Within the multielectron model of magnetic insulator with spin crossover under high pressure we have studied the mean field phase diagrams in pressure temperature plane and dynamics of a sudden excited non equilibrium spin state. We obtain the different relaxation of the magnetization, high spin/low spin occupation numbers, and the metal oxygen bond length for different values of the external pressure. We found the long living oscillations of magnetization without pressure and at small external pressure. Close to crossover pressure the smooth relaxation is accompanied with a set of sharp strongly non linear oscillations of magnetization and HS/LS occupation numbers that are accompanied by the Franck Condon resonances.
Ultrafast quantum dynamics relaxation of a photoexcited state in a strongly correlated spin crossover system LaCoO3 under a sudden perturbation is considered with the density matrix generalized master equation. The magnetization and cobalt-oxygen bond length oscillations were found. The evolution of the electronic band structure during relaxation is calculated in the framework of the LDA+GTB method.
We utilize near-infrared pump and mid-infrared probe spectroscopy to investigate the ultrafast electronic response of pressurized VO$_2$. Distinct pump-probe signals and a pumping threshold behavior are observed even in the pressure-induced metallic state showing a noticeable amount of localized electronic states. Our results are consistent with a scenario of a bandwidth-controlled Mott-Hubbard transition.
We investigate the nonequilibrium photocarrier dynamics of WTe2 under pressure using the optical pump-probe spectroscopy. The pressure dependences of the electronic relaxation manifest anomalous changes around 0.8, 3.5, and 6 GPa, indicating the abruptions in the electron-phonon interactions. In addition, the coherent phonon oscillations originating from shear mode suddenly disappears above 3.5 GPa, which marks the onset of Td-1T' structural phase transition. Supported by the theoretical calculation, we unveil the electronic topological transitions (ETTs), especially an emergence of a new type…
We report electrical resistivity, ac magnetic susceptibility and X-ray absorption spectroscopy measurements of intermediate valence YbNi$_{3}$Ga$_{9}$ under pressure and magnetic field. We have revealed a characteristic pressure-induced Yb valence crossover within the temperature-pressure phase diagram, and a first-order metamagnetic transition is found below $P_{\rm c}$ $\sim$ 9 GPa where the system undergoes a pressure-induced antiferromagnetic transition. As a possible origin of the metamagnetic behavior, a critical valence fluctuation emerging near the critical point of the first-order val…
In solid materials, the parameters relevant to quantum effects, such as the spin quantum number, are basically determined and fixed at the chemical synthesis, which makes it challenging to control the amount of quantum correlations. We propose and demonstrate a method for active control of the classical-quantum crossover in magnetic insulators by applying external pressure. As a concrete example, we perform high-field, high-pressure measurements on CsCuCl$_3$, which has the structure of weakly-coupled spin chains. The magnetization process experiences a continuous evolution from the semi-class…
Heavy Fermion superconductor CeCu$_2$Si$_2$ under high pressure: multiprobing the valence crossover
第一个重费米子超导体CeCu $_2$ Si $_2$还没有完全揭开它的神秘面纱。在高压下，超导性被认为是由价态涨落介导的，而在环境压力下，自旋涨落最有可能充当配对粘合剂。我们对高质量的CeCu $_2$ Si $_2$单晶进行了多探针（电输运、热电势、交流比热、霍尔和能斯特效应）实验，直至$7 \text{GPa}$。可靠的电阻率数据揭示了第一次的标度行为接近假定的价态转变，并允许定位在$4.5\pm0.2 \text{GPa}$和一个稍微负的温度的临界终点。在相同的压力区域，显着的功能也已被检测到的其他物理性质，作为进一步的签名的Ce价交叉和相关的临界波动。
Crossover from impurity-induced ordered phase to uniform antiferromagnetic phase under hydrostatic pressure in the doped spin-gap system TlCu$_{1-x}$Mg$_x$Cl$_3$
This work reports on the pressure dependence of the octahedra tilts and mean Fe-O bond lengths in RFeO3 (R=Nd, Sm, Eu, Gd, Tb and Dy), determined through synchrotron X-ray diffraction and Raman scattering, and their role on the pressure induced phase transition displayed by all of these compounds. For larger rare-earth cations (Nd-Sm), both anti- and in-phase octahedra tilting decrease as pressure increases, whereas the reverse behavior is observed for smaller ones (Gd-Dy). EuFeO3 stands at the borderline, as the tilts are pressure independent. For the compounds where the tilts increase with p…
We have studied the sub-picosecond quasiparticle dynamics in the perovskite manganite La0.7Ca0.3MnO3 and the layered manganite La1.4Sr1.6Mn2O7 using ultrafast optical spectroscopy. We found that for T > TC, initial relaxation proceeds on the time scale of several hundred femtoseconds and corresponds to the redressing of a photoexcited electron to its polaronic ground state. The temperature and dimensionality dependence of this polaron redressing time provides insight into the relationship between polaronic motion and spin dynamics on a sub-picosecond time scale. We also observe a crossover to …
