In previous work [C. A. Chatzidimitriou-Dreismann et al., J. Chem. Phys. 113, 2784 (2000)] we provided first results of the subfemtosecond dynamics of C–H bond dissociation of solid fully protonated polystyrene at T≈295 K, applying neutron Compton scattering (NCS). A striking anomalous shortfall of the proton scattering intensity with respect to that of the carbon nucleus has been observed. A theoretical explanation based on short-lived protonic quantum entanglement (QE) has also been given. Here we present a twofold extension of that work: Investigation of the found anomaly (i) in solid D-polystyrene with various degrees of aromatic protonation [(-CD2CDC6HxDy-)n with x+y=5] and (ii) in liquid C6H6 and C6H6–C6D6 mixtures. A striking decrease of the neutron cross-section density of H by 20% (on the average) was observed, which appeared to be weakly dependent on the H:D atomic ratio. This result indicates that the considered effect is mainly of intramolecular origin. In contrast to previous NCS experiments on metallic hydrides which revealed a strong scattering time (τscatt) dependence of the decrease of the neutron cross-section density of H, this effect is only slightly apparent in polystyrene and benzene, thus indicating different dynamics of the decoherence process due to different electronic environments. All presented results imply that short-lived QE may be highly relevant for chemical and biological systems.
In previous work [C. A. Chatzidimitriou-Dreismann et al., J. Chem. Phys. 113, 2784 (2000)] we provided first results of the subfemtosecond dynamics of C–H bond dissociation of solid fully protonated polystyrene at T≈295 K, applying neutron Compton scattering (NCS). A striking anomalous shortfall of the proton scattering intensity with respect to that of the carbon nucleus has been observed. A theoretical explanation based on short-lived protonic quantum entanglement (QE) has also been given. Here we present a twofold extension of that work: Investigation of the found anomaly (i) in solid D-polystyrene with various degrees of aromatic protonation [(-CD2CDC6HxDy-)n with x+y=5] and (ii) in liquid C6H6 and C6H6–C6D6 mixtures. A striking decrease of the neutron cross-section density of H by 20% (on the average) was observed, which appeared to be weakly dependent on the H:D atomic ratio. This result indicates that the considered effect is mainly of intramolecular origin. In contrast to previous NCS experiments on metallic hydrides which revealed a strong scattering time (τscatt) dependence of the decrease of the neutron cross-section density of H, this effect is only slightly apparent in polystyrene and benzene, thus indicating different dynamics of the decoherence process due to different electronic environments. All presented results imply that short-lived QE may be highly relevant for chemical and biological systems.
Nuclei and electrons in condensed matter and/or molecules are usually entangled, due to the prevailing electromagnetic interactions. Usually, the “environment” of a microscopic scattering system (e.g., a proton) causes an ultrafast decoherence, thus making atomic and/or nuclear entanglement effects not directly accessible to experiments. However, neutron Compton scattering (NCS) and electron Compton scattering represent ultrafast techniques operating in the sub-femtosecond timescale, thus opening a way for investigation of such dehoherence and short-lived entanglement phenomena of atoms in molecules and condensed matter. The experimental context of NCS and a new striking scattering effect from protons (H-atoms) in several condensed systems and molecules are described. In short, one observes an “anomalous” decrease of scattering intensity from protons, which seem to become partially “invisible” to the neutrons. The experiments apply large energy (several electronvolts) and momentum (10–200 Å −1 transfers, and the collisional (or scattering) time between the neutron and a struck proton is only 100–1000 attoseconds long. Similar results are also obtained with electron-atom Compton scattering at large momentum transfers. As an example, we present new NCS experimental results from a single crystal, which also provide new physical insights into the attosecond quantum dynamics of protons in molecules and condensed matter. Theoretical discussions and models are presented which show that the effect under consideration is caused by the non-unitary time evolution (due to decoherence) of open quantum systems during the ultrashort, but finite, time-window of the neutron-proton scattering process. The conceptual connection with the well known Quantum Zeno Effect is pointed out. The experimental results, together with their qualitative interpretation “from first principles,” show that epithermal neutrons being available at spallation sources, and electron spectrometers providing large momentum transfers, may represent novel tools for investigation of thus far unknown physical and chemical attosecond phenomena.
