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Chunmei Zhang

Publications and source records attributed to Chunmei Zhang.

18 recordsLinked to original sources

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 $χ^{(2)}$ 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

Bulk Photovoltaic Effect in Two-Dimensional Perovskite Oxides

Perovskite oxides ABO$_3$ host a rich interplay of charge, spin, lattice, and orbital degrees of freedom, giving rise to diverse quantum phenomena. In low-dimensional ABO$_3$, reduced symmetry can induce exotic quantum effects such as the two-dimensional electron gas and unconventional superconductivity. Using first-principles density functional theory, tight-binding modeling, and symmetry analysis, we show that ultrathin two-dimensional (2D) ABO$_3$ films -- exemplified by SrTiO$_3$ -- naturally break inversion symmetry, producing a spontaneous out-of-plane bulk photovoltaic (BPV) effect. This differs from previous studies on in-plane BPV current signals and is more applicable and experimentally detectable. Such an effect is highly tunable via thickness, strain, surface termination, crystallographic orientation, and Moiré twisting. These findings are broadly applicable to a wide range of 2D perovskite and other layer-resolved oxides.

cond-mat.mtrl-sci

Quantitative Bounds and Compactness for the Commutators of Area Integrals Associated with Self-adjoint Operators on Weighted $L^p$ and Morrey Spaces

Let $L$ be a non-negative self-adjoint operator, we consider some commutators generated by the BMO function $b$ and the area integral operator $S_H$ associated with the heat semigroup $\{e^{-tL}\}_{t>0}$ or the area integral operator $S_P$ associated with the Poisson semigroup $\{e^{-t\sqrt{L}}\}_{t>0}$. The strong-type estimates of these commutators on weighted $L^p$ spaces and weighted Morrey spaces are established. At the same time, we verified that these commutators are compact operators on weighted Morrey spaces.

math.CA

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 $\sim4~μ\mathrm{m}$ 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

Bulk Photovoltaic Effects in Helimagnets

The bulk photovoltaic (BPV) effect that converts light into electric current is highly sensitive to the system symmetry and its electronic Bloch wavefunction. To create a sizable net electric current, it is necessary to break the centrosymmetry P in its host material. While prior studies mainly focus on P-broken nonmagnetic (time reversal T-reserved) and collinear antiferromagnetic PT systems, here we adopt magnetic group theory to scrutinize how helical spin polarization breaks P that is otherwise kept in its crystalline geometry. Such spin helix widely exists in intrinsic multiferroics and magnon excitation in collinear magnets. We demonstrate that magnetic symmetries are determined by spin spiral configurations, helical propagation wavevectors, magnetic chirality, and spin winding angles at the home site, offering effective and versatile manipulation of BPV generation in helimagnets. This is illustrated by tight-binding model calculations. Furthermore, we apply our theory to monolayer NiI2, a realistic showcase for helimagnetic material. Our first-principles calculations show that it could host observable direction-dependent BPV current, which could serve as a photoelectric probe to track the subtle magnetic configurations and potential multiferroic nature. This work reveals the fundamental mechanism of the interplay between spin spiral order and nonlinear optics process.

cond-mat.mtrl-sci

Experimental demonstration of improved reference-frame-independent quantum key distribution over 175km

Reference-frame-independent (RFI) quantum key distribution (QKD) presents promising advantages, especially for mobile-platform-based implementations, as it eliminates the need for active reference frame calibration. While RFI-QKD has been explored in various studies, limitations in key rate and distance persist due to finite data collection. In this study, we experimentally demonstrate an improved RFI-QKD protocol proposed by Zhu \textit{et al.} [Opt. Lett. 47, 4219 (2022)], featuring a statistical quantity for bounding information leaked to Eve that exhibits more insensitivity to statistical fluctuations and more robustness to variations in the reference frame. Taking into account finite-size considerations and potential general attacks, RFI-QKD is implemented over a distance of 175 \si{\kilo\meter} in this work. We believe that our study extends the communication distance achievable by RFI-QKD, thereby constituting a notable advancement for its practical application.

