Efficient Emission of Highly Polarized Thermal Radiation from a Suspended Aligned Carbon Nanotube Film.

A polarized light source covering a wide wavelength range is required in applications across diverse fields, including optical communication, photonics, spectroscopy, and imaging. For practical applications, high degrees of polarization and thermal performance are needed to ensure the stability of the radiation intensity and low energy consumption. Here, we achieved efficient emission of highly polarized and broadband thermal radiation from a suspended aligned carbon nanotube film. The anisotropic nature of the film, combined with the suspension, led to a high degree of linear polarization (∼0.9) and great thermal performance. Furthermore, we performed time-resolved measurements of thermal emission from the film, revealing a fast time response of approximately a few microseconds. We also obtained visible light emission from the device and analyzed the film's mechanical breakdown behavior to improve the emission intensity. Finally, we demonstrated that suspended devices with a constriction geometry can enhance the heating performance. These results show that carbon nanotube film-based devices, as electrically driven thermal emitters of polarized radiation, can play an important role for future development in optoelectronics and spectroscopy.

Strong nonlinear optical processes with extraordinary polarization anisotropy in inversion-symmetry broken two-dimensional PdPSe.

Nonlinear optical activities, especially second harmonic generation (SHG), are key phenomena in inversion-symmetry-broken two-dimensional (2D) transition metal dichalcogenides (TMDCs). On the other hand, anisotropic nonlinear optical processes are important for unique applications in nano-nonlinear photonic devices with polarization functions, having become one of focused research topics in the field of nonlinear photonics. However, the strong nonlinearity and strong optical anisotropy do not exist simultaneously in common 2D materials. Here, we demonstrate strong second-order and third-order susceptibilities of 64 pm/V and 6.2×10-19 m2/V2, respectively, in the even-layer PdPSe, which has not been discovered in other common TMDCs (e.g., MoS2). Strikingly, it also simultaneously exhibited strong SHG anisotropy with an anisotropic ratio of ~45, which is the largest reported among all 2D materials to date, to the best of our knowledge. In addition, the SHG anisotropy ratio can be harnessed from 0.12 to 45 (375 times) by varying the excitation wavelength due to the dispersion of χ ( 2 ) values. As an illustrative example, we further demonstrate polarized SHG imaging for potential applications in crystal orientation identification and polarization-dependent spatial encoding. These findings in 2D PdPSe are promising for nonlinear nanophotonic and optoelectronic applications.

Reversible non-volatile electronic switching in a near-room-temperature van der Waals ferromagnet.

Non-volatile phase-change memory devices utilize local heating to toggle between crystalline and amorphous states with distinct electrical properties. Expanding on this kind of switching to two topologically distinct phases requires controlled non-volatile switching between two crystalline phases with distinct symmetries. Here, we report the observation of reversible and non-volatile switching between two stable and closely related crystal structures, with remarkably distinct electronic structures, in the near-room-temperature van der Waals ferromagnet Fe5-δGeTe2. We show that the switching is enabled by the ordering and disordering of Fe site vacancies that results in distinct crystalline symmetries of the two phases, which can be controlled by a thermal annealing and quenching method. The two phases are distinguished by the presence of topological nodal lines due to the preserved global inversion symmetry in the site-disordered phase, flat bands resulting from quantum destructive interference on a bipartite lattice, and broken inversion symmetry in the site-ordered phase.

Observation of interplay between phonon chirality and electronic band topology.

The recently demonstrated chiral modes of lattice motion carry angular momentum and therefore directly couple to magnetic fields. Notably, their magnetic moments are predicted to be strongly influenced by electronic contributions. Here, we have studied the magnetic response of transverse optical phonons in a set of Pb1-xSnxTe films, which is a topological crystalline insulator for x > 0.32 and has a ferroelectric transition at an x-dependent critical temperature. Polarization-dependent terahertz magnetospectroscopy measurements revealed Zeeman splittings and diamagnetic shifts, demonstrating a large phonon magnetic moment. Films in the topological phase exhibited phonon magnetic moment values that were larger than those in the topologically trivial samples by two orders of magnitude. Furthermore, the sign of the effective phonon g-factor was opposite in the two phases, a signature of the topological transition according to our model. These results strongly indicate the existence of interplay between the magnetic properties of chiral phonons and the topology of the electronic band structure.

