Philosophical Transactions of the Royal Society A Mathematical Physical and Engineering Sciences
Quantum dynamics of excitations and decoherence in many-spin systems detected with Loschmidt echoes: its relation to their spreading through the Hilbert space
Claudia M. Sánchez, Patricia R. Levstein, L. Buljubasich, Horacio M. Pastawski, Ana Karina Chattah
In this work, we overview time-reversal nuclear magnetic resonance (NMR) experiments in many-spin systems evolving under the dipolar Hamiltonian. The Loschmidt echo (LE) in NMR is the signal of excitations which, after evolving with a forward Hamiltonian, is recovered by means of a backward evolution. The presence of non-diagonal terms in the non-equilibrium density matrix of the many-body state is directly monitored experimentally by encoding the multiple quantum coherences. This enables a spin counting procedure, giving information on the spreading of an excitation through the Hilbert space and the formation of clusters of correlated spins. Two samples representing different spin systems with coupled networks were used in the experiments. Protons in polycrystalline ferrocene correspond to an 'infinite' network. By contrast, the liquid crystal N-(4-methoxybenzylidene)-4-butylaniline in the nematic mesophase represents a finite proton system with a hierarchical set of couplings. A close connection was established between the LE decay and the spin counting measurements, confirming the hypothesis that the complexity of the system is driven by the coherent dynamics.
In this work, we overview time-reversal nuclear magnetic resonance (NMR) experiments in many-spin systems evolving under the dipolar Hamiltonian. The Loschmidt echo (LE) in NMR is the signal of excitations which, after evolving with a forward Hamiltonian, is recovered by means of a backward evolution. The presence of non-diagonal terms in the non-equilibrium density matrix of the many-body state is directly monitored experimentally by encoding the multiple quantum coherences. This enables a spin counting procedure, giving information on the spreading of an excitation through the Hilbert space and the formation of clusters of correlated spins. Two samples representing different spin systems with coupled networks were used in the experiments. Protons in polycrystalline ferrocene correspond to an 'infinite' network. By contrast, the liquid crystal N-(4-methoxybenzylidene)-4-butylaniline in the nematic mesophase represents a finite proton system with a hierarchical set of couplings. A close connection was established between the LE decay and the spin counting measurements, confirming the hypothesis that the complexity of the system is driven by the coherent dynamics.
In this work we present solid-state nuclear magnetic-resonance experiments to study decoherence in the dynamics of many-spin systems. We characterize the global Loschmidt echo and the distribution of multiple-quantum coherence orders during the evolution under dipolar and double-quantum Hamiltonians. To study an infinite 1H system and a closed cluster of nuclear spins we use polycrystalline adamantane and the liquid crystal 5CB in the nematic mesophase, respectively, as model systems. The infinite or finite nature of the system is clearly manifested through spin counting measurements. Comparison between experimental and numerical results gives insights on the decoherence mechanisms in these systems. Contrastingly, the dominating mechanism in 5CB affects all coherence orders in the same way, while in adamantane higher orders of coherence decay faster than the lower ones.
We performed Loschmidt echo nuclear magnetic resonance experiments to study decoherence under a scaled dipolar Hamiltonian by means of a symmetrical time-reversal pulse sequence denominated Proportionally Refocused Loschmidt (PRL) echo. The many-spin system represented by the protons in polycrystalline adamantane evolves through two steps of evolution characterized by the secular part of the dipolar Hamiltonian, scaled down with a factor |k| and opposite signs. The scaling factor can be varied continuously from 0 to 1/2, giving access to a range of complexity in the dynamics. The experimental results for the Loschmidt echoes showed a spreading of the decay rates that correlate directly to the scaling factors |k|, giving evidence that the decoherence is partially governed by the coherent dynamics. The average Hamiltonian theory was applied to give an insight into the spin dynamics during the pulse sequence. The calculations were performed for every single radio frequency block in contrast to the most widely used form. The first order of the average Hamiltonian numerically computed for an 8-spin system showed decay rates that progressively decrease as the secular dipolar Hamiltonian becomes weaker. Notably, the first order Hamiltonian term neglected by conventional calculations yielded an explanation for the ordering of the experimental decoherence rates. However, there is a strong overall decoherence observed in the experiments which is not reflected by the theoretical results. The fact that the non-inverted terms do not account for this effect is a challenging topic. A number of experiments to further explore the relation of the complete Hamiltonian with this dominant decoherence rate are proposed.
We present an improved approach for the study of the evolution of spin correlations and decoherence in multiple quantum nuclear magnetic resonance experiments. The infinite system, constituted by the protons of a polycrystalline adamantane sample, evolves under a double quantum Hamiltonian. The distribution of multiple quantum coherence orders is represented by a contribution of spin clusters with different sizes that exchange spins, increasing their size with the evolution time. A cluster with nearly exponential growth at all times is observed, in agreement with previous models. Remarkably, a small cluster that stabilizes in a size corresponding to 18 correlated spins is revealed. In addition, by performing a renormalization of the obtained data with the experimental Loschmidt echo, the contribution of the different clusters to the observable signal is determined. This procedure accounts for the effect of decoherence on the evolution of the system, and allows setting the range of confidence of the experimental data. Our analysis confirms the natural hint that, correlated states involving higher coherence orders are far more sensitive to the uncontrolled decoherent interactions, than those involving lower orders.
