arXiv subjects

Kaili Jiang

Publications and source records attributed to Kaili Jiang.

26 records · Page 2Linked to original sources

arXiv2017

Non-additive Non-interacting Kinetic Energy of Rare Gas Dimers

Approximations of the non-additive non-interacting kinetic energy (NAKE) as an explicit functional of the density are the basis of several electronic structure methods that provide improved computational efficiency over standard Kohn-Sham calculations. However, within most fragment-based formalisms, there is no unique exact NAKE, making it difficult to develop general, robust approximations for it. When adjustments are made to the embedding formalisms to guarantee uniqueness, approximate functionals may be more meaningfully compared to the exact unique NAKE. We use numerically accurate inversions to study the exact NAKE of several rare-gas dimers within Partition Density Functional Theory, a method that provides the uniqueness for the exact NAKE. We find that the NAKE decreases nearly exponentially with atomic separation for the rare gas dimers. We compute the logarithmic derivative of the NAKE with respect to the bond length for our numerically accurate inversions as well as for several approximate NAKE functionals. We show that standard approximate NAKE functionals do not reproduce the correct behavior for this logarithmic derivative, and propose two new NAKE functionals that do. The first of these is based on a re-parametrization of a conjoint PBE functional. The second is a simple, physically-motivated non-decomposable NAKE functional that matches the asymptotic decay constant without fitting.

physics.chem-ph↗

arXiv2016

The Importance of being consistent

We review the role of self-consistency in density functional theory. We apply a recent analysis to both Kohn-Sham and orbital-free DFT, as well as to Partition-DFT, which generalizes all aspects of standard DFT. In each case, the analysis distinguishes between errors in approximate functionals versus errors in the self-consistent density. This yields insights into the origins of many errors in DFT calculations, especially those often attributed to self-interaction or delocalization error. In many classes of problems, errors can be substantially reduced by using `better' densities. We review the history of these approaches, many of their applications, and give simple pedagogical examples.

physics.chem-ph↗

arXiv2016

Accurate Reference Data for the Non-Additive Non-Interacting Kinetic Energy in Covalent Bonds

The non-additive non-interacting kinetic energy is calculated exactly for fragments of H$_2$, Li$_2$, Be$_2$, C$_2$, N$_2$, F$_2$, and Na$_2$ within partition density-functional theory. The resulting fragments are uniquely determined and their sum reproduces the Kohn-Sham molecular density of the corresponding XC functional. We compare the use of fractional orbital occupation to the usual PDFT ensemble method for treating the fragment energies and densities. We also compare Thomas-Fermi and von Weiz{ä}cker approximate kinetic energy functionals to the numerically exact solution and find significant regions where the von Weiz{ä}cker solution is nearly exact.

physics.chem-ph↗

arXiv2015

Monolayer charge-neutral graphene on platinum with extremely weak electron-phonon coupling

Epitaxial growth of graphene on transition metal substrates is an important route for obtaining large scale graphene. However, the interaction between graphene and the substrate often leads to multiple orientations, distorted graphene band structure, large doping and strong electron-phonon coupling. Here we report the growth of monolayer graphene with high crystalline quality on Pt(111) substrate by using a very low concentration of an internal carbon source with high annealing temperature. The controlled growth leads to electronically decoupled graphene: it is nearly charge neutral and has extremely weak electron-phonon coupling (coupling strength $λ$ $\approx$ 0.056) as revealed by angle-resolved photoemission spectroscopic measurements. The thermodynamics and kinetics of the carbon diffusion process is investigated by DFT calculation. Such graphene with negligible graphene-substrate interaction provides an important platform for fundamental research as well as device applications when combined with a nondestructive sample transfer technique.

cond-mat.mtrl-sci↗

arXiv2015

Silicene Nanomesh

Similar to graphene, zero band gap limits the application of silicene in nanoelectronics despite of its high carrier mobility. By using first-principles calculations, we reveal that a band gap is opened in silicene nanomesh (SNM) when the width W of the wall between the neighboring holes is even. The size of the band gap increases with the reduced W and has a simple relation with the ratio of the removed Si atom and the total Si atom numbers of silicene. Quantum transport simulation reveals that the sub-10 nm single-gated SNM field effect transistors show excellent performance at zero temperature but such a performance is greatly degraded at room temperature.

cond-mat.mtrl-sci↗

arXiv2010

Multiplexed five-color molecular imaging of cancer cells and tumor tissues with carbon nanotube Raman tags in the near-infrared

Single-walled carbon nanotubes (SWNTs) with five different C13/C12 isotope compositions and well-separated Raman peaks have been synthesized and conjugated to five targeting ligands in order to impart molecular specificity. Multiplexed Raman imaging of live cells has been carried out by highly specific staining of cells with a five-color mixture of SWNTs. Ex vivo multiplexed Raman imaging of tumor samples uncovers a surprising up-regulation of epidermal growth factor receptor (EGFR) on LS174T colon cancer cells from cell culture to in vivo tumor growth. This is the first time five-color multiplexed molecular imaging has been performed in the near-infrared (NIR) region under a single laser excitation. Near zero interfering background of imaging is achieved due to the sharp Raman peaks unique to nanotubes over the low, smooth autofluorescence background of biological species.

cond-mat.mtrl-sci↗

arXiv2008

Protein Microarrays with Carbon Nanotubes as Multi-Color Raman Labels

Detection of biomolecules is important in proteomics and clinical diagnosis and treatment of diseases. Here, we apply functionalized, macromolecular, single walled carbon nanotubes SWNTs as multi-color Raman labels to protein arrays for highly sensitive, multiplexed protein detection. Raman detection utilizes the sharp peaks of SWNTs with minimal background interference, affording a high signal to noise ratio needed for ultra-sensitive detection. Surface-enhanced Raman scattering SERS combined with the strong resonance Raman intensity of SWNTs, affords detection sensitivity down to 1 fM, a three order of magnitude improvement over most of reported fluorescence-based protein detections. We show that human autoantibodies to Proteinase 3 aPR3, a biomarker for the autoimmune disease Wegeners granulomatosis, is detected by Raman in human serum up to a 107 dilution. Moreover, SWNT Raman tags are stable against photobleaching and quenching, and by conjugating different antibodies to pure 12C and 13C SWNT isotopes, we demonstrate two-color SWNT Raman-based protein detection in a multiplexed fashion.

cond-mat.mtrl-sci↗

arXiv2008

Multiplexed Multi-Color Raman Imaging of Live Cells with Isotopically Modified Single Walled Carbon Nanotubes

We show that single walled carbon nanotubes with different isotope compositions exhibit distinct Raman Gband peaks and can be used for multiplexed multi-color Raman imaging of biological systems. Cancer cells with specific receptors are selectively labeled with 3 differently colored SWNTs conjugated with various targeting ligands including Herceptin, anti-Her2, Erbitux, anti-Her1, and RGD peptide, allowing for multi-color Raman imaging of cells in a multiplexed manner. SWNT Raman signals are highly robust against photo-bleaching, allowing long term imaging and tracking. With narrow peak features, SWNT Raman signals are easily differentiated from the auto-fluorescence background. The SWNT Raman excitation and scattering photons are in the near-infrared region, which is the most transparent optical window for biological systems in vitro and in vivo. Thus, SWNTs are novel Raman tags promising for multiplexed biological detection and imaging.

cond-mat.mtrl-sci↗