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Nikolaj Moll

Publications and source records attributed to Nikolaj Moll.

34 records · Page 2Linked to original sources
arXiv2020

Probing molecular excited states by atomic force microscopy

By employing single charge injections with an atomic force microscope, we investigated redox reactions of a molecule on a multilayer insulating film. First, we charged the molecule positively by attaching a single hole. Then we neutralized it by attaching an electron and observed three channels for the neutralization. We rationalize that the three channels correspond to transitions to the neutral ground state, to the lowest energy triplet excited states and to the lowest energy singlet excited states. By single-electron tunneling spectroscopy we measured the energy differences between the transitions obtaining triplet and singlet excited state energies. The experimental values are compared with density functional theory calculations of the excited state energies. Our results show that molecules in excited states can be prepared and that energies of optical gaps can be quantified by controlled single-charge injections. Our work demonstrates the access to, and provides insight into, ubiquitous electron-attachment processes related to excited-state transitions important in electron transfer and molecular optoelectronics phenomena on surfaces.

cond-mat.mes-hall↗
arXiv2020

Time-resolved tomography of a driven adiabatic quantum simulation

A typical goal of a quantum simulation is to find the energy levels and eigenstates of a given Hamiltonian. This can be realized by adiabatically varying the system control parameters to steer an initial eigenstate into the eigenstate of the target Hamiltonian. Such an adiabatic quantum simulation is demonstrated by directly implementing a controllable and smoothly varying Hamiltonian in the rotating frame of two superconducting qubits, including longitudinal and transverse fields and iSWAP-type two-qubit interactions. The evolution of each eigenstate is tracked using time-resolved state tomography. The energy gaps between instantaneous eigenstates are chosen such that depending on the energy transition rate either diabatic or adiabatic passages are observed in the measured energies and correlators. Errors in the obtained energy values induced by finite $T_1$ and $T_2$ times of the qubits are mitigated by extrapolation to short protocol times.

quant-ph↗
arXiv2019

Short-depth trial-wavefunctions for the variational quantum eigensolver based on the problem Hamiltonian

For the variational quantum eigensolver we propose to generate trial wavefunctions from a small amount of selected Pauli terms of the problem Hamiltonian. Two different approaches, one inspired by the quantum approximate optimization algorithm and the other by imaginary-time evolution, are proposed and studied in detail. Using numerical calculations, we study the efficiency of these trial wavefunctions for finding the ground-state energy of three molecules: H2, LiH and H2O. We find that only a small number of Pauli terms are needed to reach chemical accuracy, leading to short-depth quantum circuits with a small number of variational parameters. For the LiH molecule, the quantum circuit consists of 36 two-qubit gates, 45 one-qubit gates, and four variational parameters, with a favorable scaling for larger molecules.

quant-ph↗
arXiv2019

Molecular structure elucidation with charge-state control

The charge state of a molecule governs its physicochemical properties, such as conformation, reactivity and aromaticity, with implications for on-surface synthesis, catalysis, photo conversion and applications in molecular electronics. On insulating, multilayer NaCl films we control the charge state of organic molecules and resolve their structures in neutral, cationic, anionic and dianionic states by atomic force microscopy, obtaining atomic resolution and bond-order discrimination using CO functionalized tips. We detect changes in conformation, adsorption geometry and bond-order relations for azobenzene, tetracyanoquinodimethane and pentacene in multiple charge states. Moreover, for porphine we investigate the charge-state-dependent change of aromaticity and conjugation pathway in the macrocycle. This work opens the way to studying chemical-structural changes of individual molecules for a wide range of charge states.

cond-mat.mes-hall↗
arXiv2018

Gate-efficient simulation of molecular eigenstates on a quantum computer

A key requirement to perform simulations of large quantum systems on near-term quantum hardware is the design of quantum algorithms with short circuit depth that finish within the available coherence time. A way to stay within the limits of coherence is to reduce the number of gates by implementing a gate set that matches the requirements of the specific algorithm of interest directly in hardware. Here, we show that exchange-type gates are a promising choice for simulating molecular eigenstates on near-term quantum devices since these gates preserve the number of excitations in the system. Complementing the theoretical work by Barkoutsos et al. [PRA 98, 022322 (2018)], we report on the experimental implementation of a variational algorithm on a superconducting qubit platform to compute the eigenstate energies of molecular hydrogen. We utilize a parametrically driven tunable coupler to realize exchange-type gates that are configurable in amplitude and phase on two fixed-frequency superconducting qubits. With gate fidelities around 95% we are able to compute the eigenstates within an accuracy of 50 mHartree on average, a limit set by the coherence time of the tunable coupler.

