Understanding the coherent interplay of light with the magnetization in metals has been a longstanding

problem in ultrafast magnetism. While it is known that when laser light acts on a metal it can

induce magnetization via the process known as the inverse Faraday effect (IFE), the most basic

ingredients of this phenomenon are still largely unexplored. In particular, given a strong recent interest

in orbital non-equilibrium dynamics and its role in mediating THz emission in transition metals, the

exploration of distinct features in spin and orbital IFE is pertinent. Here, we present a first complete

study of the spin and orbital IFE in 3d, 4d and 5d transition metals of groups IV–XI from first-principles.

By examining the dependence on the light polarization and frequency, we show that the laser-induced

spin and orbitalmoments may vary significantly both in magnitude and sign.Weunderpin the interplay

between the crystal field splitting and spin-orbit interaction as the key factor which determines the

magnitude and key differences between the spin and orbital response. Additionally, we highlight the

anisotropy of the effect with respect to the ferromagnetic magnetization and to the crystal structure.

The here-provided complete map of IFE in transition metals is a key reference point in the field of optomagnetics.

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