Dynamics of recombination via conical intersection in a semiconductor nanocrystal

doi:10.1039/c7sc04221c

Title: Dynamics of recombination via conical intersection in a semiconductor nanocrystal

The ultrafast dynamics of nonradiative recombination at dangling bond defects is elucidated by nanoscale multireferenceab initiomolecular dynamics simulations.

Authors:

Peng, Wei-Tao ^[1] ; ; ;

Michigan State Univ., East Lansing, MI (United States). Dept. of Chemistry
Stanford Univ., CA (United States). Dept. of Chemistry; SLAC National Accelerator Lab., Menlo Park, CA (United States). Photon Ultrafast Laser Science and Engineering Inst. (PULSE)
Univ. of Minnesota, Minneapolis, MN (United States). Dept. of Chemistry

Publication Date:: 2018-11-13

Grant/Contract Number:: CHE-1565634; AC02-76SF00515

Type:: Accepted Manuscript

Journal Name:: Chemical Science

Additional Journal Information:: Journal Volume: 9; Journal Issue: 3; Journal ID: ISSN 2041-6520

Publisher:: Royal Society of Chemistry

Research Org:: SLAC National Accelerator Lab., Menlo Park, CA (United States)

Sponsoring Org:: USDOE; National Science Foundation (NSF)

Country of Publication:: United States

Language:: English

Subject:: 77 NANOSCIENCE AND NANOTECHNOLOGY; 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; Nanocrystal; Conical intersection

OSTI Identifier:: 1419973

Alternate Identifier(s):: OSTI ID: 1475548


                    Peng, Wei-Tao, Fales, B. Scott, Shu, Yinan, and Levine, Benjamin G.. Dynamics of recombination via conical intersection in a semiconductor nanocrystal.  United States: N. p.,  
        Web.  doi:10.1039/c7sc04221c.

Copy to clipboard


                    Peng, Wei-Tao, Fales, B. Scott, Shu, Yinan, & Levine, Benjamin G.. Dynamics of recombination via conical intersection in a semiconductor nanocrystal.  United States.  doi:10.1039/c7sc04221c.

Copy to clipboard


                    Peng, Wei-Tao, Fales, B. Scott, Shu, Yinan, and Levine, Benjamin G.. 2018.  
        "Dynamics of recombination via conical intersection in a semiconductor nanocrystal".  United States.  
        doi:10.1039/c7sc04221c.  https://www.osti.gov/servlets/purl/1419973.

Copy to clipboard


                    
@article{osti_1419973,

  title        = {Dynamics of recombination via conical intersection in a semiconductor nanocrystal},

  author       = {Peng, Wei-Tao and Fales, B. Scott and Shu, Yinan and Levine, Benjamin G.},

  abstractNote = {The ultrafast dynamics of nonradiative recombination at dangling bond defects is elucidated by nanoscale multireferenceab initiomolecular dynamics simulations.},

  doi          = {10.1039/c7sc04221c},

  journal      = {Chemical Science},

  number       = 3,

  volume       = 9,

  place        = {United States},

  year         = {2018},

  month        = {11}

}

Copy to clipboard

Free Publicly Accessible Full Text
Accepted Manuscript (DOE)
Publisher's Version of Record
10.1039/c7sc04221c
https://doi.org/10.1039/c7sc04221c

Works referenced in this record:

Optical gain in silicon nanocrystals
journal, November 2000

Pavesi, L.; Dal Negro, L.; Mazzoleni, C.
Nature, Vol. 408, Issue 6811, p. 440-444
DOI: 10.1038/35044012

Silicon quantum wire array fabrication by electrochemical and chemical dissolution of wafers
journal, September 1990

Canham, L. T.
Applied Physics Letters, Vol. 57, Issue 10, p. 1046-1048
DOI: 10.1063/1.103561

Biodegradable luminescent porous silicon nanoparticles for in vivo applications
journal, February 2009

Park, Ji-Ho; Gu, Luo; von Maltzahn, Geoffrey
Nature Materials, Vol. 8, Issue 4, p. 331-336
DOI: 10.1038/nmat2398

General atomic and molecular electronic structure system
journal, November 1993

Schmidt, Michael W.; Baldridge, Kim K.; Boatz, Jerry A.
Journal of Computational Chemistry, Vol. 14, Issue 11, p. 1347-1363
DOI: 10.1002/jcc.540141112

