Tianqi Li

Femtosecond Population Inversion and Stimulated Emission of Dense Dirac Fermions in Graphene

We show that strongly photoexcited graphene monolayers with 35 fs pulses quasi-instantaneously build up a broadband, inverted Dirac fermion population. Optical gain emerges and directly manifests itself via a negative conductivity at the near-infrared region for the first 200 fs, where stimulated emission completely compensates absorption loss in the graphene layer. Our experiment-theory comparison with two distinct electron and hole chemical potentials reproduce absorption saturation and gain at 40 fs, revealing, particularly, the evolution of the transient state from a hot classical gas to a dense quantum fluid with increasing the photoexcitation.

Femtosecond switching of magnetism via strongly correlated spin-charge quantum excitations

The technological demand to push the gigahertz (109 hertz) switching speed limit of today’s magnetic memory and logic devices into the terahertz (1012 hertz) regime underlies the entire field of spin-electronics and integrated multi-functional devices. This challenge is met by all-optical magnetic switching based on coherent spin manipulation. By analogy to femtosecond chemistry and photosynthetic dynamics—in which photoproducts of chemical and biochemical reactions can be influenced by creating suitable superpositions of molecular states—femtosecond-laser-excited coherence between electronic states can switch magnetic order by ‘suddenly’ breaking the delicate balance between competing phases of correlated materials: for example, manganites exhibiting colossal magneto-resistance suitable for applications. Here we show femtosecond (10−15 seconds) photo-induced switching from antiferromagnetic to ferromagnetic ordering in Pr0.7Ca0.3MnO3, by observing the establishment (within about 120 femtoseconds) of a huge temperature-dependent magnetization with photo-excitation threshold behaviour absent in the optical reflectivity. The development of ferromagnetic correlations during the femtosecond laser pulse reveals an initial quantum coherent regime of magnetism, distinguished from the picosecond (10−12 seconds) lattice-heating regime characterized by phase separation without threshold behaviour. Our simulations reproduce the nonlinear femtosecond spin generation and underpin fast quantum spin-flip fluctuations correlated with coherent superpositions of electronic states to initiate local ferromagnetic correlations. These results merge two fields, femtosecond magnetism in metals and band insulators, and non-equilibrium phase transitions of strongly correlated electrons, in which local interactions exceeding the kinetic energy produce a complex balance of competing orders.

Ultrafast observation of critical nematic fluctuations and giant magnetoelastic coupling in iron pnictides

Many of the iron pnictides have strongly anisotropic normal-state characteristics, important for the exotic magnetic and superconducting behaviour these materials exhibit. Yet, the origin of the observed anisotropy is unclear. Electronically driven nematicity has been suggested, but distinguishing this as an independent degree of freedom from magnetic and structural orders is difficult, as these couple together to break the same tetragonal symmetry. Here we use time-resolved polarimetry to reveal critical nematic fluctuations in unstrained Ba(Fe1-xCox)2As2. The femtosecond anisotropic response, which arises from the two-fold in-plane anisotropy of the complex refractive index, displays a characteristic two-step recovery absent in the isotropic response. The fast recovery appears only in the magnetically ordered state, whereas the slow one persists in the paramagnetic phase with a critical divergence approaching the structural transition temperature. The dynamics also reveal a gigantic magnetoelastic coupling that far exceeds electron-spin and electron-phonon couplings, opposite to conventional magnetic metals.

Transient charge and energy balance in graphene induced by ultrafast photoexcitation.

Ultrafast optical pump-probe spectroscopy measurements on monolayer graphene reveal significant optical nonlinearities. We show that strongly photoexcited graphene monolayers with 35 fs pulses quasi-instantaneously build up a broadband, inverted Dirac-fermion population. Optical gain emerges and directly manifests itself via a negative conductivity at the near-infrared region for the first 200 fs, where stimulated emission completely compensates for absorption loss in the graphene layer. To quantitatively investigate this transient, extremely dense photoexcited Dirac-fermion state, we construct a two-chemical-potential model, in addition to a time-dependent transient carrier temperature above the lattice temperature, to describe the population inverted electronic state metastable on the time scale of tens of femtoseconds generated by a strong exciting pulse. The calculated transient optical conductivity reveals a complete bleaching of absorption, which sets the saturation density during the pulse propagation. In particular, the model calculation reproduces the negative optical conductivity at lower frequencies in the states close to saturation, corroborating the observed femtosecond stimulated emission and optical gain in the wide near-infrared window.

Ultrafast probes of nonequilibrium hole spin relaxation in the ferromagnetic semiconductor GaMnAs

We directly measure the hole spin lifetime in ferromagnetic GaMnAs via time- and polarization-resolved spectroscopy. Below the Curie temperature Tc, an ultrafast photoexcitation with linearly-polarized light is shown to create a non-equilibrium hole spin population via the dynamical polarization of holes through p-d exchange scattering with ferromagnetically-ordered Mn spins, and we characterize their relaxation dynamics. The observed relaxation consists of a distinct three-step recovery : (i) femtosecond (fs) hole spin relaxation ~

Post-transient relaxation in graphene after an intense laser pulse

160-200 fs, (ii) picosecond (ps) hole energy relaxation ~ 1-2 ps, and (iii) a coherent, damped Mn spin precession with a period of ~ 250 ps. The transient amplitude of the hole spin component diminishes with increasing temperature, directly following the ferromagnetic order, while the hole energy amplitude shows negligible temperature change, consistent with our interpretation. Our results thus establish the hole spin lifetimes in ferromagnetic semiconductors and demonstrate a novel spectroscopy method for studying non-equilibrium hole spins in the presence of correlation and magnetic order.

Quantum Femtosecond Magnetism in a Strongly Correlated Manganese Oxide

High intensity laser pulses were recently shown to induce a population inverted transient state in graphene [T. Li, et al., Phys. Rev. Lett. 108, 167401 (2012)]. Using a combination of hydrodynamic arguments and a kinetic theory we determine the post-transient state relaxation of hot, dense, population inverted electrons towards equilibrium. The cooling rate and charge-imbalance relaxation rate are determined from the Boltzmann-equation including electron-phonon scattering. We show that the relaxation of the population inversion, driven by inter-band scattering processes, is much slower that the relaxation of the electron temperature, which is determined by intra-band scattering processes. This insight may be of relevance for the application of graphene as an optical gain medium.

Speeding up of transient carrier relaxation during non-equilibrium photoinduced phase transition in manganites

We show a photoinduced magnetic phase transition from antiferromagnetic to ferromagnetic ordering in a strongly correlated manganite during ~100 fs laser pulses when optical polarization still interacts with spins. This reveals an initial quantum coherent regime of magnetism, which is driven by fast quantum spin-flip fluctuations correlated with a coherent superposition of many-body electronic states.

Femtosecond Magneto-Optics: Quantum Spin Switching

We observe a distinct excitation-fluence-dependent transient carrier relaxation in a strongly correlated colossal magnetoresistive manganite that correlates with photoinduced magnetic and electronic phase transitions characterized by nonlinear photoexcitation behaviors.

Dynamic decoupling of spin-lattice-charge excitations in iron pnictides using time-resolved laser ellipsometry

The challenge to push the gigahertz switching speed of today’s logic and magnetic memory devices into the terahertz regime underlies the entire field of information processing, communication and integrated photonic-electronic-magnetic multi-functional devices.