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Jacques Doumani

Publications and source records attributed to Jacques Doumani.

10 recordsLinked to original sources

Chip-Scale Aligned Chiral Carbon Nanotubes Exhibiting Giant Second Harmonic Generation

Chiral carbon nanotubes (CNTs) are direct-gap semiconductors with optical properties governed by one-dimensional excitons with enormous oscillator strengths. Each species of chiral CNTs has an enantiomeric pair of left- and right-handed CNTs with nearly identical properties, but enantiomer-dependent phenomena can emerge, especially in nonlinear optical processes. Theoretical studies have predicted strong second-order nonlinearities in chiral CNTs, but no experimental quantitative verification has been reported due to the lack of macroscopically ordered assemblies of single-enantiomer chiral CNTs. Here, we report the synthesis of centimeter-scale, densely packed, aligned single-enantiomer chiral CNT films that are microfabrication-compatible. We observe giant second harmonic generation (SHG) emission from the chiral CNT film, which originates from the intrinsic chirality and inversion symmetry breaking of the atomic structure of chiral CNTs. The observed nonlinear susceptibility of the as-fabricated film reaches $4.9\times 10^2$\,pm/V at a pump wavelength of 1030\,nm, corresponding to the lowest-energy excitonic resonance, indicating $χ_{xyz} = 1.6\times 10^3$\,pm/V for a perfectly aligned CNT crystal. Our calculations based on many-body theory correctly estimate the spectrum and magnitude of such excitonically enhanced optical nonlinearity. These results are promising for the development of scalable chiral-CNT electronics and nonlinear photonics.

physics.app-ph

Vacuum-dressed superconductivity in NbN observed in a high-$Q$ terahertz cavity

Emerging theoretical frameworks suggest that physical properties of matter can be altered within an optical cavity by harnessing quantum vacuum electromagnetic fluctuations, even in the total absence of external driving fields. Among the most intriguing predictions is the potential to noninvasively manipulate superconductivity. Here, we experimentally observe modified superconductivity in niobium nitride (NbN) thin films within high-quality-factor ($Q$) terahertz cavities. Using terahertz time-domain spectroscopy, we characterize the NbN response both in free space and within a high-$Q$ photonic-crystal cavity. Our analysis reveals significant cavity-induced modifications to the optical conductivity. A theoretical model indicates that these changes originate from a substantial ($\sim13\,\%$) reduction in the superfluid density and a minor ($\sim2\,\%$) reduction in the superconducting gap, driven by cavity vacuum fluctuations. These results demonstrate a platform for engineering ground states via vacuum--matter coupling, opening frontiers in cavity materials science.

physics.optics

Terahertz Chiral Optics with Ordered Carbon Nanotube Architectures

Chiral optical terahertz (THz) devices have significant technological implications for telecommunications, spectroscopy, and sensing. Engineering tunable, broadband, and cost-effective THz chiral materials has long been recognized as a challenging endeavor and has been the bottleneck hindering the full exploitation of the THz spectrum. Here, we present an artificial structure based on aligned carbon nanotube films that exhibit a tunable broadband circular dichroism (CD) up to 2.8 degrees. Its behavior is reciprocal. The developed theoretical simulations are in agreement with the experiments and predict a further increase of CD signal up to ~30 degrees when more CNT layers are added.

physics.optics

Lattice-induced spin dynamics in Dirac magnet CoTiO3

Spin-lattice coupling is crucial for understanding the spin transport and dynamics for spintronics and magnonics applications. Recently, cobalt titanate (CoTiO3), an easy-plane antiferromagnet, has been found to host axial phonons with a large magnetic moment, which may originate from spin-lattice coupling. Here, we investigate the effect of light-driven lattice dynamics on the magnetic properties of CoTiO3 using time-resolved spectroscopy with a THz pump and a magneto-optic probe. We found resonantly driven Raman active phonons, phonon-polariton-induced excitation of the antiferromagnetic magnons, and a slow increase in the polarization rotation of the probe, all indicating symmetry breaking that is not intrinsic to the magnetic space group. The temperature dependence confirmed that the observed spin dynamics is related to the magnetic order, and we suggest surface effects as a possible mechanism. Our results of THz-induced spin-lattice dynamics signify that extrinsic symmetry breaking may contribute strongly and unexpectedly to light-driven phenomena in bulk complex oxides.

