arXiv subjects

Nanlin Wang

Publications and source records attributed to Nanlin Wang.

At least 19 recordsLinked to original sources

arXiv2026

Temperature-driven sodium-ion dynamical-to-static crossover in the zig-zag ordered phase of Na$_{0.5}$CoO$_2$

We employ polarization-resolved Raman spectroscopy combined with first-principles calculations to study the sodium-ion lattice dynamics in a sodium zig-zag ordered cobaltate compound Na$_{0.5}$CoO$_2$. We detect two sodium phonon modes for the first time, and their mode frequencies are consistent with first-principles phonon calculations based on an orthorhombic unit cell. We find that they appear below around $T^*\sim300\pm50$K with large linewidth broadening, much lower than the sodium zig-zag ordering temperature $T_\text{S}\sim460$K, and then narrow at lower temperatures. We interpret the sodium-phonon anomalies occurring at $T^*$ as a dynamical-to-static crossover involving mainly the motion of sodium ions. Our results suggest that the gradual freezing of the sodium ions and the well-defined static sodium-zigzag order below $T^*$ set the stage for the emergent electronic and magnetic orders in the CoO$_2$ layer of Na$_{0.5}$CoO$_2$.

cond-mat.mtrl-sci↗

arXiv2026

Ultrafast Terahertz and Optical Spectroscopy under Synergetic Extreme Conditions

Elucidating and manipulating emergent phases in complex materials requires direct access to their low-energy collective modes. Terahertz (THz) time-domain and ultrafast optical spectroscopies have emerged as indispensable experimental tools, enabling the probing of intrinsic electrodynamics and the coherent control of non-equilibrium states. At the Synergetic Extreme Condition User Facility (SECUF), we have developed a suite of intense ultrashort light sources covering the near-infrared, mid-infrared, and THz spectral ranges. By integrating these strong-field pulses with extreme sample environments, such as low temperatures, strong magnetic fields, and high pressures, we have established several state-of-the-art spectroscopy platforms. In this article, we outline the technical specifications of each setup and highlight representative user experiments. The presented results underscore the exceptional capability of the THz experimental unit (A4-2) to explore ultrafast dynamics across a multi-parameter thermodynamic phase space.

physics.optics↗

arXiv2026

Multimodal Terahertz Spectroscopy of the Pairing Symmetry and Normal-State Pseudogap in (La,Pr)$_3$Ni$_2$O$_7$ Films

The discovery of ambient-pressure superconductivity in compressively strained (La,Pr)$_3$Ni$_2$O$_7$ thin films has intensified efforts to identify the pairing mechanism. However, the symmetry of the superconducting order parameter and the character of the normal state remain unsettled. Here we combine bulk-sensitive terahertz (THz) time-domain spectroscopy with THz third-harmonic generation to present spectroscopic insights into these issues. Linear THz spectroscopy reveals a bulk superconducting response in the (La,Pr)$_3$Ni$_2$O$_7$ films, evidenced by the suppression of low-frequency spectral weight below the onset critical temperature, $T_\mathrm{c}^{\mathrm{onset}}$. A weak coherence peak near $T_\mathrm{c}^{\mathrm{onset}}$, together with substantial residual low-frequency conductivity as $T\to 0$, is consistent with disordered $s_{\pm}$-wave pairing. In the nonlinear regime, the third-harmonic signal rises sharply on cooling through $T_\mathrm{c}^{\mathrm{onset}}$, providing an independent signature of the transition. Strikingly, the nonlinear response persists above $T_\mathrm{c}^{\mathrm{onset}}$, pointing to either disorder-enhanced nonlinearity or a distinct correlated normal state. Motivated by angle-resolved photoemission spectroscopy on similarly grown films that identifies a comparable temperature scale, we associate the anomalous normal-state terahertz nonlinearity with a pseudogap. These results establish (La,Pr)$_3$Ni$_2$O$_7$ as a bulk superconductor with $s_{\pm}$-like pairing that coexists with, and may compete with, a distinct ordered state, providing a platform for exploring unconventional superconductivity beyond cuprates and pnictides.

cond-mat.supr-con↗

arXiv2026

Efficient high-harmonic generation in van der Waals ferroelectric NbOI$_2$ crystals

