journal article·2018-04-01Open access

From coherent quasi-irreversible quantum dynamics towards the second law of thermodynamics: The model boron rotor B13+

Dongming Jia, Jörn Manz, Yonggang Yang

AIP Advances· Volume 8· Issue 4

Abstract

The planar boron cluster B13+ provides a model to investigate the microscopic origin of the second law of thermodynamics in a small system. It is a molecular rotor with an inner wheel that rotates in an outer bearing. The cyclic reaction path of B13+ passes along thirty equivalent global minimum structures (GMi, i = 1, 2, ..., 30). The GMs are embedded in a cyclic thirty-well potential. They are separated by thirty equivalent transition states with potential barrier Vb. If the boron rotor B13+ is prepared initially in one of the thirty GMs, with energy below Vb, then it tunnels sequentially to its nearest, next-nearest etc. neighbors (520 fs per step) such that all the other GMs get populated. As a consequence, the entropy of occupying the GMs takes about 6 ps to increases from zero to a value close to the maximum value for equi-distribution. Perfect recurrences are practically not observable.
Source: crossref · Quality: baseline

Research context

OpenAlex topics: Protein Structure and Dynamics · Advanced Chemical Physics Studies · Crystallography and molecular interactions

SciVX discovery tags are terminology-based. OpenAlex topics are source-provided classifications.

Affiliations

State Key Laboratory of Quantum Optics and Quantum Optics Devices, Institute of Laser Spectroscopy, Shanxi University 1 , Taiyuan 030006, China

Institut für Chemie und Biochemie, Freie Universität Berlin 2 , 14195 Berlin, Germany

Collaborative Innovation Center of Extreme Optics, Shanxi University 3 , Taiyuan 030006, China

Funding

the Program for Changjiang Scholars and Innovative Research Team · Deutsche Forschungsgemeinschaft · National Natural Science Foundation of China

References (39)

Show source-provided references
1. The art of building small: From molecular switches to motors (nobel lecture)10.1002/anie.201702979 ↗
2. From chemical topology to molecular machines (nobel lecture)10.1002/anie.201702992 ↗
3. Mechanically interlocked molecules (MIMs)-molecular shuttles, switches, and machines, (nobel lecture)10.1002/anie.201703216 ↗
4. Artificial molecular rotors10.1021/cr0300993 ↗
5. The art of building small: From molecular switches to molecular motors10.1021/jo070394d ↗
6. Quantum control of unidirectional rotations of a chiral molecular motor10.1039/b815047h ↗
7. Biologically inspired molecular machines driven by light. Optimal control of a unidirectional rotor10.1088/1367-2630/12/7/075007 ↗
8. Theoretical studies on a carbonaceous molecular bearing: Association thermodynamics and dual-mode rolling dynamics10.1039/c5sc00335k ↗
9. A reversible, unidirectional molecular rotary motor driven by chemical energy10.1126/science.1117090 ↗
10. Dynamic control of chiral space in a catalytic asymmetric reaction using a molecular motor10.1126/science.1199844 ↗
11. Allosteric regulation of the rotational speed in a light-driven molecular motor10.1021/jacs.6b06467 ↗
12. Crystalline arrays of pairs of molecular rotors: Correlated motion, rotational barriers, and space-inversion symmetry breaking due to conformational mutations10.1021/ja4044517 ↗
13. Molecular dynamics simulation of an electric field driven dipolar molecular rotor attached to a quartz glass surface10.1021/ja0348851 ↗
14. Surface-mounted altitudinal molecular rotors in alternating electric field: Single-molecule parametric oscillator molecular dynamics10.1073/pnas.0506183102 ↗
15. Synthesis of triptycene-based molecular rotors for Langmuir–Blodgett monolayers10.1021/acs.joc.5b01753 ↗
16. 2015
17. Unravelling phenomenon of internal rotation in B13+ through chemical bonding analysis10.1039/c1cc10821b ↗
18. B13+: A photodriven molecular Wankel engine10.1002/anie.201202674 ↗
19. Structure and fluxionality of B13+ probed by infrared photodissociation spectroscopy10.1002/anie.201609766 ↗
20. A universal mechanism of the planar boron rotors B11−, B13+, B15+, and B19−: Inner wheels rotating in pseudo-rotating outer bearings10.1039/c6nr09074e ↗
21. B11−: A moving subnanoscale tank tread10.1039/c5nr03732h ↗
22. Dynamical behavior of boron clusters10.1039/c6nr06383g ↗
23. Chemical bonding and dynamic fluxionality of a B 15+ cluster: A nanoscale double-axle tank tread10.1039/c6cp02544g ↗
24. A concentric planar doubly π-aromatic B19− cluster10.1038/nchem.534 ↗
25. B19−: An aromatic Wankel motor10.1002/anie.201001275 ↗
26. Understanding boron through size-selected clusters: Structure, chemical bonding, and fluxionality10.1021/ar400310g ↗
27. Photoelectron spectroscopy of size-selected boron clusters: From planar structures to borophenes and borospherenes10.1080/0144235x.2016.1147816 ↗
28. Beyond organic chemistry: Aromaticity in atomic clusters10.1039/c5cp07465g ↗
29. Effects of molecular symmetry on the directions of nuclear flux densities during tunnelling in double well potentials10.1080/00268976.2013.800599 ↗
30. Capture of heavy hydrogen isotopes in a metal-organic framework with active Cu (I) sites10.1038/ncomms14496 ↗
31. Toward reliable density functional methods without adjustable parameters: The PBE0 model10.1063/1.478522 ↗
32. Balanced basis sets of split valence, triple zeta valence and quadruple zeta valence quality for H to Rn: Design and assessment of accuracy10.1039/b508541a ↗
33. 2010
34. Rotating molecules trapped in pseudorotating cages10.1021/ja00526a007 ↗
35. Quantum theory of concerted electronic and nuclear fluxes associated with adiabatic intramolecular processes10.1039/c5cp03982g ↗
36. A selection rule for the directions of electronic fluxes during unimolecular pericyclic reactions in the electronic ground state10.1080/00268976.2011.648666 ↗
37. On the impossibility of localized states for molecular rotors with cyclic potentials
38. On the unimolecular dissociation of large molecules10.1016/0009-2614(89)85180-2 ↗
39. The quantum harmonic Otto cycle10.3390/e19040136 ↗