Abstract If a magnetic polarization excess is locally injected in a crystal of interacting spins in thermal equilibrium, this ‘excitation’ would spread as consequence of spin–spin interactions. Such an apparently irreversible process is known as spin diffusion and it can lead the system back to ‘equilibrium’. Even so, a unitary quantum dynamics would ensure a precise memory of the non-equilibrium initial condition. Then, if at a certain time, say t / 2 , an experimental protocol reverses the many-body dynamics by changing the sign of the effective Hamiltonian, it would drive the system back to the initial non-equilibrium state at time t . As a matter of fact, the reversal is always perturbed by small experimental imperfections and/or uncontrolled internal or environmental degrees of freedom. This limits the amount of signal M ( t ) recovered locally at time t . The degradation of M ( t ) accounts for these perturbations, which can also be seen as the sources of decoherence. This general idea defines the Loschmidt echo (LE), which embodies the various time-reversal procedures implemented in nuclear magnetic resonance. Here, we present an invitation to the study of the LE following the pathway induced by the experiments. With such a purpose, we provide a historical and conceptual overview that briefly revisits selected phenomena that underlie the LE dynamics including chaos, decoherence, localization and equilibration. This guiding thread ultimately leads us to the discussion of decoherence and irreversibility as an emergent phenomenon. In addition, we introduce the LE formalism by means of spin–spin correlation functions in a manner suitable for presentation in a broad scope physics journal. Last, but not least, we present new results that could trigger new experiments and theoretical ideas. In particular, we propose to transform an initially localized excitation into a more complex initial state, enabling a dynamically prepared LE. This induces a global definition of the LE in terms of the raw overlap between many-body wave functions. Our results show that as the complexity of the prepared state increases, it becomes more fragile towards small perturbations.
If a magnetic polarization excess is locally injected in a crystal of interacting spins in thermal equilibrium, this 'excitation' would spread as consequence of spin-spin interactions. Such an apparently irreversible process is known as spin diffusion and it can lead the system back to 'equilibrium'. Even so, a unitary quantum dynamics would ensure a precise memory of the non-equilibrium initial condition. Then, if at a certain time, say , an experimental protocol reverses the many-body dynamics by changing the sign of the effective Hamiltonian, it would drive the system back to the initial non-equilibrium state at time t. As a matter of fact, the reversal is always perturbed by small experimental imperfections and/or uncontrolled internal or environmental degrees of freedom. This limits the amount of signal M(t) recovered locally at time t. The degradation of M(t) accounts for these perturbations, which can also be seen as the sources of decoherence. This general idea defines the Loschmidt echo (LE), which embodies the various time-reversal procedures implemented in nuclear magnetic resonance. Here, we present an invitation to the study of the LE following the pathway induced by the experiments. With such a purpose, we provide a historical and conceptual overview that briefly revisits selected phenomena that underlie the LE dynamics including chaos, decoherence, localization and equilibration. This guiding thread ultimately leads us to the discussion of decoherence and irreversibility as an emergent phenomenon. In addition, we introduce the LE formalism by means of spin-spin correlation functions in a manner suitable for presentation in a broad scope physics journal. Last, but not least, we present new results that could trigger new experiments and theoretical ideas. In particular, we propose to transform an initially localized excitation into a more complex initial state, enabling a dynamically prepared LE. This induces a global definition of the LE in terms of the raw overlap between many-body wave functions. Our results show that as the complexity of the prepared state increases, it becomes more fragile towards small perturbations.
In the long quest to identify and compensate the sources of decoherence in many-body systems far from the ground state, the varied family of Loschmidt echoes (LEs) became an invaluable tool in several experimental techniques. A LE involves a time-reversal procedure to assess the effect of perturbations in a quantum excitation dynamics. However, when addressing macroscopic systems one is repeatedly confronted with limitations that seem insurmountable. This led to the formulation of the central hypothesis of irreversibility stating that the timescale of decoherence, T3, is proportional to the timescale of the many-body interactions we reversed, T2. We test this by implementing two experimental schemes based on Floquet Hamiltonians where the effective strength of the dipolar spin-spin coupling, i.e., 1/T2, is reduced by a variable scale factor k. This extends the perturbation timescale, ${T}_{\mathrm{\ensuremath{\Sigma}}}$, in relation to T2. Strikingly, we observe the superposition of the normalized Loschmidt echoes for the bigger values of k. This manifests the dominance of the intrinsic dynamics over the perturbation factors, even when the Loschmidt echo is devised to reverse that intrinsic dynamics. Thus, in the limit where the reversible interactions dominate over perturbations, the LE decays within a timescale, ${T}_{3}\ensuremath{\approx}{T}_{2}/R$ with $R=(0.15\ifmmode\pm\else\textpm\fi{}0.01)$, confirming the emergence of a perturbation independent regime. These results support the central hypothesis of irreversibility.