Layered NbOX$_2$ ($X=\mathrm{Cl,\,Br,\,I}$), a member of the van der Waals ferroelectric family, exhibits intrinsic ferroelectricity and pronounced nonlinear optical responses, making it a promising candidate for integrated nanophotonics applications. While previous studies have emphasized the material's strong second-order nonlinear responses, higher-order nonlinear responses are still mostly unexplored. This work systematically investigates NbOI$_2$ using high harmonic generation (HHG) spectroscopy. Driven by an intense mid-infrared laser field centered at $\sim4~\mu\mathrm{m}$ wavelength, highly anisotropic odd- and even-order harmonics up to the 16th order are generated at a low peak intensity of $0.4~\mathrm{TW\,cm^{-2}}$, extending beyond the material's bandgap. Both bulk and flake forms of NbOI$_2$ display pronounced harmonic emission from the near-infrared to the deep-ultraviolet spectral region, with a notably high overall conversion efficiency compared to other known materials. Polarization-resolved measurements reveal that even-order harmonics remain aligned with the crystal polar axis regardless of the driving-field orientation, whereas odd-order harmonics are dynamically affected. First-principles calculations suggest that the flat valence band associated with Peierls dimerization enhances HHG efficiency through electron correlation. These findings provide fresh perspectives on HHG in van der Waals ferroelectric materials and facilitate the development of compact and tunable quantum light sources.

cond-mat.mtrl-sci↗

arXiv2025

Anomalous terahertz nonlinearity in disordered s-wave superconductor close to the superconductor-insulator transition

Detection of the Higgs mode in superconductors using nonlinear terahertz spectroscopy is a key area of interest in condensed matter physics. We investigate the influence of disorder on the nonlinear terahertz response and the Higgs mode in NbN thin films with varying Ioffe-Regel parameters ($k_Fl$). In strongly disordered films near the superconductor-insulator transition (SIT), we observe an anomalous third-harmonic generation (THG) signal above $T_c$, which is absent in both cleaner superconducting and non-superconducting counterparts. The persistence of this normal-state THG signal in a high magnetic field excludes superconducting fluctuations as its origin. Below $T_c$, the THG intensity increases sharply, indicating a dominant contribution from the driven Higgs mode. The THG spectrum of the strongly disordered sample exhibits a broadened, multi-peak structure, which we attribute to quantum path interference between distinct channels involving unpaired electrons and Cooper pairs within emergent superconducting islands. Our findings not only demonstrate how disorder tunes the nonlinear terahertz response but also uncover a strong coupling between electrons responsible for normal-state THG and the superconducting Higgs mode below $T_c$ in strongly disordered samples.

cond-mat.supr-con↗

arXiv2025

Ultrafast giant enhancement of second harmonic generation in a strongly correlated cobaltite

In quantum materials, nonlinear optical responses are highly sensitive to electronic structure and many-body interactions. Probing and manipulating such nonlinear processes is a complex and subtle endeavor, yet it offers deep insights into emerging physics and functionalities. Here, we report an anomalous ultrafast enhancement of second harmonic generation (SHG) in a strongly correlated cobaltite YbBaCo$_4$O$_7$. Above-bandgap femtosecond pumping increases SHG intensity by up to 60 % within 200 fs, with the enhancement persisting for tens of picoseconds. The enhancement is strongly anisotropic, with substantial amplification of in-plane susceptibility tensors, whereas the out-of-plane counterpart shows negligible change. We attribute these anomalies to ultrafast photodoping-induced modulation of the on-site Coulomb repulsion, which dynamically renormalizes the band structure and selectively amplifies specific $\chi^{(2)}$ components. These nonlinear dynamics encode rich information about the orbital symmetries and energies of the states involved, opening new avenues for all-optical probing of electronic structure in strongly correlated materials.

cond-mat.str-el↗

arXiv2025

Structural contribution to light-induced gap suppression in Ta$_2$NiSe$_5$

An excitonic insulator is a material that hosts an exotic ground state, where an energy gap opens due to spontaneous condensation of bound electron-hole pairs. Ta$_2$NiSe$_5$ is a promising candidate for this type of material, but the coexistence of a structural phase transition with the gap opening has led to a long-standing debate regarding the origin of the insulating gap. Here we employ MeV ultrafast electron diffraction to obtain quantitative insights into the atomic displacements in Ta$_2$NiSe$_5$ following photoexcitation, which has been overlooked in previous time-resolved spectroscopy studies. In conjunction with first-principles calculations using the measured atomic displacements, we find that the structural change can largely account for the photoinduced reduction in the energy gap without considering excitonic effects. Our work illustrates the importance of a quantitative reconstruction of individual atomic pathways during nonequilibrium phase transitions, paving the way for a mechanistic understanding of a diverse array of phase transitions in correlated materials where lattice dynamics can play a pivotal role.

