TY - JOUR
T1 - Rigorous quantum treatment of inelastic neutron scattering spectra of a heteronuclear diatomic molecule in a nanocavity
T2 - HD in the small cage of structure II clathrate hydrate
AU - Xu, Minzhong
AU - Ulivi, Lorenzo
AU - Celli, Milva
AU - Colognesi, Daniele
AU - Bačić, Zlatko
N1 - Funding Information:
Z.B. thanks the NSF for generous support of this research through Grant No. CHE-1112292 . The computational resources at NYU used in this work were funded in part by the NSF MRI Grant CHE-0420810 . Z.B. has also been supported by the China 111 Project B1202. This work was partially supported by the Italian Ministry of Education, University and Research (Ministero dell’Istruzione, Università e Ricerca, MIUR) under the project PRIN 2008 AFW2JS and by Consiglio Nazionale delle Ricerche (Italy) through the Cooperation Agreement No. 01/9001 with STFC (U.K.).
PY - 2013/3/20
Y1 - 2013/3/20
N2 - We present a novel methodology which allows rigorous quantum calculation of the inelastic neutron scattering (INS) spectra of a heteronuclear diatomic molecule confined inside a nanoscale cavity of an arbitrary shape. This generalizes the approach recently developed by us for the quantum simulation of the INS spectra of nanoconfined homonuclear diatomics. The key distinguishing feature of our approach is the use of the fully coupled 5D translation-rotation (TR) energy levels and wave functions as the initial and final states of the INS transitions. The computed INS spectra embody the full complexity of the quantum TR dynamics of the guest heteronuclear molecule in the anisotropic confinement and are therefore highly realistic. Utilizing this methodology, we compute at several temperatures the INS spectra of HD molecule in the small cage of the structure II clathrate hydrate, which are in very good overall agreement with the experimental INS spectra.
AB - We present a novel methodology which allows rigorous quantum calculation of the inelastic neutron scattering (INS) spectra of a heteronuclear diatomic molecule confined inside a nanoscale cavity of an arbitrary shape. This generalizes the approach recently developed by us for the quantum simulation of the INS spectra of nanoconfined homonuclear diatomics. The key distinguishing feature of our approach is the use of the fully coupled 5D translation-rotation (TR) energy levels and wave functions as the initial and final states of the INS transitions. The computed INS spectra embody the full complexity of the quantum TR dynamics of the guest heteronuclear molecule in the anisotropic confinement and are therefore highly realistic. Utilizing this methodology, we compute at several temperatures the INS spectra of HD molecule in the small cage of the structure II clathrate hydrate, which are in very good overall agreement with the experimental INS spectra.
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U2 - 10.1016/j.cplett.2013.01.013
DO - 10.1016/j.cplett.2013.01.013
M3 - Article
AN - SCOPUS:84874940816
SN - 0009-2614
VL - 563
SP - 1
EP - 8
JO - Chemical Physics Letters
JF - Chemical Physics Letters
ER -