Browsing by Author "Zhang, T."
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Item Open Access Chiral ceramic nanoparticles and peptide catalysis(American Chemical Society, 2017) Jiang S.; Chekini, M.; Qu, Z.-B.; Wang Y.; Yeltik A.; Liu, Y.; Kotlyar, A.; Zhang, T.; Li, B.; Demir, Hilmi Volkan; Kotov, N. A.The chirality of nanoparticles (NPs) and their assemblies has been investigated predominantly for noble metals and II-VI semiconductors. However, ceramic NPs represent the majority of nanoscale materials in nature. The robustness and other innate properties of ceramics offer technological opportunities in catalysis, biomedical sciences, and optics. Here we report the preparation of chiral ceramic NPs, as represented by tungsten oxide hydrate, WO3-x·H2O, dispersed in ethanol. The chirality of the metal oxide core, with an average size of ca. 1.6 nm, is imparted by proline (Pro) and aspartic acid (Asp) ligands via bio-to-nano chirality transfer. The amino acids are attached to the NP surface through C-O-W linkages formed from dissociated carboxyl groups and through amino groups weakly coordinated to the NP surface. Surprisingly, the dominant circular dichroism bands for NPs coated by Pro and Asp are different despite the similarity in the geometry of the NPs; they are positioned at 400-700 nm and 500-1100 nm for Pro- and Asp-modified NPs, respectively. The differences in the spectral positions of the main chiroptical band for the two types of NPs are associated with the molecular binding of the two amino acids to the NP surface; Asp has one additional C-O-W linkage compared to Pro, resulting in stronger distortion of the inorganic crystal lattice and greater intensity of CD bands associated with the chirality of the inorganic core. The chirality of WO3-x·H2O atomic structure is confirmed by atomistic molecular dynamics simulations. The proximity of the amino acids to the mineral surface is associated with the catalytic abilities of WO3-x·H2O NPs. We found that NPs facilitate formation of peptide bonds, leading to Asp-Asp and Asp-Pro dipeptides. The chiroptical activity, chemical reactivity, and biocompatibility of tungsten oxide create a unique combination of properties relevant to chiral optics, chemical technologies, and biomedicine.Item Open Access Magneto-optical studies of CdSe/CdMnS/CdS core/multi-shell colloidal nanoplatelets(SPIE, 2016) Petrou, A.; Scrace, T. A.; Murphy, J. R.; Zhang, P.; Norden, T.; Zhang, T.; Thomay, T.; Cartwright, A. N.; Delikanlı, Savaş; Akgül, Mehmet Zafer; Demir, Hilmi VolkanWe studied the photoluminescence (PL)) from CdSe/CdMnS/CdS core/multi-shell colloidal nanoplatelets, a versatile platform to study the interplay of optical properties and nanomagnetism. The photoluminescence (PL) exhibits σ+ polarization in the applied magnetic field. Our measurement detects the presence of even a single magnetic monolayer shell. The PLL consists of a higher and a lower energy component; the latter exhibits a circular polarization peak. The time-resolved PL (trPL) shows a red shift as function of time delay. At early (later) times the trPL spectra coincide with the high (low) energy PL component. A model is proposed to interpret these results.Item Open Access Time resolved photoluminescence study of magnetic CdSe/CdMnS/CdS core/multi-shell nanoplatelets(SPIE, 2017) Murphy, J. R.; Delikanlı, Savaş; Zhang, T.; Scrace, T. A.; Zhang, P.; Norden, T.; Thomay, T.; Cartwright, A. N.; Demir, Himli Volkan; Petrou, A.Colloidal semiconductor nanoplatelets (NPLs) are quasi 2D-nanostructures that are grown and processed inexpensively using a solution based method and thus have recently attracted considerable attention. We observe two features in the photoluminescence spectrum, suggesting two possible recombination channels. Their intensity ratio varies with temperature and two distinct temperature regions are identified; a low temperature region (10K < T < 90K) and a high temperature region (90K < T < 200K). This ratio increases with increasing temperature, suggesting that one recombination channel involves holes that are weakly localized with a localization energy of 0.043meV. A possible origin of these localized states are energy-variations in the xy-plane of the nanoplatelet. The presence of positive photoluminescence circular polarization in the magnetically-doped core/multi-shell NPLs indicates a hole-dopant exchange interaction and therefore the incorporated magnetic Manganese ions act as a marker that determines the location of the localized hole states.1 Time-resolved measurements show two distinct timescales (τfast and τslow) that can be modeled using a rate equation model. We identify these timescales as closely related to the corresponding recombination times for the channels. The stronger hole localization of one of these channels leads to a decreased electron-hole wave function overlap and thus a decreased oscillator strength and an increased lifetime. We show that we can model and understand the magnetic interaction of doped 2D-colloidal nanoplatelets which opens a pathway to solution processable spin controllable light sources. Copyright © 2017 SPIE.Item Open Access Voxel-based state space modeling recovers task-related cognitive states in naturalistic fMRI experiments(Frontiers Media S.A., 2021-05-06) Zhang, T.; Gao, J. S.; Çukur, Tolga; Gallant, J. L.Complex natural tasks likely recruit many different functional brain networks, but it is difficult to predict how such tasks will be represented across cortical areas and networks. Previous electrophysiology studies suggest that task variables are represented in a low-dimensional subspace within the activity space of neural populations. Here we develop a voxel-based state space modeling method for recovering task-related state spaces from human fMRI data. We apply this method to data acquired in a controlled visual attention task and a video game task. We find that each task induces distinct brain states that can be embedded in a low-dimensional state space that reflects task parameters, and that attention increases state separation in the task-related subspace. Our results demonstrate that the state space framework offers a powerful approach for modeling human brain activity elicited by complex natural tasks.