cond-mat.mtrl-sci

Terahertz Cavity Phonon Polaritons in Lead Telluride in the Deep-Strong Coupling Regime

Lead telluride is an important thermoelectric material due to its large Seebeck coefficient combined with its unusually low thermal conductivity that is related to the strong anharmonicity of phonons in this material. Here, we have studied the resonant and nonperturbative coupling of transverse optical phonons in lead telluride with cavity photons inside small-mode-volume metallic metasurface cavities that have photonic modes with terahertz frequencies. We observed a giant vacuum Rabi splitting on the order of the bare phonon and cavity frequencies. Through terahertz time-domain spectroscopy experiments, we systematically studied the vacuum Rabi splitting as a function of sample thickness, temperature, and cavity length. Under the strongest light-matter coupling conditions, the strength of coupling exceeded the bare phonon and cavity frequencies, putting the system into the deep-strong coupling regime. These results demonstrate that this uniquely tunable platform is promising for realizing and understanding predicted cavity-vacuum-induced ferroelectric instabilities and exploring applications of light-matter coupling in the ultrastrong and deep-strong coupling regimes in quantum technology.

physics.optics

Zeeman polaritons as a platform for probing Dicke physics in condensed matter

The interaction of an ensemble of two-level atoms and a quantized electromagnetic field, described by the Dicke Hamiltonian, is an extensively studied problem in quantum optics. However, experimental efforts to explore similar physics in condensed matter typically employ bosonic matter modes (e.g., phonons, magnons, and plasmons) that are describable as simple harmonic oscillators, i.e., an infinite ladder of equally spaced energy levels. Here, we examine ultrastrong coupling between a coherent light mode and an ensemble of paramagnetic spins, a finite-multilevel system, in Gd$_3$Ga$_5$O$_{12}$. The electron paramagnetic resonance of Gd$^{3+}$ ions is tuned by a magnetic field into resonance with a Fabry--Pérot cavity mode, resulting in the formation of spin--photon hybrid states, or Zeeman polaritons. We observe that the light--matter coupling strength, measured through the vacuum Rabi splitting, decreases with increasing temperature, which can be explained by the temperature-dependent population difference between the lower and higher-energy states, a trait of a finite-level system. This finding demonstrates that a spin--boson system is more compatible with the Dicke model and has advantages over boson--boson systems for pursuing experimental realizations of phenomena predicted for ultrastrongly coupled light--matter hybrids.

quant-ph

Graphene Terahertz Devices for Sensing and Communication

Graphene-based terahertz (THz) devices have emerged as promising platforms for a variety of applications, leveraging graphene's unique optoelectronic properties. This review explores recent advancements in utilizing graphene in THz technology, focusing on two main aspects: THz molecular sensing and THz wave modulation. In molecular sensing, the environment-sensitive THz transmission and emission properties of graphene are utilized for enabling molecular adsorption detection and biomolecular sensing. This capability holds significant potential, from the detection of pesticides to DNA at high sensitivity and selectivity. In THz wave modulation, crucial for next-generation wireless communication systems, graphene demonstrates remarkable potential in absorption modulation when gated. Novel device structures, spectroscopic systems, and metasurface architectures have enabled enhanced absorption and wave modulation. Furthermore, techniques such as spatial phase modulation and polarization manipulation have been explored. From sensing to communication, graphene-based THz devices present a wide array of opportunities for future research and development. Finally, advancements in sensing techniques not only enhance biomolecular analysis but also contribute to optimizing graphene's properties for communication by enabling efficient modulation of electromagnetic waves. Conversely, developments in communication strategies inform and enhance sensing capabilities, establishing a mutually beneficial relationship.

