWNT reduced state bears the character of a conduction band injected electron ([SWNT •– ] CB ). This reaction thus gives rise to relaxed, nongeminate SWNT electron and hole polarons on the same nanotube; these polarons react on a 10 2 ps time scale independent of the electronic structure of these SWNT-PDI superstructures.

anions↗

DOE OSTI2026

A Vibrational Probe of Electrical Doping in N2200 and Fermi-Level Alignment at Polymer Cathode/Metal Cocatalyst/Electrolyte Junctions

Hybrid (photo)cathodes consisting of conjugated polymer and hydrogen evolution reaction (HER) cocatalysts are an emerging platform for low-cost solar fuel generation. Poly{[N,N′-bis(2-octyldodecyl)-naphthalene-1,4,5,8-bis(dicarboximide)-2,6-diyl]-alt-5,5′-(2,2′-bithiophene)}, known as P(NDI2OD-T2) or N2200, is a promising electron accepting material for bulk heterojunction photocathodes. Unlike inorganic (photo)electrodes, much less is known about the energetic alignment of conjugated polymer electrode/metal/electrolyte junctions. Here, in this work, we investigate the electrical doping behavior in an N2200 cathode and its Fermi-level alignment with gold nanoparticles, which is used here as a model for the hydrogen evolution metal cocatalyst. Through UV/visible, Raman, and attenuated total-reflectance infrared spectroelectrochemistry, we observe the impact of electrical doping on the vibrational frequencies of neutral, anion, and dianion species in N2200, which suggests that electron density changes within the corresponding naphthalene-diimide (NDI) units. Upon one-electron reduction, the $C=O$ stretching frequency of the NDI anion unit (polaron) shows a red shift by ∼ 68 cm –1 . Additionally, the $C=O$ stretching frequency of neutral units in the doped N2200 shows a minor red shift of ∼ 5 cm –1 , suggesting charge transfer from neighboring polaron units. Surface-enhanced Raman spectroscopy measurements of a gold nanoparticle-functionalized N2200 electrode revealed that the Au Fermi level only shifts with that of N2200 upon polaron formation; thus, the formal potential of polymer polaron formation determines the behavior of the catalyst Fermi level, which we posit will modulate reaction capability. This mechanistic study provides a new approach for understanding the nanometer-scale energetics at the conjugated polymer/cocatalyst junction and provides critical insights for the future design of HER (photo)cathodes.

charge transfer↗

DOE OSTI2011

Intense laser field effects on p-d exchange interaction in single manganese doped GaAs

We have developed a comprehensive theory about optical control of p - d exchange interaction between spins of hole and Mn{sup 2+} in single-manganese doped GaAs material irradiated by a monochromatic, linearly polarized, intense pulsed laser field (PLF) under nonresonant conditions. The p - d exchange interaction leads to formation of magnetic polaron. While the PLF induces a dressed acceptor Coulomb potential, which transforms single center problem into the one with two virtual positively charged centers, resembling hydrogen molecule ion (H{sub 2}{sup +}). The dichotomy of hole wave functions, determined by the laser-intensity, affects strongly the p - d exchange interaction as well as binding energy of magnetic polaron. Increasing the laser intensity reduces the magnetic polaron binding energy. At larger excitation intensity, the magnetic polaron can be completely dissolved.

36 MATERIALS SCIENCE↗

DOE OSTI2015

Superlight bipolarons in High-T{sub c} superconductors

We present numerical results of the recently derived polaronic t-J{sub p} model, which accounts for realistic long range Coulomb repulsion and strong Fröhlich electron-phonon interactions for high temperature superconductivity in doped polar insulators. Different cluster geometries of 18-sites with two particles are studied. It appears that ground state energy decreases with hopping of polarons indicating an increase in tendency of the polarons to couple with each other. The entropy curves show that the system goes to more ordered state with the increase of polaron hopping for all cluster geometries.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