quant-ph

Optical Measurement of Photorecombination Time Delays

Recollision physics and attosecond pulse generation meld the precision of optics with collision physics. As a follow-up to our previous work, we reveal a new direction for the study of electronic structure and multielectron dynamics by exploiting the collision-physics nature of recollision. We show experimentally that, by perturbing recollision trajectories with an infrared field, photorecombination time delays can be measured entirely optically using the Cooper minimum in argon as an example. In doing so, we demonstrate the relationship between recollision trajectories and the transition moment coupling the ground and continuum states. In particular, we show that recollision trajectories are influenced by their parent ion, while it is commonly assumed they are not. Our work paves the way for the entirely optical measurement of ultrafast electron dynamics and photorecombination delays due to electronic structure, multielectron interaction, and strong-field driven dynamics in complex molecular systems and correlated solid-state systems.

physics.atom-ph

Two-dimensional hourglass Weyl nodal loop in monolayer Pb(ClO$_{2}$)$_{2}$ and Sr(ClO$_{2}$)$_{2}$

The hourglass fermions in solid-state materials have been attracting significant interest recently. However, realistic two-dimensional (2D) materials with hourglass-shaped band structures are still very scarce. Here, through the first-principles calculations, we identify the monolayer Pb(ClO$_{2}$)$_{2}$ and Sr(ClO$_{2}$)$_{2}$ materials as the new realistic materials platform to realize 2D hourglass Weyl nodal loop. We show that these monolayer materials possess an hourglass Weyl nodal loop circling around the $Γ$ point and Weyl nodal line on the Brillouin zone (BZ) boundary in the absence of spin-orbit coupling (SOC). Through the symmetry analysis, we demonstrate that the hourglass Weyl nodal loop and Weyl nodal line are protected by the nonsymmorphic symmetries, and are robust under the biaxial strains. When we include the SOC, a tiny gap will be opened in the hourglass nodal loop and nodal line, and the nodal line can be transformed into the spin-orbit Dirac points. Our results provide a new realistic material platform for studying the intriguing physics associated with the 2D hourglass Weyl nodal loop and spin-orbit Dirac points.

cond-mat.mtrl-sci

Tailoring Bulk Photovoltaic Effects in Magnetic Sliding Ferroelectric Materials

The bulk photovoltaic effect that is intimately associated with crystalline symmetry has been extensively studied in various nonmagnetic materials, especially ferroelectrics with a switchable electric polarization. In order to further engineer the symmetry, one could resort to spin-polarized systems possessing an extra magnetic degree of freedom. Here, we investigate the bulk photovoltaic effect in two-dimensional magnetic sliding ferroelectric (MSFE) systems, illustrated in VSe2, FeCl2, and CrI3 bilayers. The transition metal elements in these systems exhibit intrinsic spin polarization, and the stacking mismatch between the two layers produce a finite out-of-plane electric dipole. Through symmetry analyses and first-principles calculations, we show that photoinduced in-plane bulk photovoltaic current can be effectively tuned by their magnetic order and the out-of-plane dipole moment. The underlying mechanism is elucidated from the quantum metric dipole distribution in the reciprocal space. The ease of the fabrication and manipulation of MSFEs guarantee practical optoelectronic applications.

cond-mat.mtrl-sci

On weighted Compactness of Commutators of square function and semi-group maximal function associated to Schrodinger operator

In this paper, the object of our investigation is the following Littlewood-Paley square function $g$ associated with the Schrödinger operator $L=-Δ+V$ which is defined by: $g(f)(x)=\Big(\int_{0}^{\infty}\Big|\frac{d}{dt}e^{-tL}(f)(x)\Big|^2tdt\Big)^{1/2},$ where $Δ$ is the laplacian operator on $\mathbb{R}^n$ and $V$ is a nonnegative potential. We show that the commutators of $g$ are compact operators from $L^p(w)$ to $L^p(w)$ for $1 0}|e^{-tL}f(x)|.$

math.CA

Switchable Topological Phase Transition and Novel Nonlinear Optical Properties in ReC2H Monolayer

