Intersubband Transitions Research Articles

Bound and Continuum Intersubband Transitions in Colloidal Quantum Wells.

Quantum well intersubband transitions are critical for quantum cascade lasers and infrared photodetectors. Control of band offsets allows bound-to-bound intersubband transitions, with confinement of both initial and final states, and bound-to-continuum transitions, in which only the initial state is energetically confined within the potential well. Both types of transitions are also achieved in colloidal CdSe wells by changing the heterostructure shell. Bare wells have narrow intersubband transitions spanning the near-infrared spectrum following effective mass predictions. Atomically precise core/shells enable a readily adjusted potential well for electrons. For CdSe/ZnS, bound-to-bound transitions are narrow and redshift with shell thickness. By contrast, broad bound-to-continuum absorptions are found in CdSe/CdS. Due to small conduction band offsets, higher conduction band states of the well are more delocalized into the CdS shell. These measurements provide unique data to understand the electronic structure of colloidal quantum wells and chart a path to atomically precise optoelectronic materials for the mid-infrared.

Transport dynamics of photo-induced carriers in GaN quantum well infrared photodetectors influenced by triangular potentials.

The intrinsic spontaneous and piezoelectric polarizations of GaN lead to the formation of triangular wells and barriers, resulting in the manifestation of chaotic transport models in GaN quantum well intersubband transition (ISBT) infrared detectors and giving rise to various adverse effects. The APSYS software was utilized to construct a novel GaN quantum well ISBT infrared detector in this study. By endeavoring to modify the quantum well structure, our objective was to precisely adjust the energy level of the first excited state (E1) to align with the apex of the triangular barrier. The objective is to reduce the transport barrier for photo-induced carriers and simultaneously investigate the mechanisms through which the triangular potentials influence the transport modes of ISBT infrared detectors. The construction of a GaN/AlGaN quantum well device reveals that the inclusion of 10 periods of 1.7/2.0 nm GaN/Al0.8Ga0.2N in the device structure results in an ISBT absorption wavelength of approximately 1550 nm. In comparison to the deep well structure featuring 2.0/2.0 nm GaN/AlN, the polarization field strengths of both wells and barriers in the quantum well region exhibit a reduction of 23% and 36%, respectively, while the depth of the well decreases by 0.35 eV. The E1 energy level penetrates the region of a triangular barrier, resulting in an approximate 18.5-fold enhancement of the absorption coefficient. By employing innovative transient spectroscopy techniques in conjunction with AC impedance spectroscopy, we have conducted an in-depth analysis of the transport dynamics of photo-induced carriers. The results reveal that the time constant for carrier transport within the E1 energy level, situated in the region of a triangular barrier, amounts to 318.9 ps, thereby indicating a remarkable enhancement in the overall transport process. Furthermore, based on impedance spectroscopy data, this work has successfully derived equivalent circuit models for various quantum well structures and distinct carrier transport pathways, thus providing valuable theoretical insights to optimize photo-induced carrier transportation.

Vertical Quantum Confinement in Bulk MoS2.

We experimentally observe quantum confinement states in bulk MoS2 by using angle-resolved photoemission spectroscopy (ARPES). The band structure at the Γ̅ point reveals quantum well states (QWSs) linked to vertical quantum confinement of the electrons, confirmed by the absence of dispersion in kz and a strong intensity modulation with the photon energy. Notably, the binding energy dependence of the QWSs versus n does not follow the quadratic dependence of a two-dimensional electron gas. Instead, a linear behavior is observed that is consistent with a parabolic-like quantum well. This confinement arises from the mechanical exfoliation preparation method, which leads to the detachment of a multilayer stack from the underlying bulk. This is confirmed by density functional theory (DFT) calculations. The quantum confinement in bulk-like MoS2 not only offers the opportunity to explore intersubband transitions to exploit optical properties but also provides a means to study fundamental quantum phenomena in multilayer stacks of different thicknesses.

THE INTERSUBBAND OPTICAL ABSORPTION COEFFICIENT OF THE QD WITH ACCEPTOR IMPURITY UNDER APPLIED ELECTRIC FIELD

In this work, a spherical quantum dot (QD) under the influence of an external electric field is investigated. A multi-band model of the valence band is applied. The influence of off-center acceptor impurity, electric field and QD size dispersion on the absorption coefficient during intersubband transitions between hole states has been analyzed. The results show that an electric field combined with an off-center impurity induces the appearance of two distinct absorption bands corresponding to different magnetic quantum numbers. The intensity of absorption bands depends on the direction and strength of the electric field, and significant differences are observed between fields of opposite polarity. It is important to note that there is a critical field strength that restores the degeneracy of the energy levels, narrowing the broadband absorption tail for systems with small or large dispersion sizes. This research aims to improve the understanding and optimization of the optical properties of nanomaterials.

