Ultrafast laser pulses can be used to drive materials into nonequilibrium states that have unusual properties and are promising for technological applications. Different classes of phenomena are observed during and after the optical illumination. This Colloquium discusses the recent developments in this field, and the prospects for using these techniques to create materials with novel functionalities in a controlled way.

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Colloquium: Nonthermal pathways to ultrafast control in quantum materials

Cavity control of quantum matter may offer new ways to study and manipulate many-body systems. A particularly appealing idea is to use cavities to enhance superconductivity, especially in unconventional or high-$T_c$ systems. Motivated by this, we propose a scheme for coupling Terahertz resonators to the antiferromagnetic fluctuations in a cuprate parent compound, which are believed to provide the glue for Cooper pairs in the superconducting phase. First, we derive the interaction between magnon excitations of the Ne\'el-order and polar phonons associated with the planar oxygens. This mode also couples to the cavity electric field, and in the presence of spin-orbit interactions mediates a linear coupling between the cavity and magnons, forming hybridized magnon-polaritons. This hybridization vanishes linearly with photon momentum, implying the need for near-field optical methods, which we analyze within a simple model. We then derive a higher-order coupling between the cavity and magnons which is only present in bilayer systems, but does not rely on spin-orbit coupling. This interaction is found to be large, but only couples to the bimagnon operator. As a result we find a strong, but heavily damped, bimagnon-cavity interaction which produces highly asymmetric cavity line-shapes in the strong-coupling regime. To conclude, we outline several interesting extensions of our theory, including applications to carrier-doped cuprates and other strongly-correlated systems with Terahertz-scale magnetic excitations. 

/pdf/cavity-magnon-polaritons-in-cuprate-parent-compounds-eu0vy03j.pdf

Cavity magnon-polaritons in cuprate parent compounds

Strong-laser-field physics is a research direction that relies on the use of high-power lasers and has led to fascinating achievements ranging from relativistic particle acceleration to attosecond science. On the other hand, quantum optics has been built on the use of low photon number sources and has opened the way for groundbreaking discoveries in quantum technology, advancing investigations ranging from fundamental tests of quantum theory to quantum information processing. Despite the tremendous progress, until recently these directions have remained disconnected. This is because the majority of the interactions in the strong-field limit have been successfully described by semi-classical approximations treating the electromagnetic field classically, as there was no need to include the quantum properties of the field to explain the observations. The link between strong-laser-field physics, quantum optics, and quantum information science has been developed in the recent past. Studies based on fully quantized and conditioning approaches have shown that intense laser-matter interactions can be used for the generation of controllable entangled and non-classical light states. These achievements open the way for a vast number of investigations stemming from the symbiosis of strong-laser-field physics, quantum optics, and quantum information science. Here, after an introduction to the fundamentals of these research directions, we report on the recent progress in the fully quantized description of intense laser-matter interaction and the methods that have been developed for the generation of non-classical light states and entangled states. Also, we discuss the future directions of non-classical light engineering using strong laser fields, and the potential applications in ultrafast and quantum information science. 

Strong–laser–field physics, non–classical light states and quantum information science

Photodoped states are widely observed in laser-excited Mott insulators, in which charge excitations are quickly created and can exist beyond the duration of the external driving. Despite the fruitful experimental explorations, theoretical studies on the microscopic models face the challenge to simultaneously deal with exponentially separated time scales, especially in multiband systems, where the longtime behaviors are often well beyond the reach of state-of-the-art numerical tools. Here, we address this difficulty by introducing a steady-state description of photodoped Mott insulators using an open-system setup, where the photodoped system is stabilized as a nonequilibrium steady state by a weak external driving. Taking advantage of the stationarity, we implement and discuss the details of an efficient numerical tool using the steady-state dynamical mean-field theory combined with the noncrossing approximation. We demonstrate that these stationary photodoped states exhibit the same properties of their transient counterparts, while being solvable with reasonable computational efforts. Furthermore, they can be parametrized by just a few physical quantities, including the effective temperature and the density of charge excitations, which confirms the universal nature of photodoped states indeed independent of the excitation protocols. As a first application, we consider the stationary photodoped states in a two-band Hubbard model with intertwined spin-and-orbital ordering and find a family of hidden phases unknown from the previous studies, implying an apparently unexplored time regime of the relaxation of the intertwined orders.

Nonequilibrium steady-state theory of photodoped Mott insulators

Magnetism in topological materials creates phases exhibiting quantized transport phenomena with potential technological applications. The emergence of such phases relies on strong interaction between localized spins and the topological bands, and the consequent formation of an exchange gap. However, this remains experimentally unquantified in intrinsic magnetic topological materials. Here, this interaction is quantified in MnBi2Te4, a topological insulator with intrinsic antiferromagnetism. This is achieved by optically exciting Bi‐Te p states comprising the bulk topological bands and interrogating the consequent Mn 3d spin dynamics, using a multimodal ultrafast approach. Ultrafast electron scattering and magneto‐optic measurements show that the p states demagnetize via electron‐phonon scattering at picosecond timescales. Despite being energetically decoupled from the optical excitation, the Mn 3d spins, probed by resonant X‐ray scattering, are observed to disorder concurrently with the p spins. Together with atomistic simulations, this reveals that the exchange coupling between localized spins and the topological bands is at least 100 times larger than the superexchange interaction, implying an optimal exchange gap of at least 25 meV in the surface states. By quantifying this exchange coupling, this study validates the materials‐by‐design strategy of utilizing localized magnetic order to manipulate topological phases, spanning static to ultrafast timescales.