quant-ph↗
arXiv2018

Adiabatic quantum simulations with driven superconducting qubits

We propose a quantum simulator based on driven superconducting qubits where the interactions are generated parametrically by a polychromatic magnetic flux modulation of a tunable bus element. Using a time-dependent Schrieffer-Wolff transformation, we analytically derive a multi-qubit Hamiltonian which features independently tunable $XX$ and $YY$-type interactions as well as local bias fields over a large parameter range. We demonstrate the adiabatic simulation of the ground state of a hydrogen molecule using two superconducting qubits and one tunable bus element. The time required to reach chemical accuracy lies in the few microsecond range and therefore could be implemented on currently available superconducting circuits. Further applications of this technique may also be found in the simulation of interacting spin systems.

quant-ph↗
arXiv2018

Quantum algorithms for electronic structure calculations: particle/hole Hamiltonian and optimized wavefunction expansions

In this work we investigate methods to improve the efficiency and scalability of quantum algorithms for quantum chemistry applications. We propose a transformation of the electronic structure Hamiltonian in the second quantization framework into the particle-hole (p/h) picture, which offers a better starting point for the expansion of the trial wavefunction. The state of the molecular system at study is parametrized in a way to efficiently explore the sector of the molecular Fock space that contains the desired solution. To this end, we explore several trial wavefunctions to identify the most efficient parameterization of the molecular ground state. Taking advantage of known post-Hartree Fock quantum chemistry approaches and heuristic Hilbert space search quantum algorithms, we propose a new family of quantum circuits based on exchange-type gates that enable accurate calculations while keeping the gate count (i.e., the circuit depth) low. The particle-hole implementation of the Unitary Coupled Cluster (UCC) method within the Variational Quantum Eigensolver approach gives rise to an efficient quantum algorithm, named q-UCC , with important advantages compared to the straightforward 'translation' of the classical Coupled Cluster counterpart. In particular, we show how a single Trotter step can accurately and efficiently reproduce the ground state energies of simple molecular systems.

quant-ph↗
arXiv2018

Entanglement generation in superconducting qubits using holonomic operations

We investigate a non-adiabatic holonomic operation that enables us to entangle two fixed-frequency superconducting transmon qubits attached to a common bus resonator. Two coherent microwave tones are applied simultaneously to the two qubits and drive transitions between the first excited resonator state and the second excited state of each qubit. The cyclic evolution within this effective 3-level $Λ$-system gives rise to a holonomic operation entangling the two qubits. Two-qubit states with 95\% fidelity, limited mainly by charge-noise of the current device, are created within $213~\rm{ns}$. This scheme is a step toward implementing a SWAP-type gate directly in an all-microwave controlled hardware platform. By extending the available set of two-qubit operations in the fixed-frequency qubit architecture, the proposed scheme may find applications in near-term quantum applications using variational algorithms to efficiently create problem-specific trial states.

quant-ph↗
arXiv2017

Quantum optimization using variational algorithms on near-term quantum devices

Universal fault-tolerant quantum computers will require error-free execution of long sequences of quantum gate operations, which is expected to involve millions of physical qubits. Before the full power of such machines will be available, near-term quantum devices will provide several hundred qubits and limited error correction. Still, there is a realistic prospect to run useful algorithms within the limited circuit depth of such devices. Particularly promising are optimization algorithms that follow a hybrid approach: the aim is to steer a highly entangled state on a quantum system to a target state that minimizes a cost function via variation of some gate parameters. This variational approach can be used both for classical optimization problems as well as for problems in quantum chemistry. The challenge is to converge to the target state given the limited coherence time and connectivity of the qubits. In this context, the quantum volume as a metric to compare the power of near-term quantum devices is discussed. With focus on chemistry applications, a general description of variational algorithms is provided and the mapping from fermions to qubits is explained. Coupled-cluster and heuristic trial wave-functions are considered for efficiently finding molecular ground states. Furthermore, simple error-mitigation schemes are introduced that could improve the accuracy of determining ground-state energies. Advancing these techniques may lead to near-term demonstrations of useful quantum computation with systems containing several hundred qubits.

quant-ph↗
arXiv2017

Analysis of parametrically driven exchange-type (iSWAP) and two-photon (bSWAP) interactions between superconducting qubits

A current bottleneck for quantum computation is the realization of high-fidelity two-qubit quantum operations between two and more quantum bits in arrays of coupled qubits. Gates based on parametrically driven tunable couplers offer a convenient method to entangle multiple qubits by selectively activating different interaction terms in the effective Hamiltonian. Here, we study theoretically and experimentally a superconducting qubit setup with two transmon qubits connected via a capacitively coupled tunable bus. We develop a time-dependent Schrieffer-Wolff transformation and derive analytic expressions for exchange-interaction gates swapping excitations between the qubits (iSWAP) and for two-photon gates creating and annihilating simultaneous two-qubit excitations (bSWAP). We find that the bSWAP gate is generally slower than the more commonly used iSWAP gate, but features favorable scalability properties with less severe frequency crowding effects, which typically degrade the fidelity in multi-qubit setups. Our theoretical results are backed by experimental measurements as well as exact numerical simulations including the effects of higher transmon levels and dissipation.