We present results of magnetic susceptibility and thermal expansion measurements performed on high-quality single crystals of EuPd$_2$(Si$_{1-x}$Ge$_x$)$_2$ for 0 $\leq$ x $\leq$ 0.2 and temperatures 2 K $\leq T \leq$ 300 K. Data were taken at ambient pressure and finite He-gas pressure $p$ $\leq$ 0.5 GPa. For x = 0 and ambient pressure we observe a pronounced valence-change crossover centred around $T'_V$ $\approx$ 160 K with a non-magnetic ground state. This valence-change crossover is characterized by an extraordinarily strong pressure dependence of d$T'_V$ /d$p$ = (80 $\pm 10)$ K/GPa. We o…
At ambient pressure, lithium molybdenum purple bronze (Li0.9Mo6O17) is a quasi-one dimensional solid in which the anisotropic crystal structure and the linear dispersion of the underlying bands produced by electronic correlations possibly bring about a rare experimental realization of Tomomaga-Luttinger liquid physics. It is also the sole member of the broader purple molybdenum bronzes family where a Peierls instability has not been identified at low temperatures. The present study reports a pressure-induced series of phase transitions between 0 and 12 GPa. These transitions are strongly refle…
Based on the Phase Hamiltonian, two types of solitons are found to exist in the crossover region between band insulator and Mott insulator in one-dimension. Both of these solitons have fractional charges but with different spins, zero and 1/2, respectively. The results are in accord with the experimental results by Kanoda et al. for TTF-Chloranil under pressure.
Within the framework of a realistic multi-band p-d-model, we derived an effective Hamiltonian to describe the exchange interaction effects near the spin crossover in magnetic Mott-Hubbard insulators under pressure. It is shown that single-ion mechanism of spin crossover under change of the crystal field does not lead to a thermodynamic phase transition, however, at T = 0 a quantum phase transition appears. It has been found that the cooperativity leads to a modification of the quantum phase transition to a first-order phase transition and the appearance of metastable states of the system. The …
Ultrafast Magneto-Pressure Spectroscopy and Control of Correlated Phases in a Trilayer Nickelate
Ames National Laboratory, U.S. Department of Energy（艾姆斯国家实验室）；Department of Physics and Astronomy, Iowa State University（爱荷华州立大学物理与天文学系）；Materials Science Division, Argonne National Laboratory（阿贡国家实验室材料科学部）；School of Physics, Southeast University（东南大学物理学院）；Department of Physics, University of Alabama at Birmingham（阿拉巴马大学伯明翰分校物理系）
We derived simple rules for the sign of superexchange interaction based on the multielectron calculations of the superexchange interaction in the transition metal oxides that are valid both below and above spin crossover under high pressure. The superexchange interaction between two cations in d$^n$ configurations is given by a sum of individual contributions related to the electron-hole virtual excitations to the different states of the d$^{n + 1}$ and d$^{n - 1}$ configurations. Using these rules, we have analyzed the sign of the superexchange interaction of a number of oxides with magnetic …
Superconductivity in strongly correlated systems is a remarkable phenomenon that attracts a huge interest. The study of this problem is relevant for materials as the high $T_c$ oxides, pnictides and heavy fermions. These systems also have in common the existence of electrons of several orbitals that coexist at a common Fermi-surface. In this paper we study the effect of pressure, chemical or applied on multi-band superconductivity. Pressure varies the atomic distances and consequently the overlap of the wave-functions in the crystal. This rearranges the electronic structure that we model inclu…
We report a detailed theoretical study of the electronic structure, spectral properties, and lattice parameters of bulk FeSe under pressure using a fully charge self-consistent implementation of the density functional theory plus dynamical mean-field theory method (DFT+DMFT). In particular, we perform a structural optimization and compute the evolution of the lattice parameters (volume, $c/a$ ratio, and the internal $z$ position of Se) and the electronic structure of the tetragonal (space group $P4/nmm$) paramagnetic FeSe. Our results for the lattice parameters are in good quantitative agreeme…
