2014 New's Items

Collective Effects in Linear Spectroscopy of Dipole Coupled Arrays

A. A. Kocherzhenko
J. Dawlaty
B. P. Abolins
F. Herrera
D. B. Abraham
K. B. Whaley
2014

We present a consistent analysis of linear spectroscopy for arrays of nearest-neighbor dipole-coupled two-level molecules that reveals distinct signatures of weak- and strong-coupling regimes separated for infinite-size arrays by a quantum critical point. In the weak-coupling regime, the ground state of the molecular array is disordered, but in the strong-coupling regime, it has (anti)ferroelectric ordering. We show that multiple molecular excitations [odd (even) in the weak- (strong-) coupling regime] can be accessed directly from the ground state. We analyze the scaling of...

Phase-Selective Cation-Exchange Chemistry in Sulfide Nanowire Systems

D. Zhang
A. B. Wong
Y. Yu
S. Brittman
J. Sun
A. Fu
B. Beberwyck
A. P. Alivisatos
P. Yang
2014

As a cation-deficient, p-type semiconductor, copper sulfide (Cu2–xS) shows promise for applications such as photovoltaics, memristors, and plasmonics. However, these applications demand precise tuning of the crystal phase as well as the stoichiometry of Cu2–xS, an ongoing challenge in the synthesis of Cu2–xS materials for a specific application. Here, a detailed transformation diagram of cation-exchange (CE) chemistry from cadmium sulfide (CdS) into Cu2–xS nanowires (...

Optimizing Broadband Terahertz Modulation with Hybrid Graphene/Metasurface Structures

S. F. Shi
B. Zeng
H. L. Han
X. Hong
H. Z. Tsai
H. S. Jung
A. Zettl
M. F. Crommie
F. Wang
2014

We demonstrate efficient terahertz (THz) modulation by coupling graphene strongly with a broadband THz metasurface device. This THz metasurface, made of periodic gold slit arrays, shows near unity broadband transmission, which arises from coherent radiation of the enhanced local-field in the slits. Utilizing graphene as an active load with tunable conductivity, we can significantly modify the local-field enhancement and strongly modulate the THz wave transmission. This hybrid device also provides a new platform for future nonlinear THz spectroscopy study of graphene.

Relating the Physical Structure and Optoelectronic Function of Crystalline TIPS-Pentacene

S. Sharifzadeh
C. Y. Wong
H. Wu
B. L. Cotts
L. Kronik
N. S. Ginsberg
J. B. Neaton
2014

Theory and experiment are combined to investigate the nature of low-energy excitons within ordered domains of 6,13-bis(triisopropylsilylethynyl)-pentacene (TIPS-PEN) polycrystalline thin films. First-principles density functional theory and many-body perturbation theory calculations, along with polarization-dependent optical absorption spectro-microscopy on ordered domains, show multiple low-energy absorption peaks that are composed of excitonic states delocalized over several molecules. While the first absorption peak is composed of a single excitonic transition and retains the...

The Low-Lying Electronic Excited States of Pentacene Oligomers: A Comparative Electronic Structure Study in the Context of Singlet Fission

P. B. Coto
S. Sharifzadeh
J. B. Neaton
M. Thoss
2014

The lowest-lying electronic excited states of pentacene and its oligomers are investigated using accurate multireference wave function methods (CASPT2/CASSCF) and the many-body Greens’s function approach (GW/BSE). The results obtained for dimers and trimers of different geometry reveal a complex electronic structure, which includes locally excited, charge transfer, and multiexciton states. For singlets of single-excitation character, both approaches yield excitation energies that are in good overall quantitative agreement. While the multiexciton states are located relatively high in...

Nanocatalysis I: Synthesis of Metal and Bimetallic Nanoparticles and Porous Oxides and Their Catalytic Reaction Studies

K. An
G. A. Somorjai
2014

In recent heterogeneous catalysis, much effort has been made in understanding how the size, shape, and composition of nanoparticles and oxide-metal interfaces affect catalytic performance at the molecular level. Recent advances in colloidal synthetic techniques enable preparing diverse metallic or bimetallic nanoparticles with well-defined size, shape, and composition and porous oxides as a high surface support. As nanoparticles become smaller, new chemical, physical, and catalytic properties emerge. Geometrically, as the smaller the nanoparticle the greater the relative number of...

Structure-Based Design of Functional Amyloid Materials

D. Li
E. M. Jones
M. R. Sawaya
H. Furukawa
F. Luo
M. Ivanova
S. A. Sievers
W. Wang
O. M. Yaghi
C. Liu
D. S. Eisenberg
2014

Amyloid fibers, once exclusively associated with disease, are acquiring utility as a class of biological nanomaterials. Here we introduce a method that utilizes the atomic structures of amyloid peptides, to design materials with versatile applications. As a model application, we designed amyloid fibers capable of capturing carbon dioxide from flue gas, to address the global problem of excess anthropogenic carbon dioxide. By measuring dynamic separation of carbon dioxide from nitrogen, we show that fibers with designed amino acid sequences double the carbon dioxide binding capacity of...