cond-mat.mtrl-sci↗

arXiv2025

Mn4Al11: A Half-Semimetal Candidate with Anomalous Electronic Behaviors

Half-semimetals, characterized by their spin-polarized electronic states, hold significant promise for spintronic applications but remain scarce due to stringent electronic and magnetic criteria. Through a combination of transport measurements and optical spectroscopy, we investigated the intermetallic compound Mn4Al11, which features an exceptionally low carrier concentration and undergoes a magnetic phase transition near 68 K. Transport measurements reveal anomalies that deviate from typical metallic behavior at low temperatures. Optical spectroscopy indicates a small, nearly frequency-independent optical conductivity in the far-infrared region, with spectral weight decreasing as the temperature drops from 300 K to 50 K. These behaviors suggest a temperaturedependent carrier density and significant scattering of charge carriers. Combining experimental findings with calculated electronic band structures, we propose that Mn4Al11 is a novel half-semimetal candidate exhibiting a ferrimagnetic ground state.

cond-mat.str-el↗

arXiv2025

Collapse of density wave and emergence of superconductivity in pressurized-La$_4$Ni$_3$O$_{10}$ evidenced by ultrafast spectroscopy

Recent discoveries of superconductivity in Ruddlesden-Popper nickelates realize a rare category of superconductors. However, the use of high-pressure diamond anvil cells limits spectroscopic characterization of the density waves and superconducting gaps. Here, we systematically studied the pressure evolution of La$_{4}$Ni$_{3}$O$_{10}$ using ultrafast optical pump-probe spectroscopy. We found that the transition temperature and energy gap of density waves are suppressed with increasing pressure and disappear suddenly near 17 GPa where structural transition appears. In addition, the observation of a single density wave gap indicates that the spin density wave and charge density wave remain coupled as pressure increases, rather than decoupling. After the density wave collapse, a distinct low-temperature regime emerges, characterized by a small gap consistent with potential superconducting pairing. The separated phase region of superconductivity and density waves suggests that superconductivity in pressurized-La$_4$Ni$_3$O$_{10}$ competes strongly with density waves, offering new insights into the interplay between these two phenomena.

cond-mat.supr-con↗

arXiv2025

Field-induced spin continuum in twin-free Na$_3$Co$_2$SbO$_6$ revealed by magneto-THz spectroscopy

The honeycomb magnet Na$_3$Co$_2$SbO$_6$ recently emerged as a promising candidate for realizing Kitaev quantum spin liquid with relatively low levels of structural disorder. While the precise spin Hamiltonian remains controversial, the potential existence of a quantum spin liquid or other novel quantum magnetic phases continues to stimulate investigation. Here, we study the temperature and magnetic field-dependent spin excitations of Na$_3$Co$_2$SbO$_6$ on a twin-free single crystal using magneto-terahertz (THz) spectroscopy, focusing on magnetic anisotropy and field-induced unusual phases. We observe a low-energy continuum excitation above $T_N$ and a 0.5 THz (2 meV) spin wave excitation in magnetic order under zero field. Upon applying an in-plane magnetic field, the spin waves transform to a magnetic continuum over an intermediate field range, above which the system enters a spin-polarized state. Crucially, the spin excitation spectra reveal striking anisotropy between the $\textbf{a}$ and $\textbf{b}$ crystallographic axes, demanding description by a strongly anisotropic spin model. These findings establish Na$_3$Co$_2$SbO$_6$ as a model system for investigating field-tunable quantum magnetism and potential spin liquid behavior in highly anisotropic systems.

cond-mat.str-el↗

arXiv2025

Ultrafast Orbital-Selective Photodoping Melts Charge Order in Overdoped Bi-based Cuprates

High-temperature superconductivity in cuprates remains one of the enduring puzzles of condensed matter physics, with charge order (CO) playing a central yet elusive role, particularly in the overdoped regime. Here, we employ time-resolved X-ray absorption spectroscopy and resonant X-ray scattering at a free-electron laser to probe the transient electronic density of states and ultrafast CO dynamics in overdoped (Bi,Pb)$_{2.12}$Sr$_{1.88}$CuO$_{6+δ}$. We reveal a striking pump laser wavelength dependence - the 800 nm light fails to suppress CO, whereas the 400 nm light effectively melts it. This behavior originates from the fact that 400 nm photons can promote electrons from the Zhang-Rice singlet band to the upper Hubbard band or apical oxygen states, while 800 nm photons lack the energy to excite electrons across the charge-transfer gap. The CO recovery time ($\sim$3 ps) matches that of the underdoped cuprates, indicating universal electronic instability in the phase diagram. Additionally, melting overdoped CO requires an order-of-magnitude higher fluence highlighting the role of lattice interactions. Our findings demonstrate orbital-selective photodoping and provide a route to ultrafast control of emergent quantum phases in correlated materials.

