Letter abstract


Nature Materials 6, 39 - 43 (2007)
doi:10.1038/nmat1803

Triggering dynamics of the high-pressure benzene amorphization

Lucia Ciabini1,2, Mario Santoro1,3, Federico A. Gorelli1,3, Roberto Bini1,2, Vincenzo Schettino1,2 and Simone Raugei4

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Success in designing and tailoring solid-state reactions depends on the knowledge of the mechanisms regulating the reactivity at the microscopic level. In spite of several attempts to rationalize the reactivity of crystals1, 2, 3, 4, 5, the question of the existence of a critical distance for a reaction to occur remains unsolved. In this framework, the role of lattice phonons, which continuously tune the relative distance and orientation of the molecules, is still not fully understood. Here, we show that at the onset of the transformation of crystalline benzene to an amorphous hydrogenated carbon the intermolecular C–C distance is always the same (about 2.6 Å) once collective motions are taken into account, and it is independent of the pressure and temperature conditions. This conclusion is supported by first-principles molecular-dynamics simulations. This is a clear demonstration of the role of lattice phonons in driving the reactivity in the crystalline phase by fine-tuning of the nearest-neighbour distances. The knowledge of the critical C–C distance can be crucial in planning solid-state reactions at moderate pressure.

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  1. LENS, European Laboratory for Non-Linear Spectroscopy and INFM, Via Carrara 1, I-50019 Sesto Fiorentino, Firenze, Italy
  2. Dipartimento di Chimica dell'Università di Firenze, Via della Lastruccia 3, I-50019 Sesto Fiorentino, Firenze, Italy
  3. CRS-SOFT-INFM-CNR, Università di Roma La Sapienza, P.zza A. Moro 2, I-00185 Roma, Italy
  4. International School for Advanced Studies (SISSA/ISAS) and INFM-DEMOCRITOS MOdeling Center for Research In aTOmistic Simulation, Via Beirut 2-4,34014-Trieste, Italy

Correspondence to: Roberto Bini1,2 e-mail: bini@chim.unifi.it

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