In general, nuclei and electrons in condensed matter and/or molecules are entangled, due to the prevailing (electromagnetic) interactions. As a matter of fact, the "environment" interacting with a microscopic system of interest (e.g. a proton) causes the destruction of the entanglement. This process, called decoherence, has until now prevented experimenters from directly accessing atomic and/or nuclear entanglement effects in real experiments. However, our neutron and electron Compton scattering experiments from protons (H-atoms) in several condensed systems and molecules at ambient conditions demonstrated a new striking effect, i.e. an "anomalous" decrease of scattering intensity from protons, which seem to become partially "invisible" to the neutrons. This effect, which has no interpretation within conventional neutron scattering theory, is proposed to be caused by the non-unitary time evolution (due to decoherence) during the ultrashort, but finite, time-window of the neutron-proton scattering process. Due to the large energy (several eV) and momentum (20-200 Å −1 ) transfers of these experiments the collisional time between the probe particle and a struck proton is 100–1000 attoseconds long. It is shown that, due to this short timescale, the scattering process must be theoretically treated within quantum dynamics of open quantum systems. New experimental neutron Compton scattering results from a single crystal KHCO 3 are presented. They provide the first direct evidence for a connection between the momentum distribution and the "anomalous" scattering intensity of H. Additionally, recent experiments with electron-atom Compton scattering at momentum transfers are mentioned, which reveal the presence of this effect even in scattering from single H 2 molecules in the gas phase. Theoretical discussions "from first principles" are presented, also in relation to the quantum Zeno effect, which underline the crucial role of decoherence in the considered experiments. The experimental results and their qualitative interpretation show that epithermal neutrons being available at spallation sources (e.g. ISIS/UK, SNS/USA or ESS/Sweden), and electron spectrometers with large scattering angles, provide tools for investigating new physical and chemical phenomena in the sub-femtosecond timescale.
Several recent experiments have shown that protons, and to some extent also deuterons, show anomalous cross sections when the neutrons have energies in the range 10-100 eV (this results in a Compton scattering process where an essential part of the energy is transferred to one of the scattering particles). Here, an experiment on partially deuterated water, carried out by Chatzidimitriou-Dreismann et al., is analyzed in terms of a theory, which assumes that during the short duration (<10(-15) s) of this scattering process, protons are exchange correlated and cannot be considered as independent scattering objects. The quantum decoherence time for protons in liquid water is estimated from a simple model for the interaction of the water protons with hydrogen bonds.
Nuclei and electrons in condensed matter and/or molecules are usually entangled, due to the prevailing (mainly electromagnetic) interactions. However, the "environment" of a microscopic scattering system (e.g. a proton) causes ultrafast decoherence, thus making atomic and/or nuclear entanglement effects not directly accessible to experiments. However, our neutron Compton scattering experiments from protons (H-atoms) in condensed systems and molecules have a characteristic collisional time about 100–1000 attoseconds. The quantum dynamics of an atom in this ultrashort, but finite, time window is governed by non-unitary time evolution due to the aforementioned decoherence. Unexpectedly, recent theoretical investigations have shown that decoherence can also have the following energetic consequences. Disentangling two subsystems A and B of a quantum system AB is tantamount to erasure of quantum phase relations between A and B. This erasure is widely believed to be an innocuous process, which e.g. does not affect the energies of A and B . However, two independent groups proved recently that disentangling two systems, within a sufficiently short time interval, causes increase of their energies. This is also derivable by the simplest Lindblad-type master equation of one particle being subject to pure decoherence. Our neutron-proton scattering experiments with H 2 molecules provide for the first time experimental evidence of this effect. Our results reveal that the neutron-proton collision, leading to the cleavage of the H-H bond in the attosecond timescale, is accompanied by larger energy transfer (by about 2–3%) than conventional theory predicts. Preliminary results from current investigations show qualitatively the same effect in the neutron-deuteron Compton scattering from D 2 molecules. We interpret the experimental findings by treating the neutron-proton (or neutron-deuteron) collisional system as an entangled open quantum system being subject to fast decoherence caused by its "environment" (i.e., two electrons plus second nucleus of H 2 or D 2 ). The presented results seem to be of generic nature, and may have considerable consequences for various processes in condensed matter and molecules, e.g. in elementary chemical reactions.
Several recent experiments on liquid and solid samples containing protons or deuterons show an interesting anomaly, which is a shortfall in the intensity of energetic neutrons scattered by the samples. Previously we demonstrated that quantum correlations in the spatial and spin degrees of freedom of the hydrogen isotopes lead to entanglement in scattering and a reduction in the scattered intensity. The viability of short-lived quantum correlations as the cause of the observed anomalies is further explored and found to be entirely feasible. General features of the basic premiss, that quantum entanglement reduces the scattered signal, are discussed and the interpretation of the neutron scattering experiments is set in context to related work on other systems. For the experiments in question, the duration of a scattering event, τ s , is a fraction of a femtosecond which is extremely short compared to solid-state relaxation times. Increasing τ s , by suitably changing experimental conditions, restores the intensity to the standard value calculated from the single atom cross-section and concentration of particles. Our physical picture of the restoration is evolution with increasing τ s from a pure state of the particles (described by a wavefunction) to a mixed state (described by a density matrix) that is created, through decoherence, by steadily engaging the solid-state environment of the particles.