Creating a near-perfect circularly polarized terahertz beam through the nonreciprocity of a magnetoplasma.

Compared to other parts of the electromagnetic spectrum, the terahertz frequency range lacks efficient polarization manipulation techniques, which is impeding the proliferation of terahertz technology. In this work, we demonstrate a tunable and broadband linear-to-circular polarization converter based on an InSb plate containing a free-carrier magnetoplasma. In a wide spectral region (∼ 0.45 THz), the magnetoplasma selectively absorbs one circularly polarized mode due to electron cyclotron resonance and also reflects it at the edges of the absorption band. Both effects are nonreciprocal and contribute to form a near-zero transmission band with a high isolation of -36 dB, resulting in the output of a near-perfect circularly polarized terahertz wave for an incident linearly polarized beam. The near-zero transmission band is tunable with magnetic field to cover a wide frequency range from 0.3 to 4.8 THz.

Engineering chirality at wafer scale with ordered carbon nanotube architectures.

Creating artificial matter with controllable chirality in a simple and scalable manner brings new opportunities to diverse areas. Here we show two such methods based on controlled vacuum filtration - twist stacking and mechanical rotation - for fabricating wafer-scale chiral architectures of ordered carbon nanotubes (CNTs) with tunable and large circular dichroism (CD). By controlling the stacking angle and handedness in the twist-stacking approach, we maximize the CD response and achieve a high deep-ultraviolet ellipticity of 40 ± 1 mdeg nm-1. Our theoretical simulations using the transfer matrix method reproduce the experimentally observed CD spectra and further predict that an optimized film of twist-stacked CNTs can exhibit an ellipticity as high as 150 mdeg nm-1, corresponding to a g factor of 0.22. Furthermore, the mechanical rotation method not only accelerates the fabrication of twisted structures but also produces both chiralities simultaneously in a single sample, in a single run, and in a controllable manner. The created wafer-scale objects represent an alternative type of synthetic chiral matter consisting of ordered quantum wires whose macroscopic properties are governed by nanoscopic electronic signatures and can be used to explore chiral phenomena and develop chiral photonic and optoelectronic devices.

High-Speed Modulation of Polarized Thermal Radiation from an On-Chip Aligned Carbon Nanotube Film.

Spectroscopic analysis with polarized light has been widely used to investigate molecular structure and material behavior. A broadband polarized light source that can be switched on and off at a high speed is indispensable for reading faint signals, but such a source has not been developed. Here, using aligned carbon nanotube (CNT) films, we have developed broadband thermal emitters of polarized infrared radiation with switching speeds of ≲20 MHz. We found that the switching speed depends on whether the electrical current is parallel or perpendicular to the CNT alignment direction with a significantly higher speed achieved in the parallel case. Together with detailed theoretical simulations, our experimental results demonstrate that the contact thermal conductance to the substrate and the conductance to the electrodes are important factors that determine the switching speed. These emitters can lead to advanced spectroscopic analysis techniques with polarized radiation.

Angle-resolved photoemission spectroscopy with an in situ tunable magnetic field.

Angle-resolved photoemission spectroscopy (ARPES) is a powerful tool for probing the momentum-resolved single-particle spectral function of materials. Historically, in situ magnetic fields have been carefully avoided as they are detrimental to the control of photoelectron trajectory during the photoelectron detection process. However, magnetic field is an important experimental knob for both probing and tuning symmetry-breaking phases and electronic topology in quantum materials. In this paper, we introduce an easily implementable method for realizing an in situ tunable magnetic field at the sample position in an ARPES experiment and analyze magnetic-field-induced artifacts in the ARPES data. Specifically, we identified and quantified three distinct extrinsic effects of a magnetic field: constant energy contour rotation, emission angle contraction, and momentum broadening. We examined these effects in three prototypical quantum materials, i.e., a topological insulator (Bi2Se3), an iron-based superconductor (LiFeAs), and a cuprate superconductor (Pb-Bi2Sr2CuO6+x), and demonstrate the feasibility of ARPES measurements in the presence of a controllable magnetic field. Our studies lay the foundation for the future development of the technique and interpretation of ARPES measurements of field-tunable quantum phases.

