We present an infrared magneto-optical study of the highly thermoelectric narrow-gap semiconductor Bi2Se3. Far-infrared and mid-infrared (IR) reflectance and transmission measurements have been performed in magnetic fields oriented both parallel and perpendicular to the trigonal c axis of this layered material, and supplemented with UV-visible ellipsometry to obtain the optical conductivity σ1(ω). With lowering of temperature we observe narrowing of the Drude conductivity due to reduced quasiparticle scattering, as well as the increase in the absorption edge due to direct electronic transitions. Magnetic fields H c dramatically renormalize and asymmetrically broaden the strongest far-IR optical phonon, indicating interaction of the phonon with the continuum freecarrier spectrum and significant magnetoelectric coupling. For the perpendicular field orientation, electronic absorption is enhanced, and the plasma edge is slightly shifted to higher energies. In both cases the direct transition energy is softened in magnetic field. arXiv:0912.2769v2 [cond-mat.str-el]

We investigate the transient photoconductivity of graphene at various gate-tuned carrier densities by optical-pump terahertz-probe spectroscopy. We demonstrate that graphene exhibits semiconducting positive photoconductivity near zero carrier density, which crosses over to metallic negative photoconductivity at high carrier density. These observations can be accounted for by the interplay between photoinduced changes of both the Drude weight and carrier scattering rate. Our findings provide a complete picture to explain the opposite photoconductivity behavior reported in (undoped) graphene grown epitaxially and (doped) graphene grown by chemical vapor deposition. Notably, we observe nonmonotonic fluence dependence of the photoconductivity at low carrier density. This behavior reveals the nonmonotonic temperature dependence of the Drude weight in graphene, a unique property of two-dimensional massless Dirac fermions. DOI: 10.1103/PhysRevLett.113.056602 PACS numbers: 72.80.Vp, 72.40.+w, 73.40.Qv, 78.20.−e Charge carriers in graphene mimic two-dimensional (2D) massless Dirac fermions with linear energy dispersion, resulting in unique optical and electronic properties [1]. They exhibit high mobility and strong interaction with electromagnetic radiation over a broad frequency range [2]. Interband transitions in graphene give rise to pronounced optical absorption in the midinfrared to visible spectral range, where the optical conductivity is close to a universal value σ 0 ¼ πe 2 =2h [3]. Free-carrier intraband transitions, on the other hand, cause lowfrequency absorption, which varies significantly with charge density and results in strong light extinction at high carrier density [4]. In addition to this density dependence, the massless Dirac particles in graphene are predicted to exhibit a distinctive nonmonotonic temperature dependence of the intraband absorption strength, or Drude weight, due to their linear dispersion [5,6]. This behavior contrasts with the temperature-independent Drude weight expected in conventional systems of massive particles with parabolic dispersion [7,8]. Although the unique behavior of the Drude weight in graphene has been considered theoretically, experimental signatures are still lacking.The intrinsic properties of Drude absorption in graphene can be revealed by studying its dynamical response to photoexcitation. In particular, optical-pump terahertz-probe spectroscopy provides access to a wide transient temperature range via pulsed optical excitation, and allows measurement of the ac Drude conductivity by a timedelayed terahertz probe pulse [9]. This technique has been applied to study transient photoconductivity (PC) in graphene, but conflicting results have been reported [9][10][11][12][13][14][15]. Positive PC was observed in epitaxial graphene on SiC (Ref.[15]), while negative PC was seen in graphene grown by chemical vapor deposition (CVD) [11][12][13][14]. It has been argued that the opposite behavior in these samples arises from their different charge densities. Here we study...

Interactions between two excitons can result in the formation of bound quasiparticles, known as biexcitons. Their properties are determined by the constituent excitons, with orbital and spin states resembling those of atoms. Monolayer transition metal dichalcogenides (TMDs) present a unique system where excitons acquire a new degree of freedom, the valley pseudospin, from which a novel intervalley biexciton can be created. These biexcitons comprise two excitons from different valleys, which are distinct from biexcitons in conventional semiconductors and have no direct analogue in atomic and molecular systems. However, their valley properties are not accessible to traditional transport and optical measurements. Here, we report the observation of intervalley biexcitons in the monolayer TMD MoS2 using ultrafast pump-probe spectroscopy. By applying broadband probe pulses with different helicities, we identify two species of intervalley biexcitons with large binding energies of 60 meV and 40 meV. In addition, we also reveal effects beyond biexcitonic pairwise interactions in which the exciton energy redshifts at increasing exciton densities, indicating the presence of many-body interactions among them.