Extensive investigations on topological phase transition (TPT) in three-dimensional compounds have been done. whereas, rare in two-dimensional systems, let alone noncentrosymmetric materials. In this work, based on first-principles calculations, we explore an inversion symmetry broken structural ReC2H monolayer. We reveal that it undergoes two TPTs, namely from normal insulator to Z2 topological insulator and back to normal insulator, at the critical biaxial strain of 2.3% and 7.8%, respectively. The band inversion occurs at the generic momentum in the first TPT, while at high symmetric K point in the second one. Usually, band inversion is identified by the exchange in the components or irreducible representations of the wavefunctions. These quantities can be easily obtained in theoretical calculation but hard to be detected in experimental techniques like Angle-resolved photoemission spectroscopy. It is well known that nonlinear optical (NLO) response is very sensitive to the components and symmetries of the engaged bands, which also incorporates information of band topology. Therefore, we study the shift current, one of the widely explored NLO responses in noncentrosymmetric systems, during the two TPTs. We find that in both cases band inversion leads to the sign change of shift vectors around the momenta where the bandgap closes and reopens. Whereas the shift current, as the overall contribution of shift vectors weighted by the absorption rate in the whole Brillouin zone, may keep its direction. This work offers insight that a scrutinized examination is highly demanded in utilizing shift current to detect TPT.

cond-mat.mtrl-sci

Correlation-driven topological and valley states in monolayer VSi$_{2}$P$_{4}$

Electronic correlations could have significant impact on the material properties. They are typically pronounced for localized orbitals and enhanced in low-dimensional systems, so two-dimensional (2D) transition metal compounds could be a good platform to study their effects. Recently, a new class of 2D transition metal compounds, the MoSi$_2$N$_4$-family materials, have been discovered, and some of them exhibit intrinsic magnetism. Here, taking monolayer VSi$_{2}$P$_{4}$ as an example from the family, we investigate the impact of correlation effects on its physical properties, based on the first-principles calculations. We find that different correlation strength can drive the system into a variety of interesting ground states, with rich magnetic, topological and valley features. With increasing correlation strength, while the system favors a ferromagnetic semiconductor state for most cases, the magnetic anisotropy and the band gap type undergo multiple transitions, and in the process, the band edges can form single, two or three valleys for electrons or holes. Remarkably, there is a quantum anomalous Hall (QAH) insulator phase, which has a unit Chern number. The boundary of the QAH phase correspond to the half-valley semimetal state with fully valley polarized bulk carriers. We further show that for phases with the out-of-plane magnetic anisotropy, the interplay between spin-orbit coupling and orbital character of valleys enable an intrinsic valley polarization for electrons but not for holes. This electron valley polarization can be switched by reversing the magnetization direction, providing a new route of magnetic control of valleytronics. Our result sheds light on the possible role of correlation effects in the 2D transition metal compounds, and it will open new perspectives for spintronic, valleytronic and topological nanoelectronic applications based on these materials.

cond-mat.mtrl-sci

Characterizing multielectron dynamics during recollision

Measuring the delay for an electron to emerge from different states is one of the major achievements of attosecond science. This delay can have two origins - the electron wave packet is reshaped during departure by the electrostatic field of the ionizing medium or it is modified by dynamic interaction with the remaining electrons. Most experiments have observed the former, but confirmation requires a complex calculation. A direct measurement of multielectron dynamics is needed. Photo-recombination - the inverse of photoionization - occurs naturally during electron recollision and can be measured by combining a perturbing beam to modify the recollision electron before recombination. These in situ methods allow us to unambiguously isolate multielectron dynamics - the reference being the spectral phase of an attosecond pulse simultaneously measured in spectral regions without multielectron interaction. Here, we measure the group delay of the recollision electron caused by plasmonic resonance dynamics in Xe, simulate the in situ measured spectral phase of a recollision electron generated in the presence of the plasmonic resonance in C$_{60}$ and present a corresponding semi-classical theory based on the strong-field approximation. Our results suggest that in situ techniques, together with 300 eV recollision electrons, will allow the ultimate time response of electronic matter to be measured.

physics.atom-ph

Near-field imaging of dipole emission modulated by an optical grating

Multiphoton-ionized electrons are born into a strong light field that will determine their short-term future. By controlling the infrared beam, we enable atoms or molecules to generate extreme ultraviolet (XUV) pulses and synthesize attosecond pulses - the shortest controlled events ever produced. Here we show that a weak obliquely incident beam imposes an optical grating on the fundamental beam, resulting in a spatially modulated attosecond pulse. We observe the modulation on a spectrally resolved near-field XUV image, encoding all information of the spectral phase of the recollision electron and, therefore, the attosecond pulse produced by structureless atoms. Near-field imaging is an efficient method for measuring the duration of attosecond pulses, especially important for soft X-ray pulses created in helium. For more complex systems, it includes auto ionization and giant plasmon resonances.