DOE OSTI2012

Tiny Bubbles in my BEC

Ultracold atomic gases provide a unique way for exploring many-body quantum phenomena that are inaccessible to conventional low-temperature experiments. Nearly two decades ago the Bose-Einstein condensate (BEC) - an ultracold gas of bosons in which almost all bosons occupy the same single-particle state - became experimentally feasible. Because a BEC exhibits superfluid properties, it can provide insights into the behavior of low-temperature helium liquids. We describe the case of a single distinguishable atom (an impurity) embedded in a BEC and strongly coupled to the BEC bosons. Depending on the strength of impurity-boson and boson-boson interactions, the impurity self-localizes into two fundamentally distinct regimes. The impurity atom can behave as a tightly localized 'polaron,' akin to an electron in a dielectric crystal, or as a 'bubble,' an analog to an electron bubble in superfluid helium. We obtain the ground state wavefunctions of the impurity and BEC by numerically solving the two coupled Gross-Pitaevskii equations that characterize the system. We employ the methods of imaginary time propagation and conjugate gradient descent. By appropriately varying the impurity-boson and boson-boson interaction strengths, we focus on the polaron to bubble crossover. Our results confirm analytical predictions for the polaron limit and uncover properties of the bubble regime. With these results we characterize the polaron to bubble crossover. We also summarize our findings in a phase diagram of the BEC-impurity system, which can be used as a guide in future experiments.

36 MATERIALS SCIENCE↗

DOE OSTI2019

Dynamic Screening and Slow Cooling of Hot Carriers in Lead Halide Perovskites

Abstract Among the exceptional properties of lead halide perovskites (LHPs) is the ultraslow cooling of hot carriers. Carrier densities below the Mott density for large polarons (≤ ≈10 18 cm −3 ) are focused on here. As in other semiconductors, a nascent hot electron distribution initially cools down via emission of longitudinal optical (LO) phonons on the 10 −14 –10 −13 s timescale. What distinguishes LHPs from conventional semiconductors is the exceptionally efficient screening in the former. The dielectric screening in LHPs on the 10 −13 s timescale results in an order‐of‐magnitude reduction in the Coulomb potential upon the formation of a large polaron, likely with ferroelectric‐like local ordering. Further LO‐phonon emission is inhibited, and this leads to partial retention of hot electron energy on the 10 −12 s timescale, more so in hybrid LHPs than in their all‐inorganic counterparts. Further cooling of hot polarons occurs on the 10 −10 s timescale, and this can be attributed to the slow diffusion of heat out of the large polaron volume due to the low thermal conductivity of LHPs. Like other carrier properties, slow hot carrier cooling in LHPs can be intimately related to efficient screening in a soft, anharmonic, and dynamically disordered lattice.

Joshi, Prakriti Pradhan↗

DOE OSTI2018

The Influence of Local Distortions on Proton Mobility in Acceptor Doped Perovskites

Optimizing proton conduction in solids remains the most promising solution for achieving intermediate temperature (~750–1000 K) solid oxide fuel cell devices, and enabling selective membranes for H 2 separation. Proton conduction, a thermally activated process, exhibits its highest rates in yttrium (Y) acceptor doped BaZrO 3 at an optimal doping level of 20% Y. The presence of extended defects such as grain boundaries has typically generated a wide variability in reported conductivity values. This has hindered a fundamental mechanistic understanding of how (acceptor) doping levels correlate with the activation energy of protons to produce an optimal doping level for fast proton transport. While isolated dopants have been suggested as the primary source of proton trapping, our results indicate that it is the local dopant-density that matters. Here in this work, we show that increasing the local dopant density promotes localized lattice distortions in the presence of point defects such as oxygen-vacancies or proton interstitials. An increasing distortion amplitude traps the point defects more strongly in the form of polarons, forming defect-clusters at higher concentrations. This leads to a monotonic increase in the activation energy (and hence a decrease in proton mobility) as observed in our measurements. The optimum doping level can now be explained as a competition between increasing proton concentration with doping levels and increasing activation energy due to defect-clusters formed by defect-polarons. Based on our findings, we demonstrate how to improve proton conductivity in doped BaZrO 3 , by inhibiting this dopant-lattice polaronic interaction. Finally, this approach should be generally applicable for ionic conduction in perovskite oxides such as oxygen-ion conduction in solid-oxide fuel cells and alkali-ion conduction in solid-state batteries where carriers might get trapped as defect-polarons.