Optical excitation typically enhances electrical conduction and low-frequency radiation absorption in semiconductors. We, however, observe a pronounced transient decrease of conductivity in doped monolayer molybdenum disulfide (MoS 2 ), a two-dimensional (2D) semiconductor, using ultrafast opticalpump terahertz-probe spectroscopy. In particular, the conductivity is reduced to only 30% of its equilibrium value at high pump fluence. This anomalous phenomenon arises from the strong many-body interactions in the 2D system, where photoexcited electron-hole pairs join the doping-induced charges to form trions, bound states of two electrons and one hole. The resultant increase of the carrier effective mass substantially diminishes the conductivity. [3,4], and intriguing coupled spin-valley physics [5][6][7][8]. These remarkable properties make TMD materials promising for developing next-generation (opto)electronics and (pseudo)spintronics. One distinctive feature of monolayer TMDs is the strong quantum confinement and reduced dielectric screening in the strict 2D limit. The resultant strong Coulomb interactions cause photoexcited electron-hole pairs to form tightly bound excitons, which govern the optical and electronic properties of the materials [9][10][11][12][13][14][15][16][17][18][19][20][21][22]. In samples with excess charges, the excitons can capture additional charges to form trions (charged excitons). These trions possess exceptionally high dissociation energies (20-50 meV), and their concentration and spin-valley configuration can be controlled by electrical gate and optical helicity, respectively [12,[23][24][25]. Although these strong many-body effects have been observed in 2D TMDs, their influence on the materials' intrinsic conductive behavior and implications for device applications have not been explored thus far.In this Letter, we report the first experimental signature of a profound trionic effect on the conductive properties of atomically thin TMD materials. By using time-resolved terahertz spectroscopy [26,27], we have observed an anomalous transient decrease of terahertz conductivity in doped monolayer MoS 2 after femtosecond laser excitation at T ¼ 4-350 K. The negative photoconductivity saturates at high pump fluence, where the conductivity is substantially reduced to ∼30% of its equilibrium value. This behavior contrasts with the positive photoconductivity found in multilayer and bulk MoS 2 , and in other conventional semiconductors (e.g., Si, Ge, and GaAs) [26,27]. Our results reflect the strong many-body interactions in monolayer MoS 2 , where photoexcited carriers form trions with the original free electrons. The resultant increase of effective mass significantly diminishes the carrier mobility and conductivity. This interaction-driven photoreduction of conductivity represents an intrinsic property of monolayer MoS 2 crystals, in contrast to the negative photoconductivity arising from trapping or spatial transfer of charges in some semiconductor systems with high defect density or heteroge...

We present a detailed infrared study of the insulator-to-metal transition ͑IMT͒ in vanadium dioxide ͑VO 2 ͒ thin films. Conventional infrared spectroscopy was employed to investigate the IMT in the far field. Scanning near-field infrared microscopy directly revealed the percolative IMT with increasing temperature. We confirmed that the phase transition is also percolative with cooling across the IMT. We present extensive near-field infrared images of phase coexistence in the IMT regime in VO 2 . We find that the coexisting insulating and metallic regions at a fixed temperature are static on the time scale of our measurements. A distinctive approach for analyzing the far-field and near-field infrared data within the Bruggeman effective medium theory was employed to extract the optical constants of the incipient metallic puddles at the onset of the IMT. We found divergent effective carrier mass in the metallic puddles that demonstrates the importance of electronic correlations to the IMT in VO 2 . We employ the extended dipole model for a quantitative analysis of the observed near-field infrared amplitude contrast and compare the results with those obtained with the basic dipole model.

Published Version

When light is absorbed by a semiconductor, photoexcited charge carriers enhance the absorption of far-infrared radiation due to intraband transitions. We observe the opposite behavior in monolayer graphene, a zero-gap semiconductor with linear dispersion. By using time domain terahertz (THz) spectroscopy in conjunction with optical pump excitation, we observe a reduced absorption of THz radiation in photoexcited graphene. The measured spectral shape of the differential optical conductivity exhibits non-Drude behavior. We discuss several possible mechanisms that contribute to the observed low-frequency non-equilibrium optical response of graphene

We investigated the ab-plane optical properties of single crystals of WTe2 for light polarized parallel and perpendicular to the W-chain axis over a broad range of frequency and temperature. At far-infrared frequencies, we observed a striking dependence of the reflectance edge on light polarization, corresponding to anisotropy of the carrier effective masses. We quantitatively studied the temperature dependence of the plasma frequency, revealing a modest increase of the effective mass anisotropy in the ab-plane upon cooling. We also found strongly anisotropic interband transitions persisting to high photon energies. These results were analyzed by comparison with ab initio calculations. The calculated and measured plasma frequencies agree to within 10% for both polarizations, while the calculated interband conductivity shows excellent agreement with experiment.