We report measurements of the physical properties and electronic structure of the hexagonal compounds Yb2Ni12Pn7 (Pn = P, As) by measuring the electrical resistivity, magnetization, specific heat and partial fluorescence yield x-ray absorption spectroscopy (PFY-XAS). These demonstrate a crossover upon reducing the unit cell volume, from an intermediate valence state in Yb2Ni12As7 to a heavy-fermion paramagnetic state in Yb2Ni12P7, where the Yb is nearly trivalent. Application of pressure to Yb2Ni12P7 suppresses T_FL, the temperature below which Fermi liquid behavior is recovered, suggesting th…
The recently discovered kagome superconductors AV3Sb5 exhibit tantalizing high-pressure phase diagrams, in which a new dome-like superconducting phase emerges under moderate pressure. However, its origin is as yet unknown. Here, we carried out the high-pressure electrical measurements up to 150 GPa, together with the high-pressure X-ray diffraction measurements and first-principles calculations on CsV3Sb5. We find the new superconducting phase to be rather robust and inherently linked to the interlayer Sb2-Sb2 interactions. The formation of Sb2-Sb2 bonds at high pressure tunes the system from …
The localized-itinerant nature of Ce-4$f$ valence electrons in heavy fermion compound CeIn$_{3}$ under pressure is studied thoroughly by means of the combination of density functional theory and single-site dynamical mean-field theory. The detailed evolutions of electronic structures of CeIn$_{3}$, including total and partial density of states, momentum-resolved spectral functions, and valence state histograms etc., are calculated in a wide pressure range where the corresponding volume compression $V/V_0 \in [0.6,1.0]$ (here $V_0$ is the experimental crystal volume) at $T \cong 116$ K. Upon in…
We present a first evaluation of the potential for spin crossover (SCO) compounds to be considered as a new class of giant mechanocaloric effect material. From literature data on the variation of the spin crossover temperature with pressure, we estimate the maximum available adiabatic temperature change for several compounds and the relatively low pressures that may be required to observe these effects.
The correlated polar semimetal Ca$_3$Ru$_2$O$_7$ exhibits a rich phase diagram including two magnetic transitions ($T_N$=56 K and $T_C$=48 K) with the appearance of an insulating-like pseudogap (at $T_C$). In addition, there is a crossover back to metallic behavior at $T^*$=30 K, the origin of which is still under debate. We utilized ultrafast optical pump optical probe spectroscopy to investigate quasiparticle dynamics as a function of temperature in this enigmatic quantum material. We identify two dynamical processes, both of which are influenced by the onset of the pseudogap. This includes …
Structural, magnetic and electrical-transport properties of α-LiFeO2, crystallizing in the rock salt structure with random distribution of Li and Fe ions, have been studied by synchrotron X-ray diffraction, 57Fe Mössbauer spectroscopy and electrical resistance measurements at pressures up to 100 GPa using diamond anvil cells. It was found that the crystal structure is stable at least to 82 GPa, though a significant change in compressibility has been observed above 50 GPa. The changes in the structural properties are found to be on a par with a sluggish Fe3+ high- to low-spin (HS-LS) transition…
X-ray diffraction pressure studies at room temperature demonstrate that the spinel FeAl$_{2}$O$_{4}$ transforms to a tetragonal phase at ~18 GPa. This tetragonal phase has a highly irregular unit-cell volume versus pressure dependence up to ~45 GPa, after which a transformation to a Cmcm post-spinel phase is onset. This is attributable to pressure driven Fe-Al site inversion at room temperature, corroborated by signatures in the 57Fe Mössbauer spectroscopy pressure data. At the tetragonal to post-spinel transition, onset in the range 45-50 GPa, there is a concurrent emergence of a non-magnetic…
Layered magnetic transition-metal thiophosphate NiPS3 has unique two-dimensional (2D) magnetic properties and electronic behavior. The electronic band structure and corresponding magnetic state are expected to sensitive to the interlayer interaction, which can be tuned by external pressure. Here, we report an insulator-metal transition accompanied with magnetism collapse during the 2D-3D crossover in structure induced by hydrostatic pressure. A two-stage phase transition from monoclinic (C2=m) to trigonal (P-31m) lattice is identified by ab initio simulation and confirmed by high-pressure XRD …
We present the results of $^{75}$As nuclear magnetic resonance (NMR), nuclear quadrupole resonance (NQR), and resistivity measurements in KFe$_2$As$_2$ under pressure ($p$). The temperature dependence of the NMR shift, nuclear spin-lattice relaxation time ($T_1$) and resistivity show a crossover between a high-temperature incoherent, local-moment behavior and a low-temperature coherent behavior at a crossover temperature ($T^*$). $T^*$ is found to increase monotonically with pressure, consistent with increasing hybridization between localized $3d$ orbital-derived bands with the itinerant elect…