physics.optics

Observation of the Magnonic Dicke Superradiant Phase Transition

Two-level atoms coupled with single-mode cavity photons are predicted to exhibit a quantum phase transition when the coupling strength exceeds a critical value, entering a phase in which atomic polarization and photonic field are finite even at zero temperature and without external driving. However, this phenomenon, the superradiant phase transition (SRPT), is forbidden by a no-go theorem due to the existence of the diamagnetic term in the Hamiltonian. Here, we present spectroscopic evidence for a magnonic SRPT in ErFeO$_3$, where the role of the photonic mode (two-level atoms) in the photonic SRPT is played by an Fe$^{3+}$ magnon mode (Er$^{3+}$ spins). The absence of the diamagnetic term in the Fe$^{3+}$-Er$^{3+}$ exchange coupling ensures that the no-go theorem does not apply. Terahertz and gigahertz magnetospectroscopy experiments revealed the signatures of the SRPT -- a kink and a softening, respectively, of two spin-magnon hybridized modes at the critical point.

quant-ph

Macroscopically Self-Aligned and Chiralized Carbon Nanotubes: From Filtration to Innovation

Because of their natural one-dimensional (1D) structure combined with intricate chiral variations, carbon nanotubes (CNTs) exhibit various exceptional physical properties, such as ultrahigh electrical and thermal conductivity, exceptional mechanical strength, and chirality-dependent metallicity. These properties make CNTs highly promising for diverse applications, including field-effect transistors, sensors, photodetectors, and thermoelectric devices. While CNTs excel individually at the nanoscale, their 1D and chiral nature can be lost on a macroscopic scale when they are randomly assembled. Therefore, the alignment and organization of CNTs in macroscopic structures is crucial for harnessing their full potential. In this review, we explore recent advancements in understanding CNT alignment mechanisms, improving CNT aligning methods, and demonstrating macroscopically 1D properties of ordered CNT assemblies. We also focus on a newly discovered class of CNT architectures, combining CNT alignment and twisting mechanisms to create artificial radial and chiral CNT films at wafer scales. Finally, we summarize recent developments related to aligned and chiral CNT films in optoelectronics, highlighting their unique roles in solar cells, thermal emitters, and optical modulators.

physics.app-ph

Controlled synthetic chirality in macroscopic assemblies of carbon nanotubes

There is an emerging recognition that successful utilization of chiral degrees of freedom can bring new scientific and technological opportunities to diverse research areas. Hence, methods are being sought for creating artificial matter with controllable chirality in an uncomplicated and reproducible manner. Here, we report the development of two straightforward methods for fabricating wafer-scale chiral architectures of ordered carbon nanotubes (CNTs) with tunable and giant circular dichroism (CD). Both methods employ simple approaches, (i) mechanical rotation and (ii) twist-stacking, based on controlled vacuum filtration and do not involve any sophisticated nanofabrication processes. We used a racemic mixture of CNTs as the starting material, so the intrinsic chirality of chiral CNTs is not responsible for the observed chirality. In particular, by controlling the stacking angle and handedness in (ii), we were able to maximize the CD response and achieve a record-high deep-ultraviolet ellipticity of 40 $\pm$ 1 mdeg/nm. Our theoretical simulations using the transfer matrix method reproduce the salient features of the experimentally observed CD spectra and further predict that a film of twist-stacked CNTs with an optimized thickness will exhibit an ellipticity as high as 150 mdeg/nm. The created wafer-scale objects represent a new class of synthetic chiral matter consisting of ordered quantum wires whose macroscopic properties are governed by nanoscopic electronic signatures such as van Hove singularities. These artificial structures with engineered chirality will not only provide playgrounds for uncovering new chiral phenomena but also open up new opportunities for developing high-performance chiral photonic and optoelectronic devices.

physics.optics