Publications

The Mott transition is observed experimentally in materials that are magnetically frustrated so that long-range order does not hide the Mott transition at finite temperature. Using the dynamical cluster approximation for the half-filled Hubbard model on the triangular lattice, we show that a) the Widom line that extends above the critical point of the first-order Mott transition exists in the thermodynamic limit; b) the presence of this line argues for the existence of the Mott transition in the thermodynamic limit; c) the loss of spectral weight in the metal to Mott insulator transition for strong interactions is momentum dependent, the hallmark of a pseudogap; d) the pseudogap to Mott insulator crossover line is a Frenkel line, analogous to the recently discovered crossover discussed in the statistical physics of the liquid-gas transition. Since the Mott transition and the liquid-gas transition are both in the Ising universality class, the Widom and Frenkel lines can be considered as very general emergent phenomena that arise in both ordinary liquids and electron liquids.

We theoretically propose a biphoton entanglement-enhanced multidimensional spectroscopic technique as a probe for the dissipative polariton dynamics in the ultrafast regime. It is applied to the cavity-confined monomeric photosynthetic complex that represents a prototypical multi-site excitonic quantum aggregate. The proposed technique is shown to be particularly sensitive to inter-manifold polariton coherence between the two and one-excitation subspaces. It is demonstrated to be able to monitor the dynamical role of cavity-mediated excitonic correlations, and dephasing in the presence of phonon-induced dissipation. The non-classicality of the entangled biphoton sources is shown to enhance the ultra-fast and broadband correlation features of the signal, giving an indication about the underlying state correlations responsible for long-range cavity-assisted exciton migration.

Long-range vacuum fluctuations break the integer quantum Hall topological protection Cavitronics—a portmanteau of cavity and electronics —are devices with certain properties that can be controlled by the light waves bouncing inside the cavity in which the device sits. In quantum mechanical terms, this interaction between light and matter is done by the standing light waves inside the cavity known as vacuum field states. A major advantage of this setup for generating light-matter coupling is the ability to induce certain properties inside a material that otherwise require the use of a strong external electric or magnetic field (see the image). On page 1030 of this issue, Appugliese et al. (1) provide a special case of cavitronics. Their experimental setup modifies one of the most prominent quantum phenomena in materials, known as the quantum Hall effect (QHE). They found a drastic change in its Hall resistance, opening the path to designing materials functionalities by vacuum-field engineering.

This perspective provides a brief introduction into the theoretical complexity of polaritonic chemistry, which emerges from the hybrid nature of strongly coupled light-matter states. To tackle this complexity, the importance of ab initio methods is highlighted. Based on those, novel ideas and research avenues are developed with respect to quantum collectivity, as well as for resonance phenomena immanent in reaction rates under vibrational strong coupling. Indeed, fundamental theoretical questions arise about the mesoscopic scale of quantum-collectively coupled molecules, when considering the depolarization shift in the interpretation of experimental data. Furthermore, to rationalise recent QEDFT findings, a simple, but computationally efficient, Langevin framework is proposed, based on well-established methods from molecular dynamics. It suggests the emergence of cavity induced non-equilibrium nuclear dynamics, where thermal (stochastic) resonance phenomena could emerge in the absence of external periodic driving. Overall, we believe the latest ab initio results indeed suggest a paradigmatic shift for ground-state chemical reactions under vibrational strong coupling, from the collective quantum interpretation towards a more local, (semi)-classically and non-equilibrium dominated perspective. Finally, various extensions towards a refined description of cavity-modified chemistry are introduced in the context of QEDFT and future directions of the field are sketched.

We theoretically study the interplay between magnetism and a heavy Fermi liquid in the AB stacked transition metal dichalcogenide bilayer system MoTe

Characterizing chirality is highly important for applications in the pharmaceutical industry, as well as in the study of dynamical chemical and biological systems. However, this task has remained challenging, especially due to the ongoing increasing complexity and size of the molecular structure of drugs and active compounds. In particular, large molecules with many active chirality centers are today ubiquitous, but remain difficult to structurally analyze due to their high number of stereoisomers. Here we theoretically explore the sensitivity of high harmonic generation (HHG) to the chirality of molecules with a varying number of active chiral centers. We find that HHG driven by bi-chromatic non-collinear lasers is a sensitive probe for the stereo-configuration of a chiral molecule. We first show through calculations (from benchmark chiral molecules with up to three chirality centers) that the HHG spectrum is imprinted with information about the handedness of each chirality center in the driven molecule. Next, we show that using both classical- and deep-learning-based reconstruction algorithms, the composition of an unknown mixture of stereoisomers can be reconstructed with high fidelity by a single-shot HHG measurement. Our work illustrates how the combination of non-linear optics and machine learning might open routes for ultra-sensitive sensing in chiral systems.

First-principles methods for time-resolved angular resolved photoelectron spectroscopy play a pivotal role in providing interpretation and microscopic understanding of the complex experimental data and in exploring novel observables or observation conditions that may be achieved in future experiments. Here we describe an efficient, reliable and scalable first-principles method for tr-ARPES based on time-dependent density functional theory including propagation and surface effects usually discarded in the widely used many-body techniques based on computing the non-equilibrium spectral function and discuss its application to a variety of pump-probe conditions. We identify four conditions, depending on the length of the probe relative to the excitation in the materials on the one hand and on the overlap between pump and probe on the other hand. Within this paradigm different examples of observables of time-resolved ARPES are discussed in view of the newly developed and highly accurate time-resolved experimental spectroscopies.

The density matrix renormalization group (DMRG) method has already proved itself as a very efficient and accurate computational method, which can treat large active spaces and capture the major part of strong correlation. Its application on larger molecules is, however, limited by its own computational scaling as well as demands of methods for treatment of the missing dynamical electron correlation. In this work, we present the first step in the direction of combining DMRG with density functional theory (DFT), one of the most employed quantum chemical methods with favourable scaling, by means of the projection-based wave function (WF)-in-DFT embedding. On the two proof-of-concept but important molecular examples, we demonstrate that the developed DMRG-in-DFT approach provides a very accurate description of molecules with a strongly correlated fragment.

We consider two-dimensional metals of fermions coupled to quantum critical scalars, the latter representing order parameters or emergent gauge fields. We show that at low temperatures (T), such metals generically exhibit strange metal behavior with a T-linear resistivity arising from spatially random fluctuations in the fermion-scalar Yukawa couplings about a non-zero spatial average. We also find a T (1/T) specific heat, and a rationale for the Planckian bound on the transport scattering time. These results are obtained in the large N expansion of an ensemble of critical metals.

Tensor network representations of quantum many-body states provide powerful tools for strongly correlated systems, tailored to capture local correlations such as ground states exhibiting entanglement area laws. When applying tensor network states to interacting fermionic systems, a proper choice of basis or orbitals can greatly reduce the bond dimension of tensors and speed up calculations. We introduce such a change of basis with unitary gates obtained via compressing fermionic Gaussian states into quantum circuits corresponding to various tensor networks. These circuits can reduce the ground state entanglement entropy and improve the performance of algorithms such as the density matrix renormalization group. We study the 1D single impurity Anderson model to show the power of the method in improving computational efficiency and interpreting impurity physics. Furthermore, fermionic Gaussian circuits also show potential for suppressing entanglement during the time evolution of a low-lying excited state that is used to compute the impurity Green's function. Lastly, we consider Gaussian multi-scale entanglement renormalization ansatz (GMERA) circuits which compress fermionic Gaussian states hierarchically. The emergent coarse-grained physical models from these GMERA circuits are studied in terms of their entanglement properties and suitability for performing time evolution.