Extreme Polarization Anisotropy in Resonant Third-Harmonic Generation from Aligned Carbon Nanotube Films.

Carbon nanotubes (CNTs) possess extremely anisotropic electronic, thermal, and optical properties owing to their 1D character. While their linear optical properties have been extensively studied, nonlinear optical processes, such as harmonic generation for frequency conversion, remain largely unexplored in CNTs, particularly in macroscopic CNT assemblies. In this work, macroscopic films of aligned and type-separated (semiconducting and metallic) CNTs are synthesized and polarization-dependent third-harmonic generation (THG) from the films with fundamental wavelengths ranging from 1.5 to 2.5 µm is studied. Both films exhibited strongly wavelength-dependent, intense THG signals, enhanced through exciton resonances, and third-order nonlinear optical susceptibilities of 2.50 × 10-19  m2  V-2 (semiconducting CNTs) and 1.23 × 10-19  m2  V-2 (metallic CNTs), respectively are found, for 1.8 µm excitation. Further, through systematic polarization-dependent THG measurements, the values of all elements of the susceptibility tensor are determined, verifying the macroscopically 1D nature of the films. Finally, polarized THG imaging is performed to demonstrate the nonlinear anisotropy in the large-size CNT film with good alignment. These findings promise applications of aligned CNT films in mid-infrared frequency conversion, nonlinear optical switching, polarized pulsed lasers, polarized long-wave detection, and high-performance anisotropic nonlinear photonic devices.

Transition from Diffusive to Superdiffusive Transport in Carbon Nanotube Networks via Nematic Order Control.

The one-dimensional confinement of quasiparticles in individual carbon nanotubes (CNTs) leads to extremely anisotropic electronic and optical properties. In a macroscopic ensemble of randomly oriented CNTs, this anisotropy disappears together with other properties that make them attractive for certain device applications. The question however remains if not only anisotropy but also other types of behaviors are suppressed by disorder. Here, we compare the dynamics of quasiparticles under strong electric fields in aligned and random CNT networks using a combination of terahertz emission and photocurrent experiments and out-of-equilibrium numerical simulations. We find that the degree of alignment strongly influences the excited quasiparticles' dynamics, rerouting the thermalization pathways. This is, in particular, evidenced in the high-energy, high-momentum electronic population (probed through the formation of low energy excitons via exciton impact ionization) and the transport regime evolving from diffusive to superdiffusive.

Phonon-Assisted Intertube Electronic Transport in an Armchair Carbon Nanotube Film.

The electrical conductivity of a macroscopic assembly of nanomaterials is determined through a complex interplay of electronic transport within and between constituent nano-objects. Phonons play dual roles in this situation: their increased populations tend to reduce the conductivity via electron scattering, while they can boost the conductivity by assisting electrons to propagate through the potential-energy landscape. We identified a phonon-assisted coherent electron transport process between neighboring nanotubes in temperature-dependent conductivity measurements on a macroscopic film of armchair single-wall carbon nanotubes. Through atomistic modeling of electronic states and calculations of both electronic and phonon-assisted junction conductances, we conclude that phonon-assisted conductance is the dominant mechanism for observed high-temperature transport in armchair carbon nanotubes. The unambiguous manifestation of coherent intertube dynamics proves a single-chirality armchair nanotube film to be a unique macroscopic solid-state ensemble of nano-objects promising for the development of room-temperature coherent electronic devices.

Perfect intrinsic squeezing at the superradiant phase transition critical point.

Some of the most exotic properties of the quantum vacuum are predicted in ultrastrongly coupled photon-atom systems; one such property is quantum squeezing leading to suppressed quantum fluctuations of photons and atoms. This squeezing is unique because (1) it is realized in the ground state of the system and does not require external driving, and (2) the squeezing can be perfect in the sense that quantum fluctuations of certain observables are completely suppressed. Specifically, we investigate the ground state of the Dicke model, which describes atoms collectively coupled to a single photonic mode, and we found that the photon-atom fluctuation vanishes at the onset of the superradiant phase transition in the thermodynamic limit of an infinite number of atoms. Moreover, when a finite number of atoms is considered, the variance of the fluctuation around the critical point asymptotically converges to zero, as the number of atoms is increased. In contrast to the squeezed states of flying photons obtained using standard generation protocols with external driving, the squeezing obtained in the ground state of the ultrastrongly coupled photon-atom systems is resilient against unpredictable noise.