/pdf/large-exchange-coupling-between-localized-spins-and-127dzrr3.pdf

Large Exchange Coupling Between Localized Spins and Topological Bands in MnBi2Te4

We investigate quasiparticle relaxation dynamics in URu$_{2-x}$Fe$_{x}$Si$_{2}$ single crystals using ultrafast optical-pump optical-probe (OPOP) spectroscopy as a function of temperature ($T$) and Fe substitution ($x$), crossing from the hidden order (HO) phase ($x$ = 0) to the large moment antiferromagnet (LMAFM) phase ($x$ = 0.12). At low $T$, the dynamics for $x$ = 0 and $x$ = 0.12 are consistent with the low energy electronic structure of the HO and LMAFM phases that emerge from the high $T$ paramagnetic (PM) phase. In contrast, for $x$ = 0.1, two transitions occur over a narrow $T$ range (from ~15.5 - 17.5 K). A PM to HO transition occurs at an intermediate $T$ followed by a transition to the LMAFM phase at lower $T$. While the data at low $T$ are consistent with the expected coexistence of LMAFM and HO, the data in the intermediate $T$ phase are not, and instead suggest the possibility of an unexpected coexistence of HO and PM. Additionally, the dynamics in the PM phase reflect the presence of a hybridization gap as well as strongly interacting spin and charge degrees of freedom. OPOP yields insights into meV-scale electrodynamics with sub-Kelvin $T$ resolution, providing a complementary approach to study low energy electronic structure in quantum materials.

Quasiparticle relaxation dynamics in URu 2 − x Fe x Si 2 single crystals

In this work we investigate single crystal $\mathrm{Gd}\mathrm{Ti}{\mathrm{O}}_{3}$, a promising candidate material for Floquet engineering and magnetic control, using ultrafast optical pump-probe reflectivity and magneto-optical Kerr spectroscopy. $\mathrm{Gd}\mathrm{Ti}{\mathrm{O}}_{3}$ is a Mott-Hubbard insulator with a ferrimagnetic and orbitally ordered ground state (${T}_{C}$ = 32 K). We observe multiple signatures of the magnetic phase transition in the photoinduced reflectivity signal, in response to above band-gap 660-nm excitation. Magnetic dynamics measured via Kerr spectroscopy reveal optical perturbation of the ferrimagnetic order on spin-lattice coupling timescales, highlighting the competition between the ${\mathrm{Gd}}^{3+}$ and ${\mathrm{Ti}}^{3+}$ magnetic sub-lattices. Furthermore, a strong coherent oscillation is present in the reflection and Kerr dynamics, attributable to an acoustic strain wave launched by the pump pulse. The amplitude of this acoustic mode is highly dependent on the magnetic order of the system, growing sharply in magnitude at ${T}_{C}$, indicative of strong magneto-elastic coupling. The driving mechanism, involving strain-induced modification of the magnetic exchange interaction, implies an indirect method of coupling light to the magnetic degrees of freedom and emphasizes the potential of $\mathrm{Gd}\mathrm{Ti}{\mathrm{O}}_{3}$ as a tunable quantum material.

Magnetoelastic coupling to coherent acoustic phonon modes in the ferrimagnetic insulator Gd Ti O 3

Recent optical conductivity measurements reveal the presence of Hubbard excitons in certain Mott insulators. In light of these results, it is important to revisit the dynamics of these materials to account for excitonic correlations. We investigate time-resolved excitation and relaxation dynamics as a function of temperature in perovskite-type ${\mathrm{LaVO}}_{3}$ thin films using ultrafast optical pump-probe spectroscopy. ${\mathrm{LaVO}}_{3}$ undergoes a series of phase transitions at roughly the same critical temperature ${T}_{C}\ensuremath{\cong}140$ K, including a second-order magnetic phase transition ($\mathrm{PM}\stackrel{}{\ensuremath{\rightarrow}}\mathrm{AFM}$) and a first-order structural phase transition, accompanied by $C$-type spin order and $G$-type orbital order. Ultrafast optical pump-probe spectroscopy at 1.6 eV monitors changes in the spectral weight of the Hubbard exciton resonance which serves as a sensitive reporter of spin and orbital fluctuation dynamics. We observe dramatic slowing down of the spin, and orbital dynamics in the vicinity of ${T}_{C}\ensuremath{\cong}140$ K, reminiscent of a second-order phase transition, despite the (weakly) first-order nature of the transition. We emphasize that since it is spectral weight changes that are probed, the measured dynamics are not reflective of conventional exciton generation and recombination, but are related to the dynamics of Hubbard exciton formation in the presence of a fluctuating many-body environment.

/pdf/influence-of-spin-and-orbital-fluctuations-on-mott-hubbard-4zcifn1seq.pdf

Influence of spin and orbital fluctuations on Mott-Hubbard exciton dynamics in LaVO 3 thin films

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Papers

Quasiparticle relaxation dynamics in URu 2 − x Fe x Si 2 single crystals

Magnetoelastic coupling to coherent acoustic phonon modes in the ferrimagnetic insulator Gd Ti O 3

Influence of spin and orbital fluctuations on Mott-Hubbard exciton dynamics in LaVO 3 thin films