Vibron-vibron coupling from ab initio molecular dynamics simulations of a silicon cluster

We study the temperature-dependent dynamical processes of a Si10H16 cluster and obtain a blue shift of the Si-Si vibrational modes with transverse acoustic character and a red shift of the other vibrational modes with increasing temperature. We link this behavior to the bond length expansion and the...

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Published inNew journal of physics Vol. 15; no. 4; pp. 43039 - 14
Main Authors Han, Peng, Vil iauskas, Linas, Bester, Gabriel
Format Journal Article
LanguageEnglish
Published IOP Publishing 22.04.2013
Subjects
Blue shift
Clusters
Computer simulation
Coupling (molecular)
Doppler effect
Molecular dynamics
Occupation
Strength
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Abstract We study the temperature-dependent dynamical processes of a Si10H16 cluster and obtain a blue shift of the Si-Si vibrational modes with transverse acoustic character and a red shift of the other vibrational modes with increasing temperature. We link this behavior to the bond length expansion and the varying sign of the Grüneisen parameter. We further present a computational approach able to extract the vibron-vibron coupling strength in clusters or molecules. Our approach is based on ab initio Born-Oppenheimer molecular dynamics and a projection formalism able to deliver the individual vibron occupation numbers. From the Fourier transform of the vibron energy autocorrelation function, we obtain the coupling strength of each vibron to the most strongly coupled vibronic states. We find the vibron-vibron coupling strength up to 2.5 THz with a moderate increase of about 5% when increasing the temperature from 50 to 150 K.
AbstractList We study the temperature-dependent dynamical processes of a Si sub(10)H sub(16) cluster and obtain a blue shift of the Si-Si vibrational modes with transverse acoustic character and a red shift of the other vibrational modes with increasing temperature. We link this behavior to the bond length expansion and the varying sign of the Gruneisen parameter. We further present a computational approach able to extract the vibron-vibron coupling strength in clusters or molecules. Our approach is based on ab initio Born-Oppenheimer molecular dynamics and a projection formalism able to deliver the individual vibron occupation numbers. From the Fourier transform of the vibron energy autocorrelation function, we obtain the coupling strength of each vibron to the most strongly coupled vibronic states. We find the vibron-vibron coupling strength up to 2.5 THz with a moderate increase of about 5% when increasing the temperature from 50 to 150 K.
We study the temperature-dependent dynamical processes of a Si10H16 cluster and obtain a blue shift of the Si-Si vibrational modes with transverse acoustic character and a red shift of the other vibrational modes with increasing temperature. We link this behavior to the bond length expansion and the varying sign of the Grüneisen parameter. We further present a computational approach able to extract the vibron-vibron coupling strength in clusters or molecules. Our approach is based on ab initio Born-Oppenheimer molecular dynamics and a projection formalism able to deliver the individual vibron occupation numbers. From the Fourier transform of the vibron energy autocorrelation function, we obtain the coupling strength of each vibron to the most strongly coupled vibronic states. We find the vibron-vibron coupling strength up to 2.5 THz with a moderate increase of about 5% when increasing the temperature from 50 to 150 K.
We study the temperature-dependent dynamical processes of a Si _10 H _16 cluster and obtain a blue shift of the Si–Si vibrational modes with transverse acoustic character and a red shift of the other vibrational modes with increasing temperature. We link this behavior to the bond length expansion and the varying sign of the Grüneisen parameter. We further present a computational approach able to extract the vibron–vibron coupling strength in clusters or molecules. Our approach is based on ab initio Born–Oppenheimer molecular dynamics and a projection formalism able to deliver the individual vibron occupation numbers. From the Fourier transform of the vibron energy autocorrelation function, we obtain the coupling strength of each vibron to the most strongly coupled vibronic states. We find the vibron–vibron coupling strength up to 2.5 THz with a moderate increase of about 5% when increasing the temperature from 50 to 150 K.
Author Bester, Gabriel
Han, Peng
Vil iauskas, Linas
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CitedBy_id crossref_primary_10_1103_PhysRevB_91_085305
crossref_primary_10_1142_S0219876218501086
crossref_primary_10_1364_OE_25_014192
crossref_primary_10_1016_j_molstruc_2016_05_103
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Snippet We study the temperature-dependent dynamical processes of a Si10H16 cluster and obtain a blue shift of the Si-Si vibrational modes with transverse acoustic...
We study the temperature-dependent dynamical processes of a Si sub(10)H sub(16) cluster and obtain a blue shift of the Si-Si vibrational modes with transverse...
We study the temperature-dependent dynamical processes of a Si _10 H _16 cluster and obtain a blue shift of the Si–Si vibrational modes with transverse...
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SubjectTerms Blue shift
Clusters
Computer simulation
Coupling (molecular)
Doppler effect
Molecular dynamics
Occupation
Strength
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Title Vibron-vibron coupling from ab initio molecular dynamics simulations of a silicon cluster
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