Nonlinear optical response and bistability of intersubband polariton in a planar microcavity: Role of dynamic Coulomb coupling

We theoretically investigate the steady-state bistable intersubband polariton response of quantum-well (QW) structures embedded into planar semiconductor microcavity to intense plane wave incident radiation. A rigorous semiclassical approach employs the transfer matrix formalism and the sheet model, which includes the dynamic depolarization effect. Results of comprehensive numerical simulations on reflectance characteristics of the structures with strong coupling between the ground cavity mode of the electromagnetic field and intersubband excitations in QWs are presented. The mechanism of the polariton-based optical bistability (OB) is revealed. Both the mirror-based optical bistability (MOB) and the intrinsic optical bistability (IOB) are investigated, with the focus on the MOB. Polariton-based bistabilities driven by cyclically changing intensity of the incident radiation, frequency of the incident radiation, and the angle of incidence are considered. It is found that the presence of the dynamic depolarization effect brings novel features to the OB reflectance characteristics of the structures. Effect of accumulation of the MOB cooperativity parameter is revealed. The concept of effective QW is proposed to describe a tremendously enhanced MOB response of multiple identical QWs particularly located in the cavity. A remarkable possibility of MOB in systems of multiple particularly located QWs with big values of dephasing rate is demonstrated. It is shown that the transition from bistability to multiple bistability and to multistability for two QWs can be controlled by slight manipulation of the angle of incidence. A possibility is found for an outstanding width of the hysteresis of the angular-domain OB, being about one degree.

The impact of barrier modulation on carriers transport in GaN quantum well infrared detectors

The impact of barrier modulation on carriers transport in GaN quantum well infrared detectors

Photodetectors performance of nanostructured materials in antimony III-V InGaAsSb/AlGaAsSb interband cascade structures

The aim of the study is to increase the performance of solar conversion by integrating nanostructured materials within conventional solar cells by employing multi-energy stages (i.e., interband and intersubband) in cascade systems to overcome the absorption length barrier and achieve large photo-generated carrier values. Specifically, InGaAsSb/Al GaAsSb MQWs are investigated with narrow well widths (2-20 nm) and transition energies of the structures are calculated for varied well/barrier widths and depths using numerical modelling. The results show that both interband and intersubband transitions are valuable for improving photovoltaic and photodetection applications, but their mechanisms and applications are distinct, so understanding and controlling these transitions within semiconductor materials is essential for optimising the performance of devices in both areas of optoelectronics, including strain as an important parameter of integrity. The data suggests that a single electron requires multiple photons to be transported, with the formation of a type-I broken-gap alignment between AlGa AsSb (barrier) and InGaAsSb (well). A wide range of wavelengths, from visible to medium infrared (MIR), will greatly enhance solar spectrum absorption. The long-term goal is to combine the thermal properties of antimonies (GaSbInSb) with a low band gap and the optical properties of arsenide (GaAsAlAs) with a large band gap.

Autler-Townes splitting and linear dichroism in colloidal CdSe nanoplatelets driven by near-infrared pulses.

Coherent interaction between light fields and matter has led to many exotic physical phenomena, one of which is the Autler-Townes splitting originating from the optical Stark effect of a three-level system. It has been well documented for atoms, molecules, and low-dimensional, epitaxial-grown semiconductors but rarely for solution-processed samples. Here, we report on Autler-Townes splitting observed in CdSe nanoplatelets. The strong intersubband transition of these nanoplatelets situated in the near-infrared allows us to coherently drive it with femtosecond near-infrared pulses, and meanwhile, their strong interband transition in the visible records the resultant spectral changes. The splitting is most prominent with cross-polarized, linear pump-probe pulses, consistent with the orthogonal polarizations of interband and intersubband transition dipoles. When the nanoplatelets are driven from tilted incident angles, we observe anomalous spectral lineshapes arising from a competition between interband and intersubband drivings, which are nevertheless quantitatively captured by our dressed-state model simulation.

Transmission coefficient and probability of intersubband transitions in [formula omitted] superlattices: Effect of non-parabolicity

Transmission coefficient and probability of intersubband transitions in [formula omitted] superlattices: Effect of non-parabolicity

Hot Electron Cooling in n-Doped Colloidal Nanoplatelets Following Near-Infrared Intersubband Excitation.