Dicke-Cooperativity-Assisted Ultrastrong Coupling Enhancement in Terahertz Metasurfaces.

A system of N two-level atoms cooperatively interacting with a photonic field can be described as a single giant atom coupled to the field with interaction strength ∝N. This enhancement, known as Dicke cooperativity in quantum optics, has recently become an indispensable element in quantum information technology. Here, we extend the coupling beyond the standard light-matter interaction paradigm, enhancing Dicke cooperativity in a terahertz metasurface with N meta-atoms. The cooperative enhancement is manifested through the hybridization of the localized surface plasmon resonance in individual meta-atoms and surface lattice resonance due to the periodic array. Furthermore, through engineering of the capacitive split-gap in the meta-atoms, we were able to enhance the coupling rate into the ultrastrong coupling regime by a factor of N. Our strategy can serve as a new platform for demonstrating effective control of fermionic systems by weak pumping, superradiant emission, and ultrasensitive sensing of molecules.

K-point longitudinal acoustic phonons are responsible for ultrafast intervalley scattering in monolayer MoSe2.

In transition metal dichalcogenides, valley depolarization through intervalley carrier scattering by zone-edge phonons is often unavoidable. Although valley depolarization processes related to various acoustic phonons have been suggested, their optical verification is still vague due to nearly degenerate phonon frequencies on acoustic phonon branches at zone-edge momentums. Here we report an unambiguous phonon momentum determination of the longitudinal acoustic (LA) phonons at the K point, which are responsible for the ultrafast valley depolarization in monolayer MoSe2. Using sub-10-fs-resolution pump-probe spectroscopy, we observed coherent phonons signals at both even and odd-orders of zone-edge LA mode involved in intervalley carrier scattering process. Our phonon-symmetry analysis and first-principles calculations reveal that only the LA phonon at the K point, as opposed to the M point, can produce experimental odd-order LA phonon signals from its nonlinear optical modulation. This work will provide momentum-resolved descriptions of phonon-carrier intervalley scattering processes in valleytronic materials.

Ultrahigh strength, modulus, and conductivity of graphitic fibers by macromolecular coalescence.

Theoretical considerations suggest that the strength of carbon nanotube (CNT) fibers be exceptional; however, their mechanical performance values are much lower than the theoretical values. To achieve macroscopic fibers with ultrahigh performance, we developed a method to form multidimensional nanostructures by coalescence of individual nanotubes. The highly aligned wet-spun fibers of single- or double-walled nanotube bundles were graphitized to induce nanotube collapse and multi-inner walled structures. These advanced nanostructures formed a network of interconnected, close-packed graphitic domains. Their near-perfect alignment and high longitudinal crystallinity that increased the shear strength between CNTs while retaining notable flexibility. The resulting fibers have an exceptional combination of high tensile strength (6.57 GPa), modulus (629 GPa), thermal conductivity (482 W/m·K), and electrical conductivity (2.2 MS/m), thereby overcoming the limits associated with conventional synthetic fibers.

Magnetic Control of Soft Chiral Phonons in PbTe.

PbTe crystals have a soft transverse optical phonon mode in the terahertz frequency range, which is known to efficiently decay into heat-carrying acoustic phonons, resulting in anomalously low thermal conductivity. Here, we studied this phonon via polarization-dependent terahertz spectroscopy. We observed softening of this mode with decreasing temperature, indicative of incipient ferroelectricity, which we explain through a model including strong anharmonicity with a quartic displacement term. In magnetic fields up to 25 T, the phonon mode splits into two modes with opposite handedness, exhibiting circular dichroism. Their frequencies display Zeeman splitting together with an overall diamagnetic shift with increasing magnetic field. Using a group-theoretical approach, we demonstrate that these observations are the result of magnetic field-induced morphic changes in the crystal symmetries through the Lorentz force exerted on the lattice ions. Thus, our Letter reveals a novel process of controlling phonon properties in a soft ionic lattice by a strong magnetic field.

