For centuries, practitioners of origami ('ori', fold; 'kami', paper) and kirigami ('kiru', cut) have fashioned sheets of paper into beautiful and complex three-dimensional structures. Both techniques are scalable, and scientists and engineers are adapting them to different two-dimensional starting materials to create structures from the macro- to the microscale. Here we show that graphene is well suited for kirigami, allowing us to build robust microscale structures with tunable mechanical properties. The material parameter crucial for kirigami is the Föppl-von Kármán number γ: an indication of the ratio between in-plane stiffness and out-of-plane bending stiffness, with high numbers corresponding to membranes that more easily bend and crumple than they stretch and shear. To determine γ, we measure the bending stiffness of graphene monolayers that are 10-100 micrometres in size and obtain a value that is thousands of times higher than the predicted atomic-scale bending stiffness. Interferometric imaging attributes this finding to ripples in the membrane that stiffen the graphene sheets considerably, to the extent that γ is comparable to that of a standard piece of paper. We may therefore apply ideas from kirigami to graphene sheets to build mechanical metamaterials such as stretchable electrodes, springs, and hinges. These results establish graphene kirigami as a simple yet powerful and customizable approach for fashioning one-atom-thick graphene sheets into resilient and movable parts with microscale dimensions.

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We outline a novel numerical method, called Ultrafast Ultrafast (UF2) spectroscopy, for calculating the nth-order wavepackets required for calculating n-wave mixing signals. The method is simple to implement, and we demonstrate that it is computationally more efficient than other methods in a wide range of use cases. The resulting spectra are identical to those calculated using the standard response function formalism but with increased efficiency. The computational speed-ups of UF2 come from (a) nonperturbative and costless propagation of the system time-evolution, (b) numerical propagation only at times when perturbative optical pulses are nonzero, and (c) use of the fast Fourier transform convolution algorithm for efficient numerical propagation. The simplicity of this formalism allows us to write a simple software package that is as easy to use and understand as the Feynman diagrams that organize the understanding of n-wave mixing processes.

Nonlinear optical spectroscopies are powerful tools for probing quantum dynamics in molecular and nanoscale systems. While intuition about ultrafast spectroscopies is often built by considering impulsive optical pulses, actual experiments have finite-duration pulses, which can be important for interpreting and predicting experimental results. We present a new freely available open source method for spectroscopic modeling, called Ultrafast Ultrafast (UF2) spectroscopy, which enables computationally efficient and convenient prediction of nonlinear spectra, such as treatment of arbitrary finite duration pulse shapes. UF2 is a Fourier-based method that requires diagonalization of the Liouvillian propagator of the system density matrix. We also present a Runge–Kutta–Euler (RKE) direct propagation method. We include open system dynamics in the secular Redfield, full Redfield, and Lindblad formalisms with Markovian baths. For non-Markovian systems, the degrees of freedom corresponding to memory effects are brought into the system and treated nonperturbatively. We analyze the computational complexity of the algorithms and demonstrate numerically that, including the cost of diagonalizing the propagator, UF2 is 20–200 times faster than the direct propagation method for secular Redfield models with arbitrary Hilbert space dimension; it is similarly faster for full Redfield models at least up to system dimensions where the propagator requires more than 20 GB to store; and for Lindblad models, it is faster up to Hilbert space dimension near 100 with speedups for small systems by factors of over 500. UF2 and RKE are part of a larger open source Ultrafast Software Suite, which includes tools for automatic generation and calculation of Feynman diagrams.

Time-resolved spectroscopy is commonly used to study diverse phenomena in chemistry, biology, and physics. Pump–probe experiments and coherent two-dimensional (2D) spectroscopy have resolved site-to-site energy transfer, visualized electronic couplings, and much more. In both techniques, the lowest-order signal, in a perturbative expansion of the polarization, is of third order in the electric field, which we call a one-quantum (1Q) signal because in 2D spectroscopy it oscillates in the coherence time with the excitation frequency. There is also a two-quantum (2Q) signal that oscillates in the coherence time at twice the fundamental frequency and is fifth order in the electric field. We demonstrate that the appearance of the 2Q signal guarantees that the 1Q signal is contaminated by non-negligible fifth-order interactions. We derive an analytical connection between an nQ signal and (2n + 1)th-order contaminations of an rQ (with r < n) signal by studying Feynman diagrams of all contributions. We demonstrate that by performing partial integrations along the excitation axis in 2D spectra, we can obtain clean rQ signals free of higher-order artifacts. We exemplify the technique using optical 2D spectroscopy on squaraine oligomers, showing clean extraction of the third-order signal. We further demonstrate the analytical connection with higher-order pump–probe spectroscopy and compare both techniques experimentally. Our approach demonstrates the full power of higher-order pump–probe and 2D spectroscopy to investigate multi-particle interactions in coupled systems.