Intersubband transition was recently discovered in colloidal nanoplatelets, but the associated intersubband carrier relaxation dynamics remains poorly understood. In particular, it is crucial to selectively excite the intersubband transition and to follow the hot electron dynamics in the absence of valence-band holes. This is achieved herein by exciting the predoped electrons in CdSe/ZnS nanoplatelets using near-infrared femtosecond pulses and monitoring nonequilibrium electron dynamics using broad-band visible pulses. We find that the n = 2 electrons relax to the n = 1 subband and establish a Fermi-Dirac distribution within 200 fs, and finally reach an equilibrium with the lattice within a few ps. The cooling dynamics depend mainly on the excitation fluence but weakly on the doping density and the lattice temperature. These characteristics are well captured by our numerical simulation that explicitly accounts for the state occupation effect and optical phonon scattering.

A Colloidal Route for Ubiquotous Mid-Wave Infrared Sensing

The rapid emergence of the Internet of Things, machine vision, and artificial intelligence have imposed critical requirements on the miniaturization, energy efficiency, and cost-effectiveness of infrared detectors. To meet these requirements, new sensor technologies that can reduce the fabrication cost associated with semiconductor epitaxy and remove the stringent requirement for cryogenic cooling are under active investigation. In the technologically important spectral region of mid-wavelength infrared (3–5 µm), colloidal quantum dots are currently at the forefront of this endeavor, with wafer-scale monolithic integration and Auger suppression being the key material capabilities to minimize the sensor's size, weight, power consumption, and cost (SWaP-C). Infrared sensors based on colloidal quantum dots have been studied for decades, and harnessing the interband transition in these quantum-confined nanostructures has been the mainstream theme in optoelectronic research. More unique photophysical properties can be harnessed by utilizing the transitions within the conduction levels or valence levels, known as intraband (intersubband) transitions. In this presentation, we discuss the progress, challenges, and opportunities of MWIR sensors fabricated from Ag2Se intraband colloidal quantum dots, a heavy metal-free colloidal nanomaterial that has merits for wide-scale adoption in consumer and industrial sectors.

Optical absorption properties in multi-layer InGaN/GaN core-shell quantum dots: The influences of ternary mixed crystal effect and hydrogen-like impurity

Optical absorption properties in multi-layer InGaN/GaN core-shell quantum dots: The influences of ternary mixed crystal effect and hydrogen-like impurity

Effects of hydrostatic pressure, aluminium composition, and external magnetic field on intersubband and intrasubband transitions characteristics in symmetric potential quantum wells

Effects of hydrostatic pressure, aluminium composition, and external magnetic field on intersubband and intrasubband transitions characteristics in symmetric potential quantum wells

Enhanced terahertz ISBT in GaAsBi/AlGaAs quantum well: impact of doping modulation

One of the pivotal characteristics of quantum wells (QW) designed for applications in filters or modulators is its absorption coefficient. This study investigates the combined influence of doping and active layer thickness on the absorption coefficient in GaAsBi/AlGaAs quantum wells. The self-consistent coupling between Schrödinger and Poisson equations was employed for this purpose. A comprehensive analysis of conduction band structure, energy levels, potentials, and densities is presented. This analysis discerns the effects of doping on intersubband transitions (ISBTs) in the terahertz (THz) frequency domain. An introduction of a donor impurity into the system greatly influenced the intersubband absorption coefficient, increasing its intensity and causing the optical response to shift toward the lowest frequency. The obtained resonant peak energies, situated within the terahertz spectrum, hint at promising applications for GaAsBi-based devices within this frequency band.

Electrically tunable third-harmonic generation using intersubband polaritonic metasurfaces

Nonlinear intersubband polaritonic metasurfaces, which integrate giant nonlinear responses derived from intersubband transitions of multiple quantum wells (MQWs) with plasmonic nanoresonators, not only facilitate efficient frequency conversion at pump intensities on the order of few tens of kW cm-2 but also enable electrical modulation of nonlinear responses at the individual meta-atom level and dynamic beam manipulation. The electrical modulation characteristics of the magnitude and phase of the nonlinear optical response are realized through Stark tuning of the resonant intersubband nonlinearity. In this study, we report, for the first time, experimental implementations of electrical modulation characteristics of mid-infrared third-harmonic generation (THG) using an intersubband polaritonic metasurface based on MQW with electrically tunable third-order nonlinear response. Experimentally, we achieved a 450% modulation depth of the THG signal, 86% suppression of zero-order THG diffraction tuning based on local phase tuning exceeding 180 degrees, and THG beam steering using phase gradients. Our work proposes a new route for electrically tunable flat nonlinear optical elements with versatile functionalities.