Carbon Nanotube Devices for Quantum Technology.

Carbon nanotubes, quintessentially one-dimensional quantum objects, possess a variety of electrical, optical, and mechanical properties that are suited for developing devices that operate on quantum mechanical principles. The states of one-dimensional electrons, excitons, and phonons in carbon nanotubes with exceptionally large quantization energies are promising for high-operating-temperature quantum devices. Here, we discuss recent progress in the development of carbon-nanotube-based devices for quantum technology, i.e., quantum mechanical strategies for revolutionizing computation, sensing, and communication. We cover fundamental properties of carbon nanotubes, their growth and purification methods, and methodologies for assembling them into architectures of ordered nanotubes that manifest macroscopic quantum properties. Most importantly, recent developments and proposals for quantum information processing devices based on individual and assembled nanotubes are reviewed.

Hall effect in gated single-wall carbon nanotube films.

The presence of hopping carriers and grain boundaries can sometimes lead to anomalous carrier types and density overestimation in Hall-effect measurements. Previous Hall-effect studies on carbon nanotube films reported unreasonably large carrier densities without independent assessments of the carrier types and densities. Here, we have systematically investigated the validity of Hall-effect results for a series of metallic, semiconducting, and metal-semiconductor-mixed single-wall carbon nanotube films. With carrier densities controlled through applied gate voltages, we were able to observe the Hall effect both in the n- and p-type regions, detecting opposite signs in the Hall coefficient. By comparing the obtained carrier types and densities against values derived from simultaneous field-effect-transistor measurements, we found that, while the Hall carrier types were always correct, the Hall carrier densities were overestimated by up to four orders of magnitude. This significant overestimation indicates that thin films of one-dimensional SWCNTs are quite different from conventional hopping transport systems.

Macroscopic weavable fibers of carbon nanotubes with giant thermoelectric power factor.

Low-dimensional materials have recently attracted much interest as thermoelectric materials because of their charge carrier confinement leading to thermoelectric performance enhancement. Carbon nanotubes are promising candidates because of their one-dimensionality in addition to their unique advantages such as flexibility and light weight. However, preserving the large power factor of individual carbon nanotubes in macroscopic assemblies has been challenging, primarily due to poor sample morphology and a lack of proper Fermi energy tuning. Here, we report an ultrahigh value of power factor (14 ± 5 mW m-1 K-2) for macroscopic weavable fibers of aligned carbon nanotubes with ultrahigh electrical and thermal conductivity. The observed giant power factor originates from the ultrahigh electrical conductivity achieved through excellent sample morphology, combined with an enhanced Seebeck coefficient through Fermi energy tuning. We fabricate a textile thermoelectric generator based on these carbon nanotube fibers, which demonstrates high thermoelectric performance, weavability, and scalability. The giant power factor we observe make these fibers strong candidates for the emerging field of thermoelectric active cooling, which requires a large thermoelectric power factor and a large thermal conductivity at the same time.

Ultrastrong magnon-magnon coupling dominated by antiresonant interactions.

Exotic quantum vacuum phenomena are predicted in cavity quantum electrodynamics systems with ultrastrong light-matter interactions. Their ground states are predicted to be vacuum squeezed states with suppressed quantum fluctuations owing to antiresonant terms in the Hamiltonian. However, such predictions have not been realized because antiresonant interactions are typically negligible compared to resonant interactions in light-matter systems. Here we report an unusual, ultrastrongly coupled matter-matter system of magnons that is analytically described by a unique Hamiltonian in which the relative importance of resonant and antiresonant interactions can be easily tuned and the latter can be made vastly dominant. We found a regime where vacuum Bloch-Siegert shifts, the hallmark of antiresonant interactions, greatly exceed analogous frequency shifts from resonant interactions. Further, we theoretically explored the system's ground state and calculated up to 5.9 dB of quantum fluctuation suppression. These observations demonstrate that magnonic systems provide an ideal platform for exploring exotic quantum vacuum phenomena predicted in ultrastrongly coupled light-matter systems.