اشترك بالحزمة الذهبية واحصل على وصول غير محدود شمرا أكاديميا
تسجيل مستخدم جديدA Parallel Iterative Method for Computing Molecular Absorption Spectra
474
0
0.0
(
0
)
اسأل ChatGPT حول البحث
ﻻ يوجد ملخص باللغة العربية
We describe a fast parallel iterative method for computing molecular absorption spectra within TDDFT linear response and using the LCAO method. We use a local basis of dominant products to parametrize the space of orbital products that occur in the LCAO approach. In this basis, the dynamical polarizability is computed iteratively within an appropriate Krylov subspace. The iterative procedure uses a a matrix-free GMRES method to determine the (interacting) density response. The resulting code is about one order of magnitude faster than our previous full-matrix method. This acceleration makes the speed of our TDDFT code comparable with codes based on Casidas equation. The implementation of our method uses hybrid MPI and OpenMP parallelization in which load balancing and memory access are optimized. To validate our approach and to establish benchmarks, we compute spectra of large molecules on various types of parallel machines. The methods developed here are fairly general and we believe they will find useful applications in molecular physics/chemistry, even for problems that are beyond TDDFT, such as organic semiconductors, particularly in photovoltaics.
قيم البحث
اقرأ أيضاً
We present a systematic study of the photo-absorption spectra of various Si$_{n}$H$_{m}$ clusters (n=1-10, m=1-14) using the time-dependent density functional theory (TDDFT). The method uses a real-time, real-space implementation of TDDFT involving f
ull propagation of the time dependent Kohn-Sham equations. Our results for SiH$_{4}$ and Si$_{2}$H$_{6}$ show good agreement with the earlier calculations and experimental data. We find that for small clusters (n<7) the photo-absorption spectrum is atomic-like while for the larger clusters it shows bulk-like behaviour. We study the photo-absorption spectra of silicon clusters as a function of hydrogenation. For single hydrogenation, we find that in general, the absorption optical gap decreases and as the number of silicon atoms increase the effect of a single hydrogen atom on the optical gap diminishes. For further hydrogenation the optical gap increases and for the fully hydrogenated clusters the optical gap is larger compared to corresponding pure silicon clusters.
Graphene is considered one of the most promising materials for future electronic. However, in its pristine form graphene is a gapless material, which imposes limitations to its use in some electronic applications. In order to solve this problem many
approaches have been tried, such as, physical and chemical functionalizations. These processes compromise some of the desirable graphene properties. In this work, based on ab initio quantum molecular dynamics, we showed that a two-dimensional carbon allotrope, named biphenylene carbon (BPC) can be obtained from selective dehydrogenation of porous graphene. BPC presents a nonzero bandgap and well-delocalized frontier orbitals. Synthetic routes to BPC are also addressed.
Coherence among rotational ion channels during photoionization is exploited to control the anisotropy of the resulting photoelectron angular distributions at specific photoelectron energies. The strategy refers to a robust and single parameter contro
l using two ultra-short light pulses delayed in time. The first pulse prepares a superposition of a few ion rotational states, whereas the second pulse serves as a probe that gives access to a control of the molecular asymmetry parameter $beta$ for individual rotational channels. This is achieved by tuning the time delay between the pulses leading to channel interferences that can be turned from constructive to destructive. The illustrative example is the ionization of the $E(1Sigma_{g}^{+})$ state of Li$_{2}$. Quantum wave packet evolutions are conducted including both electronic and nuclear degrees of freedom to reach angle-resolved photoelectron spectra. A simple interference model based on coherent phase accumulation during the field-free dynamics between the two pulses is precisely exploited to control the photoelectron angular distributions from almost isotropic, to marked anisotropic.
We investigate the photo-doubleionization of $H_2$ molecules with 400 eV photons. We find that the emitted electrons do not show any sign of two-center interference fringes in their angular emission distributions if considered separately. In contrast
, the quasi-particle consisting of both electrons (i.e. the dielectron) does. The work highlights the fact that non-local effects are embedded everywhere in nature where many-particle processes are involved.
The vibrational properties of alkaline-earth metal fluoride clusters (BaF2)n (n=1-6) are investigated in the framework of density functional theory. The calculated Raman and Infrared (IR) spectra reveals shift in Raman and IR peak position towards lo
wer frequency region with the increase in the cluster size. Further the calculated spectra have been compared with the experimental vibrational spectra of bulk BaF2 crystal. Even though the smaller size cluster lacks translational symmetry, the structural and vibrational characteristic of (BaF2)5-6 are nearer to bulk counterpart.
سجل دخول لتتمكن من نشر تعليقات
التعليقات
جاري جلب التعليقات
سجل دخول لتتمكن من متابعة معايير البحث التي قمت باختيارها