cond-mat.supr-con↗

arXiv2025

Origin of the density wave instability in trilayer nickelate La$_{4}$Ni$_{3}$O$_{10}$ revealed by optical and ultrafast spectroscopy

In the intricate phase diagram of unconventional superconductors characterized by intertwined electronic orders and superconductivity, a key step in understanding the superconducting mechanism is to investigate the parent compounds from which superconductivity emerges through doping or pressure. In this study, we employed optical spectroscopy and ultrafast reflectivity measurements to examine the density wave instability in the trilayer nickelate La$_{4}$Ni$_{3}$O$_{10}$, which displays pressure-induced superconductivity up to 30 K. Our optical spectroscopy measurements reveal that La$_{4}$Ni$_{3}$O$_{10}$ behaves as a metal with a high plasma frequency. Upon cooling, we observed a distinct formation of a density wave energy gap in both optical conductivity and pump-probe measurements. The gap feature is more pronounced compared to the bilayer nickelate La$_{3}$Ni$_{2}$O$_{7}$. Through a comparison of the experimentally determined plasma frequency with first-principles calculations, we classify La$_{4}$Ni$_{3}$O$_{10}$ as a moderately electron-correlated material, resembling the parent compound of iron-based superconductors but exhibiting weaker correlation than the bilayer nickelate La$_{3}$Ni$_{2}$O$_{7}$. The enhanced gap feature and weaker electronic correlation in La$_{4}$Ni$_{3}$O$_{10}$ may explain its lower superconductivity transition temperature under high pressure. These findings significantly advance our comprehension of the density wave and superconductivity mechanisms in the trilayer nickelate La$_{4}$Ni$_{3}$O$_{10}$.

cond-mat.str-el↗

arXiv2025

Photo-induced Dynamics and Momentum Distribution of Chiral Charge Density Waves in 1T-TiSe$_{2}$

Exploring the photoinduced dynamics of chiral states offers promising avenues for advanced control of condensed matter systems. Photoinduced or photoenhanced chirality in 1T-TiSe$_{2}$ has been suggested as a fascinating platform for optical manipulation of chiral states. However, the mechanisms underlying chirality training and its interplay with the charge density wave (CDW) phase remain elusive. Here, we use time-resolved X-ray diffraction (tr-XRD) with circularly polarized pump lasers to probe the photoinduced dynamics of chirality in 1T-TiSe$_{2}$. We observe a notable ($\sim$20%) difference in CDW intensity suppression between left- and right-circularly polarized pumps. Additionally, we reveal momentum-resolved circular dichroism arising from domains of different chirality, providing a direct link between CDW and chirality. An immediate increase in CDW correlation length upon laser pumping is detected, suggesting the photoinduced expansion of chiral domains. These results both advance the potential of light-driven chirality by elucidating the mechanism driving chirality manipulation in TiSe$_2$, and they demonstrate that tr-XRD with circularly polarized pumps is an effective tool for chirality detection in condensed matter systems.

cond-mat.str-el↗

arXiv2025

Interlayer Hopping between Surface Mott Insulator and Bulk Band Insulator in layered 1T-TaS_{2}

In condensed matter physics, various mechanisms give rise to distinct insulating phases. The competition and interplay between these phases remain elusive, even for the seemingly most distinguishable band and Mott insulators. In multilayer systems, such interplay is mediated by interlayer hopping, which competes with the Coulomb repulsion to determine the nature of insulators. The layered compound 1T-TaS_{2} provides an ideal platform for investigating this phenomenon, as it naturally hosts coexisting Mott and band insulating states. However, distinguishing these distinct insulating states and characterizing the evolution remain challenging. In this study, we employ a dual approach utilizing surface-sensitive High-Resolution Electron Energy Loss Spectroscopy (HREELS) and bulk-sensitive Fourier-transform Infrared Spectroscopy (FTIR) to investigate the electronic excitation spectrum of 1T-TaS_{2}. Our methodology effectively identifies the features originating from the Mott and band insulators by analyzing the differences in their bulk and surface spectral weights, along with their energy distinctions. Based on the previous identification, we further investigate the evolution of insulating state features in the homostructure as they are modulated by temperature. The measurements and Dynamical Mean-Field Theory (DMFT) calculations suggest that the softening and broadening of Hubbard excitations in the Mott state with increasing temperature result from enhanced interlayer hopping between the Mott and band insulators.