Similar Records

Similar records in DOE PAGES and OSTI.GOV collections:

Dynamics of recombination via conical intersection in a semiconductor nanocrystal

Journal Article Peng, Wei-Tao ; Fales, B. Scott ; Shu, Yinan ; ... January 2018 - Chemical Science

The ultrafast dynamics of nonradiative recombination at dangling bond defects is elucidated by nanoscale multireferenceab initiomolecular dynamics simulations.
Full Text Available
Ultrafast Electronic Relaxation through a Conical Intersection: Nonadiabatic Dynamics Disentangled through an Oscillator Strength-Based Diabatization Framework

Journal Article Medders, Gregory R. ; Alguire, Ethan C. ; Jain, Amber ; ... January 2017 - Journal of Physical Chemistry. A, Molecules, Spectroscopy, Kinetics, Environment, and General Theory

Here, we employ surface hopping trajectories to model the short-time dynamics of gas-phase and partially solvated 4-(N,N-dimethylamino)benzonitrile (DMABN), a dual fluorescent molecule that is known to undergo a nonadiabatic transition through a conical intersection. To compare theory vs time-resolved fluorescence measurements, we calculate the mixed quantum–classical density matrix and the ensemble averaged transition dipole moment. We introduce a diabatization scheme based on the oscillator strength to convert the TDDFT adiabatic states into diabatic states of L _a and L _b character. Somewhat surprisingly, we find that the rate of relaxation reported by emission to the ground state is almost 50%more »« less
Full Text Available
Imaging CF ₃I conical intersection and photodissociation dynamics with ultrafast electron diffraction

Journal Article Yang, Jie ; Zhu, Xiaolei ; Wolf, Thomas J. A. ; ... July 2018 - Science

Conical intersections play a critical role in excited-state dynamics of polyatomic molecules because they govern the reaction pathways of many nonadiabatic processes. However, ultrafast probes have lacked sufficient spatial resolution to image wave-packet trajectories through these intersections directly. Here in this paper, we present the simultaneous experimental characterization of one-photon and two-photon excitation channels in isolated CF ₃I molecules using ultrafast gas-phase electron diffraction. In the two-photon channel, we have mapped out the real-space trajectories of a coherent nuclear wave packet, which bifurcates onto two potential energy surfaces when passing through a conical intersection. In the one-photon channel, we havemore »« less
Cited by 1
Dynamic mapping of conical intersection seams: A general method for incorporating the geometric phase in adiabatic dynamics in polyatomic systems

Journal Article Xie, Changjian ; Malbon, Christopher L. ; Yarkony, David R. ; ... July 2017 - Journal of Chemical Physics

The incorporation of the geometric phase in single-state adiabatic dynamics near a conical intersection (CI) seam has so far been restricted to molecular systems with high symmetry or simple model Hamiltonians. This is due to the fact that the ab initio determined derivative coupling (DC) in a multi-dimensional space is not curl-free, thus making its line integral path dependent. In a recent work [C. L. Malbon et al., J. Chem. Phys. 145, 234111 (2016)], we proposed a new and general approach based on an ab initio determined diabatic representation consisting of only two electronic states, in which the DC ismore »« less
Cited by 4Full Text Available
Enhanced photovoltaic performance of ultrathin Si solar cells via semiconductor nanocrystal sensitization: Energy transfer vs. optical coupling effects

Journal Article Hoang, Son ; Ashraf, Ahsan ; Eisaman, Matthew D. ; ... December 2015 - Nanoscale

Excitonic energy transfer (ET) offers exciting opportunities for advances in optoelectronic devices such as solar cells. While recent experimental attempts have demonstrated its potential in both organic and inorganic photovoltaics (PVs), what remains to be addressed is quantitative understanding of how different ET modes contribute to PV performance and how ET contribution is differentiated from the classical optical coupling (OC) effects. In this study, we implement an ET scheme using a PV device platform, comprising CdSe/ZnS nanocrystal energy donor and 500 nm-thick ultrathin Si acceptor layers, and present the quantitative mechanistic description of how different ET modes, distinguished from themore »« less
Cited by 4Full Text Available

Access journal articles and accepted manuscripts resulting from DOE research funding

Title: Dynamics of recombination via conical intersection in a semiconductor nanocrystal

Access journal articles and accepted manuscripts
resulting from DOE research funding