36 MATERIALS SCIENCE↗

DOE OSTI2018

Role of Point Defects in Enhancing the Conductivity of BiVO 4

We report that bismuth vanadate is a promising photoanode for solar-to-fuel photocatalytic applications, and it has been extensively studied in recent years. However, the microscopic mechanism underlying the observed changes in electronic conductivity due to oxygen vacancies and nitrogen dopants remains unclear. Here, we combine electronic structure calculations at the hybrid density functional theory (DFT) level with constrained DFT, and we elucidate the role of defects in enhancing the transport properties of the material. We show that at low temperature, oxygen vacancies give rise to deep levels within the fundamental gap of BVO; however even as deep levels, oxygen vacancies can act as effective n-dopants and polaronic charge carriers, due to their favorable position in energy relative to polarons in the pristine bulk. In addition, we show that N atoms can be easily introduced in n-doped BiVO 4 and that the presence of substitutional nitrogen affects the formation energy of polarons, effectively contributing to an increase of the carrier mobility in the material. Lastly, our results reconcile apparently conflicting experiments and they may be generalized to other transition metal oxides, thus providing a foundation for polaronic defect engineering in photoanodes for water photocatalysis.

36 MATERIALS SCIENCE↗

DOE OSTI2022

Visible Light Absorption and Hot Carrier Trapping in Anatase TiO 2 : The Role of Surface Oxygen Vacancies

Anatase TiO 2 is an efficient water splitting photocatalyst using UV light, but solar energy harvesting requires the presence of midgap states to increase visible light absorption. Despite numerous studies, important questions remain regarding the photophysics in O vacancy doped TiO 2 . Here, by employing extreme ultraviolet reflection–absorption (XUV-RA) spectroscopy at the Ti M2,3-edge, spectral signatures of both large and small polaron states are identified, allowing ultrafast electron and hole dynamics in these states to be independently resolved. Results show that visible light absorption occurs via promotion of an electron from the small polaron state to the TiO 2 conduction band. In contrast, absorption of UV light results in direct band gap excitation followed by carrier relaxation during which hot holes trap as small polarons in 45 ± 42 fs, and hot electrons couple to polar optical phonons leading to vibrational coherence and large polaron formation in 945 ± 92 fs.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2016

Interfacial Coupling-Induced Ferromagnetic Insulator Phase in Manganite Film

Interfaces with subtle differences in atomic and electronic structures in perovskite ABO 3 heterostructures often yield intriguingly different properties, yet their exact roles remain elusive. Here, we report an integrated study of unusual transport, magnetic, and structural properties of Pr 0.67 Sr 0.33 MnO 3 film on SrTiO 3 substrate. The variations in the out-of-plane lattice constant and BO 6 octahedral rotation across the Pr 0.67 Sr 0.33 MnO 3 /SrTiO 3 interface strongly depend on the thickness of the Pr 0.67 Sr 0.33 MnO 3 film. In the 12-nm film, a new interface-sensitive ferromagnetic polaronic insulator (FI') phase is formed during the cubic-to-tetragonal phase transition of SrTiO 3 , apparently due to the enhanced electron–phonon interaction and atomic disorder in the film. The transport properties of the FI' phase in the 30-nm film are masked because of the reduced interfacial coupling and smaller interface-to-volume ratio. In conclusion, this work demonstrates how thickness-dependent interfacial coupling leads to the formation of a theoretically predicted ferromagnetic–polaronic insulator, as illustrated in a new phase diagram, that is otherwise ferromagnetic metal (FM) in bulk form.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

DOE OSTI2024

Chirality manipulation of ultrafast phase switches in a correlated CDW-Weyl semimetal

Light engineering of correlated states in topological materials provides a new avenue of achieving exotic topological phases inaccessible by conventional tuning methods. Here we demonstrate a light control of correlation gaps in a model charge-density-wave (CDW) and polaron insulator (TaSe 4 ) 2 I recently predicted to be an axion insulator. Our ultrafast terahertz photocurrent spectroscopy reveals a two-step, non-thermal melting of polarons and electronic CDW gap via the fluence dependence of a longitudinal circular photogalvanic current. This helicity-dependent photocurrent reveals continuous ultrafast phase switches from the polaronic state to the CDW (axion) phase, and finally to a hidden Weyl phase as the pump fluence increases. Additional distinctive attributes aligning with the light-induced switches include: the mode-selective coupling of coherent phonons to the polaron and CDW modulation, and the emergence of a non-thermal chiral photocurrent above the pump threshold of CDW-related phonons. The demonstrated ultrafast chirality control of correlated topological states here holds large potentials for realizing axion electrodynamics and advancing quantum-computing applications.

36 MATERIALS SCIENCE↗