quant-ph↗
arXiv2017

Fermionic Hamiltonians for quantum simulations: a general reduction scheme

Many-body fermionic quantum calculations performed on analog quantum computers are restricted by the presence of k-local terms, which represent interactions among more than two qubits. These originate from the fermion-to-qubit mapping applied to the electronic Hamiltonians. Current solutions to this problem rely on perturbation theory in an enlarged Hilbert space. The main challenge associated with this technique is that it relies on coupling constants with very different magnitudes. This prevents its implementation in currently available architectures. In order to resolve this issue, we present an optimization scheme that unfolds the k-local terms into a linear combination of 2-local terms, while ensuring the conservation of all relevant physical properties of the original Hamiltonian, with several orders of magnitude smaller variation of the coupling constants.

quant-ph↗
arXiv2016

Optimizing qubit resources for quantum chemistry simulations in second quantization on a quantum computer

Quantum chemistry simulations on a quantum computer suffer from the overhead needed for encoding the fermionic problem in a bosonic system of qubits. By exploiting the block diagonality of a fermionic Hamiltonian, we show that the number of required qubits can be reduced by a factor of two or more. There is no need to go into the basis of the Hilbert space for this reduction because all operations can be performed in the operator space. The scheme is conceived as a pre-computational step that would be performed on a classical computer prior to the actual quantum simulation. We apply this scheme to reduce the number of qubits necessary to simulate both the Hamiltonian of the two-site Fermi-Hubbard model and the hydrogen molecule. Both quantum systems can then be simulated with a two-qubit quantum computer.

quant-ph↗
arXiv2014

Investigating Atomic Contrast in Atomic Force Microscopy and Kelvin Probe Force Microscopy on Ionic Systems using Functionalized Tips

Noncontact atomic force microscopy (NC-AFM) and Kelvin probe force microscopy (KPFM) have become important tools for nanotechnology; however, their contrast mechanisms on the atomic scale are not entirely understood. Here we used chlorine vacancies in NaCl bilayers on Cu(111) as a model system to investigate atomic contrast as a function of applied voltage, tip height, and tip functionalization. We demonstrate that the AFM contrast on the atomic scale decisively depends on both the tip termination and the sample voltage. On the contrary, the local contact potential difference (LCPD) acquired with KPFM showed the same qualitative contrast for all tip terminations investigated, which resembled the contrast of the electric field of the sample. We find that the AFM contrast stems mainly from electrostatic interactions but its tip dependence cannot be explained by the tip dipole alone. With the aid of a simple electrostatic model and by density functional theory we investigate the underlying contrast mechanisms.

cond-mat.mes-hall↗
arXiv2013

Interface dipoles of organic molecules on Ag(111) in hybrid density-functional theory

We investigate the molecular acceptors 3,4,9,10-perylene-tetracarboxylic acid dianhydride (PTCDA), 2,3,5,6-tetra uoro-7,7,8,8-tetracyanoquinodimethane (F4TCNQ), and 4,5,9,10-pyrenetetraone (PYTON) on Ag(111) using densityfunctional theory. For two groups of the HSE(α, ω) family of exchange-correlation functionals (ω= 0 and ω= 0.2Å) we study the isolated components as well as the combined systems as a function of the amount of exact-exchange (α). We find that hybrid functionals favour electron transfer to the adsorbate. Comparing to experimental work-function data, we report for (α) ca. 0.25 a notable but small improvement over (semi)local functionals for the interface dipole. Although Kohn-Sham eigenvalues are only approximate representations of ionization energies, incidentally, at this value also the density of states agrees well with the photoelectron spectra. However, increasing (α) to values for which the energy of the lowest unoccupied molecular orbital matches the experimental electron affinity in the gas phase worsens both the interface dipole and the density of states. Our results imply that semi-local DFT calculations may often be adequate for conjugated organic molecules on metal surfaces and that the much more computationally demanding hybrid functionals yield only small improvements.

cond-mat.mtrl-sci↗
arXiv2004

Observation of surface states in a truncated two-dimensional photonic crystal slab

The effect of lattice termination on the surface states in a two-dimensional truncated photonic crystal slab is experimentally studied in a high index contrast silicon-on-insulator system. A single-mode silicon strip waveguide that is separated from the photonic crystal by a trench of variable width is used to evanescently couple to surface states in the surrounding lattice. It is demonstrated that the dispersion of the surface states depends strongly on the specific termination of the lattice.

physics.optics↗