Motivated by the recent synthesis of two-dimensional monolayer AlSb, we theoretically investigate its ground state and electronic properties using the first-principles calculations coupled with Bethe-Salpeter equation. An excitonic instability is revealed as a result of larger exciton binding energy than the corresponding one-electron energy gap by $\sim$0.1 eV, which is an indicative of a many-body ground state accompanied by spontaneous exciton generation. Including the spin-orbit coupling is proven to be a must to correctly predict the ground state. At room temperature, the two-dimensional monolayer AlSb is a direct gap semiconductor with phonon-limited electron and hole mobilities both around 1700 cm$^2$/V$\cdot$s. These results show that monolayer AlSb may provide a promising platform for realization of the excitonic insulator and for applications in the next-generation electronic devices.
Exploring new two-dimensional (2D) van der Waals (vdW) systems is at the forefront of materials physics. Here, through molecular beam epitaxy on graphene-covered SiC(0001), we report successful growth of AlSb in the double-layer honeycomb (DLHC) structure, a 2D vdW material which has no direct analogue to its 3D bulk and is predicted kinetically stable when freestanding. The structural morphology and electronic structure of the experimental 2D AlSb are characterized with spectroscopic imaging scanning tunneling microscopy and cross-sectional imaging scanning transmission electron microscopy, w…
Recently it was suggested that transient excitonic instability can be realized in optically-pumped two-dimensional (2D) Dirac materials (DMs), such as graphene and topological insulator surface states. Here we discuss the possibility of achieving a transient excitonic condensate in optically-pumped three-dimensional (3D) DMs, such as Dirac and Weyl semimetals, described by non-equilibrium chemical potentials for photoexcited electrons and holes. Similar to the equilibrium case with long-range interactions, we find that for pumped 3D DMs with screened Coulomb potential two possible excitonic ph…
We use a functional renormalization group (fRG) approach to investigate potential interaction-induced instabilities in a two-dimensional model for the Dirac nodal-line materials ZrSiS and ZrSiSe employing model parameters derived from {\it ab initio} calculations. Our results confirm that the excitonic instability recently found in random-phase approximation for ZrSiS is indeed the leading instability. In the simplest modeling, spin- and charge-excitonic states are degenerate. Beyond this, we show that the fRG analysis produces an energy scale for the onset of the instability in good agreement…
Electron correlation effects are studied in ZrSiS using a combination of first-principles and model approaches. We show that basic electronic properties of ZrSiS can be described within a two-dimensional lattice model of two nested square lattices. High degree of electron-hole symmetry characteristic for ZrSiS is one of the key features of this model. Having determined model parameters from first-principles calculations, we then explicitly take electron-electron interactions into account and show that at moderately low temperatures ZrSiS exhibits excitonic instability, leading to the formation…
Nonlinear light propagation in a single-mode micron-size waveguide made of semiconducting excitonic material has been theoretically studied in terms of exciton-polaritons by using an analysis based on macroscopic fields. When a light pulse is spectrally centered in the vicinity of the ground-state Wannier exciton resonance, it interacts with the medium nonlinearly. This optical cubic nonlinearity is caused by the repulsive exciton-exciton interactions in the semiconductor, and at resonance it is orders of magnitude larger than the Kerr nonlinearity (e.g., in silica). We demonstrate that a very…
The nodal-line semimetals have attracted immense interest due to the unique electronic structures such as the linear dispersion and the vanishing density of states as the Fermi energy approaching the nodes. Here, we report temperature-dependent transport and scanning tunneling microscope (spectroscopy) (STM[S]) measurements on nodal-line semimetal ZrSiSe.Our experimental results and theoretical analyses consistently demonstrate that the temperature induces Lifshitz transitions at 80 and 106 K in ZrSiSe, which results in the transport anomalies at the same temperatures. More strikingly, we obse…
Innovations in imaging technology involves finding strategies and materials suitable for detection applications over the entire infrared range. Herein, we propose a new design concept based on the unique feature of an excitonic insulator, namely, negative exciton transition energy ($E_t$). We demonstrate this concept using first-principles $GW$-BSE calculations on one-dimensional organometallic wire (CrBz)$_\infty$. The pristine (CrBz)$_\infty$ exhibits an excitonic instability due to a negative $E_t$ for the lowest exciton. Substitutional doping can continuously tune the $E_t$ from $\sim$0 to…
