Phonon Dephasing Dynamics in MoS2.

A variety of quantum degrees of freedom, e.g., spins, valleys, and localized emitters, in atomically thin van der Waals materials have been proposed for quantum information applications, and they inevitably couple to phonons. Here, we directly measure the intrinsic optical phonon decoherence in monolayer and bulk MoS2 by observing the temporal evolution of the spectral interference of Stokes photons generated by pairs of laser pulses. We find that a prominent optical phonon mode E2g exhibits a room-temperature dephasing time of ∼7 ps in both the monolayer and bulk. This dephasing time extends to ∼20 ps in the bulk crystal at ∼15 K, which is longer than previously thought possible. First-principles calculations suggest that optical phonons decay via two types of three-phonon processes, in which a pair of acoustic phonons with opposite momentum are generated.

Stabilization of the Cubic Crystalline Phase in Organometal Halide Perovskite Quantum Dots via Surface Energy Manipulation.

Surface functionalization of nanoscale materials has a significant impact on their properties. We have demonstrated the effect of different passivating ligands on the crystal phase of organometal halide perovskite quantum dots (PQDs). Using static and dynamic spectroscopy, we studied phase transitions in CH3NH3PbBr3 PQDs ligated with either octylaminebromide (P-OABr) or 3-aminopropyl triethoxysilane (P-APTES). Around 140 K, P-OABr underwent a structural phase transition from tetragonal to orthorhombic, established by the emergence of a higher energy band in the photoluminescence (PL) spectrum. This was not observed in P-APTES, despite cooling down to 20 K. Additionally, time-resolved and excitation power-dependent PL, as well as Raman spectroscopy over a range of 300-20 K, revealed that recombination rates and types of charge carriers involved are significantly different in P-APTES and P-OABr. Our findings highlight how aspects of PQD phase stabilization are linked to nanoscale morphology and the crystal phase diagram.

Increased sensitivity of thyroid hormone-mediated signaling despite prolonged fasting.

Thyroid hormones (TH) can increase cellular metabolism. Food deprivation in mammals is typically associated with reduced thyroid gland responsiveness, in an effort to suppress cellular metabolism and abate starvation. However, in prolonged-fasted, elephant seal pups, cellular TH-mediated proteins are up-regulated and TH levels are maintained with fasting duration. The function and contribution of the thyroid gland to this apparent paradox is unknown and physiologically perplexing. Here we show that the thyroid gland remains responsive during prolonged food deprivation, and that its function and production of TH increase with fasting duration in elephant seals. We discovered that our modeled plasma TH data in response to exogenous thyroid stimulating hormone predicted cellular signaling, which was corroborated independently by the enzyme expression data. The data suggest that the regulation and function of the thyroid gland in the northern elephant seal is atypical for a fasted animal, and can be better described as, "adaptive fasting". Furthermore, the modeling data help substantiate the in vivo responses measured, providing unique insight on hormone clearance, production rates, and thyroid gland responsiveness. Because these unique endocrine responses occur simultaneously with a nearly strict reliance on the oxidation of lipid, these findings provide an intriguing model to better understand the TH-mediated reliance on lipid metabolism that is not otherwise present in morbidly obese humans. When coupled with cellular, tissue-specific responses, these data provide a more integrated assessment of thyroidal status that can be extrapolated for many fasting/food deprived mammals.

High Resolution Phonon-assisted Quasi-resonance Fluorescence Spectroscopy.

High resolution optical spectroscopy methods are demanding in terms of either technology, equipment, complexity, time or a combination of these. Here we demonstrate an optical spectroscopy method that is capable of resolving spectral features beyond that of the spin fine structure and homogeneous linewidth of single quantum dots (QDs) using a standard, easy-to-use spectrometer setup. This method incorporates both laser and photoluminescence spectroscopy, combining the advantage of laser line-width limited resolution with multi-channel photoluminescence detection. Such a scheme allows for considerable improvement of resolution over that of a common single-stage spectrometer. The method uses phonons to assist in the measurement of the photoluminescence of a single quantum dot after resonant excitation of its ground state transition. The phonon's energy difference allows one to separate and filter out the laser light exciting the quantum dot. An advantageous feature of this method is its straight forward integration into standard spectroscopy setups, which are accessible to most researchers.

Magnetic field induced quantum dot brightening in liquid crystal synergized magnetic and semiconducting nanoparticle composite assemblies.

The design and development of multifunctional composite materials from artificial nano-constituents is one of the most compelling current research areas. This drive to improve over nature and produce 'meta-materials' has met with some success, but results have proven limited with regards to both the demonstration of synergistic functionalities and in the ability to manipulate the material properties post-fabrication and in situ. Here, magnetic nanoparticles (MNPs) and semiconducting quantum dots (QDs) are co-assembled in a nematic liquid crystalline (LC) matrix, forming composite structures in which the emission intensity of the quantum dots is systematically and reversibly controlled with a small applied magnetic field (<100 mT). This magnetic field-driven brightening, ranging between a two- to three-fold peak intensity increase, is a truly cooperative effect: the LC phase transition creates the co-assemblies, the clustering of the MNPs produces LC re-orientation at atypical low external field, and this re-arrangement produces compaction of the clusters, resulting in the detection of increased QD emission. These results demonstrate a synergistic, reversible, and an all-optical process to detect magnetic fields and additionally, as the clusters are self-assembled in a fluid medium, they offer the possibility for these sensors to be used in broad ranging fluid-based applications.

Optophononics with coupled quantum dots.

Modern technology is founded on the intimate understanding of how to utilize and control electrons. Next to electrons, nature uses phonons, quantized vibrations of an elastic structure, to carry energy, momentum and even information through solids. Phonons permeate the crystalline components of modern technology, yet in terms of technological utilization phonons are far from being on par with electrons. Here we demonstrate how phonons can be employed to render a single quantum dot pair optically transparent. This phonon-induced transparency is realized via the formation of a molecular polaron, the result of a Fano-type quantum interference, which proves that we have accomplished making typically incoherent and dissipative phonons behave in a coherent and non-dissipative manner. We find the transparency to be widely tunable by electronic and optical means. Thereby we show amplification of weakest coupling channels. We further outline the molecular polaron's potential as a control element in phononic circuitry architecture.

Optical spin initialization and nondestructive measurement in a quantum dot molecule.

The spin of an electron in a self-assembled InAs/GaAs quantum dot molecule is optically prepared and measured through the trion triplet states. A longitudinal magnetic field is used to tune two of the trion states into resonance, forming a superposition state through asymmetric spin exchange. As a result, spin-flip Raman transitions can be used for optical spin initialization, while separate trion states enable cycling transitions for nondestructive measurement. With two-laser transmission spectroscopy we demonstrate both operations simultaneously, something not previously accomplished in a single quantum dot.