The spin crossover of iron in Fe$^{3+}$-bearing bridgmanite, the most abundant mineral of the Earth's lower mantle, is by now a well-established phenomenon, though several aspects of this crossover remain unclear. Here we investigate effects of disorder, iron concentration, and temperature on this crossover using ab initio LDA + U$_{sc}$ calculations. The effect of concentration and disorder are addressed using complete statistical samplings of coupled substituted configurations in super-cells containing up to 80 atoms. Vibrational/thermal effects on the crossover are addressed within the quas…
X-ray diffraction studies to ~90 GPa at room temperature show that Fe$_{2}$TiO$_{4}$ ferrous inverse spinel undergoes the following sequence of structural transitions : cubic (Fd3m) to tetragonal (I41/amd)to orthorhombic(Cmcm) to orthorhombic(Pmma),at the indicated onset transition pressures. Within the Cmcm phase, site-specific spin crossover is initiated and involves only highly distorted octahedral sites constituting ~25% of all Fe locations. This is manifest as a steeper volume decrease of dV/V0 ~ 3.5% beyond ~40 GPa and an emergent diamagnetic component discerned in 57Fe Mössbauer spectro…
High-pressure properties of MnPS$_3$ are investigated by using the hybrid functional, we report a spin-crossover pressure of 35 GPa consisting with experimental observation (30 GPa), less than half of existing report (63 GPa) using the Hubbard U correction. Interestingly, a spin-crossover induced antiferromagnetism-to-ferromagnetism transition combined with stacking-order change from monoclinic to rhombohedral are founded, and the ferromagnetism origins from the partially occupied $t_{2g}$ orbitals. Different from previous understanding, the Mott metal-insulator transition of MnPS$_3$ does not…
The family of hole-doped Pr-based perovskite cobaltites, Pr$_{0.5}$Ca$_{0.5}$CoO$_{3}$ and (Pr$_{1-y}$RE$_{y}$)$_{0.3}$Ca$_{0.7}$CoO$_{3}$ (where RE is rare earth) has recently been found to exhibit simultaneous metal-insulator, spin-state, and valence transitions. We have investigated magnetic-field-induced phase transitions of (Pr$_{1-y}$Y$_{y}$)$_{0.7}$Ca$_{0.3}$CoO$_{3}$ by means of magnetization measurements at 4.2$-$100 K up to an ultrahigh magnetic field of 140 T with the chemical pressure varied by $y$ = 0.0625, 0.075, 0.1. The observed magnetic-field-induced transitions were found to …
A detailed defect energy level map was investigated for heterostructures of 26 unit cells of LaAlO3 on SrTiO3 prepared at a low oxygen partial pressure of 10-6 mbar. The origin is attributed to the presence of dominating oxygen defects in SrTiO3 substrate. Using femtosecond laser spectroscopy, the transient absorption and relaxation times for various transitions were determined. An ultrafast relaxation process of 2-3 picosecond from the conduction band to the closest defect level and a slower process of 70-92 picosecond from conduction band to intra-band defect level were observed. The results…
The pairing of interacting fermions leading to superfluidity has two limiting regimes: the Bardeen-Cooper-Schrieffer (BCS) scheme for weakly interacting degenerate fermions and the Bose-Einstein condensation (BEC) of bosonic pairs of strongly interacting fermions. While the superconductivity that emerges in most metallic systems is the BCS-like electron pairing, strongly correlated electrons with poor Fermi liquidity can condense into the unconventional BEC-like pairs. Quantum spin liquids harbor extraordinary spin correlation free from order and the superconductivity that possibly emerges by …
Light-matter coupling involving classical and quantum light offers a wide range of possibilities to tune the electronic properties of correlated quantum materials. Two paradigmatic results are the dynamical localization of electrons and the ultrafast control of spin dynamics, which have been discussed within classical Floquet engineering and in the deep quantum regime where vacuum fluctuations modify the properties of materials. Here we discuss how these two extreme limits are interpolated by a cavity which is driven to the excited states. In particular, this is achieved by formulating a Schri…
Ultrafast Terahertz and Optical Spectroscopy under Synergetic Extreme Conditions
Beijing National Laboratory for Condensed Matter Physics, Institute of Physics, Chinese Academy of Sciences（中国科学院物理研究所凝聚态物理国家实验室）；School of Physical Sciences, University of Chinese Academy of Sciences（中国科学院大学物理科学学院）；Tsung-Dao Lee Institute, Department of Physics and Astronomy, Shanghai Jiao Tong University（上海交通大学物理与天文学院紫江研究院）；International Center for Quantum Materials, School of Physics, Peking University（北京大学物理学院量子材料科学中心）