The structural phase transition in Ta$_2$NiSe$_5$ has been envisioned as driven by the formation of an excitonic insulating phase. However, the role of structural and electronic instabilities on crystal symmetry breaking has yet to be disentangled. Meanwhile, the phase transition in its complementary material Ta$_2$NiS$_5$ does not show any experimental hints of an excitonic insulating phase. We present a microscopic investigation of the electronic and phononic effects involved in the structural phase transition in Ta$_2$NiSe$_5$ and Ta$_2$NiS$_5$ using extensive first-principles calculations.…
First-principles calculations reveal an unusual electronic state (dubbed as half excitonic insulator) in monolayer 1T-MX2 (M = Co, Ni and X = Cl, Br). Its one spin channel has a many-body ground state due to excitonic instability, while the other is characterized by a conventional band insulator gap. This disparity arises from a competition between the band gap and exciton binding energy, which exhibits a spin-dependence due to different orbital occupations. Such a state can be identified by optical absorption measurements and angle-resolved photoemission spectroscopy. Our theory not only prov…
Motivated by the iron pnictides, we examine the spin excitations in an itinerant antiferromagnet where a spin-density wave (SDW) originates from an excitonic instability of nested electron-like and hole-like Fermi pockets. Using the random phase approximation (RPA), we derive the Dyson equation for the transverse susceptibility in the excitonic SDW state. The Dyson equation is solved for two different two-band models, describing an antiferromagnetic insulator and metal, respectively. We determine the collective spin-wave dispersions and also consider the single-particle continua. The results f…
We use the LDA+U approach to search for possible ordered ground states of LaSrCoO$_4$. We find a staggered arrangement of magnetic multipoles to be stable over a broad range of Co $3d$ interaction parameters. This ordered state can be described as a spin-denity-wave-type condensate of $d_{xy} \otimes d_{x^2-y^2}$ excitons carrying spin $S=1$. Further, we construct an effective strong-coupling model, calculate the exciton dispersion and investigate closing of the exciton gap, which marks the exciton condensation instability. Comparing the layered LaSrCoO$_4$ with its pseudo cubic analog LaCoO$_…
The excitonic insulator (EI) state is a strongly correlated many-body ground state, arising from an instability in the band structure towards exciton formation. We show that the flat valence and conduction bands of a semiconducting diatomic Kagome lattice, as exemplified in a superatomic graphene lattice, can possibly conspire to enable an interesting triplet EI state, based on density functional theory (DFT) calculations combined with many-body GW and Bethe-Salpeter Equation(BSE). Our results indicate that massive carriers in flat bands with highly localized electron and hole wavefunctions si…
Transition metal dichalcogenides (TMDs), whether in bulk or in monolayer form, exhibit a rich variety of charge-density-wave (CDW) phases and stronger periodic lattice distortions. While the actual role of nesting has been under debate, it is well understood that the microscopic interaction responsible for the CDWs is the electron-phonon coupling. The case of TiSe$_2$ is however unique in this family in that the normal state above the critical temperature $T_\mathrm{CDW}$ is characterized by a small quasiparticle bandgap as measured by ARPES, so that no nesting-derived enhancement of the susce…
Electron-hole mixing-induced fine structure in alkaline earth hexaborides leads to lower energy (temperature) scales, and thus stronger tendency toward an excitonic instability, than in their doped counterparts (viz. Ca(1-x)La(x)B(6), x=0.005), which are high Curie temperature, small moment ferromagnets. Comparison of Fermi surfaces and spectral distributions with de Haas - van Alphen (dHvA), optical, transport, and tunneling data indicates that SrB6 remains a fermionic semimetal down to (at least) 5 K, rather than forming an excitonic condensate. For the doped system the Curie temperature is …
A new bosonic, excitonic method for interacting electrons is developed. For two-dimensional electron liquid, it reveals a noncompensated quantum crystal phase ranging from the high density, or vanishing Coulomb interaction, limit: $r_s=0$, to a lower density $r_s\sim 10$, where a condensation of exciton pairs and the loss of the Fermi step is possible. The correlation energy and the static susceptibility, calculated using the method, are in agreement with the independent studies. A proof of the instability of the Fermi surface in the limit $r_s\to 0$ is given. The concept of quantum crystal is…
Two-dimensional molecular crystals have been beyond the reach of systematic investigation because of the lack or instability of their well-defined forms. Here, we demonstrate drastically enhanced photostability and Davydov splitting in single and few-layer tetracene (Tc) crystals sandwiched between inorganic 2D crystals of graphene or hexagonal BN. Molecular orientation and long-range order mapped with polarized wide-field photoluminescence imaging and optical second-harmonic generation revealed high crystallinity of the 2D Tc and its distinctive orientational registry with the 2D inorganic cr…