Electric field-induced electronic structure and intersubband transitions of a hydrogen molecular ion in a gaussian-type quantum ring

In this work, the influence of an external electric field on the electronic structure and intersubband transitions of a singly ionized double-donor system in a GaAs quantum ring defined by Gaussian-type potentials is investigated theoretically. Within the framework of the effective mass approach, the two-dimensional diagonalization method is used for the solution of the Schrödinger equation to obtain the eigen energies and corresponding wave functions. Numerical results reveal that the electronic energy spectrum and the linear optical absorption coefficient of the ring are remarkably affected by the strength of the lateral electric field, internuclear distance and parameters defining the confinement potential. Also, it has been shown that beyond the anti-crossing point, the wave functions exchange their symmetries without mixing, which is a characteristic feature of energy-level anti-crossing.

Tip‐Enhanced Imaging and Control of Infrared Strong Light‐Matter Interaction

AbstractOptical antenna resonators enable control of light‐matter interactions on the nano‐scale via electron–photon hybrid states in strong coupling. Specifically, mid‐infrared (MIR) nano‐antennas coupled to saturable intersubband transitions in multi‐quantum‐well (MQW) semiconductor heterostructures allow for the coupling strength to be tuned through antenna resonance and field intensity. Here, tip‐enhanced nano‐scale variation of antenna‐MQW coupling across the antenna is demonstrated, with a spatially‐dependent coupling strength varying from 73 (strong coupling) to 24 (weak coupling). This behavior is modeled based on the spatially dependent local constructive and destructive interference between tip and antenna fields. Using a quantum‐mechanical density‐matrix model of the MQW system with its designed values of transition dipole moment, doping density, and population decay time, the picosecond IR pulse coupling to intersubband transitions and the associated tip induced strong‐field saturation effects are described. These results present a new regime of nonlinear IR light‐matter control based on the dynamic manipulation of quantum hybrid states on the nanoscale and in the infrared, with a perspective regarding extension to molecular vibrations.

Intersubband polaritonic metasurfaces for high-contrast ultra-fast power limiting and optical switching

Nonlinear intersubband polaritonic metasurfaces support one of the strongest known ultrafast nonlinear responses in the mid-infrared frequency range across all condensed matter systems. Beyond harmonic generation and frequency mixing, these nonlinearities can be leveraged for ultrafast optical switching and power limiting, based on tailored transitions from strong to weak polaritonic coupling. Here, we demonstrate synergistic optimization of materials and photonic nanostructures to achieve large reflection contrast in ultrafast polaritonic metasurface limiters. The devices are based on optimized semiconductor heterostructure materials that minimize the intersubband transition linewidth and reduce absorption in optically-saturated nanoresonators, achieving a record-high reflection contrast of 54% experimentally. We also discuss opportunities to further boost the metrics of performance of this class of ultrafast limiters, showing that reflection contrast as high as 94% may be realistically achieved using all-dielectric intersubband polaritonic metasurfaces.

The effect of hydrostatic pressure, temperature and impurity factor on linear and nonlinear optical properties of InxGa1-xAs tuned quantum dot with modified Gaussian potential under the action of a vertical magnetic field

The effect of hydrostatic pressure, temperature and impurity factor on linear and nonlinear optical properties of InxGa1-xAs tuned quantum dot with modified Gaussian potential under the action of a vertical magnetic field

Giant optical second- and third-order nonlinearities at a telecom wavelength.

A material platform that excels in both optical second- and third-order nonlinearities at a telecom wavelength is theoretically and experimentally demonstrated. In this TiN-based coupled metallic quantum well structure, electronic subbands are engineered to support doubly resonant inter-subband transitions for an exceptionally high second-order nonlinearity and provide single-photon transitions for a remarkable third-order nonlinearity within the 1400-1600 nm bandwidth. The second-order susceptibility χ(2) reaches 2840 pm/V at 1440 nm, while the Kerr coefficient n2 arrives at 2.8 × 10-10 cm2/W at 1460 nm. The achievement of simultaneous strong second- and third-order nonlinearities in one material at a telecom wavelength creates opportunities for multi-functional advanced applications in the field of nonlinear optics.