physics.atom-ph

Characterizing Fano Resonances During Recollision

When intense light irradiates a quantum system, an ionizing electron recollides with its parent ion within the same light cycle and, during that very brief (few femtosecond) encounter, its kinetic energy sweeps from low to high energy and back. Therefore, recollision offers unprecedented time resolution and it is the foundation on which attosecond science is built. For simple systems, recolliding trajectories are shaped by the strong field acting together with the Coulomb potential and they can be readily calculated and measured. However, for more complex systems, multielectron effects are also important because they dynamically alter the recolliding wave packet trajectories. Here, we theoretically study Fano resonances, one of the most accessible multielectron effects, and we show how multielectron dynamics can be unambiguously isolated when we use in situ measurement. The general class of in situ measurement can provide key information needed for time-dependent ab initio electronic structure theory and will allow us to measure the ultimate time response of matter.

physics.atom-ph

Surface Adhesion of Back-Illuminated Ultrafast Laser-Treated Polymers

We report a decreased surface wettability when polymer films on a glass substrate are treated by ultra-fast laser pulses in a back-illumination geometry. We propose that back-illumination through the substrate confines chemical changes beneath the surface of polymer films, leaving the surface blistered but chemically intact. To confirm this hypothesis, we measure the phase contrast of the polymer when observed with a focused ion beam. We observe a void at the polymer-quartz interface that results from the expansion of an ultrafast laser-induced plasma. A modified polymer layer surrounds the void, but otherwise the film seems unmodified. We also use X-ray photoelectron spectroscopy to confirm that there is no chemical change to the surface. When patterned with partially overlapping blisters, our polymer surface shows increased hydrophobicity. The increased hydrophobicity of back-illuminated surfaces can only result from the morphological change. This contrasts with the combined chemical and morphological changes of the polymer surface caused by a front-illumination geometry.

physics.app-ph

Control of $\text{N}_2^+$ Air Lasing

A near-infrared laser generates gain on transitions between the $\text{B}^{\text{2}} Σ_{\text{u}}^{\text{+}}$ and $\text{X}^{\text{2}} Σ_{\text{g}}^{\text{+}}$ states of the nitrogen molecular cation in part by coupling the $\text{X}^{\text{2}} Σ_{\text{g}}^{\text{+}}$ and $\text{A}^{\text{2}} Π_{\text{u}}$ states in the V-system. Traditional time resolved pump-probe measurements rely on post-ionization coupling by the pump pulse to initialize dynamics in the $\text{A}^{\text{2}} Π_{\text{u}}$ state. Here we show that a weak second excitation pulse reduces ambiguity because it acts only on the ion independent of ionization. The additional control pulse can increase gain by moving population to the $\text{A}^{\text{2}} Π_{\text{u}}$ state, which modifies the lasing emission in two distinct ways. The presence of fast decoherence on $\text{X}^{\text{2}} Σ_{\text{g}}^{\text{+}}$ to $\text{A}^{\text{2}} Π_{\text{u}}$ transitions may prevent the formation of a coherent rotational wave packet in the ground state in our experiment, but the control pulse can reverse impulsive alignment by the pump pulse to remove rotational wave packets in the $\text{B}^{\text{2}} Σ_{\text{u}}^{\text{+}}$ state.

physics.optics

Asymmetric sending or not-sending twin-field quantum key distribution in practice

Quantum key distribution (QKD) offers a secret way to share keys between legitimate users which is guaranteed by the law of quantum mechanics. Most recently, the limitation of transmission distance without quantum repeaters was broken through by twin-field QKD [Nature (London) 557, 400 (2018)]. Based on its main idea, sending or not-sending (SNS) QKD protocol was proposed [Phys. Rev. A 98, 062323 (2018)], which filled the remaining security loopholes and can tolerate large misalignment errors. In this paper, we give a more general model for SNS QKD, where the two legitimate users, Alice and Bob, can possess asymmetric quantum channels. By applying the method present in the work, the legitimate users can achieve dramatically increased key generation rate and transmission distance compared with utilizing the original symmetric protocol. Therefore, our present work represents a further step along the progress of practical QKD.

quant-ph