cond-mat.mtrl-sci↗

arXiv2024

Selective excitation of collective modes in multiband superconductor MgB2

Recent developments in nonequilibrium and nonlinear terahertz (THz) spectroscopies have significantly advanced our understanding of collective excitations in superconductors. However, there is still debate surrounding the identification of Higgs or Leggett modes, as well as BCS charge fluctuations, in the well-known two-band superconductor MgB$_2$. Here, we utilized both multi-cycle and single-cycle THz pump-broadband THz probe techniques to investigate the THz nonlinear response of MgB$_2$. Through multicycle THz pump-THz probe experiments on MgB$_2$, we observed distinct nonlinear signals at both the fundamental frequency ($ω$) and the second harmonic frequency (2$ω$) of the pump pulses, which exhibited resonant enhancement at temperatures where their frequencies respectively match 2$Δ_π(T)$. They are mainly attributed to the $π$-band Higgs mode. By adjusting the THz pump pulse to a single-cycle waveform that satisfies non-adiabatic excitation criteria, we observed an over-damped oscillation corresponding to the Leggett mode. Our findings contribute to solving the ongoing debates and demonstrate the selective excitation of collective modes in multiband superconductors, offering new insights into the interaction between Higgs and Leggett modes.

cond-mat.supr-con↗

arXiv2024

Room-temperature non-volatile optical manipulation of polar order in a charge density wave

Utilizing ultrafast light-matter interaction to manipulate electronic states of quantum materials is an emerging area of research in condensed matter physics. It has significant implications for the development of future ultrafast electronic devices. However, the ability to induce long-lasting metastable electronic states in a fully reversible manner is a long-standing challenge.Here, by using ultrafast laser excitations, we demonstrate the capability to manipulate the electronic polar states in the charge-density-wavematerial EuTe4 in a non-volatile manner. The process is completely reversible and is achieved at room temperature with an all-optical approach. Each induced non-volatile state brings about modifications to the electrical resistance and second harmonic generation intensity. The results point to layer-specific phase inversion dynamics by which photoexcitation mediates the stacking polar order of the system. Our findings extend the scope of non-volatile all-optical control of electronic states to ambient conditions, and highlight a distinct role of layerdependent phase manipulation in quasi-two-dimensional systems with inherent sublayer stacking orders.

cond-mat.str-el↗

arXiv2024

Using magnetic dynamics to measure the spin gap in a candidate Kitaev material

Materials potentially hosting Kitaev spin-liquid states are considered crucial for realizing topological quantum computing. However, the intricate nature of spin interactions within these materials complicates the precise measurement of low-energy spin excitations indicative of fractionalized excitations. Using Na$_{2}$Co$_2$TeO$_{6}$ as an example, we study these low-energy spin excitations using the time-resolved resonant elastic x-ray scattering (tr-REXS). Our observations unveil remarkably slow spin dynamics at the magnetic peak, whose recovery timescale is several nanoseconds. This timescale aligns with the extrapolated spin gap of $\sim$ 1 $μ$eV, obtained by density matrix renormalization group (DMRG) simulations in the thermodynamic limit. The consistency demonstrates the efficacy of tr-REXS in discerning low-energy spin gaps inaccessible to conventional spectroscopic techniques.

cond-mat.str-el↗

arXiv2023

Revealing the frequency-dependent oscillations in the nonlinear terahertz response induced by the Josephson current

Nonlinear responses of superconductors to intense terahertz radiation has been an active research frontier. Using terahertz pump-terahertz probe spectroscopy, we investigate the c-axis nonlinear optical response of a high-temperature superconducting cuprate. After excitation by a single-cycle terahertz pump pulse, the reflectivity of the probe pulse oscillates as the pump-probe delay is varied. Interestingly, the oscillatory central frequency scales linearly with the probe frequency, a fact widely overlooked in pump-probe experiments. By theoretically solving the nonlinear optical reflection problem on the interface, we show that our observation is well explained by the Josephson-type third-order nonlinear electrodynamics, together with the emission coefficient from inside the material into free space. The latter results in a strong enhancement of the emitted signal whose physical frequency is around the Josephson plasma edge. Our result offers a benchmark for and new insights into strong-field terahertz spectroscopy of related quantum materials.

cond-mat.supr-con↗